Upload
duongphuc
View
297
Download
15
Embed Size (px)
Citation preview
VIETNAM ATOMIC ENERGY INSTITUTE
SCIENCE AND TECHNICS PUBLISHING HOUSE
TheANNUAL REPORT
For 2013
VIETNAM ATOMIC ENERGY INSTITUTE
ANNUAL REPORTfo r 2013
Editorial Board:Dr. Tran Chi Thanh, Chief Editor Dr. Cao Dinh Thanh Dr. Nguyen Thi Kim Dung Eng. Nguyen Hoang Anh M.Sc. Nguyen Thi Dinh B.A. Nguyen Thi Phuong Lan
Hanoi, November 2014
The VINATOM Annual Report for 2013 has been prepared as an account of
works carried out at VINATOM for the period 2013. Many results presented in
the report have been obtained in collaboration with scientists from national and
overseas universities and research institutions.
The ANNUAL REPORT for 2013
Edited by
Vietnam Atomic Energy Institute
59 Ly Thuong Kiet, Ha Noi, Vietnam
President: Dr. Tran Chi Thanh
Tel: +84-4-39423434
Fax: +84-4-39424133
This report is available from:
Training and Information Division
Dept. of Planning and R&D Management
Vietnam Atomic Energy Institute
59 Ly Thuong Kiet, Ha Noi,Vietnam
Tel: +84-4-39423591
Fax: +84-4-39424133
E-mail: [email protected]
Preface
The research activities of the Vietnam Atomic Energy Institute (VINATOM) during
the period from 1 January to 31 December 2013 are presented in this report. The research activities are focused on the following fields:
1. Nuclear Physics, Reactor Physics;
2. Research Reactor, Nuclear Power Technology, Nuclear Safety, Nuclear Power Economy;
3. Instrumentation, Nuclear Electronics;
4. Industrial Applications;
5. Applications in Ecology, Environment and Geology;
6. Applications in Biology, Agriculture and Medicine;
7. Radiation Protection and Radioactive Waste Management;
8. Radiation Technology;
9. Radiochemistry and Materials Science;
10. Computation and Other Related Topics.
The total number of permanent staff working at the VINATOM as December 31, 2013 is 743 including the clerical service staff. The VINATOM was funded from the Government with the total amount to 172.253 billion VND for FY 2013, an increase of 12.22% compared to the last fiscal year. The international support of 250,000 USD for the VINATOM activities is committed to the operating projects including equipment, staff training and expert services (3 VIE projects, 10 FNCA projects, 18 RAS projects and 11 research contracts with the IAEA).
Main results of fundamental and applied research implemented in the year were presented in 236 scientific articles, reports and contributions published in many journals, proceedings of conferences, etc.
During the time of year 2013, in the VINATOM there were 7 to be graduated in Ph.D. courses; about 155 people have been trained abroad in the fields of nuclear science and technology.
Dr. Tran Chi Thanh
President, VINATOM
9
CONTENTS
Page Preface 5
1. CONTRIBUTIONS 13
1.1- NUCLEAR PHYSICS, REACTOR PHYSICS 15
Investigation for Calculation Methods Used in Analyzing the Physics Characteristics
of Nuclear Power Reactor. 17
Nguyen Tuan Khai, Nguyen Minh Tuan, Tran Quoc Duong, Hoang Van Khanh, Phan Quoc
Vuong, Tran Viet Phu, Tran Vinh Thanh, Nguyen Thi Mai Huong, Nguyen Thi Dung and
Le Tran Chung.
Studying, Surveying the Capabilities of Determining Short-lived Radionuclides of
Instrumental Neutron Activation Analysis Using Pneumatic Transfer System at The
No.13-2 Channel and Thermal Column.
22
Ho Van Doanh, Cao Dong Vu, Tran Quang Thien, Pham Ngoc Son and Nguyen Thi Sy.
Improvement of the DHP Program and Apply for Fission Product Decay Heat
Calculations of 233
U, 235
U, 238
U, 232
Th and 239
Pu. 27
Pham Ngoc Son, Tran Tuan Anh, Nguyen Xuan Hải, Ho Huu Thang and Mai Xuan Trung.
1.2- RESEARCH REACTOR, NUCLEAR POWER TECHNOLOGY, NUCLEAR
SAFETY, NUCLEAR POWER ECONOMY 33
Study on Safety Analysis of PWR Reactor Core in Transient and Severe Accident
Conditions. 35
Le Dai Dien, Hoang Minh Giang, Nguyen Thi Thanh Thuy, Nguyen Thi Tu Oanh, Le Thi
Thu, Pham Tuan Nam, Tran Van Trung, Bui Thi Hoa, Nguyen Huu Tiep and Le Tri Dan.
A Neutronic Feasibility Study of the VVER Assembly Type Design Loaded With Fully
Ceramic Micro-encapsulated Fuel. 43
Hoang Van Khanh, Phan Quoc Vuong, Tran Vinh Thanh.
Calculation of Fuel and Moderator Temperature Coefficients in APR1400 Nuclear
Reactor by MVP Code. 48
Pham Tuan Nam, Le Thi Thu, Nguyen Huu Tiep and Tran Viet Phu.
Establishing Quality Assurance Program for Calculation in Core and Fuel
Management of The Dalat Nuclear Research Reactor Using Low Enriched Fuel. 52
Huynh Ton Nghiem, Luong Ba Vien, Le Vinh Vinh, Nguyen Kien Cuong, Nguyen Manh
Hung, Nguyen Minh Tuan, Pham Quang Huy, Tran Quoc Duong, Vo Doan Hai Đang,
Pham Hong Son, Tran Tri Vien and Tran Thanh Tram.
A SRAC Calculation of The VVER-1000 Core’s Effective Multiplication Factor. 61 Tran Vinh Thanh, Phan Quoc Vuong, Tran Viet Phu, Hoang Van Khanh and Ta Duy Long.
Modeling and Analysis of Thermal Hydraulic Phenomena for VVER-1000 Reactor
when Trip Out of One or Two Main Coolant Pumps by RELAP/SCDAPSIM Code. 69
Le Thi Thu, Pham Tuan Nam, Nguyen Thi Tu Oanh and Nguyen Huu Tiep.
1.3- INSTRUMENTATION, NUCLEAR ELECTRONICS 79
Study the Operation of Sub-system for Cyclotron Kotron13 with the Purpose of
Operation and Maintenance of This Equipment. 81
Nguyen Tien Dung, Pham Minh Duc, Le Viet Phong, Vu Duy Truong and Nguyen Xuan
Truong.
10
Application of Prompt Gamma Neutron Activation Analysis at the N0.2 Horizontal
Channel of the Dalat Nuclear Research Reactor Using a Compton-Suppression
Spectrometer.
84
Tran Tuan Anh, Nguyen Xuan Hai, Nguyen Canh Hai, Pham Ngoc Son, Ho Huu Thang
and Dang Lanh.
Research and Production of Calorimeter for Measuring Irradiation Doses on 10MeV
Electron Beam Accelerator. 90
Cao Van Chung, Nguyen Hoang Hai, Nguyen Anh Tuan and Tran Van Hung.
Researching, Building a Soft-Processor and Ethernet Interface Circuit Using EDK. 95 Tuong Thi Thu Huong, Pham Ngoc Tuan, Truong Van Dat, Dang Lanh and Chau Thi Nhu
Quynh
A Study of Characteristics of Helium-3 (He-3) Proportional Counters in Order to
Design Electronic Circuits for Neutron Detection. 100
Vu Van Tien, Nguyen Van Sy, Nguyen Thi Bao My, Nguyen Thi Thuy Mai and Ho Quang
Tuan.
1.4- INDUSTRIAL APPLICATIONS 107
Corrosion Surveillance in Pipe by Computed Radiography. 109 Nguyen The Man, Dao Duy Dung, Dang Thu Hong, Le Duc Thinh, Ha Hong Thu and
Nguyen Trong Nghia.
Study of Preparation and Survey of Radioisotopes Tracer Applications of Gold
Nanoparticles in the Multi-phase Industrial Processes. 114
Huynh Thai Kim Ngan, Trịnh Cong Son, Duong Thi Bich Chi, Tran Tri Hai, Nguyen Huu
Quang, Bui Trong Duy, Le Trong Nghia and Ngo Duc Tin.
1.5 - APPLICATIONS IN ECOLOGY, ENVIRONMENT AND GEOLOGY 119
Assessing Soil Erosion Rates for a Large Catchment in the Central Highlands of
Vietnam Using Fallout Radionuclides. 121
Phan Son Hai, Nguyen Thanh Binh, Nguyen Minh Dao, Nguyen Thi Huong Lan, Nguyen
Thi Mui, Le Xuan Thang and Phan Quang Trung.
Study on Method for Simulation of Partitioning Tracers in Double Porosity Model of
Fractured Basement Formations. 129
To Ba Cuong, Nguyen Hong Phan, Tran Tri Hai, Le Van Son and Le Van Loc.
Studying the Possibilities of Using The Radium Isotopes to Determine the Mass Ages
and Circulation of the Coastal Water. 138
Nguyen Thi Huong Lan, Phan Son Hai, Nguyen Van Phuc, Phan Quang Trung,
Nguyen Thi Mui and Nguyen Minh Dao.
Studying, Determining the Radionuclide of Tritum in the Water Samples (Rain,
Surface Water) by Using Liquid Scintillation Counting (TRi-carb 3180TR/SL). 142
Nguyen Thi Linh, Nguyen Dinh Tung, Truong Y, Le Nhu Sieu, Nguyen Van Phuc, Nguyen
Van Phu and Nguyen Kim Thanh.
1.6 - APPLICATIONS IN BIOLOGY, AGRICULTURE AND MEDICINE 149
Study on Preparation of 177
Lu, Labeling With Dotatate for Using in Diagnosis and
Treatment Neuroendocrine Tumors. 151
Duong Van Dong, Bui Van Cuong, Pham Ngoc Dien, Chu Van Khoa, Mai Phuoc Tho,
Nguyen Thi Thu and Vo Thi Cam Hoa.
Envisagement of Analytical Process for 13
C/12
C Isotope Ratio (13
C) in Benthic Bivalve
Samples by the Isotope Ratio Mass Spectrometry (EA-IRMS). 162
Ha Lan Anh, Vo Tuong Hanh, Vo Thi Anh and Nguyen Hong Thinh.
11
Techniques for Induction of Premature Chromosome Condensation (PCC) by
Calyculin - A and Micronucleus Assay for Biodosimetry in Vietnam. 167
Pham Ngoc Duy, Tran Que, Hoang Hung Tien, Bui Thi Kim Luyen, Nguyen Thi Kim Anh
and Ha Thi Ngoc Lien.
Field Test of Capability To Prevent Cabbage Clubroot Disease Caused by
Plasmodiophora Brassicae of Silver Nanoparticles Synthesized by Gamma Radiation. 174
Pham Thi Le Ha, Nguyen Tan Man, Nguyen Duy Hang, Le Hai, Tran Thi Tam,
Pham Thi Sam, Le Huu Tu, Tran Thu Hong, Tran Thi Thuy and Nguyen Tuong Ly Lan.
Study on Irradiated Vietnam Java Rambutan Fruit Which Was Postharvested
Treatment to Prolong The Shelflife for Export Purposes. 180
Nguyen Thuy Khanh, Nguyen Thi Ly, Doan Thi The, Cao Van Chung and Nguyen Van
Phong.
Research and Establishment of the Analytical Procedure for/of Sr-90 in Milk Samples. 191 Tran Thi Tuyet Mai, Duong Duc Thang, Nguyen Thi Linh and Bui Thi Anh Duong.
Preliminary Assessment About Genetic Diversity, the Stability of Potential Mutants
From Two Varieties of Chrysanthemum Morifolium Ramat. (Bronze Doa and Purple
Farm) Via Gamma Irradiation.
197
Nguyen Tuong Mien, Le Ngoc Trieu, Le Tien Thanh, Pham Van Nhi and Huynh Thi Trung.
Establishment of Illumination System for Investigation of Monochromatic Lights
Combination Effects on In Vitro Plant Growth. 208
Le Tien Thanh, Le Ngoc Trieu, Nguyen Tuong Mien, Huynh Thi Trung and Phan Quoc
Minh.
Application of In Vitro Flowering Technique on Evaluating of Mutation Capacity and
Color Selection of Torenia Fournieri L. Following Irradiation. 218
Le Van Thuc, Le Thi Thuy Linh, Hoang Hung Tien, Dang Thi Dien, Le Thi Bich Thy and Han
Huynh Dien.
1.7- RADIATION PROTECTION AND RADIOACTIVE WASTE MANAGEMENT 223
Establishing the Stand ard X-ray Beam Qualities for Calibration of Dosimeters Used
in Diagnostic Radiology Following IAEA-TRS457. 225
Duong Van Trieu, Ho Quang Tuan and Bui Duc Ky.
Research on Stabilization of Radioactive Waste by Method of Synrock Ceramic. 232 Nguyen Hoang Lan, Nguyen Ba Tien, Vuong Huu Anh and Nguyen An Thai.
Calculation and Measurement Dose Rate at the Control Area of Electron Beam
Accelerator UELR-10-15S2 at Research and Development Center for Radiation
Technology.
237
Nguyen Anh Tuan, Tran Van Hung, Cao Van Chung and Nguyen Hoang Hai.
1.8 - RADIATION TECHNOLOGY 245
Study on Improving Antioxydant and Antibacterial Activities of Silk Fibroin by
Irradiation Treatment. 247
Tran Bang Diep, Nguyen Van Binh, Hoang Phuong Thao, Pham Duy Duong, Hoang Dang
Sang and Nguyen Thuy Huong Trang.
Study on Preparing Carboxymethyl Starch Hydrogel Radiation-crosslinked on the
Electron Beam Accelerator To Do the Moisturizing Material in Cosmetic. 255
Nguyen Thanh Duoc, Doan Binh, Pham Thi Thu Hong and Nguyen Anh Tuan.
Research on Degradation of Silk Fibroin by Combination of Electron Beam
Irradiation and Hydrothermal Processing. 261
Nguyen Thi Kim Lan, Dang Van Phu, Le Anh Quoc and Nguyen Quoc Hien.
12
Synthesis of Fe3O4-chitosan Magnetic Nanocomposites by Gamma Irradiation for
Absorbing of Heavy Metals in Aqueous Solutions. 269
Tran Minh Quynh, Nguyen Van Binh, Nguyen Quang Long and Hoang Dang Sang.
Studies on Sterilization Process for Some Traditional Products of Herbal Medicine by
Gamma Radiation. 276
Hoang Phuong Thao, Nguyen Van Binh, Tran Bang Diep, Hoang Dang Sang, Nguyen Thuy
Huong Trang, Pham Duy Duong and Tran Minh Quynh.
1.9 - RADIOCHEMISTRY AND MATERIALS SCIENCE 281
Study on Beneficiation Technology of Dong Pao Rare-Earth-Barite-Fluorite with Two
Product Plans About Content and Recovery of Rare-Earth Fine Ores. 283
Duong Van Su, Truong Thi Ai, Bui Ba Duy, Bui Thi Bay, Nguyen Hong Ha, Le Thi Hong
Ha, Doan Thi Mo, Doan Dac Ban and Nguyen Hoang Son.
Improving Technology and Setting-up a Production Line for High Quality Zinc Oxide
(99.5%) With a Capacity of 150 Ton/year by Reduction-Oxidation Process. 297
Pham Minh Tuan, Tran The Dinh, Tran Ngoc Vuong, Tuong Duy Nhan, Tran Trung Son,
Le Huu Thiep, Nguyen Trung Dung, Le Thi Hong, Luong Manh Hung and Bui Huy Cuong.
Determination of Rare Earth and Other Elements in Yen-phu Rare Earth Ore and
Other Intermediate Products From the Floatation And Hydrometallurgical Process on
Portable XRF Si-Pin Detector.
305
Doan Thanh Son, Phung Vu Phong and Nguyen Hanh Phuc.
Studying of Preparation Silver Nano-Particles Using Spinning Disc Reactor. 309 Hoang Van Duc, Nguyen Thanh Chung, Tran Ngoc Ha, Ho Minh Quang and Nguyen Thi
Thuc Phuong.
Research on Technology of Making Rare Earth Alloy Having Rare Earth Content ≥
30% from Ore ( ≥ 40% Reo) Using Aluminum Thermal Technology in Arc Furnace. 314
Ngo Xuan Hung, Ngo Trong Hiep, Tran Duy Hai and Nguyen Huu Phuc.
A Test Study on the Recovery of Zinc Oxide from Bac-Kan Low Grade Zinc Ore. 320 Tran Ngoc Vuong, Pham Minh Tuan, Luong Manh Hung and Bui Huy Cuong.
1.10- COMPUTATION AND OTHER RELATED TOPICS 327
Research to Build The Advanced Training Programs for Nuclear Power Plan. 329 Nguyen Manh Hung, Le Van Hong, Cao Dinh Thanh and Nguyen Ba Tien.
Collect, Analyze and Data Base for Building Up the Investment Reports of the Center
for Nuclear Science and Technology Project. 333
Pham Quang Minh, Tran Chi Thanh, Cao Dinh Thanh, Mai Dinh Trung, Hoang Sy Than,
Nguyen Nhi Dien, Trinh Van Giap, Le Ba Thuan and Vu Tien Ha.
2. IAEA TC PROJECTS AND RESEARCH CONTRACTS 341
2.1 - List of VIE Projects 2013. 343
2.2 - List of FNCA Projects Operating in 2013. 344
2.3 - List of Active Regional/Interregional Projects 2013. 345
2.4 - List of Research Contracts 2013. 347
VINATOM-AR 13--01
The Annual Report for 2013, VINATOM
17
INVESTIGATION FOR CALCULATION METHODS USED IN ANALYZING
THE PHYSICS CHARACTERISTICS OF NUCLEAR POWER REACTOR
Nguyen Tuan Khai1, Nguyen Minh Tuan
2, Tran Quoc Duong
2, Hoang Van Khanh
1,
Phan Quoc Vuong1, Tran Viet Phu
1, Tran Vinh Thanh
1, Nguyen Thi Mai Huong
1,
Nguyen Thi Dung1 and Le Tran Chung
1
1Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 - Hoang Quoc Viet, Ha Noi
2Nuclear Research Institute, Vietnam Atomic Energy Institute
1- Nguyen Tu Luc, Dalat, Lam Dong
ABSTRACT: The project aims at nuclear human resource development and enhancement in research
capability in reactor physics and kinetics at Nuclear Energy Center (Institute for Nuclear Science and
Technology) and Nuclear Reactor Center (Nuclear Research Institute, Dalat). The main research items of
the project can be summarized as follows: i) Considering possibility on using modern calculation techniques
and methods in investigating neutronic characteristics and neutronics-thermalhydraulics coupling. This item is
proposed to carry out based on international collaboration with Prof. Le Trong Thuy, San Jose University, US.
ii) Carrying out the collaborative activities in research and training between Nuclear Energy Center (Institute
for Nuclear Science and Technology) and Nuclear Reactor Center (Nuclear Research Institute, Dalat). iii)
Opening two-week training course on nuclear reactor engineering (25/Nov. -12/Dec. 2013) in collaboration
with Japan Atomic Energy Agency (JAEA).
1. INTRODUCTION
Development of nuclear human resource and enhancement in research capability in reactor
physics and kinetics including both research and power reactors are one of the priority targets for
research orientations of Vietnam Atomic Energy Institute (VINATOM) in period 2014-2020. This
task is assigned to Nuclear Energy Center, Institute for Nuclear Science and Technology (INST)
and Nuclear Reactor Center, Dalat Nuclear Research Institute (NRI). At present most of the staffs
who are working at Nuclear Energy Center (INST) are young and less experienced. They were
supported by VINATOM to pursue the above mentioned research, including:
- Research project at basis level in 2010 on calculations for some physics and thermal-
hydraulic parameters for VVER-1000 type by Pham Tuan Nam,
- Research project at basis level in 2011 on calculations for some physics parameters for
fuel assembly of VVER-1000 using MCNP4C2 by Nguyen Van Hien,
- Research project at basis level in 2012 on consideration for neutronic characteristics of
PWR 900 MWe of Japanese technology by Phan Quoc Vuong,
Project information:
- Code: 17/2013/HD-NVCB
- Managerial Level: Ministry
- Allocated Fund: 280,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--01
The Annual Report for 2013, VINATOM
18
- Research projects at basis level in 2010, 2011 and 2012 on neutronic characteristics of
the OTTO recycling for new generation of reactors by Hoang Van Khanh.
Since 2010 VINATOM has proposed a long-term strategy in nuclear power human resource
development via establishing the qualified research groups at INST. Therefore, the target of this
project is to develop the qualified human resource, gradually enhance research capability on power
reactor physics and kinetics.
2. CONTENTS AND RESULTS
The project has been deployed and carried out based on the research contents written in the
proposal. The obtained results can be summarized as follow:
- Item 1: Investigating possibility of using some modern calculation methods and
techniques in analysis of reactor physics and kinetics characteristics. This is carried out based on
collaboration with Prof. Le Trong Thuy at San Jose University, US through two scientific seminars
on (1) Conventional methods of calculation for light water reactors, and (2) Some orientations for
calculation of reactor core physics characteristics from light water reactor (LWR) to high
temperature gas cool reactor (HTGR) presented by Prof. Thuy. Also we had a detail discussion with
Prof. Thuy on how we can establish a long-term collaboration on research and training, especially
for the goal of research capability enhancement for young people in coming years.
In framework of this research item we have performed scientific reports focusing on the
calculation methods for neutron transport and neutronic characteristics in reactor core, including:
(1) Numerical methods for neutron transport research
(2) Nuclear data edition for reactor physics calculations
(3) Multi-group analysis in reactor core calculations of LWR
(4) Multi-group diffusion theory and harmonic functions
(5) Monte-Carlo simulation method in analysis for neutron transport and diffusion
(6) A calculation program written for neutron transport in reactor core of PWR
These are very fundamental knowledge that the young researchers should be equipped in
order for approaching to high-level research requirements. We have proposed to investigate and
resolve the neutron transport and diffusion in moderator of light water reactor (LWR) as an
illustration for the calculation methods and technique mentioned in the above reports. The obtained
main results were presented in a paper “Simulation for neutron transport in reactor moderator and
proper thickness of light water reflector” which will be published in scientific conference of young
researchers at VINATOM on this October 2014, and also in master thesis written by Phan Quoc
Vuong, a young researcher at Nuclear Energy Center, INST. The thesis is planned for defend in this
August at Institute for Nuclear Technique and Environmental Physics, Hanoi University of
Technology (HUT). The figures 1-3 show the main results of the paper.
VINATOM-AR 13--01
The Annual Report for 2013, VINATOM
19
Figure 3: Simulation results on neutron backscattering, absorption
and leakage fractions as a function of the reflector thickness.
We have regularly seminars presented by young researcher who are responsible for a given
topics. The reports have been reviewed by the experienced scientists.
- Item 2: Deployment for research collaboration and training activities between Nuclear
Energy Center, INST and Nuclear Reactor Center, Dalat NRI.
In 2013 two young researchers (Le Tran Chung and Ta Duy Long) from Nuclear Energy
Center, INST have been sent to Dalat NRI for 4 months to participate in some oriented research
collaborations such as analysis for neutronic characteristics of HEU and LEU assemblies, and
neutronic-thermal hydraulic coupling calculations.
In framework of this item we have performed 4 scientific reports, including:
(1) Analysis for neutronic characteristics of HEU (36%) and LEU (19.7%) assemblies of
VVR-M2 using MCNP and SRAC codes.
Figure 2: Neutron energy spectrum
at the fuel rod.
Figure 1: Energy decrease of 2 MeV neutrons with
number of collisions in Hydrogen and Oxygen.
VINATOM-AR 13--01
The Annual Report for 2013, VINATOM
20
(2) Analysis for neutronic-thermal hydraulic characteristics for steady state of PWR
assembly at burnup 0 GWd/ton and 45 GWd/ton using MCNP and COBRA-EN.
(3) Analysis for Main Steam Line Break incident for VVER-1000 (AES92) using RELAP5.
(4) A series of practical assignments with PCTRAN prepared for training course on nuclear
reactor engineering at INST in framework of NUTECH program between VINATOM and JAEA.
This is a good basis for us to prepare a joint-research project on comprehensive neutronic
characteristics of VVER-1000 technology between Nuclear Energy Center, INST and Nuclear
Reactor Center, Dalat NRI.
Item 3: Cooperation in nuclear human resource development with JAEA.
In framework of NUTECH program between VINATOM and JAEA, a training course on
nuclear reactor engineering (Follow-up Training Course-FTC) was held for the first time in
Northern region from 25/Nov. -12/Dec. 2013 at INST, Hanoi. The JAEA has dispatched three
Japanese experts to participate in and give the lectures for the course. We invited eight Vietnamese
lecturers coming from VINATOM and VARANS to give the lectures for the course, three of them
are young researchers at INST who have participated in the instructor training course (ITC) at
IAEA. The course has recruited 20 participants from the organizations and universities concerning
national nuclear power program of the country such as Vietnam Agency for Radiation and Nuclear
Safety (VARANS), Vietnam Atomic Energy Agency (VAEA), VINATOM, Hanoi University of
Technology (HUT), Hanoi University of Science (HUS), Hanoi University of Electricity and
Institute of Energy (IOE).
The course was successfully taken place, where the lectures are well prepared, and the
participants followed fully and actively. The JAEA experts have appreciated the contents and
obtained results of the course, and recommended these FTCs should be continued in next years.
3. CONCLUSION
The project members have fully carried out the registered contents which can be
summarized as follows:
- Investigating the methods of physics and mathematics, and nuclear data update to
resolve the neutron transport and diffusion problem in reactor core. The research content has been
presented in 6 scientific reports and a calculation program on the neutron transport and diffusion.
The obtained main results are written in a paper for the scientific conference of young researchers
on this October 2014, and are scientific content of a master thesis.
- Giving a support for young researchers in research and training collaboration on reactor
physics and safety analysis between Nuclear Energy Center, INST and Nuclear Reactor Center,
Dalat NRI.
- Giving an active contribution in VINATOM-JAEA cooperation on nuclear human
resource development via the training courses on reactor engineering at INST.
In conclusion in development strategy of VINATIOM for the 2014-2020 period, research on
power reactor technology is one of the prioritized orientations. We have prepared a proposal with
the items on (1) the current manpower status, (2) research and training orientation and (3) staff
planning on vision to 2020. We wish that VINATOM kindly consider and support for us in
implementing the scientific and training targets proposed.
VINATOM-AR 13--01
The Annual Report for 2013, VINATOM
21
REFERENCES
[1] John R. Lamarsh, “Introduction to Nuclear Engineering”, Prentice Hall, Upper Saddle River,
New Jersey 07458, 2001.
[2] J. Leppọnen, “Diffusion Code Group Constant Generation Using the Monte Carlo Method”,
In Proc. XII Meeting on Reactor Physics Calculations in the Nordic Countries. Halden,
Norway, May 17-18, 2005.
[3] J. J. Duderstadt and L. J. Hamilton, “Nuclear Reactor Analysis”, John Wiley & Sons, Inc.,
1976.
[4] National Nuclear Data Center, Brookhaven National Laboratory, http://nndc.bnl.gov.
[5] J. Leppọnen, “A new assemply-level Monte-Carlo neutron transportation code for reactor
physics calculation”, In Proc. International Topical Meeting on Mathematics and
Computation, Supercomputing, Reactor Physics and Nuclear and Biological Applications,
M&C 2005. Avignon, France, Sept. 12-15, 2005.
[6] George I. Bell & Samuel Glasstone, “Nuclear reactor theory”, Van Nostrand Reinhold
Company, 450 West 33rd Street, New York, N.Y 10001.
[7] MCNP manual Vol I, II, III-Los Alamos National Laboratory.
[8] Thermal-Hydraulics of Nuclear Reactor-Uchida Masaaki, Tokai Training Center, Nuclear
Technology and Education Center, Japan Atomic Energy Research Institute.
VINATOM-AR 13--02
The Annual Report for 2013, VINATOM
22
STUDYING, SURVEYING THE CAPABILITIES OF DETERMINING
SHORT-LIVED RADIONUCLIDES OF INSTRUMENTAL NEUTRON
ACTIVATION ANALYSIS USING PNEUMATIC TRANSFER SYSTEM
AT THE NO.13-2 CHANNEL AND THERMAL COLUMN
Ho Van Doanh, Cao Dong Vu, Tran Quang Thien, Pham Ngoc Son and Nguyen Thi Sy
Center for Analytical Techniques, Nuclear Research Institute, Vietnam Atomic Energy Institute
ABTRACT: The Nuclear Research Institute (NRI) has recently installed a new automatic pneumatic transfer
system at the Dalat nuclear research reactor for rapid neutron activation analysis based on very short-lived
nuclides. This system can be used to perform short irradiations in seconds either in the vertical channel 13-2 or
in the thermal column of the reactor with thermal neutron flux of 4.2 1012
n.cm-2
.s-1
or 1.2 1011
n.cm-2
.s-
1, respectively. The transferring time of sample from irradiation position to detector position is proximately 3.2
seconds. A loss-free counting system using HPGE detector has been also setup in compacting with the
pneumatic transfer system for measurement of sample’s activity, automatically starting for data acquisition at
irradiated sample’s arrival. Therefore, short-lived nuclides such as 20
F, 77m
Se, 179m
Hf, 46m
Sc, 110
Ag can be used
for INAA at NRI. This report presents the results of detection limit of short-lived nuclides (half-lives < 9,5
min), and the development of a reliable analytical procedure utilizing short-lived radionuclides for INAA:
Procedures for determining Se in biological and geological samples, procedure for determining F in geological
sample. Neutron spectrum parameters at irradiation positions and efficiency of detector were also determined
in order to establish the k0-NAA analytical procedure.
I. INTRODUCTION
Instrumental neutron activation analysis (INAA) has been developed and applied at the 500
kW Dalat research reactor (DNRR) since 1984. Until now, it is capable of analyzing more than 40
elements based on radionuclides with short, medium and long-lived time. For short-lived nuclides
with half-lives from 2 minutes to 2.6 hours, samples are often irradiated at the neutron channel
No.7-1 of Dalat research reactor through a semi-auto pneumatic transfer system (PTS) with valid
irradiation time from 45 seconds to 20 minutes. Measurements are often performed using a gamma
spectrometer coupled with a HPGe (GMX-30190), but with manual manipulation between loading
and counting procedures. Therefore, the shortest-lived nuclides that could be detected are 28
Al (T1/2
= 2.24 min), 52
V (T1/2 = 3.75 min), and 51
Ti (T1/2 = 5.76 min).
Project information:
- Code: CS/13/01-01
- Managerial Level: Institute
- Allocated Fund: 65,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. H.V. Doanh and and et al. Surveying, installing, calibrating and initial assessing the capabilities of
automatic neutron activation analysis via short-lived nuclides. The proceedings of the conference at a
postgraduate deparment of Dalat University, 10/2013. (in Vietnamese)
2. H.V. Doanh, C.D. Vu, T.Q. Thien, P.N. Son, N.T. Sy, N. Giang and N.N. Dien, “A new rapid neutron
activation analysis system at Dalat nuclear research reactor”, Journal of Nuclear Science and
Technology, 2014.
3. H.V. Doanh and et al., “Determination of selenium in biological standard material by short-time
neutron activation analysis using 77m
Se at Dalat reactor”, Journal of Nuclear Science and Technology,
2014 (being reviewed).
VINATOM-AR 13--02
The Annual Report for 2013, VINATOM
23
In the recent years, through the IAEA TC Project RER/4/028, a new automatic PTS for
rapid neutron activation analysis (Fig.1) based on short-lived nuclides has been developed. This
PTS system can be used to perform short irradiations in seconds. The return time of sample from
irradiation position to counting position is about 3.2 s. Timing information for both irradiation and
counting will be instantly delivered to the activation analysis workstation computer. The digital
gamma spectrometer is selected and tuned for accurate measurement at high and varying counting
rates, using loss-free counting technology. Accordingly, shorter-lived nuclides (half-life < 1 min)
such as 20
F, 77m
Se, 179m
Hf, 46m
Sc, and 110
Ag can be used for INAA at Dalat reactor, which the former
system can not detect.
The main purpose of this work is to determine detection limit of short-lived nuclides (half-
lives < 9,5 min), and the development of a reliable analytical procedure utilizing short-lived
radionuclides for INAA: Procedures for determining Se in biological and geological samples,
procedure for determining F in geological sample. Neutron spectrum parameters at irradiation
positions and efficiency of detector were also determined in order to establish the k0-NAA
analytical procedure.
Figure1: Diagram of the auto-pneumatic transfer system installed at DNRR.
II. EXPERIMENT
The neutron spectrum parameters including thermal neutron flux th, fast neutron flux f, the
thermal flux to epithermal neutron flux (epi) ratio, the deviation factor of the epithermal neutron
flux from the ideal 1/E law approximated by a 1/E1+
shape and neutron temperature were measured
at sample irradiation positions in channel No.13-2 and thermal column using Au, Zr, Ni and Lu
monitors. Typically monitors with masses of 4 mg for Al-0.1%Au foil (IRMM-530R) and Al-0,1%
Lu foil, 30 mg for pure Ni (wire), 10 mg for Zr (foil) were inserted into a high purity polyethylene
vial and loaded into rabbit (capsule) for irradiation. This monitors were irradiated for 10 min at 13-2
channel and for 2 h at thermal column. After a suitable delay time, the activity measurements were
carried out by a calibrated gamma-ray spectrometer combined with HPGe detector (GMX-30190).
The measured spectra were analyzed by using the k0-IAEA program.
The measurement of efficency of HPGe detector (GMX40-76-PL) were determined by
Monte Carlo code and ETNA software (Efficiency Transfer for Nuclide Activity measurements).
VINATOM-AR 13--02
The Annual Report for 2013, VINATOM
24
A variety of reference materials (Tuna Fish IAEA-436, Oyster tissue NIST 1566b, Bovine
Liver NIST 1577, Bovine Liver NIST 1577b, Montana Soil NIST 2711a and Obsidian Rock NIST
278) were selected to assess reliability of this system on the short-time activation application. All of
the samples were irradiated at a neutron flux of 4.21012
n.cm-2
.s-1
in the 13-2 channel, and then
counted on the calibrated HPGe gamma-ray spectrometer (GMX40-76-PL).
III. RESULTS AND DISCUSSION
As the results of this study, neutron spectrum parameters (Table 1) at irradiation position of
the thermal column (7/2012, 3/2013 and 4/2013) and the channel No.13-2 (8/2012, 02/2013 and
3/2013) were determined by irradiating Au, Zr, Ni, Lu monitors. In addition, the efficiency curves
(Fig.2) of detector (GMX40-76-PL) for NAA sample at a distance of 5, 10 and 15 cm were
determined by MCNP and ETNA. Analytical procedures for determining Se via 77m
Se in biological
samples and F via 20
F in geological sample were also established.
Table 1: The results of the determination of neutron spectrum parameters
at irradiation facilities of the Dalat research reactor.
Neutron spectrum parameters No.13-2 channel Thermal column
Thermal neutron flux (n/cm2/s) (4.2 0.1) x 10
12 (1.25 0.03) x 10
11
Fast neutron flux (n/cm2/s) (6.6 0.9) x 10
12 (8.4 0.5) x 10
8
The ratio of thermal to epithermal neutron
flux 10.7 6.0 195 11
The deviation factor of the epithermal neutron
flux -0.069 0.008 -0.164 0.186
Neutron temperature (K) 312 12 298 19
MCNP Efficiency of HPGe Det. for NAA Sample
0.000
0.001
0.010
0.100
10 100 1000 10000
E gamma (KeV)
Eff
icie
ncy
MCNP-5cm MCNP-10cm
MCNP-15cm ETNA-5cm
ETNA-10cm ETNA-15cm
Figure 2: Efficiency curves of HPGe detector for NAA sample by MCNP
in comparation with ETNA.
VINATOM-AR 13--02
The Annual Report for 2013, VINATOM
25
Table 2: The results of concentration (in ppm) analysis
for Se in biological reference materials.
Reference material Certificated value
This work
k-zero method The relative
method
IAEA 463 4.63 0.48 4.55 0.50 4.19 0.46
NIST 1566b 2.06 0.15 2.48 0.57 2.18 0.42
NIST 1577 1.10 0.10 1.24 0.31 1.17 0.22
NIST 1577b 0.73 0.06 0.70 0.11 0.80 0.17
The accuracy for determination of Selenium using the short-lived nuclide 77m
Se was
evaluated by analyzing a number of certified reference materials with different levels of Se (IAEA
436, NIST 1566b, NIST 1577 and NIST 1577b). The agreement between measured and certified
values was generally acceptable, as shown in Table 2.
IV. CONCLUSION
A fast pneumatic sample transfer system for analyzing of extremely short-lived nuclides by
neutron activation analysis has been installed and operated at Dalat nuclear research reactor. In this
study, efficency of detector for NAA sample and neutron spectrum parameters of the thermal
column and channel No.13-2 were determined in order to establish analytical procedures using the
k0-NAA method. The system was applied to determine the concentration of Se in the biological
sample and F in geological sample by using the short-lived nuclide 77m
Se and 20
F. The results
obtained through this research have opened a new possibility on using INAA technique for
measurement of extremely short-lived nuclides at Nuclear Research Institute.
REFERENCES
[1] P. V, Guinn., A. D, Miller., Recent instrument neutron activation analysis studies utilizing
very short-lived activities, Journal of Radioanalytical Chemistry, 1976.
[2] A. D, Becker., Characterization and use of the new NIST rapid pneumatic tube irradiation
facility, Journal of Radioanalytical Chemistry, 1998.
[3] Y.-S. Chung, et al., Characteristics of a new pneumatic transfer system for a neutron
activation analysis at the HANARO research reactor, Nuclear Engineering and Technology,
2009.
[4] S.S. Ismail, A new automated sample transfer system for instrumental neutron activation
analysis, journal of Automated Methods and Management in Chemistry, 2010.
[5] U.M.EL-Ghawi, Determination of Selenium in Libyan Food Items Using Pseudocyclic
Instrumental Neutron Activation Analysis, Journal of Radioanalytical and Nuclear
Chemistry, 2004.
[6] N.C. Hải, P.N. Sơn, Nghiên cứu áp dụng kỹ thuật phân tích kích hoạt neutron lặp vòng dựa
trên các đồng vị sống ngắn để phân tích hàm lượng một số nguyên tố sử dụng hệ chuyển mẫu
tại kênh 13-2 và cột nhiệt của lò phản ứng hạt nhân Đà Lạt, Viện Năng lượng nguyên tử Việt
Nam, 2005.
[7] D.A. Miller, Instrumental neutron activation analysis using short-lived radionuclides,
University of California, Irvine, 1976.
VINATOM-AR 13--02
The Annual Report for 2013, VINATOM
26
[8] A. D, Miller., P. V, Guinn., Precision high-speed neutron activation nanlysis via very short-
lived activities, Journal of Radioanalytical Chemistry, 1976.
[9] H.M. Dũng, Nghiên cứu phát triển phương pháp k-zero trong phân tích kích hoạt nơtrôn lò
phản ứng hạt nhân cho xác định đa nguyên tố, Luận án tiến sĩ, ĐH KHTN TP.HCM, 2003.
[10] X. Lin, et al., The program "MULTINAA" for various standardization methods in neutron
activation analysis, journal of Radioanalytical and Nuclear Chemistry, 1997.
[11] A. Chhav, et al., Full energy peak efficiency calibration of HPGe detector for point and
extended sources using Monte Carlo code, Journal of Radioanalytical Chemistry, 2011.
[12] D. Radu, et al., Transfer of detector efficiency calibration from a point source to other
geometries using ETNA software, Romanian Reports in Physics, 2010.
[13] M. Blaauw, The Holistic analysis of gamma-ray spectra in instrument analysis, PhD. Thesis,
Interfaculty Reactor Institute, Delft University of Technology, 1993.
[14] Quality aspects of research reactor operations for instrumental neutron activation analysis,
IAEA-TECDOC-1218, 2001.
[15] M.U. Rajput, et al., Characteristic absolute efficiency response curves of a high purity
germanium detector in the energy range 50–1500 keV, Journal of Radioanalytical and
Nuclear Chemistry, 2002.
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
27
IMPROVEMENT OF THE DHP PROGRAM AND APPLY
FOR FISSION PRODUCT DECAY HEAT CALCULATIONS
OF 233
U, 235
U, 238
U, 232
Th AND 239
Pu
Pham Ngoc Son, Tran Tuan Anh, Nguyen Xuan Hải,
Ho Huu Thang and Mai Xuan Trung
Department of Nuclear Physics and Electronics, Nuclear Research Institute,
Vietnam Atomic Energy Institute
ABTRACT: The program, DHP (Decay Heat Power) for calculation of nuclear decay heat from fission
products has been improved, based on the previous DHP version developed under the MEXT program at
JAEA in 2007. In this improved version, the previous individual calculation functions were combined in to a
complete program, made it easy for user in providing input information by a visualize interface dialog. Based
on the agreement results of comparison between calculation data and experimental valises, the program is
estimated that the calculation functions and the new algorithms applied in this program are properly
implemented. The duration for a calculation with cooling time of 1010
s is about 120s. This program can be
effectively used for decay data, fission yield evaluation and/or products inventory calculations in research
work or training.
I. INTRODUCTION
Gamma and beta decay energy released from the natural decay of the fission products (FP)
contributes approximately 7% to 12% of the total energy generated through the fission process, and
is called “Decay Heat”. After a reactor is shutdown, this source of radioactive decay energy still
remains to maintain a moderate level of heating in the reactor core. The precise data of decay heat
calculations are important need for safety design of a nuclear facility, design of shielding for fuel
discharges, fuel storage and transport flasks, and the management of spent fuel.
In the recent years, with the great efforts of improvement for the evaluation nuclear data
libraries and for new measurements, decay heat calculations are expected to predict the truth data of
decay heat. In this study, an update version of DHP-decay heat calculation program has been
improved for FP decay heat calculations, uncertainty analysis. The method used in the program is
summation calculation, in which the inventories of FP nuclides following a fission process are
calculated by a new numerical algorithm for exactly analysis. Furthermore, the window interface of
the program is designed with optional properties which is easy for users to perform a calculation
Project information:
- Code: CS/13/01-01
- Managerial Level: Institute
- Allocated Fund: 50,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. Pham Ngoc Son. Calculation of fission product concentrations for time following a fission burst. Asian
Journal of Science and Technology, Vol. 5 pp. 295-298, 2014.
2. Pham Ngoc Son. Decay heat uncertainty analysis. Reported at the Scientific Symposium of Dong Nai
University, P.125 (2014); The 11th
National conference of nuclear science and technology, Aug. 2013
Vung Tau, Vietnam.
3. Pham Ngoc Son. Fission product decay heat calculation of U-235. Accepted to be published in
International Journal of Nuclear Science and Engineering-IJNESE.
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
28
process, and the calculated results can be directly displayed in graphical form together with
experimental values, and can be saved as an output data file in tabular form.
II. DEVELOPMENT OF THE DHP PROGRAM
2.1. Development of computational code
The DHP program is developed using the C++ compiler, and the window interface of the
program is designed with optional style. That makes it easy for user to utilize the program, and the
user can choose optionally to calculate FP decay heat after a fission burst or after a period of
irradiation. The input data for the program is loaded from the decay data and fission yield data
libraries with ENDF/B-6 format such as FP Decay data File and fission yield data file from JENDL,
JEFF or other evaluated nuclear data library. In addition, the experimental and recommended values
for comparison are loaded from files in table form. The method used in the program is summation
calculation, in which the inventories of FP nuclides following a fission process are calculated by a
new numerical algorithm for exactly analysis. The window interface of the program is designed
with optional selection of input parameters which is easy for users to perform a calculation process.
The calculated results can be directly displayed in a window interface and can be saved as an output
data file in tabular form. The new update structure of the calculation procedure is presented in
Figure 1. The interface window of program is shown in Figure 2.
Figure 1: Block diagram of the DHP program.
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
29
Figure 2: The new window interface of DHP program.
2.2. Test and validation
The program DHP has been improved for some computational function such as update
nuclear decay and fission yield data, new window user interface, update function for uncertainty
analysis, code for fission product concentration inventory and average energy calculations. After
coding, a testing for the program validation was carried out by comparing the results of calculated
average energies for several FP nuclides with data from literatures, Table 1.
The formulas applied for average energy and energy spectra calculation in DHP that given
results in comparison with reference data. From the results shown in Figure 2 and Table 1, the data
calculated by DHP program are good agreement with calculated reference values from [8] and
experimental value reported in [9, 10].
0 1
1
22
2/1 )()1()1()(Q
E
gg
g
dEdEEFEEpEEmcESTE (1)
0 1
1
22
2/1 )()1()()(Q
E
ggg
g
dEdEEFEEpEEQmcESTE (2)
e
l
EQ
E
exceeeexceexcexcee dEECmEEEQEZFESEQEZTEP 2/14222
2/1 )())(,()(),,()(
(3)
where:
Sβ(E): The Beta strength function,
f(Z, Qβ-E): the integrated Fermi function,
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
30
Qβ : beta decay energy,
T1/2: beta decay half-life,
E: the excitation energy in the daughter nuclide.
F stands for the Fermi function, and p for the electron momentum.
Eg is related to the excitation energy Ei as Eg = -(Ei -1).
m is electron rest mass, and c is the light velocity.
ξΩ(Z, Ee, Q-Eexc): Shape factor,
Ee: Beta-ray energy,
Eexc: Excitation energy in daughter nuclide,
EL: Maximum level energy experimentally observed in daughter nuclide,
Table 1: The results of calculation for Gamma-ray and Beta average energies in Beta decay
for several fission products, comparison with data from reference [8].
Nuclide Q-value T1/2 <E > (MeV) <E > (MeV)
(MeV) (s) DHP [8] DHP [8]
Rb-89 4.496 909 0.9303 0.9355 2.2313 2.2293
Rb-90 6.587 158 1.9060 1.9162 2.2712 2.2706
Rb-90m 6.696 265 1.0811 1.1180 3.9332 3.8690
Rb-91 5.891 58.4 1.3739 1.3684 2.6876 2.7064
Rb-93 7.462 5.84 2.1544 2.1881 2.5402 2.5765
Sr-93 4.137 445 0.7860 0.7915 2.1724 2.1675
Sr-94 3.508 75.2 0.8309 0.8416 1.4380 1.4192
Sr-95 6.087 23.9 1.8928 1.9013 1.7990 1.7897
Y-94 4.917 1120 1.8111 1.8294 0.7875 0.7570
Y-95 4.453 618 1.3793 1.4147 1.2471 1.1799
Cs-138 5.374 2010 1.2223 1.2250 2.4047 2.4078
Cs-138m 5.457 916 0.2565 0.2250 0.4211 0.4930
Cs-139 4.213 556 1.6487 1.6707 0.3451 0.3050
Cs-140 6.22 63.7 1.8399 1.9102 1.9520 1.8178
III. RESULTS OF CALCULATIONS
The results of calculations for decay heat from fission products of U-233, U-235, are shown
in Figures 3-4. The results of uncertainty analysis are shown in Figure 5.
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
31
Figure 3: Result of decay heat calculation for U-233 fast
neutron fission,decay data from JENDL3.3.
Figure 4: Result of decay heat calculation for U-235 thermal
neutron fission, decay data from JENDL3.3.
U-235 Thermal pulse fission
Total Decay Heat
0.4
0.6
0.8
1.0
1.2
1.4
1.6
1.8
1.E+00 1.E+01 1.E+02 1.E+03 1.E+04
Cooling Time (s)
Decay H
eat
t*f(
t) (
MeV
/fis
sio
n)
JENDL3.3
Uncertainty
Figure 5: The results of total decay heat uncertainty analysis
with JENDL 3.3 data for U-235 thermal neutron fission.
VINATOM-AR 13--03
The Annual Report for 2013, VINATOM
32
IV. CONCLUSIONS
The DHP application program has been developed and improved for FP decay heat
calculation and its uncertainty analysis. In the present program, the fission product inventory for all
of decay chains and 12 decay modes are taken into account by the internal calculation procedures.
The main advantages of this program are exact calculation, fast and easy to use.
REFERENCES
[1] Fred L. Wilsson: “Fermi’s Theory of Beta Decay”, American Journal of Physics Volume
36, Number 12. December 1968.
[2] G. Rudstam, et al: Atom. Data and Nucl. Data Tables. 45. 239 (1990).
[3] H. V Klapdor: “The shape of the beta strength function and consequences for nuclear
physics and astrophysics”, Prog. Part. Nucl. Phys. 10, 131. 1983.
[4] Kanji TASAKA, Junichi MIWA, Junichi KATAKURA, Tadashi YOSHIDA, Kiyoshi
KAWADE, Toshio KATOH, Takahiro TACHIBANA, Masami YAMADA and Ryuzo
NAKASIMA: “Calculation of Beta-Ray Spectra from Individual and Aggregate Fission
Products”. Journal of Nuclear Science and Technology, 29[4], pp. 303-312. April 1992.
[5] Pham Ngoc Son and Jun-ichi KATAKURA: “Applications of TAGS Data in Beta Decay
Energies and Decay Heat Calculations”. JAEA-Research 2007-068. Octorber 2007.
[6] M. G. Stamatelatos, T. R. England: “Beta-Energy Averaging and Beta Spectra”, UC-34c.
August 1976.
[7] J. Katakura, T. Yoshida, K. Oyamatsu, T. Tachibana, JENDL FP Decay Data File 2000,
JAERI 1343, Japan Atomic Energy Research Institute. 2001.
[8] N. Hagura, T. Yoshida and T. Tachibana, J. Nucl. Sci. Tech., 43, 497 (2006).
[9] M. Akiyama and S. An, “ Measurement of fission products decay heat for fast reactor”,
Proc. of Int. Conf. on Nucl. Data for Science and Techno. , Antwerp Belgium, P.237
(1982).
[10] J. K. Dickens et al., “Fission Products Energy Release for Time following Thermal Neutron
Fission of 235U between 2 and 14000 seconds”, ORNL/NUREG-14 (1977); Nul. Sci. Eng.,
74, 106 (1980).
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
35
STUDY ON SAFETY ANALYSIS OF PWR REACTOR CORE
IN TRANSIENT AND SEVERE ACCIDENT CONDITIONS
Le Đai Dien, Hoang Minh Giang, Nguyen Thi Thanh Thuy, Nguyen Thi Tu Oanh,
Le Thi Thu, Pham Tuan Nam, Tran Van Trung, Bui Thi Hoa,
Nguyen Huu Tiep and Le Tri Dan
Nuclear Safety Center, Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
Le Van Hong
Vietnam Atomic Energy Institute
Vo Thi Huong
University of Science and Technology, Korea
ABSTRACT: The cooperation research project on the “Study on Safety Analysis of PWR Reactor Core in
Transient and Severe Accident Conditions” between Institute for Nuclear Science and Technology (INST),
VINATOM and Korean Atomic Energy Research Institute (KAERI), Korea has been setup to strengthen the
capability of researches in nuclear safety not only in mastering the methods and computer codes, but also in
qualifying of young researchers in the field of nuclear safety analysis. Through the studies on the using of
thermal hydraulics computer codes like RELAP5, COBRA, FLUENT and CFX the thermal hydraulics research
group has made progress in the research including problems for safety analysis of APR1400 nuclear reactor,
PIRT methodologies and sub-channel analysis. The study of severe accidents has been started by using
MELCOR in collaboration with KAERI experts and the training on the fundamental phenomena occurred in
postulated severe accident. For Vietnam side, VVER-1000 nuclear reactor is also intensively studied. The
design of core catcher, reactor containment and severe accident management are the main tasks concerning
VVER technology. The research results are presented in the 9th National Conference on Mechanics, Ha Noi,
December 8-9, 2012, the 10th
National Conference on Nuclear Science and Technology, Vung Tau, August
14-15, 2013, as well as published in the journal of Nuclear Science and Technology, Vietnam Nuclear Society
and other journals. The skills and experience from using computer codes like RELAP5, MELCOR, ANSYS
and COBRA in nuclear safety analysis are improved with the nuclear reactors APR1400, Westinghouse 4 loop
PWR and especially the VVER-1000 chosen for the specific studies. During cooperation research project, man
power and capability of Nuclear Safety center of INST have been strengthen. Three masters were graduated, 2
researchers are engaging in Ph.D course at Hanoi University of Science and Technology and University of
Science and Technology, Korea, respectively.
Project information:
- Code: 22/2012/HĐ-NĐT
- Managerial Level: Government
- Allocated Fund: 2,995,000,000 VND
- Implementation time: 24 months (Jan 2012-Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. Le Dai Dien, Nguyen Tu Oanh. Analysis of DVI line break in ATLAS test facility using RELAP5
code. J. Nuclear Science and Technology, No. 4, pp.33-41, VINATOM, 2011.
2. Le Dai Dien, Le Tri Dan. Analysis of Steam Generator Tube Rupture Accident for Korean Reactor
APR1400. J. Nuclear Science and Technology, Vol. 3, No. 2, pp.7-14, VINATOM, 2013.
3. Le Dai Dien, Bui Thi Hoa, Vo Thi Huong. Application of MELCOR code to Westinghouse 4-loop
PWR Severe Accident and Evaluation of RPV Lower Head Performance. . J. Nuclear Science and
Technology, Vol. 4, No.2, VINATOM, 2014
4. Tae Woon Kim, Jinho Song, Vo Thi Huong, Dong Ha Kim, Bo Wook Rhee, Shripad Revankar.
Sensitivity study on severe accident core melt progression for advanced PWR using
MELCOR code. Nuclear Engineering and Design (2013) http:www.elsevier.com/ locate/nucengdes.
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
36
1. INTRODUCTION
Safety analysis is one of the requirements for the construction and operation of NPP.
Understanding of physical phenomena - as well as thermal hydraulics computational simulation is
an important tool to confirm safety of NPP in the postulated accidents. The cooperation between
VINATOM and KAERI in the safety analysis of PWR has been established since 2009 and the first
phase has been successful carried out in 2010. In order to strengthen the capability of researchers at
INST, VINATOM the second phase of the project (2012-2013) is supported.
The objectives of the project are as follows:
- Enhancement of capability of implementation of computer codes in the safety analysis
work for NPP including system code and sub-channel code.
- Training of young researchers in safety analysis in thermal hydraulics as well as in
severe accident study.
For the cooperation, the common objectives are the establishments of application system of
thermal hydraulic safety analysis code for PWR, including: Evaluation of system TH code like
RELAP5, MARS and MELCOR for severe accidents. The other important objective is exchange of
human resources between Korea-Vietnam through on the job training (OJT) for Vietnamese code
users and lectures for code technology and safety analysis in the fields of thermal hydraulics and
severe accident.
With the above mentioned targets, the research topics focus on main studies which has been
shown to be effective through research works:
1. To complete basic problems in safety analysis report (SAR) of APR1400 reactor along
with the problems had been done in the first phase (2009-2010) to make a complete safety analysis
problems for APR1400 reactor.
2. To start studing the severe accident in NPP from fundamental phenomena to some key
issues such as skills using MELCOR code, expanding the scope of the research to VVER-1000
reactor, thereby helping staff to participate in the activities that support to Ninh Thuan 1 projects in
future.
3. The study results demonstrated by the thematic research activities, simulations using
computer codes (RELAP5, MELCOR, COBRA, MARS, ANSYS FLUENT, ANSYS CFX) for
some specific problems. There have been some reports in national scientific conferences and the
results demonstrated in Master thesis as well as contribution to doctoral thesis under progress.
The contents of the study are shown systematically in Figure 1. including roadmap for
research towards building expertise in thermal hydraulics safety analysis and severe accident.
Thermal hydraulics phenomena are important in most of accidents in DBA as well as
BDBA. The thermal hydraulic safety concerns with:
- Safety analysis of DBA for evaluating the adequacy of the design to cope with transient
and accident conditions
- Safety analysis of BDBA for evaluating if consequences can be considered as
acceptable
- Safety analysis of Severe accident and Accident management (AM) development to
prevent or mitigate accident consequences
To address these safety concerns, thermal hydraulic codes are studied for simulation of
Korean APR1400 reactor. The main problems in SAR have been studied during the years 2009-
2010 [1] and continued to study in order to make a full set of safety analysis including LOCA,
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
37
LOCA and SBO, REA, FWB, LOFA, SGTR, MSLB. Based on these studies, the group of
researchers in thermal hydraulics safety analysis has been set up.
The studies in severe accident have been intensively performed. The training on the basic
phenomena in severe accident with the lectures presented by experts from KAERI was held in
INST.
Figure 1: Implementation strategy of computer codes and research
works for the cooperation.
2. THE MAIN RESULTS AND DISSCUSION
2.1. Improvement of capability of using RELAP5
Three safety analysis problems including LOCA and SBO, SGTR and MSLB have been
performed for APR1400 reactor. Especially in the SGTR analysis, the simulation results has been
compared with the simulated ones by MARS-3D reported by KAERI [2].
Figure 2 shows the primary and secondary system pressures during the simulation for the
SGTR event. When a steam generator tube is ruptured, the reactor coolant system pressure
immediately drops as a tube break and the PRZ backup heater is actuated as designed. After the
ECCS is actuated, water level in PZR increases again. The water levels in PZR and in both steam
generators (intact and broken) are shown in figure 3. It is also noted, that the starting point used in
[2] included steady state (run for 300s) as indicated in the figure. The results simulated by RELAP5
performed by us are in good agreements with the KAERI report [2].
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
38
Figure 2: Pressure changes in the primary and secondary loop in SGTR accident
in comparison between calculations by RELAP5 (Right) and MARS-3D(Left)[2].
Figure 3: Collapsed water levels in PZR and narrow range of SG (broken and intact) in SGTR
accident in comparison between calculations by RELAP5 (Right) and MARS-3D(Left)[2].
2.2. Analysis of severe accident in NPP
This study refers to the phenomena and processes occurring in severe accident, the safety
and prevention systems to minimize the accident consequences, the researchers are initially
equipped with the basic knowledge not only in phenomena review but also in study of MELCOR
code by the help of KAERI experts. The modeling of Westinghouse 4-loop PWR was simulated and
SBO with RCP seal leakage is simulated. According to [3], the results reported in WASH-
1400 indicated that breaks of an equivalent diameter in the range of 0.5 to 2 inches in the RCS
pressure boundary are an important events which may lead to core-melt. The overall probability of
core-melt due to SBLOCA could be dominated by events such as RCP seal failures was also
interested.
The water mass in the reactor core and lower plenum decreases and then recovered by water
injection when RCS pressure reaches the set point of accumulators. At about 8h after reactor trip,
the core is uncovered again and collapse in fuel ring 1 occurred. The core center (ring 1) is totally
failed at 9.7h. The sequences are presented in figure 4.
The cladding temperature heat-up and exceeds the melting temperature, the cladding failure
starts to occur from top of ring 1 at 8.16 hours after that it spreads to other areas as shown in figure
4.
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
39
The simulations performed in this study are comparable with another simulations by
MELCOR [4].
T = 29400 s (8.17h)
Collapse in ring1 began
T = 31620 (8.78 h)
Debris in Lower Head
T = 36200 s (10.06h)
Collapse of ring 1
T = 36450 s (10.13h)
Failure in ring 2
T = 38200 s (10.6h)
Collapse of ring 2
T = 38230 s (10.62h)
Collapse of ring 3
T = 53050 s (14.7h)
Debris reaches lower
head
T = 63720 s (17.7h)
Melt injected to cavity
T = 90000 s (25h)
Core damage after 25h
Figure 4: Accident sequences in reactor core and lower head.
2.3. Implementation of CFD in reactor T/H
The application of CFD is studied by practice to use ANSYS software (Copyright Research
Academy version) in collaboration with ANSYS staff from Hanoi University for Science and
Technologies (HUST). Based on basic exercises, ANSYS FLUENT and CFX have been used to
simulate PSBT experiments.
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
40
Figure 5: Cross view of the void fraction at measurement position.
Simulation of two phase flow in a channel is still hard problem with CFD. For the S1
exercise of the benchmark problem mentioned in this paper there are a lot of study which are
introduced. This study introduces the utilization of two phase flow simulation with additional sub
model of MUSIG which is available in Ansys CFX 14.5. Simulations are presented in figure 5.
The results show that there is a significant improvement of the convergence for the runs
being studied. However, for various case of the two phase flow it is needed to study more
correlations for selection of appropriate key parameters for model simulation.
2.4. Thermal-hydraulic analysis for PWR
Several of important topics related to advanced light water reactor like critical heat flux, two
phase flows, departure from nucleate boiling (DNB) etc. have been studied. The updated knowledge
in thermal hydraulics safety analysis is addressed so that the following studies are intensively
performed:
The APR1400 and VVER-1000/V392 reactors have been simulated using RELAP5 and the
steady state results are given. The nodalization scheme and steady state simulations of APR1400
has been used since 2009 by the authors [1]. Followings are simulated results for VVER-
1000/V392. One nodalization based on OECD benchmark noted as “Simulation #2” and the other
developed by us noted as “Simulation #1”. Both nodalizations and steady state simulations are
satisfactory as indicated in figure 6 and table 1.
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
41
560
570
580
590
600
0 200 400 600 800 1000
Nhiệ
t độ (
K)
Thời gian (s)
Figure 6: Water temperature at the inlet and outlet calculated by the RELAP5 using
different nodalizations: “Simulation #1”(left) and “Simulation #2”(right).
The water temperature at the inlet and outlet calculated by the different nodalizations are
presented in Table 1.
Table 1: Thermal hydraulics parameters of RCS of VVER1000/V392
in the normal power operation conditions.
Main parameters Design [7] Calculated #1 Calculated #2
Thermal power, MW 3000 3000 3000
Mass flow rate through the core,
m3/h
86000 ± 2600 86532 86029
Mass flow rate / nhánh, m3/h 21500± 1000 21633 ---
Primary pressure (in PZR), MPa 15.7±0.3 15.73 15.8
Water temperature at inlet, 0C 291 (+2)(-5) 295.3 288.8
Water temperature at outlet, 0C 321±5 324.3 318.8
Pressure drop in core, MPa 0.148 0.177 ---
Pressure drop in RPV, MPa 0.387 0.38 ---
Bypass flow rate, % 3 3.1 ---
Feedwater temperature, oC 220 ± 5 220 220.15
Water level in PZR, m 8.17 8.12 ---
Water level in SG
(secondary side), m
2.7 ± 0.05 2.7 2.63
SG exit steam pressure, MPa 6.27 ± 0.1 6.08 6.27
Steam temperature, oC 278.5 276.7 ---
The steady state calculations are performed by simulations in system codes like RELAP5 for
VVER-1000/V392 in the normal power operation. The thermal hydraulics parameters calculated in
our simulations are generally in good agreements with the design. It is also noted that this
VINATOM-AR 13--04
The Annual Report for 2013, VINATOM
42
simulations are used not only in verifying the provided design data, but also in safety analysis in
transient and accident conditions.
3. CONCLUSION
Safety Analysis in which T/H studies are very important needs to be addressed not only in
NPP projects going on in Vietnam now, but also in strengthening of our understanding of safety
characteristics of NPP systems. Through joint research project, the APR1400 reactor has been
studied and safety analysis problems were performed. Based on the experience in first phase [1], the
VVER-1000 has been intensively studied, not only in core thermal hydraulics, but also in severe
accident including the containment, core catcher features etc. The severe accident phenomena are
introduced and simulation of PWR using MELCOR code is supported by KAERI. These are highly
appreciated.
The international cooperation is recognized as important factor for HRD in nuclear safety
research. The human resource development in the field of safety analysis now is under the request.
It is not only requirements of the number of researchers, but also higher qualification of researchers
as well as research works.
REFERENCE
[1] Lê Văn Hồng và các cộng sự. Báo cáo tổng kết nhiệm vụ hợp tác theo NĐT 2009-2010
“Hợp tác nghiên cứu phân tích, đánh giá an toàn vùng hoạt lò phản ứng năng lượng nước
nhẹ trong các điều kiện chuyển tiếp và sự cố”. Thư Viện Khoa học Kỹ thuật Trung ương. Hà
Nội, 1/2011.
[2] Chung B.D., et al, “Development and assessment of multi-dimensional flow models in the
thermal-hydraulic system analysis code MARS,” KAERI/TR-3011/2005, KAERI.
[3] Resolution of Generic Safety Issues: Issue 23: Reactor Coolant Pump Seal Failures (Rev. 1)
(NUREG-0933, Main Report with Supplements 1-34 ).
[4] S.G. Ashbaugh et al. “Simulation of Mixed Oxide (MOX) Versus Low Enrichment Uranium
(LEU) Fuel Severe Accident Response Using MELCOR, Sand 2005-4361c.
[5] ANSYS, Inc., Canonsburg, PA 15317, ANSYS CFX-Solver Theory Guide. (Release 14.0,
November 2011).
[6] NEA Nuclear Science Committee, NEA Committee on Safety of Nuclear Installations.
OECD/NRC BENCHMARK BASED ON NUPEC PWR SUBCHANNEL AND BUNDLE
TESTS (PSBT) Volume I: Experimental Database and Final Problem Specifications.
(November 2010).
[7] Training course “Introduction to NPP Technology”. Chapter 5-Reactor Coolant System and
Connected Systems. Risk Engineering Ltd. January 2012.
VINATOM-AR 13--05
The Annual Report for 2013, VINATOM
43
A NEUTRONIC FEASIBILITY STUDY OF THE VVER ASSEMBLY
TYPE DESIGN LOADED WITH FULLY CERAMIC
MICRO-ENCAPSULATED FUEL
Hoang Van Khanh, Phan Quoc Vuong, Tran Vinh Thanh
Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 Hoang Quoc Viet, Nghia Do, Ha Noi, Vietnam
ABSTRACT: A neutronic feasibility study is performed to evaluate the utilization of fully ceramic
microencapsulated (FCM) fuel in the VVER fuel type design. The fuel assembly features the same dimensions
as a benchmark VVER-1000 fuel assembly. On the lattice level, the MVP Monte Carlo and the JENDL-3.3
library were used based on the statistical geometry model. This work focus the results of the lattice-level
neutronic study of doubly heterogeneous FCM fuel including effect of packing fraction and TRISO size on the
neutronic characteristics of fuel pin cell and assembly. The results show that TRISO size of 500μm and
packing fraction of 0.45 has the most excellent neutronic characteristics.
Keywords: VVER, FCM, packing fraction, STRISO size.
1. INTRODUCTION
Fully ceramic microencapsulated (FCM) fuels consist of Tristructural Isotropic (TRISO)
fuel particles embedded in a silicon carbide (SiC) matrix. A TRISO particle consists of a spherical
fuel kernel that is coated with successive layers of porous carbon (buffer layer), a dense inner
pyrocarbon (IPyC), SiC, and an outer pyrocarbon (OPyC) layer. In conventional high-temperature
gas-cooled reactor (HTGR) applications, the TRISO particles are dispersed in a graphitic matrix,
producing compacts in the form of pebbles or pellets 00. Under the FCM fuel concept, the graphite
matrix is replaced with a SiC matrix that offers the following potential advantages 0: (i) improved
irradiation stability; (ii) incorporation of yet another effective barrier to fission product release; (iii)
environmental stability under operating (steady state) and transient conditions as well as long-term
storage; (iv) proliferation resistance.
This paper presents the results of the lattice-level neutronic study of doubly heterogeneous
FCM fuel of the VVER fuel type design. The impact of packing fraction and TRISO size on the
neutronic characteristics of fuel pin cell and assembly was considered to carry out their optimal
values for new fuel design.
2. OBJECTIVES
In order to begin assessing the neutronics characteristics of the FCM fuel, unit cell
calculations were performed. These unit cell calculations can provide information about the
neutronic characteristics of a whole core of similar fuel, and also would provide insight into the
influence of these types of cells heterogeneous assemblies containing UO2 pins as well. The main
objective of this work is to:
Project information:
- Code: CS/13/04-03
- Managerial Level: Ministry
- Allocated Fund: 50,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--05
The Annual Report for 2013, VINATOM
44
- Investigate neutronic characteristics of the VVER fuel type design loading FCM fuel.
- Evaluate the effects of varying the kernel size and packing fraction on the neutronic
characteristics. Preliminary evaluation of heterogeneous assemblies containing FCM pins.
- Compare these results to reference UO2 unit cells.
3. METHODOLOGY
Two calculational models, unit pin cell lattice and assembly lattice, were performed using a
Monte Carlo neutron transport MVP code developed by Japan Atomic Energy Agency 0 and the
JENDL-3.3 library 0. The lattice calculations were performed by applying the statistical geometry
model. The fuel pin cells and assembly feature the same dimensions as a benchmark VVER-1000
fuel assembly 0.
4. RESULTS
4.1. Lattice parameters
The specifications chosen for initial analysis approximate the lattice of the VVER-1000.
Initial calculations were performed by assuming that the ordinary UO2 fuel pellets are replaced with
the FCM fuel compacts. FCM fuel is constituted of TRISO fuel particles containing UO2 kernels
embedded within a SiC matrix. Table 1 shows the dimensions and densities (i.e., specific mass) of
the layers of the TRISO particles specified for these initial calculations. The simplifying assumption
was made that the kernel diameter can be varied without changing the layer thicknesses,
notwithstanding the material integrity implications.
Table 1: TRISO fuel particle dimensions and physical properties in FCM fuel.
The fuel assemblies (FA) are hexagonal in shape. They consist of a total of 331 cell
locations in a regular hexagonal array. The 331 elementary hexagonal locations in FA are occupied
by four main types of cells: 312 fuel pin cells, one central water filled instrumentation tube and 18
water filled guide tubes for control insertion. These assemblies are typical of the advanced designs
under active development in Russia for the VVER-1000 reactors 0 as description in Table 2 and
Figure 1.
Table 2: Description of cell types geometry.
VINATOM-AR 13--05
The Annual Report for 2013, VINATOM
45
Figure 1: Schematic diagram of a uniform LEU fuel assembly.
4.2. Calculation Results
This section presents on the examination of unit pin cell and assembly lattice of UO2. This
section reports on the examination of unit cells of UO2, the effect of packing fraction and TRISO
size on the neutronic characteristics are evaluated.
Figure 2 shows the initial multiplication factor (k∞) of unit pin cells versus packing fraction
(PF). When the PF increases the amount of fuel in the pin cell increases and therefore as the results
the initial k∞ increases.
Figure 2: k∞ versus packing fraction in unit pin cells.
VINATOM-AR 13--05
The Annual Report for 2013, VINATOM
46
The Figure 2 also implies that the effect of cladding material on k∞ is negligible. Both SiC
and Zr cladding result in similar k∞ value.
Compared to the original design, the infinite multiplication factor (k∞) of FCM design
slowly decreases and get higher values with higher values of packing fraction as shown in Figure 3.
Figure 3: k∞ of pin cell versus burnup with different packing fraction.
For the fuel assembly lattice, its k∞ features the same as of the fuel pin cells. With the
packing fraction of 45%, the k∞ of fuel assembly is closely similar to the one of original design
(Figure 4).
Figure 4: k∞ of fuel assembly versus burnup with different packing fraction.
The values of packing fraction, 45%, will be chosen as the first optimal packing fraction value. To
evaluate the effect of TRISO size on the neutronic characteristics, the TRISO size was increased to
600µm.
Figure 5: k∞ of fuel assembly versus burnup with different TRISO size.
VINATOM-AR 13--05
The Annual Report for 2013, VINATOM
47
Figure 6: k∞ of fuel assembly versus burnup.
With the increasing of TRISO size, the k∞ of fuel assembly increases. After 500µm, the
change of k∞ in the first burnup step (≤ 60GWd/t) is nearly unchanged. So 500µm was chosen as
the first optimal TRISO size value (Figure 5). Compared to the original design, FCM design can get
longer core life as shown in Figure 6.
5. CONCLUSIONS
A neutronic feasibility study is performed to evaluate the utilization of fully ceramic
microencapsulated (FCM) fuel in the VVER fuel type design. the results of the lattice-level
neutronic study of doubly heterogeneous FCM fuel including effect of packing fraction and TRISO
size on the neutronic characteristics of fuel pin cell and assembly. The results show that TRISO size
of 500μm and packing fraction of 0.45 has the most excellent neutronic characteristics. The effect
of cladding materials is negligible.
REFERENCES
[1] H. Nickel, H. Nabielek, G. Pott, A.W. Mehner, Nucl. Eng. Des. 217. pp. 141–151, 2002
[2] J. Phillips, C. Barnes, J. Hunn, Fabrication and comparison of fuels for advanced gas reactor
irradiation tests, in: Proceedings of HTR 2010, Prague, Czech Republic, paper 236, October
2010,
[3] K.A. Terrani, et al., Fabrication and characterization of fully ceramic microencapsulated
fuels, Journal of Nuc. Mat. 426, pp. 268-276, 2012.
[4] Nagaya, Y., Okumura, K., Mori, T., Nakagawa, M. MVP/GMVP II: general purpose
Monte Carlo codes for neutron and photon transport calculations based oncontinuous
energy and multigroup methods. JAER, I-1348, 2005.
[5] Shibata, K., et al. Japanese evaluated nuclear data library version 3 revision-3:
JENDL-3.3. J. Nucl. Sci. Technol. 39, 1125-1136, 2002.
[6] NEA/NSC/DOC 10, A VVER-1000 LEU and MOX assembly computational benchmark.
Nuclear Energy Agency, Organization for Economic Co-operation and Development, 2002.
VINATOM-AR 13--06
The Annual Report for 2013, VINATOM
48
CALCULATION OF FUEL AND MODERATOR TEMPERATURE
COEFFICIENTS IN APR1400 NUCLEAR REACTOR BY MVP CODE
Pham Tuan Nam, Le Thi Thu, Nguyen Huu Tiep and Tran Viet Phu
Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 - Hoang Quoc Viet, Ha Noi, Vietnam
ABSTRACT: In this project, these fuel and moderator temperature coefficients were calculated in APR1400
nuclear reactor by MVP code. APR1400 is an advanced water pressurized reactor, that was researched and
developed by Korea Experts, it’s electric power is 1400 MW. The neutronics calculations of full core is very
important to analysis and assess a reactor. Results of these calculation is input data for thermal-hydraulics
calculations, such as fuel and moderator temperature coefficients. These factors describe the self-safety
characteristics of nuclear reactor. After obtaining these reactivity parameters, they were used to re-run the
thermal hydraulics calculations in LOCA and RIA accidents. These thermal-hydraulics results were used to
analysis effects of reactor physics parameters to thermal hydraulics situation in nuclear reactors.
I. INTRODUCTION
The Advanced Power Reactor 1400 (APR1400) [1,2,4] is of the pressurized water type
using two reactor coolant loops. This reactor used uranium dioxide fuel, and many characteristics
that were improved from OPR1000 reactor. The simulation and calculation of this new reactor is an
important work that helps to obtain experiences and skills in analysis and assessment NPP
technology.
Fuel temperature coefficient (Doppler effects) and Moderator Temperature Coefficients
(MTC) are two important parameters that have to consider in design and operating of NPP. These
parameters have to be negative in Pressurized Water Reactor (PWR), and also in APR1400. We
carried out these factors to investigate change of reactivity that depend on temperatures of fuel and
moderator. Then these results were used to assess effects of reactor physics factors to TH state in
RIA and LOCA accidents.
II. FUEL AND NUCLEAR DESIGN OF APR1400 REACTOR
APR1400 reactor is the newest water reactor that was result of Korea government project
from 1992. This reactor has lager power, 1400 MWe. And there are many enhancements in fuel and
nuclear design. Figure 1 and table 1 describe the full core of APR1400.
Project information:
- Code: CS/13/04-05
- Managerial Level: Institute
- Allocated Fund: 50,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--06
The Annual Report for 2013, VINATOM
49
Figure 1: Reactor Core Cross Section 241 Fuel Assemblies [5].
Table 1: Mechanical Design Parameters [5].
Number of fuel assemblies in core, total 241
Number of CEAs 93
Number of fuel rod locations 56,876
Spacing between fuel assemblies, fuel rod surface to surface
inches (cm)
0.208 (0.528)
Spacing, outer fuel rod surface to core shroud, inches (cm) 0.214 (0.544)
Hydraulic diameter, nominal channel, feet (cm) 0.0393 (1.198)
Total flow area (excluding guide tubes), ft2 (m
2) 60.8 (5.649)
Total core area, ft2 (m
2) 112.3 (10.433)
Core equivalent diameter, inches (cm) 143.6 (3.647)
Core circumscribed diameter, inches (cm) 152.46 (3.872)
Total fuel loading, lb U (kg U) (assuming all rod locations are fuel
rods)
228 x 103 (103.42 x 10
3)
Total fuel weight, lb UO2 (kg UO2) (assuming all rod locations are
fuel rods)
258.6 x 103 (117.3 x 10
3)
Total weight of Zircaloy, lb (kg) 74,950 (33,996.7)
Fuel volume (including dishes), ft3 (m
3) 409.6 (11.6)
This data is adequate for thermal-hydraulics and neutronics calculations in full core of
APR1400 reactor.
III. CALCULATION OF MULTIPLIER FACTOR (K-EFF) AND REACTIVITY
COEFFICIENTS IN FULL CORE OF APR1400 REACTOR
Dopler effect is very important to design and operate a nuclear reactor [6,7,8]. When fuel
temperature changes, cross section of U238
and neutron reaction changes, and reactivity is changed.
In this project, this effect was claculated when fuel temperature changes from 68 F (293 K)-room
temperture to 2500 F (1644 K), that is reached when accident happens.
VINATOM-AR 13--06
The Annual Report for 2013, VINATOM
50
Fiure 2 is result of calculation for change of multiplier factor and reactivity when fuel
average temperature varies.
Figure 2: Dependent of multiplier factor and reactivity
on fuel temperature by MVP code.
Results that were obtained by MVP code, run in personal computer and windows OS, has
0.036% errors. This is fit with results in Safety Analysis Report (SAR) [4].
Moderator Temperature Coefficient (MTC) strongly affects to reactor physics state, too.
When moderator temperature changes, H-2, O-16 and B-10 nuclide densities change, that affects to
neutron flux and reactivity in nuclear reactor. In this project, MTC was calculated in two states, the
first state: hot zero power, 555oF (290.6
oC) water temperature, no control element assemblies
(CEA), clean, 1210 ppm acid boric; and the second state: Hot full power, 588oF (308.9
oC), no
CEAs, clean and 1088 ppm acid boric. The results are -2.19E-04 ∆ρ/oF and -2.63E-04 ∆ρ/
oF ,
corresponding to the first and second states. These results have large different that comparing to
results in SAR, MTC coefficients are -0.11E-04 ∆ρ/oF and -0.51E-04 ∆ρ/
oF.
IV. USING THE NEUTRONICS CALCULATION RESULTS FOR THE THERMAL
HYDRAULICS CALCULATIONS
The thermal hydraulics code - RELAP5 code, was used to carry out the Reactivity Initial
Accident (RIA) and Loss Off Coolant Accident (LOCA) calculation in WINDOW OS [3], on PC.
The calculations used the neutronics calculation results, that showed above. Figure 3 indicated
change of DNBR parameter in control valve - 777 in 6 s after RIA accident. Results obtained from
the new and old input data, are similar. That indicates that MTC and Doppler effects affect to
thermal hydraulics state of reactor very weakly.
VINATOM-AR 13--06
The Annual Report for 2013, VINATOM
51
Figure 3: DNBR change in RIA accident.
V. CONCLUSION
In this project, the calculated group completed all of proposed works, described detailed
structure of fuel assembly and full core in APR1400, knew and calculated multiplier factor,
reactivity coefficients, and using nuclear physics results for thermal-hyraulics calculation.
Calculated results are used for nuclear reactor safety analysis, although this data is not high correct
level but it was the first step in full core calculation for APR1400 technology, and understood effect
of and neutronics results to thermal-hydraulics states.
REFERENCES
[1] Design Features, Safety Assessment and Verification of Key Systems, and Economic
Advancements for APR1400, Sung Jae Cho, Eui Jong Lee, Engineering Support Center,
Nuclear Environment Technology Institute, Korea Hydro & Nuclear Power Co., LDT, 103-
16, Munji-Dong, Yuseong-Gu, Daejeon 305-380, Korea.
[2] APR1400 Design Description, Center for Advanced Reactors Development, Nuclear
Environment Technology Institute, 로고 Korea Hydro & Nuclear co., Ltd, 03/2002.
[3] Lê Văn Hồng và các cộng sự. Báo cáo tổng hợp kết quả nghiên cứu khoa học công nghệ nghị
định thư “Hợp tác nghiên cứu phân tích, đánh giá an toàn vùng hoạt lò phản ứng năng lượng
nước nhẹ trong các chuyển tiếp và sự cố, Viện Năng lượng Nguyên tử Việt Nam, Hà Nội,
2011.
[4] Sung-Quun Zee, Modure 2: Reactor Core and Components, Nuclear Power Reactor
Technology, Core Dseign and Analysis Technology Dept., Korea Atomic Energy Research
Institute,
<http://www.kntc.re.kr/openlec/nuc/NPRT/module2/module2_2/module2_2_2/2_2_2.htm#3.
3%20Burnable%20Poisons>
[5] Islamic Azad University. Computation of concentration changes of heavy metals in the fuel
assemblies with 1.6% enrichment by ORIGEN code for VVER-1000, Mohammad
Rahgoshay, Department of Nuclear Engineering, Faculty of Engineering, Science and
Research Branch, , Tehran, Iran, 2006.
[6] K. Okumura, T. Kugo, K. Kaneko, K. Tsuchihashi. SRAC2006: Acomprehensive Neutronics
Canculation Code System, Japan Atomic Enerrgy Angency, 2007.
[7] Y. Nagaya, T. Mori, K. Okumura, M. Nakagawa. MVP/GMVP: General Purpose Monte
Carlo Codes for Neutron and Photon Transport Camculations based on Continuous Energy
and Multigroup Methods Version 2, Japan Atomic Energy Research Institute, 2004.
[8] Lê Đại Diễn. Báo cáo tổng kết đề tài khoa học công nghệ cấp cơ sở “Sử dụng chương trình
MVP tính toán cho mô hình bó nhiên liệu HEU và LEU của lò phản ứng hạt nhân Đà Lạt”,
Hà Nội, 2007.
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
52
ESTABLISHING QUALITY ASSURANCE PROGRAM FOR
CALCULATION IN CORE AND FUEL MANAGEMENT OF THE DALAT
NUCLEAR RESEARCH REACTOR USING LOW ENRICHED FUEL
Huynh Ton Nghiem, Luong Ba Vien, Le Vinh Vinh, Nguyen Kien Cuong, Nguyen Manh Hung,
Nguyen Minh Tuan, Pham Quang Huy, Tran Quoc Duong, Vo Doan Hai Đang, Pham Hong Son,
Tran Tri Vien and Tran Thanh Tram
Reactor Center, Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: Quality assurance program for calculation in core and fuel management for research reactor
plays very important role in safety operation and effective utilization of reactor. The main objective of the
program is to ensure the safe, reliable and optimum use of nuclear fuel in the reactor. This project is carried out
to establishing the quality assurance program together with selected, verified and validated computer code
system and data libraries for calculation in core and fuel management of the Dalat Nuclear Research Reactor
(DNRR) using completely low enriched uranium (LEU) fuel assemblies. The selected computer code system,
data libraries and computational models must be fully met requirements for analyzing status and characteristics
of reactor core as well as the requirements for selecting, verifying and evaluating for codes according to the
regulations of the International Atomic Energy Agency (IAEA). When the quality assurance program and
DRRBurn computer code system are applied for calculation in core and fuel management of the DNRR, they
will contribute not only management, safety operation and effective utilization of the DNRR but also building
safety culture and experiences that will be used for other nuclear projects.
INTRODUCTION
After managing and operating of the DNRR during 30 years, staffs of Reactor Physics and
Engineering Department that belongs to Reactor Center have really developed and carried out main
tasks:
- Calculating in core and fuel management of the DNRR using high enriched uranium
(HEU) fuel [1];
- Calculating and performing in partial conversion of the DNRR core to using LEU fuel;
- Design calculation, safety analysis and implementing fully conversion using LEU fuel
of the DNRR [2, 3, 4, 5].
Many computer code systems have been investigated and applied for safety analysis as well
as operation management and utilization of the DNRR. Especially, in full core conversion project,
some selected computer codes have been served for design calculation and safety analysis. Obtained
results from full core conversion project show that calculation tools of Reactor Center were fully
met requirements about in core and fuel management and also in researching, operating
management and utilization of the DNRR.
Project information:
- Code: 03/2012/HD-NVCB
- Managerial Level: Ministry
- Allocated Fund: 500,000,000 VND
- Implementation time: 24 months (Jan 2012- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
53
However, the evaluation of computer code systems and data libraries to apply effectively for
the DNRR was not fully carried out. Procedures of calculation implementation, storage data, etc. are
not still approved and released. So
- Not having consistency in calculation;
- Neutronics calculation depending on experience of performers;
- Not ensure in elimination of errors or mistakes of users;
- Not ensure in inheritance in research.
The calculation in core and fuel management must be organized in a coherent way and in
compliance with safety requirements [15, 16, 17]. This will not only contribute to ensure the safe
operation management and effective exploitation of the reactor but also to establish safety culture
and valuable experience for other nuclear projects. In addition, the establishment and application of
quality assurance program for calculation in core and fuel management will contribute to
consistency in reactor calculations, avoiding errors or mistakes; clearly define responsibilities and
ensuring continuity professional expertise.
I. RESEARCH IN EXPERIMENT AND CALCULATION
I.1. Research in experiment
The research in experiment to reactor’s parameters always is conducted when reactor’s
working configuration is changed to ensure safe operation and effective utilization. The
experimental results are also used to verify computer codes, simulation models and nuclear data
libraries used in the design, operation management and exploitation.
Important parameters of the DNRR were determined by experiments including:
- Neutron distribution (azimuthal distribution in fuel assembly, radial distribution, axial
distribution, symmetric distribution of the reactor core and absolute neutron flux at irradiation
positions);
- Neutron spectra at important positions;
- Control rod worths and integral characteristics;
- Reactivity of fuel assemblies and Beryllium rods;
- Void effect;
- Temperature reactivity feedback coefficient of moderator;
- Xenon poisoning effect;
- Kinetics parameters.
The methods and conditions of experiments in order to reduce errors have been concerned
during implementation such experiments. The experimental results have been synthesized and
established to a set of experimental data used as the basis data for selecting, testing and evaluating
of computer codes and nuclear data libraries as well as to apply in operation management and
exploitation of the reactor.
I.2. Research in theory calculation
The primary objective of the research in theory calculation is to select, evaluate and validate
of computer codes, data libraries and computational models to serve for in core and fuel
management of the DNRR using LEU fuel.
Computer code systems have been researched and used including:
- SRAC system (PIJ, CITATION and COREBN) [11, 12];
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
54
- WIMS-ANL and REBUS [7, 9];
- MVP and MVP-Burn [13, 14];
- REBUS-MCNP linkage system [6, 8, 18, 19].
In addition, NJOY code was also used in data processing and created data libraries for other
computer codes like WIMS-D/E and MCNP.
Nuclear evaluated data have been investigated including: ENDF/B7.1 (USA) [20, 21],
JEFF3.1 (Europe) [23] and JENDL4.0 (Japan) [22].
I.2.1. Data library selection
The selection of data libraries have been done basing on three library systems: ENDF/B,
JEFF and JENDL, MCNP5 code was used to calculate for testing. The testing calculations include:
- Infinite multiplication factor for HEU and LEU fuels;
- Neutron spectra and micro cross section of 235
U and 238
U isotopes depending on energy
of HEU and LEU fuels;
- Finite multiplication factor for critical configuration with 72 LEU fuel assemblies and
working configuration with 92 LEU fuel assemblies of the DNRR.
Calculated results of the infinite multiplication factors of fuels show that results from all
three libraries have fairly consistent with each other. The results using ENDF/B7.1 and JEFF3.1 are
closer together than JENDL4.0. The results of neutron spectrum and fission cross sections show that
for HEU fuel spectrum and fission cross section of 235
U of all three libraries have resulted in very
small differences. For the fission cross section of 238
U in the thermal energy, the calculated result
using JEFF3.1 are significantly larger than the other two libraries. The calculated results of two
critical configurations are within acceptable difference.
The calculated results show that the libraries are asymptotic data together. The calculated
results using ENDF library always get in high reliability and closer to experimental values than the
calculated results using the remained two libraries. Therefore data library using for MCNP code is
mainly ENDF/B7.1.
I.2.2. Computer code system selection
A set of data consists of 14 different critical configurations with 25 positions having various
control rod positions that was established during reactor startup was selected to perform the
calculation and obtained results by using current four computer code systems were compared with
each other.
Calculated results from 4 computer code systems show that:
- Regarding to stability, errors of calculated results using MVP and MVP-Burn and
REBUS-MCNP with real geometric models are 0.12% and 0.10% respectively, the SRAC
system and WIMS-ANL, REBUS with lattice cell geometric models are 0.17% and 0.15%
respectively compared with the average value.
- In terms of absolute results, average values of multiplication factor of WIMS-ANL and
REBUS system and REBUS-MCNP system using ENDF/B7 library are 0.9997 and 0.9995
respectively, the SRAC system and MVP and MVP-Burn using ENDF/B6 library are 0.9985 and
0.9981 respectively.
So, computer code systems using real geometric models and new updated libraries give
better stability and more consistent results compared with experimental data.
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
55
Table 1 presents main characteristics of the four computer code systems based on the main
features of the method, geometric models and other features.
The calculated results show that all computer code systems can be met requirements in
neutronics calculation of research reactor. So depending on the calculation requirements as well as
the current computer code systems users can select a suitable computer code system. With these
advantages that are presented in Table 1 and the possibility of personal computers nowadays,
REBUS-MCNP was chosen as main calculation tool in the quality assurance program for
calculation in core and fuel management of the DNRR. With complex geometry as the DNRR along
with the presence of beryllium in the core, REBUS-MCNP system can fully satisfy the
computational requirements. Time consuming in calculation was overcome by using PC cluster on
MPI environment.
Table 2: Main characteristics of four computer code systems.
Feature SRAC MVP and
MVP-Burn
WIMS-ANL
and REBUS
REBUS-
MCNP
Solving equation Neutron
diffusion
Neutron
transport
Neutron
diffusion
Neutron
transport
Solving method Finite difference Monte-Carlo Finite difference Monte-Carlo
Geometry Lattice Real Lattice Real
Upgrading ability
- Program None None None Yes
- Data library None None Yes Yes
Beryllium poisoning None None None Yes
Consuming time Short Long Short Long
I.2.3. Comparing calculated results to experimental data
To validate the REBUS-MCNP system with ENDF data library, the system should be
evaluated by performing calculation almost characteristics of the reactor and compared with the
experimental data that were mainly gotten in during reactor startup with LEU fuel. The
implemented calculations include:
- Neutron flux distribution and neutron spectrum;
- Control rod worths;
- Effective reactivity of fuel assemblies and beryllium rods in the core;
- Void effect and temperature reactivity feedback coefficient of moderator;
- Xenon poisoning effect;
- Kinetics parameters.
Calculated and experimental relative thermal neutron flux, the results were normalized to
unit, at highest neutron flux in neutron trap show that.
- In radial direction of the reactor core, discrepancy between calculated results and
experimental data is less than 3%, except cell 6-4 and 12-2 with higher difference about 8%.
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
56
- In axial direction of fuel centerline, the difference between calculated and experimental
results in range from 15 cm to 65 cm is about 4%, top and bottom of fuel have higher differences
than 10%.
- In axial direction at neutron trap, the difference between calculated and experimental
results is about 4%.
The calculation of the neutron spectrum and absolute neutron flux in the experimental
irradiation positions including neutron trap, channel and two-channel wet dry 1-4 7-1 and 13-2 were
carried out. Table 2 presents experimental and calculated neutron spectrum and neutron flux that
collapsed in three energy groups at neutron trap with highest neutron flux of two configurations
with 104 HEU fuel assemblies and 92 LEU fuel assemblies. The results showed that the difference
between the calculated and experimental within 5%.
Table 2: Integral neutron flux collapsed to three energy groups at neutron trap.
Neutron flux
Mixed-core with 104
HEU fuel assemblies
Working core with 92
LEU fuel assemblies
MCNP5 SANDBP MCNP5 SANDBP
Thermal (n/cm2.s) 2.298.10
13 2.245.10
13 2.317.10
13 2.296.10
13
Epi-thermal (n/cm2.s) 7.027.10
12 7.248.10
12 6.520.10
12 6.224.10
12
Fast (n/cm2.s) 4.031.10
12 4.272.10
12 2.563.10
12 2.641.10
12
The effect of the control rod worths of working configuration with 92 LEU fuel assemblies
were calculated and compared with experimental data in Table 3 Experimental results are lower
than the calculated results in approximately 7%.
Table 3: Effect of control rod worth of working core with 92 LEU fuel assemblies.
Control rod Effective reactivity ($)
Diff. (%) Experiment Calculation
Regulating rod 0.495 0.531 6.73
Shim rod 1 2.966 3.178 6.68
Shim rod 2 3.219 3.422 5.93
Shim rod 3 2.817 2.958 4.76
Shim rod 4 2.531 2.709 6.58
Safety rod 1 2.487 2.604 4.49
Safety rod 2 2.195 2.219 1.10
The calculation of the effective reactivity of fuel assemblies and beryllium rods at different
positions in the reactor core have been conducted in order to determine the effective of reactivity
according to their positions in the reactor core. Calculated and experimental results showed that the
difference is just within 0.05$ (or 5 cent).
Calculated and experimental results also determined negative temperature reactivity
feedback coefficient of working configuration with 92 LEU fuel assemblies shows the inherent
safety of the reactor core using LEU fuel.
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
57
The calculation of negative reactivity by Xenon poisoning was done by calculating the
present of Xenon in composition of fuel after operating 130 h of the reactor and without Xenon
after cooling. The reactivity value was calculated about 1.30 $ compared with experimental value is
about 1.23 $, the difference between two values is 5.8%.
Table 4 shows the calculated results of kinetics parameters using LEU fuel by VARI3D and
MCNP5 computer codes and experimental data. The difference between calculated and
experimental results of the precursor decay constant and fraction of delayed neutron groups is about
4% and 5% respectively. These data will be used in transient calculation and safety analysis of full
core conversion from HEU to LEU fuel of the DNRR. Prompt neutron life time is determined by
8.925.10-5
s.
The calculated results of characteristic parameters of the reactor core using LEU fuel show
that REBUS-MCNP system fully meets the goal of calculation in core and fuel management of the
DNRR.
Table 4: Calculated and experimental results of precursor decay constant
and fraction of delayed neutron group.
Delayed
neutron
group
Precursor decay constant Delayed neutron fraction
Measured
value
Calculated
value Diff. (%)
Measured
value
Calculated
value Diff. (%)
1 1.358E-02 1.334E-02 1.8 2.648E-04 2.525E-04 4.9
2 3.251E-02 3.273E-02 0.7 1.363E-03 1.421E-03 4.1
3 1.236E-01 1.208E-01 2.3 1.315E-03 1.380E-03 4.7
4 3.141E-01 3.030E-01 3.7 2.902E-03 2.809E-03 3.3
5 8.182E-01 8.503E-01 3.8 1.204E-03 1.213E-03 0.8
6 2.847E+00 2.856E+00 0.3 5.033E-04 5.049E-04 0.3
Sum 7.550E-03 7.580E-03 0.4
II. ESTABLISHING COMPUTER CODE SYSTEM FOR CALCULATION IN CORE
AND FUEL MANAGEMENT
Computer code system for in core and fuel management must comply with the regulation of
core management was specified in the document “Core Management and Fuel Handling for
Research Reactors”, IAEA safety standards [17], which including regulations on: Management
objectives of the reactor core, safety requirements in core management and analysis calculation of
reactor core.
In addition, the computer code system must also suitable to manage the core of the DNRR
and ability to upgrade the system and data libraries to ensure updated when needed.
Each computer code must be evaluated and the can be applied for safety analysis-
particularly for licensing purpose. Each computer code in the system must comply with the
assessment process including the selection rules, testing, evaluation, documentation of the code as
well as the possibility of computer code user specified in the document “Safety analysis for research
reactor,” the IAEA safety report [15,16]. The preparation of input data, establishing calculational
model of the reactor core, edit input files of the codes in the system have to follow test and
evaluation procedures that specified in this document.
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
58
The computer code system was selected for in core management of the DNRR include:
- MCNP5 code: Calculate neutron flux and reaction rate;
- REBUS-Win: Burn up calculation and interested materials such as beryllium;
- Two computer codes: NJOY and WIMS-ANL is used to create and update data
libraries;
- DRRBurn code was programmed by Compaq Visual Fortran language on Window
operating system to connect and manage working system and core data management.
DRRBurn code was designed for using easily through the interaction between the user and
the display window on the screen. Calculational model and input files for all the codes in the system
has been built and evaluated. The code will automatically compose input file with core
configuration and composition of fuel material as well as beryllium materials that are updated
basing on information about changing of core configuration and historical reactor operation
supplied by the user to achieve the consistency in the whole process of core and fuel management,
less experienced user can also use the system and avoid possible errors.
The diagram of the DRRBurn computer code system is presented in Figure 1 with functions
including display, computation, management and storage.
The system has been used for core and fuel management of the DNRR from January, 2012
to March, 2014. Difference calculated and experimental excess reactivity following operation time
at maximum nominal power is about 0.08 $ and it shows that the calculated results were quite
suitable.
Figure 1: Diagram of the DRRBurn computer code system.
Update mctal
Calculate neutron
flux and reaction
rate
Composition of fuel
materials and Be in each
depletion time step
Update files MCNPCOMP,
input, a.rebcm, inp
Update multi group cross sections depending on burn
up of fission products and lumped fission product
Update library from evaluated nuclear data
Re-calculte neutron
flux and reaction rate
New depletion step
Update core
confguration: files
FNL, mcnpinpa
Update historical
reactor
operation:LSCL
REBUS_win
Burn up
DRRBurn
Fuel management,
Display
WIMS-ANL
Lattice cell calculation
MCNP5
Calculate neutron
transport
NJOY
Nuclear data processing
Files are updated:
FNL LSCL
MCNPCOMP
Input a.rebcm inp
mctal
Storage at each
depletion time
step MCNPCOMP
Input a.rebcm
inp mctal
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
59
III. CONCLUSIONS
The experiments were carried out to determine the characteristics parameters of the DNRR
fully using LEU fuel to establish the experimental data in order to operate safely and efficiently
utilization of the reactor. At the same time, the experimental data are applied in evaluating
computer codes to be used in analysis of the reactor.
Conducting theoretical calculations, carried out comparisons with experimental data and
analysis, evaluation to select, test and evaluate computer codes as well as nuclear data library in
order to validate them for putting in analysis and core management for the DNRR.
The linkage DRRBurn computer code was programmed to manage calculations, set up
computational model and input files as well as storage data to ensure compliance with the
requirements of the IAEA in core and fuel management of the DNRR.
Establishing and applying of the quality assurance program in calculation of core and fuel
management of the DNRR. The quality assurance program and DRRBurn system will really not
only contribute to ensure the management, safe operation and efficient utilization of the DNRR but
also to build safety culture and valuable experience for other nuclear projects.
REFERENCES
[1] Ngô Quang Huy và cộng sự. Các đặc trưng vật lý của Lò phản ứng hạt nhân Đà Lạt. Viện
Năng lượng nguyên tử Việt Nam, 1994.
[2] Quy trình khởi động vật lý và khởi động năng lượng để chuyển đổi toàn bộ vùng hoạt lò
phản ứng hạt nhân Đà Lạt sang sử dụng nhiên liệu độ giàu thấp. Viện Nghiên cứu Hạt nhân,
2011.
[3] Nhật ký vận hành lò phản ứng hạt nhân Đà Lạt, 2011-2012.
[4] Báo cáo kết quả khởi động vật lý và khởi động năng lượng để chuyên đôi toan bô vung hoat
Lò Phản ứng h ạt nhân Đà Lạt sang nhiên liệu độ giàu thấp . Viện Nghiên cứu Hạt nhân,
2012.
[5] Báo cáo phân tích an toàn sử dụng cho Lò Phản ứng hạt nhân Đà Lạt 2012, Viện Nghiên cứu
Hạt nhân, 2012.
[6] X-5 Monte Carlo Team, “MCNP - A General Monte Carlo N-Particle Transport Code,
Version 5”, Los Alamos national laboratory, April 2003.
[7] A.P. Olson, “A Users Guide for the REBUS-PC Code, Version 1.4”, Argonne National
Laboratory, Dec. 2001.
[8] John G. Stevens, “The REBUS-MCNP Linkage”, Argonne National Laboratory, April 2008.
[9] J.R. Deen et al., “WIMS-ANL User Manual, Rev. 5,” ANL/TD/TM99-07, Argonne National
Laboratory, Feb. 2003.
[10] Kahler, Albert C. III, MacFarlane, Robert, “The NJOY Nuclear Data Processing System,
Version 2012”, Los Alamos, 2012.
[11] Keisuke OKUMURA, Teruhico KUGO, Kunio KANEKO and Keichiro TSUCHIHASHI,
“SRAC2006: A Comprehensive Neutronics Calculation Systems”, Japan Atomic Energy
Agency, Feb. 2007.
[12] Keisuke OKUMURA, “COREBN: A Core Burn-up Calculation Module for SRAC2006”,
Japan Atomic Energy Agency, Feb. 2007.
[13] Yasunobu NAGAYA, Keisuke OKUMURA, Takamasa MORI and Masayuki
NAKAGAWA, “MVP/GMVP II: General Purpose Monte Carlo Codes for Neutron and
Photon Transport Calculations based on Continuous Energy and Multigroup Methods”,
Japan Atomic Energy Agency, Sep. 2004.
[14] Keisuke OKUMURA, Yasunobu NAGAYA and Takamasa MORI, “MVP-BURN: Burn-up
Calculation Code Using A Continuous-energy Monte Carlo Code MVP”, Japan Atomic
VINATOM-AR 13--07
The Annual Report for 2013, VINATOM
60
Energy Agency, Jan. 2005.
[15] Safety Analysis for Research Reactors, Safety Reports Series No.55, International Atomic
Energy Agency, 2008.
[16] Safety of Research Reactors, No. NS-R-4 Safety Requirement, International Atomic Energy
Agency, 2005.
[17] Core Management and Fuel Handling for Research Reactors, IAEA Safety Standards,
International Atomic Energy Agency, 2008.
[18] Daniel J. Whalen, David A. Cardon, Jenifer L. Uhle, John S. Hendricks, “ MCNP: Neutron
Benchmark Problems”, Los Alamos National Laboratory, Nov. 1991.
[19] Oscar Cabellos, “ Processing of the JEFF-3.1 Cross Section Library into a Continuous
Energy Monte Carlo Radiation Transport and Criticality Data Library”, OECD-Nuclear
Energy Agency Data Bank, May 2006.
[20] M. B. Chadwick et.al, “ENDF/B-VII.1 Nuclear Data for Science and Technology: Cross
Section, Covariances, Fission Yields and Decay Data”, Nuclear Data Sheet, Elsevier, 2011.
[21] http://t2.lanl.gov/data/endf/
[22] http://wwwndc.jaea.go.jp/ftpnd/jendl/j40p.html
[23] http://www.oecd-nea.org/dbforms/data/eva/evatapes/jeff_31/JEFF312/
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
61
A SRAC CALCULATION OF THE VVER 1000 CORE’S EFFECTIVE
MULTIPLICATION FACTOR
Tran Vinh Thanh, Phan Quoc Vuong, Tran Viet Phu, Hoang Van Khanh and Ta Duy Long
Nuclear Power Center, Institute for Nuclear Science and Technology,
Vietnam Atomic Energy Institute
179 Hoang Quoc Viet, Nghia Do, Cau Giay, Ha Noi
ABSTRACT: Neutronic characteristics for a VVER-1000 were investigated by using SRAC code and nuclear
data library JENDL-3.3 with 107 public energy groups. The elementary lattice modules, PIJ and CITATION,
have been used for modeling of the fuel rods, fuel assemblies and full core. The main Neutronic characteristics
analyzed in this work include infinite multiplication factors (kinf) versus burnup, the distribution of nuclide
concentrations in the pin cells; the pin-wise power distribution in the assembly; the effective multiplication
factors (keff), and the power distribution in the core.
Keywords: SRAC, PIJ, CITATION, effective multiplication factor, power distribution, burnup.
I. INTRODUCTION
Nuclear data libraries provide the data on cross sections and angular distributions of nuclear
reactions with neutron from experimental research and theoretical calculations. The data are used to
simulate neutronic characteristics in nuclear reactor physics. For this reason, the more accurate data
are, the more accurate simulation results become.
This report is based on the OECD benchmark paper: “A VVER-1000 LEU and MOX
Assembly Computational Benchmark. Nuclear Energy Agency, Organization for Economic Co-
operation and Development”[1]. In this report, we present characteristics of the VVER Low
Enriched Uranium (LEU) and Mixed Oxide (MOX) fuel assembly, where the calculations have
been done using 3 libraries: ENDF/B 7.0, JENDL 3.2 and JENDL 3.3. The obtained results are
compared to estimate the accuracy and usability of the data from the libraries with specific
characteristics.
II. CALCULATION SPECIFICATIONS
In this report, we used the SRAC code with PIJ and Burnup modules to modeling LEU and
MOX assemblies. The SRAC code which can be executed in UNIX and LINUX environments was
developed by Japan Atomic Energy Agency (JAEA). The code consists of 107 energy groups with
74 fast groups and 48 thermal groups providing collision probability (PIJ) and resolving neutron
diffusion and transport [2].
Project information:
- Code: CS/13/04-07
- Managerial Level: Institute
- Allocated Fund: 50,000,000 VND
- Implementation Time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Tran Vinh Thanh, Phan Quoc Vuong, Nguyen Tuan Khai. Comparative neutronic characteristics
calculations of LEU and MOX fuel assemblies of VVER reactor with various nuclear data libraries.
10th
National Conference on Nuclear Science and Technology,Vung Tau, June 2013.
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
62
II.1. LEU and MOX assemblies
The VVER hexagonal fuel assemblies consist of 331 cylindrical rods. Fuel cladding and
structural materials made by Zr-Nb composition. Fuel rods in the LEU assembly are classified into
4 types: 300 UO2 rods with 3.7%w/t enrichment, 12 absorbed burnable rods (UO2-Gd2O3-(UGD))
with 3.6%w/t UO2 and 4.0%w/t Gd2O3, a water rod put in the center of the assembly and 18 guide
tubes located at positions as shown in Figure 1.The fuel rods in MOX assembly are classified into 6
types: first layer consisting of 66 fuel rods with 2%w/t enrichment, second layer 96 fuel rods with
3%w/t, 138 fuel rods with 4.2%w/t in the center, 12 UGD rods, 1 water rod, 18 guide tubes in the
same positions as in the LEU assembly.
Figure1: LEU (left) and MOX (right) fuel assemblies.
II.2. State conditions
Table 1: State conditions.
State Description
Fuel
Temp.
(K)
Moderator
Temp. (K)
135Xe and
149Sm
Boron
concentration
in moderator
(g/kg)
S1 Operating poisoned hot state 1027 575 Eq. 0.6
S2 Operating state 1027 575 0 0.6
S3 Isothermal hot state with Boron 575 575 0 0.6
S4 Isothermal hot state without Boron 575 575 0 0
S5 Cold state 300 300 0 0
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
63
State conditions are listed in Table 1.The physical characteristics of the LEU and MOX
assemblies are calculated in the states: S1 is the operating poisoned hot state with 135
Xe and 149
Sm,
S2 is the operating hot state, S3 is the isothermal hot state with Boron, S4 is the isothermal hot state
without Boron, S5 is the cold state.
III. RESULTS AND DISCUSSIONS
III.1. Infinite multiplication factor versus burnup
Figure 2: The infinite multiplication factor versus burnup.
Figure 2 shows the infinite multiplication factor (kinf) of the LEU and MOX assemblies
versus burnup evaluated from 0GWd/t to 40GWd/t. In the LEU assembly, we can see in the burnup
range from 0 to 8GWd/t, kinf increases lightly from 1.147 to 1.155. After that, kinf decreases steadily
from 1.155 to 0.9. In the MOX assembly, kinf decreases from 1.159 to 0.895. The kinf of MOX fuel is
lower than that of the LEU. This is due to two reasons: (i) During the fuel burning 239
Pu in the
MOX produces more neutron absorbers than 235
U in the LEU, and (ii) 238
U in the LEU fuel can be
converted into fissile material 239
Pu. At the beginning of cycle, because MOX fuel produces more 135
Xe and 149
Sm than LEU fuel, the contribution of UGD rods in MOX assembly is not much as in
LEU assembly, so gradient of the kinf curve in MOX assembly is not high as in LEU assembly.
In Figure 2, the grey BM straight line is the benchmark mean value of kinf and the other ones
are kinf obtained based on three nuclear data libraries mentioned above. For the MOX fuel the kinf
values are very close to the benchmark mean value. For the LEU assembly, the library ENDF 7.0
gives the kinf value deviated 1.5% from the benchmark one, the JENDL 3.2 and JENDL 3.3give kinf
close to the benchmark in the range from 0GWd/t to 15GWd/t with a small deviation of 0.2%.
However, at the kinf values greater than 15GWd/t the deviation increases up to 1.5%. It can be
concluded that the deviation between the kinf coefficients obtained from the LEU and Benchmark is
greater than that obtained from the MOX and Benchmark, especially at the high burn-up values.
III.2. Nuclear densities versus burnup
Figure 3 shows nuclear densities of 235
U and 239
Pu versus burnup, where we can see:
- The appearance of 239
Pu in LEU fuel is caused by fuel conversion in fuel-burning
process and the appearance of 235
U in MOX fuel by contribution of UGD rods.
- In LEU assembly, the 235
U concentration at first burnup step is 2.5x10-
4atoms/barn*cm and then decreases to 5x10
-5atoms/barn*cm at the burnup 40GWd/t. The
239Pu
concentration increases dramatically at first burnup steps. This is the reason why kinf curve for LEU
fuel has one peak at 8GWd/t.
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
64
- In MOX fuel, the 235
U concentration decreases from 2.07x10-5
atoms/barn*cm at
0GWd/t to 6.45x10-5
atoms/barn*cm at 40GWd/t.
Figure 3: Nuclear densities of 235
U(left) and 239
Pu(right) versus burnup.
The 239
Pu concentration at beginning of the cycle is 2x10-4
atoms/barn*cm and then
decreases to 7x10-5
atoms/barn*cm at 40GWd/t. The 235
U and 239
Pu nuclear densities in LEU and
MOX assemblies calculated by three libraries are very similar to the benchmark mean values.
Figure 4 shows the 135
Xe and 149
Sm concentrations versus burnup plot. As known, two these
isotopes are reactor poisons, and the kinf value is affected by their products. The amount of 135
Xe
and 149
Sm increases rapidly at the first burnup steps. We can see, the 135
Xe and 149
Sm concentration
in the MOX fuel is much higher than in the LEU fuel because the yields of 135
Xe and 149
Sm from
thermal reaction of 239
Pu are higher than from 235
U.[3]
Table 2: Fission product yields (atoms per fission) from thermal fission*
In LEU fuel, the maximum 135
Xe concentration is 3.2x10-9
atoms/barn*cm at 5GWd/t and
then decreases to 2.7x10-9
atoms/barn*cm at 40GWd/t.
Figure 4: Poison density in fuel versus burnup
for two cases: 135
Xe (left) and 149
Sm (right).
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
65
In MOX assembly, the maximum 135
Xe concentration is 5.4x10-9
atoms/barn*cm at
1GWd/t and down to 3.4x10-9
atoms/barn*cm at 40GWd/t. The accumulated amount of 149
Sm
increases rapidly at first burnup steps and reaches a maximum value of 5x10-8
atoms/barn*cm at
5GWd/t. After that, 149
Sm density decreases to 4x10-8
atoms/barn*cm at 40GWd/t.
From Figure 4 we can see that result on 135
Xe and 149
Sm concentrations with three libraries
in LEU assembly are similar to the benchmark mean value at first burnup steps. However, the
deviations increase at high burnup values. The calculations using the library ENDF 7.0 gives the
most difference compared with the benchmark one, for example at burnup 40GWd/t the
corresponding deviations for135
Xe and 149
Sm are 5.82% and 5.94%. In MOX fuel, results with 3
libraries for 135
Xe concentration are higher 4% than benchmark mean value. The calculations
using the library ENDF 7.0 gives the most difference compared with the benchmark one, for
example at burnup 40GWd/t the corresponding deviations for 135
Xe 4.59% and for 149
Sm it’s very
close to the benchmark one.
Figure 5: Nuclear density versus burnup for 155
Gd (left) and 157
Gd (right).
Figure 5 presents the 155
Gd and 157
Gd nuclear densities versus burnup plot. The role of Gd in
fuel assemblies is to equalize reactivity at beginning of the cycle. In general, the Gd concentration
decreases dramatically to 0 when the burnup increases from 0GWd/t to 10GWd/t. For LEU
assembly the results for 155
Gd and 157
Gd concentrations with three libraries are similar to the
benchmark one. For MOX assembly, the corresponding results for 155
Gd concentration are higher
than benchmark one, where the ENDF 7.0 gives the greatest difference. For example, at 6GWd/t,
the corresponding deviation is 15.89%. The results for 157
Gd concentration are similar to
benchmark one in the burnup range from 0GWd/t to 6GWd/t. At high burnup steps157
Gd
concentrations are lower than benchmark, where the ENDF 7.0 gives the greatest difference,
4.76% at 8GWd/t.
III.3. Reactivity coefficients
a. Effect on Boron in moderator
The absorption effect by Boron is obtained in comparison between their activities at
Isothermal hot state with Boron (S3) and without Boron (S4). The value can be calculated by
theformular: (mk).The specific values in LEU and
MOX assemblies at 0, 20, 40GWd/t are presented in Table 3.
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
66
Table 3: Effect of Boron in moderator.
Fuel
Assembly Burnup (GWd/t)
BM EDF 7.0 JDL 3.2 JDL 3.3
Δρ Δρ Deviation Δρ Deviation Δρ Deviation
LEU
0 40.23 40.42 0.47% 40.31 0.21% 40.25 0.06%
20 43.44 43.69 0.56% 43.34 0.23% 43.13 0.72%
40 51.41 51.56 0.30% 51.00 0.80% 50.73 1.33%
MOX
0 23.20 23.10 0.42% 23.07 0.59% 22.79 1.77%
20 32.54 32.13 1.25% 31.94 1.83% 31.60 2.88%
40 42.64 41.45 2.79% 41.04 3.75% 40.71 4.54%
The BM in Table 2 is benchmark mean value, while the columns ENF 7.0, JDL 3.2 and JDL
3.3 show the results using libraries ENDF 7.0, JENDL 3.2 and JENDL 3.3.We can see in Isothermal
hot state without Boron, values are higher than in Isothermal hot state with Boron. At high
burnup steps, change in the reactivity coefficients is relatively big. This is because the Boron
concentration in moderator is kept at 0.6g/kg while the fuel reactivity decreases.
The Δρ values for LEU assembly are more much higher than in MOX assembly. This is due
to a fact that in the burning process the MOX fuel produces more neutron absorbers than LEU fuel.
For this reason, the absorption effect by Boron in MOX assembly is not strong as in LEU assembly.
Compared with the benchmark mean value, the results given by ENDF 7.0 are in good
consistence, where a minimum deviation is 0.3% and the maximum is 2.79%.The corresponding
deviations are higher in cases of the JENDL 3.2 and JENDL 3.3, the maximum deviations are
3.75% and 4.54% for JENDL 3.2 and JENDL 3.3, respectively.
b. Effect on fuel temperature
Effect on fuel temperature is obtained by the reactivity comparison between the Operating
state(S2) and Isothermal hot state(S3). The values can be calculated by theformular:
(mk).The specific values in LEU and MOX
assemblies at 0, 20, 40GWd/t are presented in Table 4.
Table 4: Effect of fuel temperature.
Fuel
Assembly Burnup (GWd/t)
BM EDF 7.0 JDL 3.2 JDL 3.3
Δρ Δρ Deviation Δρ Deviation Δρ Deviation
LEU
0 -9.86
-
10.52 6.71%
-
10.42 5.68%
-
10.46 6.06%
20
-
12.87
-
12.74 1.01%
-
12.46 3.16%
-
12.68 1.46%
40
-
15.63
-
14.97 4.24%
-
14.64 6.36%
-
14.85 5.00%
MOX 0
-
12.18
-
11.80 3.10%
-
11.68 4.11%
-
11.74 3.58%
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
67
20
-
13.84
-
13.76 0.58%
-
13.65 1.38%
-
13.68 1.18%
40
-
15.98
-
15.37 3.81%
-
15.16 5.11%
-
15.19 4.93%
In Table 4, when fuel temperature increases from 575K to 1027K, Δρ decreases from
9.86mk at 0GWd/t to 15.63mk at 40GWd/t in LEU assembly and from 12.18mk at 0GWd/t to
15.98mk at 40GWd/t in MOX assembly. Compared with the benchmark the library ENDF 7.0 gives
a greater deviation than two the other libraries. For the ENDF 7.0 the maximum deviation is 6.71%
and minimum is 0.58%, while for the JENDL 3.2 and JENDL 3.3 the maximum deviations are 6.36
and 6.06%, and the minimum ones are 1.38 and 1.18%, respectively.
c. Effect on Isothermal hot state.
Effect on Isothermal hot state is obtained by the reactivity comparison between the
Isothermal hot state without Boron (S4) and Cold State(S5). The values can be calculated by
the formular: : (mk). The specific in LEU and
MOX assemblies at 0, 20, 40GWd/t are presented in Table 5.
When the fuel and moderator temperatures increase the negative reactivity is quite high. In
LEU assembly the Δρ values increase from 41.73mk at 0GWd/t to 50.3mk at 40GWd/t. In MOX
assembly the Δρ increase from 47.96mk at 0GWd/t to 52.73mk at 40GWd/t.
Table 5: Effect on Isothermal hot state.
Fuel
Assembly Burnup (GWd/t)
BM EDF 7.0 JDL 3.2 JDL 3.3
Δρ Δρ Deviation Δρ Deviation Δρ Deviation
LEU
0
-
41.73
-
43.22 3.58%
-
42.01 0.68%
-
42.72 2.37%
20
-
47.92
-
48.78 1.80%
-
47.79 0.27%
-
47.43 1.03%
40 -50.3
-
50.99 1.38%
-
50.00 0.60%
-
48.80 2.98%
MOX
0
-
47.96
-
48.51 1.14%
-
48.62 1.38%
-
47.37 1.23%
20
-
54.28
-
54.44 0.30%
-
54.00 0.51%
-
52.34 3.58%
40
-
52.73
-
54.49 3.33%
-
53.45 1.36%
-
51.40 2.54%
Library JENDL 3.2 gives the results closest to the benchmark mean value, its maximum and
minimum deviation is, respectively, 1.38% and 0.27%. The ENDF 7.0 and JENDL 3.3 give the
results with higher deviations, typically maximum deviation of 3.58%.
VINATOM-AR 13--08
The Annual Report for 2013, VINATOM
68
IV. CONCLUSION
In this report, we presented the calculation results on the infinite multiplication factor (kinf),
nuclear densities of 235
U, 239
Pu, 135
Xe, 149
Sm, 155
Gd, 157
Gd; reactivity coefficients (Δρ) versus
burnup for LEU and MOX assemblies using three nuclear data libraries ENDF 7.0, JENDL 3.2 and
JENDL 3. All the obtained results were compared with the benchmark mean values.
The results on infinite multiplication factor, nuclear densities obtained from two libraries
JENDL 3.2 and JENDL 3.3 are closer to the benchmark than library ENDF 7.0. However, the
results on the reactivity coefficients by ENDF 7.0 is better than two the others libraries. Thus, we
can conclude on the advantage and disadvantage of each data library used in analyzing the
neutronic characteristics of VVER. As a result, the data selection depends on both physics and
calculation code.
REFERENCES
[1] NEA/NSC/DOC, “A VVER-1000 LEU and MOX Assembly Computational Benchmark.
Nuclear Energy Agency, Organization for Economic Co-operation and Development”,
10/2002.
[2] Keisuke Okumura, Teruhiko Kugo, Kunio Kaneko, Keichiro Tsuchihashi, “SRAC2006: A
Comprehensive Neutronics Calculation Code System”, 04/2007.
[3] M. E. Meek and B. F. Rider, “Compilation of Fission Product Yields,” General Electric
Company Report NEDO-12154, 1972.
[4] VVER-1000 MOX Core Computational Benchmark.
[5] NEA/NSC/DOC(2002)/6 : VVER-1000 Coolant Transient Benchmark, 2002.
[6] Nuclear fuel for VVER reactors, Fuel company of Rosatom.
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM 69
MODELING AND ANALYSIS OF THERMAL HYDRAULIC PHENOMENAFOR VVER-1000 REACTOR WHEN TRIP OUT OF ONE OR TWO MAIN
COOLANT PUMPS BY RELAP/SCDAPSIM CODE
Le Thi Thu, Pham Tuan Nam, Nguyen Thi Tu Oanh and Nguyen Huu TiepInstitute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 Hoang Quoc Viet, Nghia Do, Cau Giay, Ha Noi
ABSTRACT: RELAP5 - a thermal hydraulic system code - in recent years is used by many reseachers inVietnam for the reactor thermal-hydraulic analysis. In the other hand, VVER-1000 reactor is selected to be thenuclear reactor technology for the first nuclear power plant in Vietnam. So the studying on VVER-1000reactor is very important. The project’s purpose is modeling the thermal-hydraulic systems of VVER-1000reactor. The project also targets enhancement of experiences in using RELAP5/SCDAPSIM code andmodeling for components of VVER-1000 reactor in steady state and transient, including: steady state at 100%power, transient with switch off 1 or 2 main coolant pumps. The thermal hydraulic parameters were analysisedversus time. The thermal hydraulic parameters, such as: outlet pressure, coolant temperature, maximum fueltemperature, water level of pressurizer and steam generator, etc. were compared, analysed and assessed. Insteady state, the errors are less 10 per cent.
1. STRUCTURES AND PRINCIPLES OF VVER-1000 THERMAL HYDRAULICSYSTEMS
In this part, studied about the structures, principles of VVER-1000 thermal hydraulicsystems, including: reactor core, main coolant pump, steam generator, pressurizer.
Figure 1 illustrates the main components of VVER-1000 reactor.
Figure 1: Main components ofVVER-1000 reactor.
Project information:- Code: CS/13/04-02- Managerial Level: Institute- Allocated Fund: 50,000,000 VND- Implementation time: 12 months (Jan 2013- Dec 2013)- Contact email: [email protected] Paper published in related to the project: (None)
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM70
2. THERMAL HYDRAULIC AND GEOMETRY DATA OF THE MAINCOMPONENTS OF VVER-1000 REACTOR
In this part, collected thermal hydraulic and geometry data of VVER-1000/V392 design.Table 1 shows the main thermal hydraulic parameters of VVER-1000/V392. Table 2 shows themain geometry parameters of fuel assembly.
Table 1: The main thermal hydraulic parameters of VVER-1000/V392.
Parameters Value
1. Number of loops 42. Thermal power, MW 30003. Outlet pressure, MPa 15.74. Iutlet temperature, oC 2915. Outlet temperature, oC 3216. Core mass flow, m3/h 860007. Mass flow per a cold leg, m3/h 215008. Core mass flow when trip out of one main coolant pump, m3/h 637009. Core mass flow when trip out of two opposite main coolant pumps,m3/h
40000
10. Core mass flow when trip out of two adjacent main coolant pumps,m3/h
40800
11. Maximum linear power rate, W/cm 44812. Steam pressure at head of steam generator, MPa 6.2713. Steam temperature, oC 278.514. Steam mass flow rate/ SG, t/h 147015. Humidity not execced, % 0.216. Average burn up of fuel assembly, MWday/kgU 54.617. Maximum burn up of fuel assembly, MW ngày/kgU 56.918. By bass mass flow rate, % 319. Feedwater temperature at nominal power, oC 22020. Feedwater temperature at disconnect HPH and zero power, oC 16421. Feedwater temperature at disconnect HPH and nominal power, oC 18622. Core pressure drop, MPa 0.38723. Design parameters of primary system
- Pressure, MPa- Temperature, oC
17.64350
24. Design parameters of second system- Pressure, MPa- Temperature, oC
7.84300
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM 71
Table 2: The main geometry parameters of fuel assembly.
Parameter Value
1. Hight fuel assembly, mm 4570
2. Hight cold fuel assembly, mm:
- Bottom part of fuel
- Active fuel part
- Top part of fuel
281
3530
759
3. Number of fuel rod in a fuel assembly 312
4. Pitch distance, mm 12.75
5. Material of fuel UO2 andUO2+Gd2O3
6. Fuel mass of a fuel assembly, kg 505.4
7. Fuel density, kg/m3 (10.4 to 10.7) x103
8. Material of cladding Alloy110
9. Outside diameter of fuel pin, mm 7.6
10. Inside diameter of fuel pin, mm 1.2
11.Outside cladding diameter, mm 9.1
12. Inside cladding diameter, mm 7.73
13. Guide tube:- Number
- Material
- Total hight, mm
18
Alloy635
4222
14. Number of grid spacer 15
3. MODELING AND INPUT FILE BY RELAP/SCDAPSIMFigure 2 is the nodalization of VVER-1000 reactor in RELAP/SCDAPSIM. The
components are modeled, such as: Core, 4 main coolant pumps, 4 steam generators, pressurizer,main pipes, feed waters …
Input file included: hydrodynamics components, heat structers, trip and logic, reactorkenitics.
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM72
Figure 2: Nodalization of VVER-1000
Figure 2: Nodalization of VVER-1000 reactor
4. CALCULATION AND RESULTS ANALYSIS4.1. Steady stateThe calculation results show in table 3. This results are compared with the design data in the
steady state. The errors are less than 10 per cent. So this calculation results is good.
Table 3: Calculation at 100% power.
Parameter Calculationvalue Design value Error (%)
Thermal power 3000 MW 3000 0 %
Outlet pressure 15.7 MPa 15.7 0.3 MPa 0%
Inlet temperature 289.30 ºC 291 ºC 0.58 %
Outlet temperature 319.24 ºC 321 ºC 0.55 %
Core mass flux 83464 m3/h 86000 m3/h 2.95 %
Core pressure drop 0.3856 MPa 0.387 MPa 0.36 %
Feedwater temperature 220 ºC 220 ºC 0 %
Steam generator water level 2.51 m 2.7 m 7 %
Steam temperature 278 ºC 278.5 ºC 0.18 %
Pressurizer water level 8.194 m 8.17 m 0.29 %
Top pressurizer pressure 6.266 MPa 6.27 MPa 0.06 %
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM 73
4.2. TransientThe senarior is trip out of one main coolant pumps when the reactor was operating at 100%
power. The events is showed in table 4.
Table 4: The events of trip out of one main coolant pumps [1].
Time, s Event Setpoint for actuation
0.0 Trip out of one operating maincoolant pump sets
Initiating event
6.5 The first signal for reactor scram (isignored)
The event occurs when reactor poweris operating to exceed 75% power andone of main coolant pump sets trip outof.
17.1 The second signal for reactor scram
20.6 Start of EP control rods removement
25.6 Start of TG stop valves closing By the fact of reactor scram in 5 ssince the moment of setpoint reaching.The time of stop valves closing isassumed 0.6 s
32.0 Start of BRU-A opening in steamlines of SGs
Pressure in the steam lines exceed 7.2MPa
Control pressure is 6.67 MPa
3600.0 End of calculation
The calculation results is illustrated from figure 3 to figure 8.
Figure 3: Coastdown of main coolant pump.
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM74
Figure 4: Outlet pressure versus time.
Figure 5: Inlet and outlet temperature.
Figure 6: Head SG pressure.
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM 75
Figure 7: Water level of pressurizer.
Figure 8: % power and % mass flow rate change versus time.
The calculation results showed that the reactor was safety during occurring the transient. Infigure 8, it explain the outlet pressure and temperature changes.
Trip out of two main coolant pumps:The senarior was trip out of two main coolant pumps when the reactor was operating at
100% power. The events is showed in table 5.
Table 5: The events of trip out of one main coolant pumps [1].
Time, s Event Setpoint for actuation
0.0 Trip out of one operating maincoolant pump sets
Initiating event
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM76
6.5 The first signal for reactor scram (isignored)
The event occurs when reactor poweris operating to exceed 75% power andone of main coolant pump sets trip outof.
8.0 Start of EP control rods removement
13.0 Start of TG stop valves closing By the fact of reactor scram in 5 ssince the moment of setpoint reaching.The time of stop valves closing isassumed 0.6 s
22.5 Start of BRU-A opening in steamlines of SGs
Pressure in the steam lines exceed 7.2MPaControl pressure is 6.67 MPa
3600.0 End of calculation
The calculation results of this transient is illustrated from figure 9 to figure 14.
Figure 9: Coastdown of the main coolant pump.
Figure 10: Outlet pressure versus time.
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM 77
Figure 11: Inlet and outlet fluid temperature.
Figure 12: Head SG pressure. Figure 13: Water level of pressurizer.
Figure 14: % power and % mass flow rate change versus time.
The thermal hydraulic phenomena are the same with two transients, be only differencechanges versus time. The reactor was safety during occurring the transients (trip out of one or twomain coolant pumps).
VINATOM-AR 13--09
The Annual Report for 2013, VINATOM78
5. CONCLUSIONThe subject’s contents were studied the technology of VVER-1000 reactor and modeled the
thermal hydraulic systems of VVER-1000 in the steady state and the transients. The calculationresults compared the design data and analysised versus time. The limitation of the transientcalculations is not calculated MDNBR (Minimum Departure from Nucleate Boiling Ratio).Actually, MDNBR is one of the shutdown signals in the transient (trip out of one or two maincoolant pumps). Thus, the modeling should be validated and verified to get better results.
The studied contents were enhanced the experience of the working group. The productionsof the study are the final report and one paper. The name of the paper: thermal hydraulic analysis ofloss of flow accident in VVER-1000 reactor using RELAP5 code. This paper is preparing to presentat the national scientific conference of young staff in october 2014.
REFERENCES
[1] Risk engineering LTD. Training course "Introduction to NPP technology, Reliability, Safetyand management engineering and software development services.
[2] Rel-885-SG. Risk engineering LTD. Sofia, Bulgaria, 2012.[3] VVER-1000 Coolant Transient Benchmark. PHASE 1 (V1000CT-1) Vol. I: Main Coolant
Pump (MCP) switching On Final Specifications. Boyan Ivanov and Kostadin Ivanov NuclearEngineering Program, USA; Pavlin Groudev and Malinka Pavlova INRNE, Academy ofSciences, Bulgaria; Vasil Hadjiev Nuclear Power Plant Kozloduy, Bulgaria; US Departmentof Energy. NUCLEAR ENERGY AGENCY ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT.
[4] Nuclear Safety Analysis Division, Information Systems Laboratories, Inc.Rockville,Maryland Idaho Falls, Idaho. RELAP5/MOD3.3 CODE MANUAL VOLUME II:APPENDIX A INPUT REQUIREMENTS. January 2002.
[5] Nuclear Safety Analysis Division, Information Systems Laboratories, Inc. Rockville,Maryland Idaho Falls, Idaho. RELAP5/MOD3.3 CODE MANUAL VOLUME IV: MODELSAND CORRELATIONS. December 2001.
VINATOM-AR 13--10
The Annual Report for 2013, VINATOM
81
STUDY THE OPERATION OF SUB-SYSTEM FOR CYCLOTRON
KOTRON13 WITH THE PURPOSE OF OPERATION AND MAINTENANCE
OF THIS EQUIPMENT
Nguyen Tien Dung, Pham Minh Duc, Le Viet Phong, Vu Duy Truong and Nguyen Xuan Truong
Department of accelerator, Hanoi Irradiation Center, Vietnam Atomic Energy Institute
ABSTRACT: In the framework of bilateral collaboration between Ministry of Science and Technology Korea
and Vietnam, a new PET cyclotron center KOTRON13 has been installed at Vietnam Atomic Energy Institute
with the production of radio-isotope 18
F, 11
C,.. used for PET. The cyclotron center is also to be the training
laboratory of accelerator’s technology, radiochemistry, vacuum technique,.. for staffs of VAEI and students of
universities. The project “study the operation of sub-system for cyclotron center KOTRON13 with the purpose
of operation and maintenance this sub-system” is carrying out in order to understand the principle and
operation of it. The main subjects in 2013 are focused in 2 facts: The system for environment inside cyclotron
center such as temperature, humidity, air atmosphere, electric power supply,.. and operation of radiation
protection system. The system used for condition of environment is constructed following the guide from
cyclotron supplier SAMYUONG. The radiation protection system is designed and constructed following the
guide from IAEA. The result of project: to get training and practicing the operation of the sub-system for staffs
of KOTRON13 center. The report on safety of the radiation protection of KOTRON13 center is presented at
10th
Nuclear conference at Vungtau city in 2013.
DETAILS OF REPORT
The contents of project are focused in 2 facts: To understand the principle operation and
requirements of the sub-system for environment inside cyclotron center and the operation of
radiation protection system.
1. The principle operation and requirements of the sub-system for environment
The sub-system includes the chiller gauge, air-exhaust and air-conditioner system.
Samyuong chillers, included external cooling system and heat exchanger [4],.. is installed in
cyclotron room. The first part of Chiller, operated like the air-conditioner, decreases the temperature
of water tank to the range from 4 to 35oC. The second part, included heat exchanger and water
manifold, carry the cooling water from water tank to cyclotron in order to cool for many
components such as magnet coil, vacuum pump, target,... Air- exhaust system is constructed from
2 fan motors with the capacity of 5000 m3 per hour. The velocity of a fan motor is controlled by
inverter LS model SV055iG5A. The Air-exhaust system supplies fresh air for laboratories of the
center and keeps a negative air-pressure for cyclotron room, hot-cell and QA/QC room with the
preset value. Air conditioner system, made from DAIKIN company, is installed in each laboratory
room. The temperature inside the room is controlled from 18 to 25oC as the requirement from
SAMYUONG. After calculation the capacity for air-cooling system, 2 set of DAKIN with power
Project information:
- Code: 38/CS/HĐNV
- Managerial Level: Institute
- Allocated Fund: 50,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--10
The Annual Report for 2013, VINATOM
82
100,000 BTU are installed in cyclotron room, 1 set of 57,000 BTU is installed in hot-cell room,..
The result of the environment condition at rooms in cyclotron center is showed at following table.
Room Temp. range
(oC)
Deviation
(oC)
Humidity
(%)
Deviation
(%)
Cyclotron room 18~25 ± 3 < 60 5
Control room 18~25 ± 3 < 60 5
Hot cell room 18~25 ± 3 < 60 5
QC room 18~25 ±3 < 60 5
2. The operation of radiation protection system
The radiation protection system is designed and constructed following the guide from
IAEA[6]. It includes the radiation monitoring system and personal radiation dosimeter. When the
cyclotron operates, radiations emit from the following source: electromagnetic radiation emits from
accelerated proton, activated atom emits x-ray, activated nuclear emits gamma ray, stopping power
of electron emits the Bremsstrahlung X-ray and from nuclear reaction: 8O18
+ 1H1 9F
18 + 0n
1 .
Radioactivity from above nuclear reaction with proton 13 MeV, beam current 50 A emits a
thermal neutron with activity of about 106 particles per second [2]. In normal operation of
KOTRON13, gamma radiation dose rate inside cyclotron room is about 106 Sv/h.The radiation
detector has been designed and constructed at 9 positions inside the KOTRON13 center in order to
observe both gamma and neutron ray.
The radiation gamma and neutron are monitoring by the ADM606M station. This station
supports by the CANBERRA of “SMART” detectors for monitoring all type of radiation including
gamma and neutron. Standard communications protocol available at the serial ports is RS-485 ,
which is used for connecting with main computer in radiation protection room. The contact of
output relay from ADM606M, closed when dose rate in cyclotron room is over a limited level, is
connected with the interlock system. The data of radiation at the cyclotron center are recorded and
stored in the main computer.
The interlock system at the center, linked with radiation protection system, is designed by
handshake method. When the conditions of radiation protection is available, it permits cyclotron to
operate and to emit proton beam to target. When the cyclotron operates with radiation dose rate
inside cyclotron room over the limitation, the cyclotron door can not open in order to protect staffs
inside the cyclotron center.
With personal portable dose rate and survey meter for gamma and neutron, the equipment
RADIAGEM-2000 and PNM-200/S are used. With the RADIAGEM 2000, dose rate of gamma
radiation range from 0.01 µSv/h to 100 µSv/h. For neutron radiation, equipment PNM-200/S has
measurement range from 0.2 mrem/h to 20 rem/h with energy range of neutron from 2 keV to 15
MeV. For the hand, foot surface contamination monitor, equipment SIRIUS-5 is installed near the
output door of the cyclotron center. Both gamma and beta contamination from staff are monitoring
when they go out the KOTRON13 center.
3. Conclusion
The content of project concentrates in the 2 objects: The operation and requirement of sub-
system for environmental condition inside cyclotron center and operation of radiation protection
system. Both tasks are adapted the requirement from SAMYUONG and IAEA. The report on
safety of the radiation protection of KOTRON13 center is presented at 10th
Nuclear conference at
VINATOM-AR 13--10
The Annual Report for 2013, VINATOM
83
Vungtau city in 2013. The knowledge of sub-system operation is also helpful for staffs in the works
of the installation and maintenance of PET cyclotron center.
REFERENCES
[1] Y. S. Kim et. al., “New Design of the KIRAMS-13 cyclotron for regional cyclotron
center”; APAC’2004, Gyeongju, March 2004.
[2] Samyuong Unitech Co,. Ltd, “Site planning”.
[3] Reference manual of Canberra ADM606M Portable Multifunction Ratemeter/Scaler.
[4] Reference manual of Samyuong Chiller.
[5] Reference manual of Sirius-5™ - Hand, Cuff and Foot Surface Contamination
Monitor.
[6] IAEA technical report series number 465; Cyclotron produced radio-nuclides: Principles
and Practice.
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
84
APPLICATION OF PROMPT GAMMA NEUTRON ACTIVATION
ANALYSIS AT THE N0.2 HORIZONTAL CHANNEL OF THE DALAT
NUCLEAR RESEARCH REACTOR USING A COMPTON-SUPPRESSION
SPECTROMETER
Tran Tuan Anh, Nguyen Xuan Hai, Nguyen Canh Hai, Pham Ngoc Son,
Ho Huu Thang and Dang Lanh
Nuclear Physics and Electronics Dept., Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: A Compton-suppression spectrometer for Prompt Gamma Activation Analysis (PGNAA) has
recently been established. The thermal neutron flux was measured to be 1.03 ×106 n.cm
-2.s
-1 at the sample
position. The corresponding Cd-ratio for gold was found to be 230. The initial parameters for the Compton-
suppression system such as gains and energy cutoff were optimum. The gamma background reduces about 2
times in the Compton suppression mode in energy range below 1 MeV. The sensitivities, detection limits
(LOD) and concentrations for B, Al, Si, K, Ti, Gd, Sm, Cd, Ca, Na, Fe in geological samples and H, B, C, N,
Cl, K, Cd, Na in biological samples have been determined.
INTRODUCTION
The Prompt Gamma Neutron Activation Analysis (PGNAA) has been applied for analyzing
light elements as H, B, N, Si, K… in geological and biological materials on the thermal neutron
beam of N0. 4 horizontal channel, Dalat Research Reactor [1]. However, the detection limits of
those elements are still high due to neutron and gamma backgrounds at the channel. In 2011, a new
thermal neutron beam at the N0. 2 channel has been established and used for basic and applied
researches and training. The neutron flux of the beam is 1.03 x 106
n.cm-2
.s-1
and Cadmium ratio is
230. Besides, a new Compton-suppression spectrometer with HPGe-BGO detectors has been setup
at the beam for PGNAA [2].
The aims of the project are to establish optimal parameters for the Compton-suppression
spectrometer for qualitative analysis of various materials such as geological, biological,
environmental samples using PGNAA method.
I. EXPERIMENTS
I.1 Sample preparations
Accurate determination of traces of Boron is important for various specific requirements in
fields such as the geochemical, cosmochemical, agricultural and material sciences and more
importantly in the study of reactor materials. In order to establish a relationship between count rates
(cps) of prompt gamma ray of 478keV (10
B) and amount of B which varied from 5 µg to 50 µg. The
samples were prepared from the standard B solution (H3BO3) diluted on filter papers and heated at
Project information:
- Code: 16/CS/HĐNV
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
85
temperature of 600C and then wrapped and heat sealed in polyethylene films. For determinations of
LOD and concentrations of B, Al, Si, K, Ti, Gd, Sm, Cd, Ca, Na, Fe in geological samples and H,
B, C, N, Cl, K, Cd, Na in biological samples, 08 reference materials were chosen as follows: NIST-
2711a (Montana soil), NIST-278a (Obsidian rock), IAEA SOIL-7 (Soil), NIST-679 (Brick clay),
IAEA SL-1 (Lake sediment), NBS-1633a (Coal Fly Ash), BCR-281(Rye grass) and NBS-1577a
(Bovine liver). The samples were also heated at 120oC during 3 hours and at 45
oC during 48 hours
for geological and biological samples, respectively. The sizes of the samples were 1.5 x 1.5 cm2
corresponding to amounts of 1 - 1.5g
I.2 Experimental arrangement
The PGNAA system was placed at the thermal neutron beam of the N0.2 channel, Dalat
Research Reactor. The neutron flux of the beam was 1.03 x 106
n.cm-2
.s-1
and Cadmium ratio is 230.
The Ge detector is set with its axis perpendicular to the neutron beam at a distance of 39.5cm from
the sample position. The Compton suppression mode has been set up to obtain prompt gamma rays
by Genie 2000 software. The neutron beam guide, shielding system and block diagram of the
electronics for Compton suppression spectrometer are shown in Fig. 1 and Fig. 2.
Figure 1: The neutron beam guide, shielding system at the N0.2 neutron channel.
Figure 2: Block diagram of the electronics for Compton suppression spectrometer.
Neutron beam
Compton
suppression
spectrometer
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
86
II. RESULTS AND DISCUSSION
II.1 Analytical sensitivity and detection limit of Boron [3, 4]
05 standard samples of B were irradiated and the prompt gamma rays were measured for a
period of time to produce a statistically sufficient count. Analytical sensitivity and detection limit of
Boron were then determined from the slope of the calibration curve between count rates of 478 keV
peak (10
B) and amounts of Boron (Fig. 3). From the linear fitting curve, we determined the
analytical sensitivity and detection limit of Boron are 520 cps/mg and 1.21 g, respectively.
10 20 30 40 50
0
5
10
15
20
25
cp
s
g B
Exp data
Linear fitting
Model Line
Equation y = A + B*x
Reduced Chi-Sqr
0.0301
Adj. R-Square 0.99956
Value Standard Error
cps A -2.79 0.158620
cps B 0.520 0.00544162
Figure 3: Calibration curve of Boron at the thermal neutron beam.
II.2 Detection limit of elements in geological and biological materials [5]
The geological and biological materials have complex matrices because of various elements
in the sample. To determine detection limits of elements, reference materials are chosen for
experimental measurements. Prompt gamma rays spectra of NBS-1633a reference material in
Single and Compton suppression modes were shown in Figure 4.
Figure 4: Prompt gamma ray spectra of the Coal Fly Ash.
Single
Compton suppression
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
87
Detection limits of B, Gd, Sm, Cd, Ca, Al, Si, K, Ti, Na and Fe in geological, sediment,
environmental and biological samples are given in Table 1 and Table 2.
Table 1: Detection limits of elements.
# Element E
(keV)
Geological
sample Sediment Coal Fly Ash
1 B (g/g) 478 1.1 - 1.8 - 1.89
2 Gd (g/g) 182 2.0 - 6.4 1.35 2.56
3 Sm (g/g) 334 1.3 - 3.6 0.91 2.22
4 Cd (g/g) 559 1.8 - 5.8 0.01 0.29
5 Ca (%) 1942 0.1 - 4.5 0.19 2.35
6 Al (%) 1778 0.2 - 0.8 0.21 1.90
7 Si (%) 3539 1.2- 6.7 - 4.16
8 K (%) 771 0.2 - 1.7 0.17 0.68
9 Ti (%) 1381 0.04 - 0.1 0.04 0.11
10 Na (%) 472 0.01 - 0.03 0.01 0.03
11 Fe (%) 352 0.5 - 2.3 0.94 3.26
Table 2: Detection limits of elements in biological samples.
# Element E (keV) Rye Grass Bovine liver
1 B (g/g) 478 2.4 1.44
2 Cd (g/g) 559 0.05 0.17
3 Cl (g/g) 1165 - 0.12
4 K (%) 771 5.9 1.5
5 N 1885 - 33.2
6 Na (%) 472 - 0.9
- Detection limits of B, Gd, Sm, Cd are 0.1-5 µg/g and Ca, Al, Si, K, Ti, Na, Fe are 0.1-
7% in geological samples.
- Detection limits of B, Cd, Cl are 0.1-3 µg/g and K, N, Na are 0.1-35% in biological
samples.
II.3 Concentration of elements in geological and biological materials [6].
Concentrations of elements in analytical samples were determined by comparing to
concentrations of the reference samples in the same measured conditions. The results of
concentrations of elements in in geological and biological reference materials are given in Table 3
and Table 4.
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
88
Table 3: Concentrations of elements in a soil sample.
# Element
NIST-2711a (Montana soil)
Measured
value Reference value
U-score
(z-score)
1 B (g/g) 50.5 ± 3.0 50 (0.09)
2 Gd (g/g) 7.6 ± 3.3 5 (5.18)
3 Sm (g/g) 6.96 ± 1.07 5.93 ± 0.28 0.49
4 Ca (%) 2.43 ± 0.59 2.42 ± 0.06 0.01
5 Al (%) 7.1 ± 0.3 6.72 ± 0.06 1.24
6 Si (%) 31.7 ± 3.9 31.4 ± 0.7 0.06
7 K (%) 2.39 ± 0.3 2.53 ± 0.1 0.48
8 Ti (%) 0.29 ± 0.06 0.32 ± 0.01 0.49
9 Na (%) 2.0 ± 0.5 1.2 ± 0.01 1.71
10 Fe (%) 3.01 ± 0.35 2.82 ± 0.04 0.54
Table 4: Concentrations of elements in a grass sample.
# Element
BCR-281 (Rye grass)
Measured
value
Reference
value
U-score
(z-score)
1 B (g/g) 5.66 ± 0.64 5.64 ± 0.56 0.02
2 C (g/g) 58.0 ± 9.3 - -
3 N (g/g) 41.3 ± 25 33.2 ± 0.5 0.32
4 Cl (g/g) 0.55 ± 0.07 -
5 K (%) 31.4 ± 7.6 33 (0.48)
6 Cd (%) 0.31 ± 0.05 0.12 (15.8)
7 Na (%) 0.21 ± 0.1 - -
In this work, 10 elements of B, Gd, Sm, Ca, Al, Si, K, Ti, Na, Fe and 07 elements of B, C,
N, Cl, K, Cd, Na in geological and biological samples have been determined of concentrations by
using a comparison method. The obtained values are in quite agreement with reference values in
acceptable uncertainty from 1-20%.
III. CONCLUSIONS
The project has carried out following tasks:
- General introduction of principle, method and equipment for PGNAA including thermal
neutron beam, Compton suppression spectrometer, analytical sensitivity, detection limit and
concentration.
VINATOM-AR 13--11
The Annual Report for 2013, VINATOM
89
- Determination of detection limits and concentrations of B, Gd, Sm, Cd, Ca, Al, Si, K,
Ti, Na, Fe and B, Cd, Cl, K, N, Na in geological and biological reference materials.
- Establishment of analytical procedures for B, Gd, Sm, Cd, Ca, Al, Si, K, Ti, Na, Fe and
B, Cd, Cl, K, N, Na in geological and biological materials.
The obtained results of this work are improved that the Compton suppression spectrometer
established at the horizontal channel N0.2 of the Dalat Research Reactor has been applied for multi
element analysis, particularly for B and Si. It is expected that with the development of K0-PGNAA
method in the immediate future, the utilization of the thermal neutron beam in elemental analysis by
PGAA will certainly be more promising.
REFERENCES
[1] Nguyễn Cảnh Hải. Xây dựng quy trình phân tích định lượng các nguyên tố B, H, N, S, C, P,
Si, Cd, Gd trong mẫu đất đá và mẫu sinh học sử dụng thiết bị phân tích kích hoạt nơtron
gamma tức thời (PGNAA) mới được nâng cấp tại Lò phản ứng hạt nhân Đà Lạt. Đề tài
KHCN cấp cơ sở, 2005.
[2] Phạm Ngọc Sơn. Báo cáo tổng kết đề tài nghiên cứu khoa học cấp bộ-năm 2009-2011: Phát
triển dòng nơtron phin lọc trên kênh ngang số 2 của Lò phản ứng hạt nhân Đà Lạt. Mã số:
ĐT.08/09/NLNT, Viện Nghiên cứu hạt nhân Đà Lạt, 2012.
[3] C. YONEZAWA. Development of a neutron capture prompt gamma-ray analysis system and
basic studies of element analysis using this system. JEARI-memo 09-030, 1997.
[4] S. Baechler et al. Prompt gamma-ray activation analysis for determination of boron in
aqueous solutions. Nucl. Instrum. Methods A 488, pp. 410-418, 2002.
[5] D. A. Gedcke, How counting statistics controls detection limits and peak precision, AN59
Application Note, ORTEC.
[6] Quality aspects of research reactor operations for instrument neutron activation analysis.
IAEA-TECHDOC-1218, 2001.
VINATOM-AR 13--12
The Annual Report for 2013, VINATOM
90
RESEARCH AND PRODUCTION OF CALORIMETER FOR MEASURING
IRRADIATION DOSES ON 10MeV ELECTRON BEAM ACCELERATOR
Cao Van Chung, Nguyen Hoang Hai, Nguyen Anh Tuan and Tran Van Hung
Research and Development Center for Radiation Technology,
Vietnam Atomic Energy Institute
ABSTRACT: Calorimeter, used in measuring dose irradiated by 10MeV electron beam, was researched and
produced at VINAGAMMA. Tri-dimensional of Polystyrene disc was determined, a cylinder with 136 mm in
wide and 18 mm in thick, the same size as descripted in ISO/ASTM 51631-2003(E). Dose distribution inside
polystyrene structure versus radius and thickness were estimated. Correction factor for calorimeter produced is
0.02; the different compared with transfer calorimeter from Gex Corp. is less than 3%.
1. OBJECTIVES
- Tri-dimensional of Polystyrene disc.
- Calorimeter.
2. APPROACH
MCNP code [2] is used for evaluating dose distribution inside polystyrene disc (PD) with
various sizes in thickness and radius. The thickness and radius of PD are chosen base on depth dose
profiles and radius dose profiles.
3. RESULTS
Calorimeter determine absorption dose by the head product in irradiation processing, the
head created in side PD proportion with irradiation dose. The shape of PD directly effect to the
result measure by calorimeter. MCNP code was used for calculating dose distribution inside many
shapes of PD.
3.1 Thickness of PD
Dose distributions in polystyrene cylinder with various thicknesses were calculated (Table 1,
Figure 1). The thickness of PD normally is one third of mean free path of electron (~5 cm in water)
is 1.8 cm. With this thickness, average dose of PD is 1.17 of surface dose.
Table 1: Average dose in various thickness of PD.
Thickness of PD (mm) Average dose (kGy)
0.3 1.0915 0.001
Project information:
- Code: CS/13/07-05
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--12
The Annual Report for 2013, VINATOM
91
0
0.2
0.4
0.6
0.8
1
1.2
1.4
1.6
0 10 20 30 40 50 60 70
mm
kG
y
0.6 1.1097 0.001
1.3 1.1307 0.001
2.5 1.1577 0.001
5 1.1916 0.001
10 1.2329 0.002
18 1.2814 0.002
30 1.3653 0.003
40 1.4042 0.003
50 1.2688 0.004
60 1.0609 0.003
Figure 1: Average dose in PD with thickness from 0.3 mm to 60 mm.
PD in thickness 18 mm has the correct factor of 1.17.
3.2 Radius of PD
Table 2: Average dose in radius in 18 mm thickness PD with various radius.
Radius (mm) Average dose (kGy)
200 1.2882 0.001
130 1.2814 0.003
69 1.2692 0.003
34.5 1.2522 0.002
17.25 1.2095 0.004
8.625 1.1349 0.006
VINATOM-AR 13--12
The Annual Report for 2013, VINATOM
92
1
1.05
1.1
1.15
1.2
1.25
1.3
1.35
0 50 100 150 200 250 300 350 400 450
mm
kG
y
Figure 2: Average dose in various diameter of PD.
Figure 2 show that, with radius larger than 69 mm, bound effect is un-significantly to the
average dose.
3.3 Produce calorimeter
With tri-dimension of PD determined above, the PD was produced form polystyrene on
Toyoseiky machine at 2200C of temperature, 30 minutes and pressure of 5 kg/cm
3. Produced PD
has 1.06 in density.
Figure 3: Produce PD.
3.4 Thermistor
Measuring temperature in PD, a thermistor has proper of 2,000 ohm at 250C is used
(MCD_2K7MCD1 [3]). This thermistor then placed at 20 mm from edge of PD.
VINATOM-AR 13--12
The Annual Report for 2013, VINATOM
93
Figure 4: Structure of MCD_2K7MCD1.
A completed calorimeter is showed in Figure 5.
Figure 5: A completed calorimeter.
3.5 Determined dose via variation of temperature in calorimeter
The temperature of PD increases during irradiation process, the heat producing inside PD
proportion with the dose by the equation 1.
D = T. K (1)
where T is the heat produced in irradiation process (T = f(R1) – f(R2); K is specific heat of
polystyrene and the unit for the dose D is kGy.
In (1), a part of energy produce chemical reaction is not including; with the material as
polystyrene, this part is smaller then the other so should be skipped.
The temperature increasing is measured by resistant of thermistor. The relation between
temperature and resistant are showed in equation (2).
310
ARLn
BRft
(2)
Constants A = 5.204, B = 4291.77 and unit for temperature t is 0C.
Some time, the specific heat is a constant factor, but in this application the temperature in
equation (3) affected [4].
20108.0022.1.0108.0022.1 21 TT
TK
(3)
A foam box always protects the PD, but these are small part of heat exchange between PD
and environment, this approximate about 0.02 degrees in Celsius.
VINATOM-AR 13--12
The Annual Report for 2013, VINATOM
94
For all, dose calculate equation now can be rewrite as:
D = K [f(R1) – f(R2) – Ta] (4)
Calorimeter produced has good agreement with calorimeter supplied by Gex.Co, an expert
company in calorimetric supplier, in practices on 10 MeV electron accelerators.
Table 3: Dose measured by Gex calorimeter and produced in this article.
Taget dose
(kGy)
Gex’s calorimeter
(kGy)
Produced
calorimeter (kGy)
Diffirent
(%)
Correct
factor
5 4.20 4.38 4.2 0.02
10 9.75 9.80 0.5 0.0025
15 15.50 15.42 0.5 0.0025
20 20.98 20.98 <0.1 0
25 25.75 25.73 <0.1 0
3.6 Dose measurement procedure
a. Measure resistant of thermistor by suitable digital multi-meter has measure current
lower then 100 A.
b. Make sure that PD is subterraneous in foam box.
c. Take calorimeter on conveyer to irradiation place.
d. Quickly measuring resistant of thermistor after irradiate.
e. Use the (1), (2), (3) equation to calculate the dose.
Calorimeter shout be used again, but make sure that the resistant of thermistor must lager
then 800
4. CONCLUSIONS
With the shape of cylinder with 138 mm in diameter and 18 mm in thickness of polystyrene
material; The calorimeter has good practice in dose measurement on 10 MeV electron accelerator.
The diffirence betwen produced calorimeter with a tranfer dosimeter is petty. The produced
calorimeter has life time more than 2.000 kGy, in some case, 4.000 kGy life time is accepted.
Totaly cost for proceduce a completed calorimeter is less then 50$, cheaper than 750$ for a foreign
calorimeter.
REFENCES
[1] ISO/ASTM 51631-2003 (E) Standard Practice for Use of Calorimetric Dosimetry Systems for
Electron Beam Dose Measurements and Routine Dosimeter Calibration.
[2] J.F.Briesmeister, MCNP-A General Monte Carlo N-Particle Transport Code Version 4C2,
Transport Methods Group, Los Alamos National Laboratory, 1997.
[3] Micro-BetaCHIP Thermistor Probe (MCD).
[4] RISO, HDRL-I-11 Manufacture and Calibration of polystyrene calorimeters.
VINATOM-AR 13--13
The Annual Report for 2013, VINATOM
95
RESEARCHING, BUILDING A SOFT-PROCESSOR AND ETHERNET
INTERFACE CIRCUIT USING EDK
Tuong Thi Thu Huong, Pham Ngoc Tuan, Truong Van Dat,
Dang Lanh and Chau Thi Nhu Quynh
Nuclear Physics and Electronics Dept., Nuclear Research Institute,
Vietnam Atomic Energy Institute
ABSTRACT: The processor is an indispensable component in the measurement and automatic control systems.
This report describes the fabrication of a soft-processor (32-bits, on-chip block RAM 64K, 50M clock, internal
and peripheral bus) for receiving, sending and processing of data Ethernet packets. This processor is fabricated
using the XPS component from EDK (Xilinx) software toolkit. After that, it is configured on the FPGA named
Spartan XC3S500E circuit. A firmware of a processor for controlling the interface between processor and
Ethernet port is written in C language and can play a role of a HOST (station) which has its own IP to connect
to Ethernet network. Besides, there are some needed parts as follows: an Ethernet interfacing controller chip, a
suitable cable providing a speed up to 100Mbs and an application program running under Window XP
environment written in LabView to communicate with soft-processor.
INTRODUCTION
Nowadays, FPGA (Field Programmable Gate Array) is a device which has generally been
used because its properties as follows: reconfigurability and high flexibility in design and
fabrication. Thank to the FPGA with the afore-mentioned properties, a generation of a specific
processor is playing a role as a hardware as well as a firmware for control of hardware components
created inside the FPGA.
The advantages of FPGA can reduce computational time and simplified designs. In the
framework of the topic, in order to communicate with Ethernet via soft-processor, the XPS (support
of C command set) can be used to generate hardware components and software (firmware) of the
soft-processor and an FPGA board named Xilinx Spartan XC3S500E.
I. REQUIREMENTS AND DUTIES OF TOPIC
The purpose of the project is to design and fabricate a soft processor (called microblaze)
which is able to communicate with Ethernet. This microblaze can be embedded into the FPGA by
using the supported XPS. The application program is running under Window XP environment
written in LabView language can link and receive/transmit information between PC and the soft-
processor.
As a result, a product created through the project is a transfer system including of:
The self-excuted application program running under PC, a modem and the soft-processor as
shown in Fig. 1.
Project information:
- Code: CS/13/01-03
- Managerial Level: Institute
- Allocated Fund: 65,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--13
The Annual Report for 2013, VINATOM
96
Figure 1: Data transfer system between soft-processor and PC via modem.
II. SUPPORTED TOOLKITS AND TECHNIQUES
1. Overview of the system
1.1. The fabrication of soft-processor
The diagram of fabrication of soft-processor is shown in Fig.2.
Figure 2: Steps to create and embed an FPGA soft-processor.
VINATOM-AR 13--13
The Annual Report for 2013, VINATOM
97
1. Peripherals: LMB, PLB, OPB, Ethernet, LEDs, RS232 created in *.MSS, *.mpd,
*.MHS file.
2. Creating the library related to the soft-processor and peripherals.
3. Compiling firmware file and C-function library (mb-GCC), *.OUT file created.
4. Creating the platform to have a core and netlists.
5. A collection of *.UCF, *.ED files, core and netlists, use of iMPACT for creating *.Bit
file, *.MCS file. Finally, the MCS file will be loaded into ROM for operating.
1.2. The create of application program on PC
The basic functions supported in LabVIEW TCP: open connection, read and write data via
Ethernet.
Figure 3: TCP connection, TCP write, TCP read.
2. System design
The Xilinx Spartan XC3S500E board is used because it contains an FPGA which is able to
embed the soft-processor, and also supports RJ45 Ethernet port. The design of system is divided
into two parts: hardware part is the 32-bit microprocessor while software part is a firmware. Both of
them are created by XPS from Xilinx Company.
2.1. Hardware design
The XPS has Wizard supporting users to design conveniently. In addition to creating a 32bit
soft-processor, 64K internal RAM, and more peripherals such as Ethernet, RS232, LEDs...
After that, connection of input/output port with peripherals (*.UCF file), producing address
automatically, generating library functions relating to microprocessor software and peripherals.
VINATOM-AR 13--13
The Annual Report for 2013, VINATOM
98
Figure 4: Bus Interface of soft-processor.
2.2. Software design (firmware)
The libraries created in hardware design can be used for the software (firmware). With
support functions such as read/write registers, cache....TCP/IP protocol is used for connection and
data transfer. The firmware received and performed a TCP packet from PC and then created a
require packet. This packet was sent to PC via Ethernet.
3. Setup and verify the characteristics
In the project, the components including FPGA named XC3S500E, 50MHz internal clock,
LAN83C185 Ethernet chip, 8 LEDS display, RS232 port, Platform Flash PROM (configure the
FPGA and program the soft-processor), 10/100 Mbs Ethernet port, USB for JTAG, MAC address is
Xilinx_02:22:5E (00:0A:35:02:22:5E) were used.
MAC address of the computer is HonHaiPr_59:0B:A3 (94:39:E5:59:0B:A3), IP is
192.168.1.105, PORT is 3363.
Wireshark software was used to capture all packets going through the computer network
card as shown in Fig.5.
Figure 5: Connected, transmited, received frames captured in Wireshark.
VINATOM-AR 13--13
The Annual Report for 2013, VINATOM
99
III . CONCLUSION
The project has successfully designed and fabricated nuclear instruments based on soft-
processor including software and hardware. The advantages of this approach are as follows:
- Economics: less hardware devices, small chip, small size of ROM.
- Flexibility: design of 8, 16, 32, 64 bits microcontroller, depending on demands, creating
arbitrary RAM only changed the parameters on software, connecting with expected peripherals
easily.
- Convenience: embedded directly into the FPGA and reusable.
- Compact: all components intergrated inside FPGA.
The project has also succeeded in firmware design for TCP/IP protocol transfer data via
Ethernet. The obtained results will help remote measurement systems transfer data conveniently.
REFERENCES
[1] Xilinx, MicroBlaze Processor Reference Guide, Embedded Development Kit EDK 10.1i.
[2] Xilinx, XPS Ethernet Lite Media Access Controller.
[3] Transmit Control Protocol, Internet Protocol version 4, Address Resolution Protocol, MAC
address, check sum, http://en.wikipedia.org/wiki/
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
100
A STUDY OF CHARACTERISTICS OF HELIUM-3 (HE-3)
PROPORTIONAL COUNTERS IN ORDER TO DESIGN ELECTRONIC
CIRCUITS FOR NEUTRON DETECTION
Vu Van Tien, Nguyen Van Sy, Nguyen Thi Bao My,
Nguyen Thi Thuy Mai and Ho Quang Tuan
Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 Hoang Quoc Viet, Cau Giay, Ha Noi
Project information:
- Code: CS/13/04-01
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
ABSTRACT: This study aims to research and develop function circuits, electronic blocks, programming
software for He-3 proportional counters using commonly in neutron detection. Results are compared with
those of a neutron dosimeter available in Institute for Nuclear Science and Technology (INST). Although the
method has been known for a long time on the world, it is newly used in VietNam. If the study is applied in
reality, neutron dosimeters will be manufactured with acceptable price, high quality, and easy maintenance
which are suitable with domestic demands. It contributes to nuclear safety and economy-society development.
I. INTRODUCTION
Currently, nuclear science and technology are growing rapidly due to demands of the life
and national economy. Promotion of nuclear energy has become a major policy of the government.
However, scientific researchers and nuclear engineers are in serious shortage of both quantity and
quality, especially in the nuclear equipment. In order to improve the capability to do and use
research as well as to approach step by step and to come to master nuclear technology, there should
be appropriate investments for nuclear research and training through specific topics, scientific
research and nuclear technology projects.
In the development of science and nuclear technology, researching, designing and
manufacturing equipment for nuclear detection, especially dosimeter devices are becoming an
urgent need in our country today.
Neutron radiation is particularly dangerous for the human body due to a coefficient of high
linear energy transfer (LET). Therefore safety problems for neutron need special attention. That is
why the need to conduct research relating to the implementation of the neutron as well as the
fabrication of devices recorded neurons, especially neutron dosimeters.
II. METHOD
1. Theoretical Foundations
Neutron is a uncharged particle which does not ionize atoms directly. Neutron is detected
indirectly through charged particles and photons produced by interaction with nucleus.
If we know the mechanism of neutron interaction, we can get information of neutron from
the reaction products. There are several types of interactions are used, including elastic scattering
and absorption of neutron.
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
101
Neutron detection is performed by using 3He or BF3 gas-filled counters and scintillation
detectors doped neutron absorption elements such as Boron, Li etc. Proton- recoil is detected by
counters contained hydrogen or methane. Activation method is also used to detect neutron.
The energy of neutrons (from thermal energy to several tens of MeV) is often detected
indirectly through the absorption reaction using the absorber materials with high cross sections such
as 3He,
6Li,
10B, and
235U. Each of these reacts by emission of high energy ionized particles,
the ionization track of which can be detected by a number of means. Commonly used reactions
include 3He (n, p)
3H,
6Li (n, α)
3H,
10B (n, α)
7Li and the fission of uranium. Since these materials
are most likely to react with thermal neutrons (i.e., neutrons that have slowed to equilibrium with
their surroundings), they are typically surrounded by moderating materials. This slowing down of
neutrons is known due to ionization energy losses in elastic scattering between neutron and light
nuclei such as proton, deuterium, or carbon.
In many neutron dosimeters, counters are usually surrounded by a large volume of
moderating materials to recorded fast neutron.
Neutrons can be detected using 3He filled gas proportional counters through
3He (n, p)
3H
reaction. A typical counter consists of a gas-filled tube with a high voltage applied across the anode
and cathode. A neutron passing through the tube will interact with a He-3 atom to produce tritium
(hydrogen-3) and a proton. The proton ionizes the surrounding gas atoms to create charges, which
in turn ionize other gas atoms in an avalanche-like multiplication process. The resulting charges are
collected as measurable electrical pulses with the amplitudes proportional to the neutron energy.
The pulses are compiled to form a pulse-height energy spectrum that serves as a "fingerprint" for
the identification and quantification of the neutrons and their energies. If incident neutron is a fast
neutron with energy of En, the energy of the fusion reaction is equal to En + Q, Q is sum of kinetic
energy of 3H and proton.
2. Electronics
In order to measure neutron dose, neutron dosimeter needs to be converted to the
corresponding neutron dose. This is a filter technique made detector response as a function of
energy. The filter will reduce detector’s efficiency, which is the most difficult in designing high
sensitive neutron dosimeters. In a common neutron dosimeter, neutron counter is set at the center of
a sphere of moderating materials made by many layers of different materials. The materials slow
down kinetic energy of neutron. Polyethylene is one of those materials.
Figure 1: Logic diagram for neutron detection.
High Voltage Power
Signal process
block
PC
microchip
He-3
n
n
n n
n
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
102
R13
2 2 M
R16
2 2 M
C14
10N/3KV
G N D
2
NUETRON DETECTOR TUBLE
G N D
C17
100PF/3KV
8
1
4
3
2
U4A
TL082
8
4
7
5
6
U4B
TL082
1 2 V
1 2 V
G N D
C15
1 0 0 N
C13
1 0 P F
R14
3 0 0 k
R17
1 K
R15
2 0 K
C18
2 0 N
G N D
C16
1 0 0 N
G N D
R20
2 0 K
R26
2 0 K
R21
1 0 K
C19
1 0 u F
G N D
C21
10UF
G N D
G N D
1 2 V
R18
3 0
1
B N C
G N D
G N D
1
2
3
4
5
6
7
8
U 5
LM311N
1 2 V
C20
1 0 0 N
R19
2 0 0
G N D
G N D
R23
1 0 K
1 2 V
R24
1 0 K
R25
1 0 K
C23
2 0 p F
3
1
2
R V 2
1 0 K
C22
1 0 0 N
G N D
R22
1 0 K
R27
1 0 K
1 2 V
G N D
1
2
3
U1A
CD4093BCN
5
6
4
U1B
CD4093BCN
8
9
1 0
U1C
CD4093BCN
1 2
1 3
1 1
U1D
CD4093BCN
8
3
2
4
1
U2A
LM393N
R 2
5 6 0 k
R 1
3 3 0 k
D 1
D
C 2
1 N
1 2 V
C 5
10UF
G N D
G N D
3
1
2
R V 1
2 5 0 K
R 5
2 0 k
R 7
1 M
C 8
1 0 0 N
G N D
C 9
1 0 N
R 9
1 M
G N D
R10
2 G
G N D
U 3
LM336
G N D
R 4
1 0 0 K
1 2 V
R 8
5K6
G N D
G N D
1
1
2
2
3
3
T R 1
TRF4
1 2 V
C 3
1 0 0 N
G N D
D 2
D D 3
D
D 4
D
C 4
10N/2KV
C 1
10N/2KV
G N D
C10
10N/2KV
G N D
C11
10N/2KV
C12
10N/2KV
G N D
G N D
R11
1 0 M
V R E F
R 6
2.2M
1 2 V
1 0 0 0 T
1 0 0 T
0 T
C 7
10N/2KV
C 6
10N/2KV
D 5
D
D 6
D
R12
1 0 M
R 3
1 0 0 k
T 1
C535
1 2 V
Q 1
D438
R30
1 0 k
RA0/AN0
2
RA1/AN1
3
RA2/AN2/VREF-
4
RA3/AN3/VREF+
5
RA4/T0CKI
6
RA5/AN4/SS
7
RB0/INT
2 1
R B 1
2 2
R B 2
2 3
RB3/PGM
2 4
R B 4
2 5
R B 5
2 6
RB6/PGC
2 7
RB7/PGD
2 8
RC0/T1OSO/T1CKI
1 1
R C 1
1 2
R C 2
1 3
R C 3
1 4
R C 4
1 5
RC5/SDO
1 6
RC6/TX/CK
1 7
RC7/RX/DT
1 8
VSS
8
VSS
1
9
MCLR/VPP
1
OSC1/CLKIN
9
OSC2/CLKOUT
1 0
V
D
D
2
0
U 4
PIC16F876-04/P
G N D
V C C
1 0 0 n F
C 8
1 0 u F
C 5
G N D
G N D
3 3 p F
C 6
3 3 p F
C 7
4MHz
U 3
*
8
9
1 0
U2C
CD4011BMN
R20
1 0 k
V C C
G N D
1
2
3
RS-1 G N D
V C CG N D
1 0 u F
C 4
S 2
1 K
R14
Res3
1 2
1 3
1 1
U2D
CD4011BMN
K 1
K 2
G N D
V C C
G N D
L C D 4
L C D 5
L C D 6
L C D 7
RS_LCD
EN_LCD
R16
3 k
G N D
D 4
1N4007
D 6
4 1 4 8
A
1
K
2
D 5
4 1 4 9
G N D
3
1
2
R V 2
1 0 k
C 9
1 0 0 N
G N D
G N D
V C C
R19
1 K
R18
1 K
DS2
L E D 1
DS3
L E D 1
V C C
R13
1 0 0 K
G N D
C 2
1 0 0 P F
5 6
4
U2B
CD4011BMN
1 2
3
U2A
CD4011BMN
1
2
3
4
5
6
7
8
9
1 0
JP4
L C D
S C
1
S E
2
T C
3
G N D
4
COMP
5
V D D
6
Ipk
7
D R
8
U 8
MC33063A
G N D
C40
2 N
G N D
R39
1 0 0 K
G N D
R35
1 0 0
R37
0.2
9 V
C37
4 7 0 u F
G N D
R34
1 0 0
R36
1 k
R38
1 k
G N D
B
C
E
Q 2
H1061
G N D
G N D 1
D11
D Schottky
D 8
D Schottky
D10
D Schottky
D 9
D Schottky
C35
CAP1
C36
CAP1
C38
CAP1
C39
CAP1
+ 1 2 V
-12V
G N D
T 3
Trans CT
R40
1 M
1 2 V
Figure 2: Schematic electronic diagram.
The high voltage can be adjusted from 0 VDC to 2000 VDC giving the current from 20 mA
to 30 mA.
The neutron is converted through the nuclear reaction 3He + n ->
3H + p into charged
particles tritium (3H) and proton which then ionizes the surrounding gas atoms to create charges.
The resulting charges are collected as measurable electrical pulses with the amplitudes proportional
to the neutron energy. The pulses are amplified and convert to TTL pulse. They are sent to
microchip and then to a PC for displaying and storage.
III. RESULTS
Detector He-3 is set at the center of a 2.5 inch diameter polyethylene sphere. Polyethylene
will efficiently slow down neutrons to energies that the detector can respond to.
Figure 3: Photograph of detector.
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
103
1. A survey of characteristics of the He-3 counter
Since we don’t have a standard neutron source at INST, we used a 252
Cf neutron sources
(belonging to RAS-80/89 project) and a source from “Coal ash analysis equipment using PGNAA
technique (PGNAA_Prompt Gamma Neutron Activation Analysis)” project.
Signals, recorded every minute, are averaged over 6 to 12 measurements. The computer will
automatically save the results and stop measurement in certain time.
Figure 4: Plan view of the dose measurement.
Table 1: Variation of counting rate against applied voltages for a 3He-gas counter.
High voltage (V) 800 900 950 1000 1050 1100 1150 1200 1250
Count/min 0 19 56 105 135 165 191 192 201
High voltage (V) 1300 1350 1400 1450 1500 1550 1600 1650 1700
Count/min 201 206 217 224 227 267 311 399 616
0
100
200
300
400
500
600
700
800 1000 1200 1400 1600 1800
252Cf neutron source
Coal ash
Figure 5: Plot of variation
of counting rate against
applied voltages for a 3He-
gas counter.
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
104
The counting rate quickly rises as the voltage is increased. After the quick rise, the counting
rate levels off. This range of voltages is termed the "plateau" region. Eventually, the voltage
becomes too high and we have continuous discharge. The threshold voltage is the voltage where the
plateau region begins. Proper operation is when the voltage is in the plateau region of the curve. For
best operation, the voltages are set from 1250 VDC to 1350 VDC.
2. Counting rate corresponding to dose ratio
We used NEUTRON MONITOR 2222A He-3 to measure dose ratio at 3 positions and
compare with the result of He-3 counter.
2 µSv/h 6 µSv/h 12.5 µSv/h
Figure 6: Plan view of 3 positions in the measurement
of counting rate corresponding to dose ratio.
Table 2: Counting rate against neutron dose ratio.
Dose µSv/h Count/min
2 89
6 287
12.5 620
Figure 7: Plot of counting rate against neutron dose ratio.
R2 is equal to 0.9999. The figure shows a linear relation between counting rate and dose
ratio.
252Cf neutron source 252Cf neutron source
Coal ash Coal ash
252Cf neutron source
Coal ash
VINATOM-AR 13--14
The Annual Report for 2013, VINATOM
105
IV. CONCLUSION
The report presents a successful home-made electronics at INST for neutron detection. The
method that we had used to study neutron dose have been described. The results are in agreement
with expectation.
REFERENCE
[1] Trần Tuấn Anh. Phát triển phương pháp đo tiết diện nơtron toàn phần sử dụng ống đếm He-3
trên các dòng nơtron phin lọc lò phản ứng hạt nhân Đà Lạt, đề tài 2007.
[2] Nguyễn Văn Hùng. Nghiên cứu, thiết kế và chế tạo hệ thống thiết bị thực nghiệm để đo một
số đặc trưng vật lý neutron, phân tích kích hoạt và định liều neutron phục vụ công tác đào tạo
nhân lực hạt nhân, đề tài 2010-2011.
[3] Nguyễn Thanh Tuỳ. Nghiên cứu xây dựng hệ thiết bị phân tích sử dụng kỹ thuật PGNAA với
ống phát nơtron, đề tài 2009-2010.
[4] Nguyễn Triệu Tú. Ghi nhận và đo lượng bức xạ. (ĐHQG Hà Nội).
[5] http://quantumfireball3.blogspot.com/
[6] http://www.science.mcmaster.ca/medphys/images/files/courses/4R06/note9.pdf
[7] http://www.canberra.com/products/hp_radioprotection/pdf/Dineutron-SS-C38294.pdf
[8] http://www.parttec.com/docs/Helium3_alternatives_AAASBreakout_4-6-2010.pdf
VINATOM-AR 13--15
The Annual Report for 2013, VINATOM
109
CORROSION SURVEILLANCE IN PIPE BY COMPUTED RADIOGRAPHY
Nguyen The Man, Dao Duy Dung, Dang Thu Hong, Le Duc Thinh,
Ha Hong Thu and Nguyen Trong Nghia
Center for Non-Destructive Evaluation, Vietnam Atomic Energy Institute
Nguyen Tuan, Thanh Xuan, Ha Noi
ABSTRACT: “Computed radiography” (CR) is a technique of digital industrial radiology which is developed
to replace conventional radiography. With a CR system, the detection of the outer and inner wall surface of the
pipe is done usually by edge detection and filter algorithms of the profile line at the position under
investigation. Applying in industries, radiographic examination shall be performed in accordance with a
written procedure. This paper summarizes collected knowledge and experimental results to establish a
procedure for radiography applications in monitoring corrosion in small bore pipes.
Keywords: Radiography, corrosion, pipeline.
1. INTRODUCTION
In the oil, gas and chemical industries, corrosion is most common cause of piping failure.
Therefore, detection of corrosion has been a major problem for the oil, gas and chemical industries
for many years. Various NDT methods can be used such as ultrasonic testing, eddy current testing,
etc. But only profile radiographic testing is most suitable to examine insulated piping. Beginning
period of the subject, we study overview on corrosion, techniques for corrosion examination and
digital industrial radiology. After experimental performances, a CR procedure for corrosion
examination would be established. In the end of the subject, this procedure would be applied in
industrial service.
2. EXPERIMENTS
In Vietnam, CR-35 system of Durr manufacturer with laser scanner and white imaging
plates is used. It has basic spatial resolution at 50μm and normalized signal to noise ratio at 70.
Before application, three specimens of various diameters were tested by tangential projection
technique (see results in Table 2). After radiation exposure by radiation source, IP is read out by
scanner. Radiograph shows directly image of the pipe wall.
The corrosion evaluation in piping is based on the wall thickness measurement. So,
tangential radiographic projection technique is most suitable to use. Figure 1 shows the tangential
radiographic projection set-up.
Project information:
- Code: CS/13/09-01
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--15
The Annual Report for 2013, VINATOM
110
Figure 1: Tangential radiographic projection technique.
The arrangement 1(a) is applied for small pipes. For the larger pipes, arrangement 1(b)
should be used. Utilizing the tangential mode, the maximum penetrated wall thickness shall be used
to determine used radiation source. Table 1 shows Maximum paths through schedule 40, 80 & 160
pipes of various diameters
Table 1: Pipes of various diameters.
Nominal
Bore (inches)
Outside diameter,
OD (mm)
Schedule Wall thickness,
WT (mm)
Max Tangential
path (mm)
2 60.3
40 3.9 29.7
80 5.5 34.7
160 8.7 42.4
3 88.9
40 5.5 42.8
80 7.6 49.7
160 11.1 58.8
4 114.3
40 6.0 51.0
80 8.6 60.3
160 13.5 73.8
5 141.3
40 6.6 59.6
80 9.5 70.8
160 15.9 89.3
6 168.3 40 7.1 67.7
(b)
(a)
VINATOM-AR 13--15
The Annual Report for 2013, VINATOM
111
80 11.0 83.2
160 18.3 104.8
8 219.1
40 8.2 83.2
80 12.7 102.4
160 23.0 134.3
Figure 2: The profile of pipe.
With calibration of pixel size, the apparent wall thickness can be determined between inner
edge and outer edge of pipe wall image (see Figure 2). According to the geometrical set-up of the
tangential projection technique, the true wall thickness is:
w = w' x (f − R)/f
where: w’ is the apparent wall thickness,
R is the pipe radius (including insulation),
f is the Source-Film Distance (SFD).
Table 2: Results of experimental test.
Object Description Examination
description
Measured
value
Remark
Specimen P01
OD: 60.3 mm
WT: 2.77 mm
X-ray
- kV: 250
- mA: 1
SFD: 700mm
Laser Power: 6 mW
High Voltage: 650
RMP: 3000
Scanning
Resolution: 50 µm
2.63mm
Isulated pipe
VINATOM-AR 13--15
The Annual Report for 2013, VINATOM
112
Specimen P02
OD: 60.3 mm
WT: 2.77 mm
Se-75, 30Ci
SFD = 700 mm
Laser Power: 6 mW
High Voltage: 650
RMP: 3000
Scanning
Resolution: 25 µm
2.71mm
Specimen P03
OD: 60.3 mm
WT: 5.54 mm
Ir-192, 40Ci
SFD = 700 mm
Laser Power: 6 mW
High Voltage: 650
RMP: 3000
Scanning
Resolution: 50 µm
5.50 mm
3. CR PROCEDURE FOR CORROSION EXAMINATION
The most important part of the subject is written procedure. We have established a
procedure which defines the conditions of performing the computed radiographic examination for
corrosion in accordance with the ASTM 2007-00 Standard Guide for Computed Radiography,
ASME Boiler and Pressure Vessel Code for carbon Steel, Alloy Steel with type piping, vessel
nozzle with outside Diameter ≤ 2 inches. The procedure involves:
- Personnel: training qualification and certification requirement on digital industrial
radiology;
- Surface preparation;
- Backscattering radiation;
- System of identification: permanent identification on the radiograph traceable relating
contract/job, component, and No. of piping,…
- Equipment and materials: Radiation source, CR system and other;
- Viewing conditions, monitor, image processing and storage of digital radiographs;
- Calibration;
- Examination technique: Tangential radiographic projection technique and Double wall
radiographic projection technique;
- Locations marker;
- Use of IQIs: ASTM IQIs and duplex IQI;
- Evaluation;
- Documentation;
- Radiation safety.
VINATOM-AR 13--15
The Annual Report for 2013, VINATOM
113
4. EXAMINATION APPLICATION IN INDUSTRIAL SERVICE
Lan Tay platform and Nam Con Son Pipeline are units of petroleum industry in Viet Nam. It
supply gas a maximum 21 million cubic meters of gas a day for thermal power plants which are
responsible for around a third of the Vietnam’s power output. With time, piping system is degraded
by main reason of corrosion processes and Lan Tay platform and NCSP must be stopped to
maintenance and repair. It influences national electric output. Therefore, some process piping items
are examined in-service. 250 insulated piping were examined. One of examinations by CR is shown
in Figure 3.
Figure 3: Pipe corrosion examination by CR.
5. CONCLUSION
We have achieved positive initial result of CR application. Computed radiography was
accepted by customer as a suitable technique for corrosion evaluation piping of petroleum
processing facilities in Vietnam.
REFERENCES
[1] API 570, “Piping Inspection Code: Inspection, Repair, Alteration, and Rerating of In-Service
Piping Systems”-American Petroleum Institute.
[2] API RECOMMENDED PRACTICE 574 “Inspection Practices for Piping System
Components” -American Petroleum Institute.
[3] IAEA-TECDOC-1445 “Development of protocols for corrosion and deposits evaluation in
pipes by radiography”-IAEA, April 2005.
[4] “Radiographic Evaluation of Corrosion and Deposit: IAEA Coordinated Research Project on
Large Diameter Steel Pipes, Evaluation of Corrosion and Deposit by RT”-BAM, IAEA
(2004), 16th WCNDT Montreal, Sept. 2004.
[5] “Advances NDE Techniques and Reliability Engineering Assessments for Piping and Storage
Tanks in Refineries and Petrochemical Plants”-IIS, Italian institute of welding, 2005.
[6] “New Developments in Automated Inspection for Corrosion under Insulation” - The Welding
Institute, UK, 2006.
VINATOM-AR 13--16
The Annual Report for 2013, VINATOM
114
STUDY OF PREPARATION AND SURVEY OF RADIOISOTOPES TRACER
APPLICATIONS OF GOLD NANOPARTICLES IN THE MULTI-PHASE
INDUSTRIAL PROCESSES
Huynh Thai Kim Ngan, Trịnh Cong Son, Duong Thi Bich Chi, Tran Tri Hai, Nguyen Huu Quang,
Bui Trong Duy, Le Trong Nghia and Ngo Duc Tin
Centre for Applications of Nuclear Technique in Industry, Vietnam Atomic Energy Institute
No.1, DT 723 Street, Da Lat City, Lam Dong Province, Vietnam
ABSTRACT: Gold nanoparticles (AuNPs) were prepared by Turkevich and Brust method. The labeled gold in
liquids is the colloidal form with nano size particle of gold. This particles is of high dispersity in the liquid
phase that makes them a good physical tracer. The stability and disolve of AuNPs in solvents such as water,
toluene are hereafter discussed. The size of AuNPs was determined through UV-Visible spectroscopy (UV-
Vis) and transmission electron microscope (TEM).
Keywords: Gold nanoparticles, UV-Visible spectroscopy, transmission electron microscope.
I. INTRODUCTION
Nanotechnology is one of the fastest growing new areas in science and engineering. The
subject arises from the convergence of electronics, physics, chemistry, biology and materials
science to create new functional systems of nanoscale dimensions. Nanotechnology deals with
science and technology associated with dimensions in the range of 0.1 to 100 nm.
Two complementary approaches to nanomaterials are studied:
- The Top-Down approach - where one starts with the bulk material and machines his
way down to the nano-scale, and
- The Bottom-Up approach, starting at the molecular level and building up the material
through the small cluster level to the nanoparticle and the assembly of nanoparticles.
Gold nanoparticles present their color in the visible range of from wine red to blue or light
green. The color in terms of wave length is from 510 nm to 550 nm. The energy absorbed by the
gold particles is depended on the energy bands formed by each single particle. A single particle can
be considered as a quantum well which has various molecular orbitals (MOs). The energy gaps
between MOs in a nanoparticle will then be able to either adsorb or emit the energy from 1.0 to 1.7
eV. This feature helps to visually determine the size of gold nanoparticle.
In this study, gold nanoparticles (AuNPs) in water is created by reduction of HAuCl4 into
Au0, however the stabilizer is needed to control the particle size and avoid the precipitation. In
water phase citrate can be used for stabilization. For organics such as condensate, toluene, gold
nanoparticles is transferred from water phase by the transformer such TOAB (tetraoctylammonium
bromide) and reduced by NaBH4 (Sodium Borohydrate).
Project information:
- Code: CS/13/06-02
- Managerial Level: Institute
- Allocated Fund: 90,000,000 VND
- Implementation time: 12 months (May 2013 - Apr 2014)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--16
The Annual Report for 2013, VINATOM
115
The characteristic of AuNPs in water and in toluene are studied such as: distribution in
solution and in multiphase (water/toluene), stability in ambient or high temperature. Besides,
AuNPs is created by HAuCl4 labled Au-198 and their characteristic is disscused.
II. RESULTS AND DISCUSSION
1. Preparation of AuNPs in water
Figure 1: TEM and UV-vis spectrometry of AuNPs in water
50ml of a solution HAuCl4 0.57mM in distiled water is placed in round botom and
connected with condenser, stirred by magnetic stirrer and heated by oil. When the solution boil,
4ml of a TSC 0.1M. The reation as follows:
3(H2CCOOH)2C(OH)COO- + 2AuCl4
- 3(H2CCOOH)2C=O + 2Au + 8Cl
- + 3CO2 +
3H+
TEM photograph showing the AuNPs uniform in shape and size, average diameter is
14.34±2.37nm.
2. Preparation of AuNPs in toluene
20ml of Tetraoctylammonium bromide (TOAB) 5,04 mM in toluene is placed in 100ml
erlenmeyer, then add 7.25 ml of 3.7mM HAuCl4, stir the solution (using magnetic stirrer at No. 6)
in 10 minutes at ambient temperature until the water solution from yellow to colorless, then take the
organic phase. Then drop 0,04 M NaBH4 into the organic solution, it takes them about 15 minutes
for the entire solution turns dark red. Shortly thereafter, maintaining stirring speed and drip 3ml of
dodecanethiol (DT) 17,9 mM in 15 minutes intervals. After the 15-minute period, the vial is
removed from the stirrer and stored in ambient temperature. The size and wathlenge of AuNPs is
measured by UV-Vis and TEM.
VINATOM-AR 13--16
The Annual Report for 2013, VINATOM
116
Figure 2: TEM and UV-vis spectrometry of AuNPs in toluene.
TEM photograph showing the AuNPs uniform in shape and size, average diameter is
4,59±1,43nm.
3. Preparation of AuNPs labeling Au-198 on water and organics
The labeled gold in liquids is the colloidal form with nano size particle of gold. This
particles is of high dispersity in the liquid phase that makes them a good physical tracer.
Au is known as the metal with isotope Au-198 emmitting gamma is very common tracer due
to not absorption, chemical reaction with material and fluids. Au-198 is produced by neutron
activation of Au-197 which is of 99.6% in abundance, in the nuclear reactor. Au is weighed in the
polyethylene ampoule to charge into the reactor.
The neutron activation equation for estimation of irradiation time, weight of Au is
introduced as following:
)1.(.. .teNA
where:
A: activity, Bq
thermal neutron flux, n/cm2.s
thermal neutron cross section, cm2
N: target nuclides, atom/cm3
AvoNM
mN ..
m: sample weight, g
M: atomic mass, g
isotope abundance
0
5
10
15
20
25
2,30 3,25 3,97 4,59 5,13 5,62 6,06 6,48 6,88
Fre
qu
en
cy, %
Diameter, nm
VINATOM-AR 13--16
The Annual Report for 2013, VINATOM
117
NAvo: Avogadro Number = 6.023 x 1023
decay constant, s-1
, 2/1
)2ln(
T
t: irradiation time, s
T ½ : decaying time, s
Table 1: Parameters of irradiation Au in Đà Lạt reactor
Reaction Cross section
(barn)
T ½
Weight of
sample
Irradiation
time, min
Activity
(mCi)
197Au(n,γ)
198Au 98 2.7day 20mg 15 0.78
Radioactive material is then transferred in the calibration cylinder for calibration of activity
using detector BGO 3’x3”, MCA Digidart and simulation by MCNP code.
Ashing Au-198 by aqua regia to make HAuCl4 as following:
Au + 3HCl +HNO3 → HAuCl4 +NO2+ H2O
Then preparation of AuNPs labeling Au-198 on water and toluene by procedure as above.
4. Test of characteristic of AuNPs
Distribution of retention time of AuNPs on glass and metal is performed by AuNPs labeling
Au-198.
Figure 3: Distribution of retention time of AuNPs on glass.
Table 2: Recovery of AuNPs on glass
No Sample name Recovery, %
1 AuNPs W1 75.40
2 AuNPs W2 90.48
3 AuNPs T1 83.45
4 AuNPs T2 85.90
VINATOM-AR 13--16
The Annual Report for 2013, VINATOM
118
Table 3: Rate of absorption of AuNPs on metal from time to time
ample name Rate of absorption , %/cm2/h
AuNPs W1 0.0044
AuNPs W2 0.0025
AuNPs T1 0.0039
AuNPs T2 0.0033
III. CONCLUSION
In summary, the Project “Study of preparation and surveying of usability gold
nanoparticles serving applications of radioisotopes tracer in the multi-phase industrial processes
” was performanced from 4/2013 to 4/2014, have achieved the target set, the completion of research
content as follows:
Gold nanoparticles (AuNPs) were prepared by Turkevich and Brust method (uniform in
shape and size, average diameter is 14.34±2.37nm and 4.59±1.43nm, respectively).
This particles is of high dispersity in the liquid phase that makes them a good physical
tracer. The stability and dissolve of AuNPs in solvents such as water, toluene are tested.
However, the results obtained from this study are preliminary in development of multiphase
tracing technology. It is the need to improve in professional and industrial quality to meet the
production requirement actually.
REFERENCES
[1] Jessica Winter, Gold nanoparticles biosensor, 2007.
[2] Thi Ha Lien Nghiem, Thi Huyen La, Xuan Hoa Vu, Viet Ha Chu, Thanh Hai Nguyen,
Quang Tuan Le, Emmanuel Fort, Quang Hoa Do, And Hong Nhung Tran. Synthesis,
Capping And Binding Of Colloidal Gold Nanoparticles To Proteins, ADVANCES IN
NATURAL SCIENCES: NANOSCIENCE AND NANOTECHNOLOGY 1 025009 (5p.),
2010.
[3] Alivisatos AP, Semiconductor Clusters, Nanocrystals, and Quantum Dots, Science, 271, pp.
933-937, 1996.
[4] M. Brust, M. Walker, D. Bethell, D. J. Schiffrin, R. Whyman, Synthesis of Thiol-derivatised
Gold Nanoparticles in a Two-phase Liquid-Liquid System, Chem. Commun, 801, 1994.
[5] D. Kim et. al., Nanotechnology, 17, 4019, 2006.
[6] Kottmann, J.P. Martin, O. J. F. Smith, D. R. Schultz, B, Physical Review, 64, 2001, pp. 402.
[7] M. Kowshik et. al., Nanotechnology, 14, 95, 2003.
[8] Kress-Rogers, E. Phil, Handbook of biosensors and electronic noses. Medicine, food and the
environment, pp. 149-168.
[9] F. Mafune et. al, J. Phys. Chem, 14, 8333, 2000.
[10] M.N. Martin, J.I. Basham, P. Chando, S.K. Eah, Charged gold nanoparticles in non-polar
solvents: 10-min synthesis and 2D self-assembly, Langmuir 26, 2010, pp. 7410.
[11] Murday, J. S. AMPTIAC Newsletter, 6, 5, 2002.
[12] S.D. Perrault, W.C.W. Chan, J. Am. Chem. Soc 131, 17042, 2009.
[13] Richard L.Mc Creery, Raman spectroscopy for chemical analysis, John Wiley& Sons Ltd,
Englad, 2007.
[14] J. Turkevich, P.C.S., J. Hillier, A study of the nucleation and growth processes in the
synthesis of colloidal gold, Discuss. Faraday. Soc 11, 1951, pp. 55-75.1951.
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
121
ASSESSING SOIL EROSION RATES FOR A LARGE CATCHMENT
IN THE CENTRAL HIGHLANDS OF VIETNAM USING FALLOUT
RADIONUCLIDES
Phan Son Hai, Nguyen Thanh Binh, Nguyen Minh Dao, Nguyen Thi Huong Lan,
Nguyen Thi Mui, Le Xuan Thang and Phan Quang Trung
Environmental Research Centre, Nuclear Research Institute, Vietnam Atomic Energy Institute
Trinh Cong Tu
Central Highlands Soils, Fertilizers and Environ. Research Center
Tran Tien Dung
Southern Coastal Central Agricultural Science Institute
ABSTRACT: Fallout radionuclides Be-7 and Cs-137 were applied to assess soil erosion rates for a 270.5 km2
catchment with a variety of slope (from 0o to more than 45º), crops or vegetation (natural forest, artificial
forest, perennial crops, annual crops) and a variety of tillage and soil conservation measures. Soil erosion rates
were estimated at 90 areas within the catchment. Each sampling area has at least one feature of the slope,
rainfall, crops, farming practice different from others. Soil erosion rates in this region depend significantly on
the slope, crops and farming techniques. Averaging over crops, soil erosion rates by slopes 0 - 5º, 5 - 15º, 15 -
25º and 25 - 35º are 5.0, 12.8, 18.9 and 21.3 t ha-1
y-1
, respectively. Forest land has the least soil erosion rates,
ranging between 0.5 t ha-1
y-1
and 14 t ha-1
y-1
depending on the slope. Annual crops land has the highest soil
erosion rates, ranging between 6 t ha-1
y-1
and 42 t ha-1
y-1
when slope varies from < 5o to 32
o. Perennial crop
land has soil erosion rates in the range of 5 t ha-1
y-1
and 39 t ha-1
y-1
. In areas with the same slope, the soil
erosion rate is the highest for cashew plantations, lower for mulberry field and the lowest for tea or coffee
plantations. Soil erosion has resulted in losing a significant quantity of plant nutrients such as OM, N, P2O5 and
K2O every year. Generally, lost nutrient quantities due to soil erosion are proportional to erosion rates. Some
areas of annual crop land lost a large amount of nutrients every year, up to 1435 kg OM, 79 kg N, 54 kg P2O5
and 36 kg K2O. Similarly, perennial crop lands in this region could lost up to 1736 kg OM, 91 kg N, 66 kg
P2O5 and 40 kg K2O every year. Owing to soil erosion, the catchment has lost about 211200 tons of surface soil
per year during last 50 years, corresponding to the rate of 7.8 t ha-1
y-1
. This amount of eroded soil was
deposited in drainage of the catchment and in reservoirs. Consequently, the drainage capacity was reduced and
the frequency of flooding increased during rainy season. Additionally, life-span of irrigative or hydroelectric
reservoirs considerably decreased. Ham Thuan reservoir supplying water to a 300 MW hydroelectric power
plant in this region is a typical example with the loss of capacity of about 418 970 m3
per year. There is an
existence of farming practice models which could reduce soil erosion rates by 30% - 45% in comparison with
others having the same slope and rainfall. Although these models did not give the effectiveness as good as
Project information:
- Code: 01/2012/HD-DTCB
- Managerial Level: Ministry
- Allocated Fund: 750,000,000 VND
- Implementation time: 24 months (Jan 2012- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. Phan Son Hai, et al., Application of fallout radionuclides to estimate soil erosion rates at areas having
different farming practices in the Lamdong Region, J. Vietnam Soil Science, 43 (2014).
2. Phan Son Hai, et al., Assessment of soil erosion rates for different land uses in the region of Lamdong
province using fallout radionuclides, Journal of Science and Technology (under review).
3. Phan Son Hai, et al., Assessing the effectiveness of soil conservation measures to reduce soil erosion
rates for sloping land in the Central Highlands of Vietnam using fallout radionuclides, Submitted to
Newsletter of WOCAT/LADA.
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
122
those developed by researchers, they have been created and accepted by farmers. Popularizing these optimal
farming practices for farmer’s imitation is feasible for this region. This approach is probably suitable to current
farming culture of local farmers.
I. INTRODUCTION
About 75% of Vietnam territory is sloping land where the third of population are living with
the major practice of farming. Owing to the demand of economic growth, the use of sloping land is
more intensified with time in term of both the frequence of land use and expansion of cultivated
area. Meanwhile, soil conservation measures have not been implemented. The loss of nutrients
owing to soil erosion has been compensated by adding chemical fertilizers and growing stimulators.
By this way, the Vietnamese agricultural system has contributed to contamination of surface and
ground water in catchments. The establishment of sustainable agriculture in sloping land is essential
for our country in this stage. Soil erosion rates for different land uses at catchment level and the
effectiveness of soil conservation measures are useful informations to help set up and maintain
sustainable agriculture.
For assessment of soil erosion rates, different techniques have been applied in Vietnam.
Conventional methods have been applied for several decades, of wich runoff plots have been being
the most widely used (Thai Phien, 1998). Radionuclide Cs-137 has been applied for estimation of
soil erosion rates for more than ten years (Phan Son Hai et al., 2000, 2003, 2004, 2006; Trinh Cong
Tu et al., 2005; Nguyen Hao Quang, 2000; Nguyen Quang Long, 2004; Bui Đac Dung et al., 2005).
The combined use of Be-7 and Cs-137 to assess soil erosion rates for different periods of time, as
well as to assess the effectiveness of soil conservation measures at landscape level has been carried
out in the Central Highlads (P.S. Hai, et al., 2006, 2007, 2011).
In general, soil erosion investigations were carried out for small areas and based mainly on
runoff plots. Fallout radionuclides were also used to assess soil erosion rates for some fields with
the area of several hectares only.
This project was set up to study soil erosion for a large catchment of about 300 km2 using
fallout radionuclides. The experimental results in detail were given in the “Report on
implementation of the MOST's scientific and technological project, period of 2012 - 2013”. Only
main results of the project were presented briefly in this report.
II. STUDY AREA
The study catchment located in
Lamdong province has the area of
270.52 km2. It consists of three
communes of Bao Lam District (Tan
Lac, Loc Thanh, Loc Nam) and three
communes of Di Linh District (Hoa
Bac, Hoa Nam, Hoa Ninh) as showed
on Figure 1. It is a part of the 1280
km2 catchment of Ham Thuan
hydroelectric reservoir. This region
has the average elevation in the range
of 600 - 800 m asl and the annual rainfall varying from 2400 mm to 3000 mm, of which the total
rainfall in rainy season makes up about 60 - 91%.
Fig. 1. The location of study catchment in Lam Dong
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
123
III. METHODS OF STUDY
3.1. Classification of catchment area according to the slope
The Degital Elevation Model (DEM) of the study catchment was established based on the
topographic map of Lamdong province scaling 1:10 000 and then the catchment area was divided
into parts with following slopes: < 5º, 5-15o, 15-25
o, 25-35
o and > 35
o.
3.2. Classification of catchment area according to plantations
Based on land use maps of lamdong province, the whole area of study catchment was
classified in to four categories: (i) Natural forest land; (ii) Artificial forest land; (iii) Perennial crop
land (Tea, coffee, strawberry, cashew); (iv) Annual crop land.
3.3. Selection of representative sampling sites
Based on the digital maps of the study catchment classified by slope, plantation mentioned
above, together with rainfall, 90 sampling sites were selected according to criterions: (i) Each
location has at least one of four characteristics of slope, plantation, rainfall and soil conservation
measure different from others; (iii) To be able to go these location for collecting samples.
3.4. Sampling method
a) Sampling at referent sites
At each referent location, depth incremental samples at 2 cm intervals were collected down
to 35cm for assessment of the vertical distribution of 137
Cs and depth incremental samples at 1 cm
intervals were collected down to 5cm for assessment of the vertical distribution of 7Be. Then 3 – 5
bulk soil samples were collected for determination of the reference value with the uncertainty of
about 8 – 12% (Phan Son Hai et al., 2003). For 137
Cs measurement, soil cores (diameter 10 cm and
depth 30 cm) were collected. For 7Be measurement, soil samples were collected using a frame made
of angle section steel (thickness 5 mm, width 20 mm, height 40 mm).
b) Sampling at study sites
At each study location, bulk soil samples were taken along a sloping line. The distance
between two sampling points varied from 10 m to 30 m depending on land form. One soil sample
was taken by a cylindrical steel tube (30 cm deep and 10cm in diameter) and the other by a scraper
(20 cm wide, 40 cm long and 4 cm deep) at each sampling point for 137
Cs and 7Be measurements as
mentioned above.
3.5. Analytical methods
a) Analysis of Cs-137 and Be-7
Soil samples were dried, ground into fine powder and put into marinelli beakers with the
mass of about 550 gram and then measured for 24 hours using low background gamma
spectrometers having relative efficiency of 30%. Be-7 and Cs-137 were analyzed using the 478 keV
and 662 keV photo-peaks, respectively. All samples for analysis of Be-7 have been completely
counted for about 40 days since sampling date.
b) Analysis of organic carbon and nutrients
- Total organic carbon was determined according to: TCVN 8941 : 2011.
- Total nitrogen was determined according to: TCVN 6498 : 1999.
- Total phosphor was determined according to: TCVN 8940 : 2011.
- Total kalium was determined according to: TCVN 8660 : 2011.
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
124
c) Analysis of particle size
Particle size distribution of soil and sediment samples was determined by wet sieving and
Robinson method according to TCVN 8567:2010.
3.6. Conversion models in soil erion assessment
Conversion models used for assessment of soil erosion rates in this study were discribed in
detail by P.S. Hai et al. (2011).
IV. RESULTS AND DISCUSSION
4.1. The feature of topography and land use for study catchment
The slope distribution infered from DEM for study catchment (Fig. 2) showed that the slope
within the catchment varies in a wide range, from several degree to more than 45o. The
classification of catchment area by slope is following: 0 - 5o accounts for 36.4%; 5 - 15
o accounts
for 40.6%; 15 - 25o accounts for 18.1%; 25 - 35
o accounts for 4.7% and > 35
o accounts for 0.12%.
For land use, 31.76% is natural forest; 6.15% is artificial forest; 1.35% is annual crop land and
60.74% is perennial crop land (Tea: 16.60%; coffee: 78.08%; cashew: 0.02%; mulberry: 0.54%;
fruit-trees: 4.76%).
By combining the map of slope and the land use map, in taking account of rainfall, 90
locations around the catchment were selected for sampling, of which 14 sites in forest land, 58 sites
within perennial land and 18 sites in annual crop land.
4.2. Inventories of Be-7 and Cs-137 at reference sites
The reference inventory of Be-7 and Cs-137 more and less varies from site to site within the
catchment. The reference inventory of Cs-137 is in the range of 385 - 563 Bq/m2 (Average: 500
Bq/m2). The variation in the
inventory of Cs-137 mainly
concerned the variation of
rainfall (rainfall: 2400 –
2980 mm). Reference
inventories of Be-7 range
between 195 Bq/m2 and 340
Bq/m2 (Average: 269
Bq/m2). Owing to short life
of Be-7, the inventory value
depended on the time of
sampling apart from rainfall.
Figure 2: Digital elevation model DEM (a) and sloping map of study catchment (b)
(a) (b)
Figure 3: Soil erosion rates over 50 years according to the slope
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
125
4.3. Soil erosion ratesa) Soil erosion rates at sampling areas
Soil erosion rate within study catchment
varied from site to site depending on the slope and
land use (Figure 3). Soil erosion rates were the lowest
of all for natural forest land and vary from 0.5 t ha-1
y-
1 to 9.0 t ha
-1 y
-1 depending on the slope. Artificial
forest land had soil erosion rates varying from 1.5 t
ha-1
y-1
to 14.0 t ha-1
y-1
when the slope ranged from <
5o to > 35
o. For perennials such as tea and coffee
plantation, soil erosion rates were comparable and in
the range of 5 - 34 t ha-1
y-1
when the slope ranged
from 50 to 35
o. On the same slope area soil erosion
rate in mulberry fields was higher than that in tea and
coffee fields and lower than that in cashew fields. Soil erosion rate in annual crop land was the
highest in the all plantations, up to 40 t ha-1
y-1
at 30o slope.
b) Soil erosion rates for whole catchment
The average soil erosion rate for areas having
the slope of 0 - 5º, 5 - 15º, 15 - 25º, 25 - 35º, > 35º
was estimated by averaging soil erosion rate over
individual study sites within each gradient group.
Long-term soil erosion rates in the period of 50 years
by the slope and plantation are given on Figure 4.
Mean soil erosion rate at annual crop land is
comparable to that at tea and coffee plantations for
areas having the slope of more than 25º. These steep
areas have been natural forest before they were
reclaimed for annual crops several years ago.
Therefore, for these steep areas mean long-term soil erosion rates at annual crop fields is not higher
than that at tea and coffee plantation fields. This is contrary to results obtained for areas less than
25º.
Based on the average soil erosion rates and the area by the slope, the annual total soil loss
was assessed for study catchment. Thereby, the annual soil loss was 211,200 tons for whole
catchment in the period of last 50 years (corresponing to 7.8 t ha-1
y-1
). The structure of soil loss (%)
by plantations is given on Figure 5. The area of coffee plantation is about 47.4% of the total
catchment area but 70% of the total soil loss was derived from coffee fields.
Figure 6: Soil loss structure by the slope for each plantation type
Figure 5: Soil loss structure by plantations
Fig 4: Soil erosion rate averaging over
plantations and slope in the 50 year period
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
126
Figure 6 presents thr structure of annual soil loss by the slope corresponding to each plantation
within the catchment. The percentage of sediment contribution by slope reflected the status of land
use for study catchment in the past.
c) Soil erosion rates according to farming practices
There were several farming practices to be able to reduce soil loss in the catchment: (i)
Intercroping pantations to improve ground cover; (ii) Creating basins at the base of coffee trees to
retain water and soil; (iii) Contour farming; (iv) Terraced farming. Soil erosion investigations into
these farming practices showed that:
- In a sloping area of 23 - 25º, intercroping pineapple with cashew reduced soil erosion
rate by 40% in comparison with cashew monoculture (from 35 t ha-1
y-1
to 21 t ha-1
y-1
).
- In a sloping area of 18 - 20º, 1.2m contour lines farming decreased soil erosion rate by
36% in comparison with cultivation without contour lines for tea plantation (from 26 t ha-1
y-1
to 16
t ha-1
y-1
). Similarly, soil erosion rates at 8 - 10º tea fields with 1.4m contour lines decreased by
40% (from 17 t ha-1
y-1
to 10 t ha-1
y-1
).
- For coffee plantation, creating basins reduced soil erosion rate by 32% in comparison
with the control at 14 - 16º sloping areas (from 26 t ha-1
y-1
to 18 t ha-1
y-1
).
- Contour mulberry rows, together with intercroping corn on 10 - 12º sloping areas
decreased soil erosion rate by 33% in comparison with the control (from 23 t ha-1
y-1
to 15 t ha-1
y-1
).
4.4 Soil erosion impacts
a) On site impacts
The amount of soil nutrient lost every year due to soil erosion was assessed by using the
content of OM, N, P2O5 and K2O in the 0 – 3.5 cm soil layer and soil erosion rates. Generally, lost
nutrient quantities due to soil erosion are proportional to erosion rates. For forest land, some areas
with high soil erosion rates lost 598 kg OM, 29 kg N, 19 kg P2O5 and 12 kg K2O per hectare every
year. Some annual crop areas lost a large amount of nutrients every year, up to 1,435 kg OM, 79 kg
N, 54 kg P2O5 and 36 kg K2O per hectare. Similarly, perennial crop areas suffering severe soil
erosion lost up to 1,736 kg OM, 91 kg N, 66 kg P2O5 and 40 kg K2O every year.
Results obtained from this study showed that for most study areas OM contents in the 0-30
cm soil layer are greater than the average value in cultivated sloping land in Viet Nam (The average
of about 2% by Nguyen Van Bo et al., 2001). However, 20 investigation locations had OM contents
less than 2%.
Particle size analysis of soil samples showed that coarse fractions like sand and silt in the 0
– 3.5 cm soil layer are higher than those in the 0 – 30cm soil layer for most sampling points. This
means that soil erosion brought about the change in physical property of surface soil. For a long
time, the change in particle size compositions can result in changing other chemical and physical
properties of surface soil.
b) Off site impacts
As mentioned above, the rate of soil loss for whole catchment is 211,200 tons per year
(mean: 7.8 t ha-1
y-1
). This amount of eroded soil silted the drainage of catchment and reservoirs.
The study catchment is a subcatchment of the Ham Thuan Reservoir’s catchment.
According to research results in the year 2010, Ham Thuan Reservoir lost it’s capacity of about
418,970 m3 every year owing to sediment from it’s catchment. This means that a sediment amount
of about 523,710 tons reached the reservoir from it’s catchment, corresponding to the average
sediment yield of 4.09 t ha-1
y-1
. With the assumption that the mean soil erosion rate of study
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
127
subcatchment is comparable to that of Ham Thuan reservoir’s catchment, about 52.5% of eroded
soil within the whole catchment was deposited in Ham Thuan reservoir. The rest was deposited in
the catchment’s drainage.
4.5 Main factors affecting soil erosion in the study catchment
Owing to dry season lasting about 5 months with very little rainfall the binding between soil
particles by colloids becomes weaker. Therefore, surface soil is more susceptable to erosion under
havy rain storms at the begining of rainy season. Investigations on run-off plots by Phan Son Hai et
al. (2007) showed that the amount of soil loss in the first month of rainy season could account for
40% to 50% of total soil loss during a year. Leaving bare soil surface or bad ground cover during
the first period of rainy season would increase soil erosion rate in comparison with other period of
time under the same rainfall. Severe soil erosion at cashew land mentioned above is a typical
example on the effect of rain storms at the begining of rainy season. Cashews usually defoliate in
dry season, therefore land surface is bare during heavy rainstorms at the beginning of rainy season,
resulting in serious soil erosion. For rainfed annual crops cultivation is usually started at the
begining of rainy season. Therefore, land surface is almost bare at this time, resulting in severe soil
erosion in this stage.
The majority of study catchment area is sloping land, of which about 23% have the slope
greater 15o. During rainy season, surface water flow increases with increasing slope, resulting in
intensifying soil erosion rate. A dense tree canopy can reduce the effect of rain drops on soil surface
resulting in decreasing rainsplash erosion. However, it do not decrease surface water flow – a factor
can bring about soil erosion. Different from forest, residues are usually cleared from soil surface for
cultivated land. Therefore, surface water flow at cultivated land is usually greater than that at forest
land. Consequently, soil erosion rate at perennial land is much higher than that at forest land unnder
the same slope and rainfall. In order to reduce soil erosion rate, many soil conservation techniques
have been applied in this catchment such as terraced farming, creating basins at the base of coffee
trees, creating contour-hedgerows, contour farming.
V. CONCLUSIONS
Fallout radionuclides Be-7 and Cs-137 were applied to assess soil erosion rates for a 270.5
km2
catchment with a variety of slope (from 0o to more than 45º), crops or vegetation (natural
forest, artificial forest, perennial crops, annual crops) and a variety of tillage and soil conservation
measures. Results obtained from this research have proved the advantages of fallout radionuclide
technique in assessing soil erosion rates and the effectiveness of soil conservation measures at large
catchment level. Especially, Be-7 technique allows us to estimate quickly the effectiveness of soil
conservation techniques at landscape level.
Soil erosion rates were estimated at 90 areas arranged in 5 slope groups: 0 - 5º, 5 - 15º, 15 -
25º, 25 - 35º and > 350 within the catchment. Soil erosion rates in the catchment varied in a wide
range, from 0.5 t ha-1
y-1
to 42.2 t ha-1
y-1
depending on the slope, plantation and farming practices.
By plantations, forest land had the lowest soil erosion rate and annual crope land had the highest
soil erosion rate in all. For perennial crops, under the same slope soil erosion rates in turn reduced
as follows: cashew, mulberry and tea/coffee plantations.
Soil erosion has resulted in losing a significant quantity of plant nutrients such as OM, N,
P2O5 and K2O every year. Generally, lost nutrient quantities due to soil erosion are proportional to
erosion rates. Some areas of annual crop land lost a large amount of nutrients every year, up to
1,435 kg OM, 79 kg N, 54 kg P2O5 and 36 kg K2O. Perennial crop land suffering severe erosion
could lose up to 1,736 kg OM, 91 kg N, 66 kg P2O5 and 40 kg K2O every year.
VINATOM-AR 13--17
The Annual Report for 2013, VINATOM
128
Owing to soil erosion, the catchment has lost about 211,200 tons of surface soil per year
during last 50 years, corresponding to the rate of 7.8 t ha-1
y-1
. This amount of eroded soil was
deposited in drainage of the catchment and in reservoirs. Consequently, life-span of irrigative or
hydroelectric reservoirs fast decreased. Ham Thuan reservoir supplying water to a 300 MW
hydroelectric power plant in this region is a typical example with the loss of capacity of about
418,970 m3
per year.
There is an existence of farming practice models which could reduce soil erosion rates by
30% - 45% in comparison with the controls. Although these models did not give the effectiveness
as good as those developed by researchers, they have been created and accepted by farmers.
Existing soil conservation measures created empirically by farmers. Therefore, the effectiveness of
these models varied in a wide range and did not get the optimal conditions.
REFERENCES
[1] Bui Dac Dung, et al., Comparing soil erosion and deposition rates assessed by Cs-137
technique with those assessed by runoff plots, The Sixth National Conference on Nuclear
Science and Technologies, Dalat City, 26-27/10/2005.
[2] Nguyen Van Bo, et al., The basic information on principal soil types in Vietnam, World
Publisher, Hanoi,2001.
[3] Nguyen Quang Long. Preliminary study on combined use of Pb-210 and Cs-137 to assess
soil erosion rates and nutrient loss. Report on the Institute Project (2004), Vietnam Atomic
Energy Institute, 2004.
[4] Nguyen Hao Quang, Preliminary application of Cs-137 technique to assess soil erosion rates
in an artificial forest area at Song Da, Report on the National Project (2000), Forest Science
Institute of Vietnam, 2000.
[5] Phan Son Hai, et al. Establishing the relationship between Cs-137 loss and soil erosion.
Report on the National Project BO/01/01-03 (2003), Vietnam Atomic Energy Institute,2003.
[6] Phan Son Hai, et al., Spatial variability of 137
Cs inventory at reference sites and influence of
sampling strategy on the uncertainty in estimation of soil erosion rates, Proc. of the fifth
National Conference on Nuclear Physics and Techniques, Ho Chi Minh City, pp. 234-
237,2003.
[7] Phan Son Hai, et al., Establishment of relationship between 137
Cs loss and soil erosion rates
for the region of Central Highlands, J. Vietnam Soil Science 26, pp. 92–94, 2006.
[8] Phan Son Hai et al., Assessment of soil erosion rates and effectiveness of soil conservation
measures using fallout radionuclides and plots, J. Vietnam Soil Science, 27 (2007), pp. 154-
159, 2007.
[9] P.S. Hai et al., Application of Cs-137 and Be-7 to access the effectiveness of soil
conservation technologies in the Central Highlands of Vietnam, IAEA-TECDOC-1665, pp.
195-206, 2011.
[10] Thai Phien & Nguyen Tu Siem (Ed.). Sustainable farming on sloping lands in Vietnam –
Research results in the period of 1990-1997. Agriculture Publisher, Hanoi, 1998.
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
129
STUDY ON METHOD FOR SIMULATION OF PARTITIONING
TRACERS IN DOUBLE POROSITY MODEL OF FRACTURED
BASEMENT FORMATIONS
To Ba Cuong, Nguyen Hong Phan, Tran Tri Hai, Le Van Son and Le Van Loc
Centre for Applications of Nuclear Techniques in Industry,Vietnam Atomic Energy Institute
No.1, DT 723 Street, Da Lat City, Lam Dong Province, Vietnam
ABSTRACT: Single well tracer test (SWTT) has been widely used and accepted as a standard method for
residual oil saturation (SOR) measurement in the field. The test involves injecting of the partitioning
tracers into the reservoir, producing them back and matching their profiles using a suitable simulation
program. Most of simulation programs were first developed for sandstone reservoir using single porosity
model cannot be applied for highly heterogeneous reservoirs such as fractured basement and carbonate
reservoirs. Therefore a simulation code in double porosity model is needed to simulate tracer flow in our
fractured basement reservoirs. In this project, a finite-difference simulation code has been developed by
following the Tang’s mathematical model to simulate the partitioning tracers in double porosity medium. The
code was matched with several field tracer data and compare with results of t h e University of Texas’s
chemical simulator showing an acceptable agreement between our program and the famous UTChem
simulator. Besides, several experiments were conducted to measure residual oil saturation in 1D column and a
2D sandpad model. Results of the experiments show that the partitioning tracers can measure residual oil
saturation in glass bead models with a relatively high accuracy when the flow velocity of tracer is sufficiently
low.
I. OBJECTIVE
The objective of this project is to find out an existing mathematical method for simulating of
partitioning tracers in double porosity media, build a simulation program for single-well tracer test
in double porosity and validate the program with a physical experiment.
Based on that, we follows the JS.Tang’s mathematical model [5] for building a simulation
program of Single well tracer test in double porosity media, then we validate the program with
several field tracer data which have been reported in the literatures; and we also compare our
program with the famous simulation program of the University of Texas named UTChem. The
comparing results showed that our program gave an acceptable match with field data as well as with
results of the UTchem simulator.
Besides, we have conducted some experiments to measure residual oil saturation in glass
bead column and a 2D sandpad model. Results of the experiments show that the partitioning tracers
can measure residual oil saturation in glass bead models with a relatively high accuracy when the
flow velocity of tracer is sufficiently low; in other words, found that the higher flow rate of tracer,
the lesser oil can be detected from tracer method.
Project information:
- Code: CS/13/06-01
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 12 months (May 2013 - Apr 2014)
- Contact email: [email protected]
- Paper published in related to the project:
Phan NH, Cuong TB, Son LV, An aproach for simulation of single-well tracer test in double porosity
media, 10th National Conference on Nuclear Science and Technology, Vung Tau City, 15-16 Aug
2013 (in Vietnamese).
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
130
II. BUILDING OF SIMULATION PROGRAM FOR SINGLE WELL TRACER
TEST IN DOUBLE POROSITY MEDIA
II.1 The mathematical model of Tang
Based on the previous models of Deans[3] and Grigorievich[4], JS.Tang[5] has developed a
new mathematical model for simulating of partitioning, reacting tracers in a single-well tracer test
in double porosity media. In this model, heterogeneities of double porosity formation are described
by 2 separate regions: the flowing region or flowing pore characterizes for large fractures or
channels where fluids can move and the non-flowing region or non-flowing pore, characterizes for
rock matrix and micro fractures where there is no flow, but its fluids can exchange with the flowing
pore by molecular diffusion at the interface. The flow of tracers obeys the convection-dipersion
equation with the following assumptions:
- There is no mass transfer resistance across phases, so tracers always attain instant
equilibrium between oil and water.
- Reaction rate of the partitioning tracer to form the non-partitioning tracer is constant.
Figure 1: A basic volume of the model (left) and the calculation grid (right).
A single well tracer test was implemented in the following steps: first, a partitioning tracer
(Ester) was injected into the formation as a pulse during a short time; after that water was injected
to push the tracer bank far away from the wellbore, when the tracer bank reaches certain distance,
the well was then shut, leaving Ester to react with water to form another tracer named Alcohol that
cannot partition between oil and water. Finally the two tracers were pull back and analyzed at the
well head. In addition, to make sure that the tracers were recovered completely, a monitoring tracer
called “cover” was also injected continuously during the ester injection and water pushing periods.
The equations describe movement of tracers in dimensionless form are as below[5]:
Equation of Ester:
In flowing pore (fracture):
j,Dj,Dh
*
j,Dj,DDa
j,D
,Pe2
DD
j,D
r,PeD
DD
j,D
D
,D
D
j,D
r,D
D
j,DCKCCN
CN
r
1
r
CNr
rr
1C
r
u
r
Cu
t
C
(1)
In non-flowing pore (matrix):
*
j,D
*
j,Dh
*
j,Dj,D
*
Da
D
*
j,DCKCCN
t
C
(2)
Equation of alcohol:
In flowing pore (fracture):
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
131
j,D
,Pe2
DD
i,D
r,PeD
DD
i,D
D
,D
D
i,D
r,D
D
i,D
j
iC
Nr
1
r
CNr
rr
1C
r
u
r
Cu
t
C
1
1
j,Dj,Dh
*
i,Di,DDa CKCCN (3)
In non-flowing pore (matrix):
*
j,D
*
j,Dh
*
i,Di,D
*
Da
D
*
i,D
*
j
*
i CKCCNt
C
1
1
(4)
Equation of mass balance tracer (cover)
In flowing pore (fracture):
c,D
,Pe2
DD
c,D
r,PeD
DD
c,D
D
,D
D
c,D
r,D
D
c,D
j
cC
Nr
1
r
CNr
rr
1C
r
u
r
Cu
t
C
1
1
*
c,Dc,DDa CCN (5)
In non-flowing pore (matrix):
*
c,Dc,D
*
Da
D
*
c,D
*
j
*
c CCNt
C
1
1
(6)
in which, CD-dimensionless concentration of tracers; uD,r, uD,radial and angular
dimensionless interstitial velocities; NPe,r, NPeradial and angular Peclet numbers; NDa-
dimensionless mass transfer coefficient of tracer between flowing and non-flowing pore; Kh-
reaction rate constant of ester and is the alcohol/ester molar volume ratio.
II.2 Building of simulation program
Based on the mathematical model of
Tang[5], we have developed a simulation code
using finite difference method to solve the
equations from (1) to (6) for three tracers in a
polar coordinate system, we used the central
finite difference scheme in space, implicit time
scheme in the flowing pore (Eq. 1, 3 and 5) and
explicit time scheme in non-flowing pore (eq.
2, 4 and 6). Those equations were solved
simultaneously, then for every tracer, the mass
transfer process between flowing and non-
flowing pores was solved sequentially.
The adjacent picture is the interface of the program
The program SWTT was written in Fortran to simulate single well tracer test in double
porosity formation. The program can handle for multi layer and the effect of fluid drift.
The code was then tested by matching of several field tracer data which have been reported
in the literatures and compared with results of the University of Texas Chemical simulator
(UTChem).
V drift =
0.3m/s
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
132
Figure 2 and 3 show the matching results of 2 field data reported in the Final report of
Deans[2], in which, the partitioning tracer was used is ethyl acetate and the secondary tracer is
ethanol.
The residual oil saturation values (Sor) estimated from our program were 11% in Test#3 and
27% in Test#28, that were in range of the Sor values which have been pre-determined from other
methods (12.5 ±1.5% in test #3 and 29 ±2% in test #28).
Figure 2: Comparison of field data and simulation results (Ethyl Acetate profiles).
Figure 3: Comparison of field data and simulation results (Ethanol profiles).
III. TRACER EXPERIMENTS
In order to validate the partitioning tracer method to determine residual oil saturation,
several experiments were conducted in 1D column and a 2D sandpad model. In which, the porous
media was made by glass bead, the sewing machine oil was used as organic phase, and the tracers
used were ethyl acetate (as partitioning tracer) and ethanol (as non partitioning tracer).
III.1 Partitioning coefficients measurement
The partitioning coefficients (Kd) of ethyl acetate and ethanol between oil and water
were measured by pumping oil and a mixture of water, ethyl acetate and ethanol (1000ppm/each)
through a very long (10m) and small diameter (1/16”) pipe. Due to the small diameter and long
length of the pipe, the contacting interface between oil and water was increased thus the
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
133
concentrations of tracers in two phases reached the equilibrium state after certain time. Figure 5 is
the concentration of tracer at the effluent of the pipe. By this way, the partitioning coefficients of
two tracers was determined:
Kdethanol = 0 and KdEthyl Acetate = 1.48
Figure 4: Experimental system for Kd measurement.
Figure 5: Concentration of tracer at the effluent samples.
III.2 Tracer experiments for residual oil saturation measurement in column
Residual oil saturation
experiments were conducted
using a stainless-steel column
with diameter of 1.7cm and
length of 29.5 cm. First, the
column was packed by glass
bead with grain size of 100-150
micron to create the porous
media, then oil was injected at
0.5 mL/min to make the column
saturated with oil. After that,
water was injected through the
column at different flow rates
(0.2, 0.5, 1.5 and 5mL/min) to
observe the oil saturation
change in the column. Fig 6
shows the amount of oil left in the
column (So,%) versus the numbers
of pore volume injected (PV)
10m, 1/16”
Figure 6: Remaining oil saturation in the column at
different water injection rates.
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
134
Results of the experiments show that: the higher water injection rate, the lesser oil can be
recovered from the column. For instant: at the water injection of 0.2 mL/min, the amount of oil
left in the column was 20% after injection of 5PV, while this amount was still 31% after injection
up to 9PV when water flow rate was 5mL/min. It means that, the swept efficiency of water is lower
at high injection rate and higher at low injection rate. This is an interest remark need to be
considered for designing of water injection in the real field.
Tracer experiment
Two tracer experiments were run at 0.2 mL/min and 1.5mL/min. The mixture of ethanol and
ethyl acetate (12,000 ppm/each) were injected into the column as a pulse of 2mL and samples were
taken at the outlet for analyzing concentrations of tracer using Gas chromatography system.
Figure 7: Experiment data of tracer concentration in two experiments.
Figure 8: Comparison between true residual oil in the column
and the Sor value estimated from tracer method.
Figure 7 shows the experimental concentration of tracers in the effluent samples. The
residual oil saturation (Sor) calculated from tracer method was 16.9% pore volume in the
experiment at 0.2mL/min (corresponds to a velocity which passed through the cross-section of the
column was 0.23 cm/min). This number was really match with the true residual oil saturation
remained in the column, was 16.4%. On the contrary, in the experiment at 1.5 mL/min (corresponds
to a velocity of 1.78 cm/min), the residual oil calculated from tracer method was only 13.6% while
the true residual oil remained in the column were 28.5%. These results implied that: the higher
velocity of tracer, the lesser oil can be detected from the column. In other words, the higher
flow rate of water, the higher uncertainty in Sor value determined by tracer method. Figure 8 is the
comparison between true value of residual oil in the column and the Sor value calculated from
tracer method.
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
135
However this conclusion need to be validated by conducting more experiments at different
flow rates to investigate the effect of phase contacting time on error of the Sor value determined
from tracer method.
III. 3 Tracer experiment for residual oil saturation measurement in 2D sandpad
A physical model of 2D sandpad was built using a mica-glass box with the sizes of
42.7x18x0.8cm. The box was packed by glass bead with grain size of 300-425 micron. Water and
oil were pump into and produced from the sandpad via a line of many tiny holes located at bottom
and top of the model (Fig.9)
Figure 9: The sandpad model.
Tracer experiment was run as the same procedure with in the column: firstly, oil was
pumped though the sandpad at 0.5 mL/min to make the pad saturated with oil. Then water was
pumped at 2mL/min during 6PV. The remaining oil saturation after 6PV was 9.85% pore volume.
After that, two tracers (ethanol and ethyl acetate) was injected as a pulse of 2mL. The samples were
collected at outlet of the model. Concentration of tracers were analyzed in GC. Figure 10 (left) is
the experimental tracer response curves in sandpad experiment and (right) is the picture of residual
oil saturation during water injection in the sandpad.
Figure 10: Tracer experiment data (left) and Images of residual
oil saturation during water injection (right) in sandpad.
Injection point
Production point
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
136
The residual oil saturation value (Sor) calculated from tracer experiment was 9.1% with a
relative error of 7.6% in comparison with the true residual oil value in the sand pad (9.85%).
To validate the experimental results, a numerical model was built using the UTCHEM
reservoir simulator to simulate the movements of tracer through the sandpad. The comparison
shows that there is a little bit different between the UTchem simulation results and the experiment
data (Fig 11). The reason may be explained by the effect of “non-uniform” of flow at the injection
point, because there are just a few small holes at the injection edge in which water can flow, as
illustrated on the Fig.12.
Figure 11: Comparison of experimental data and simulation results by UTchem.
Figure 12: Illustration of the “non-uniform flow” that causes differences between the
simulation results and experiment data.
IV. CONCLUSION
In this project, we have built a simulation program to simulate the single-well tracer test in
double porosity media. The program was used to match with several field tracer data which have
been reported in the literatures and compared with the result of the University of Texas Chemical
simulator (UTchem). The comparison showed that our program gave an acceptable match with field
data as well as with UTChem’s simulated results. In addition, several experiments were conducted
to measure residual oil saturation in 1D column and a 2D sandpad model. Results of the
experiments show that the partitioning tracers can measure residual oil saturation in glass bead
models with a relatively high accuracy when the flow velocity of tracer is sufficiently low. Or in
other words, the higher velocity of flow, the higher uncertainty in Sor value determined by tracer
method.
VINATOM-AR 13--18
The Annual Report for 2013, VINATOM
137
REFERENCES
[1] Deans, H., & Carlisle, C. Single-Well Chemical Tracers Test Handbook. Chemical Tracers
Inc., Houston, TX, (307), 1988.
[2] Deans, H.A. and Majoros, S. The Single-Well Chemical Tracer Method for Measuring
Residual Oil Saturation, Final report, Contract No. DOE/BC20006-18, US DOE, 1980.
[3] Deans, H. A., & Carlisle, C. T. Single-Well Tracer Test in Complex Pore Systems. Society of
Petroleum Engineers. doi:10.2118/14886-MS, 1 January 1986.
[4] Grigorievich, B. P., & Archer, J. S. Two Tracer Test Method for Quantification of
Residual Oil in Fractured Porous Media. Society of Petroleum Engineers.
doi:10.2118/25201-MS, 1 January 1993.
[5] Tang, J. S. A New Double-Porosity Single-Well Tracer Simulator with Fluid Drift for
Residual Oil Saturation Measurement in Carbonate Reservoirs. Petroleum Society of
Canada. doi:10.2118/2002-047, 2002.
[6] Tomich, J. F., Dalton, R. L., Deans, H. A., & Shallenberger, L. K. (1973). Single-Well
Tracer Method To Measure Residual Oil Saturation. Society of Petroleum Engineers.
VINATOM-AR 13--19
The Annual Report for 2013, VINATOM
138
STUDYING THE POSSIBILITIES OF USING THE RADIUM ISOTOPES
TO DETERMINE THE MASS AGES AND CIRCULATION
OF THE COASTAL WATER
Nguyen Thi Huong Lan, Phan Son Hai, Nguyen Van Phuc, Phan Quang Trung,
Nguyen Thi Mui and Nguyen Minh Dao
Center for Environmental Research and Monitoring, Nuclear Research Institute,
Vietnam Atomic Energy Institute
ABSTRACT: Radium isotopes are the effective indicators in assessing the water mass age, mixing of water,
distribution of some radioactive elements and their behavior in coastal and marine. The pre-concentration and
analyse techniques and counting on alpha spectrometry can determine the radium isotopes in seawater where
there is a low concentration level. Radium in seawater is pre-concentrated with MnO2, Fe(OH)3 or adsorbed on
MnO2 fiber before separating radium by PbSO4. Radium isotopes are separated from Th, Ac, Po, U, Pb by
passing through ion exchange resin. The radium source is electrodeposited on stainless steel disk by ethanol
solution.
1. INTRODUCTION
The method which is used in this subject allows analyzing all the radium isotopes that are
alpha emitters. There for, the working time not only shipboard but also in laboratory can be
reduced. Furthermore, together with some analytical procedures and spectrometry, this method can
determine the radium in seawater at low concentration level.
2. EXPERIMENTS
2.1. Equipments
The Gamma Spectrometry HPGe
The Alpha Spectrometry
2.2. Reagents
- Current Generator 30 V – 1.5 A
- HDPE buckets 200 Liters
- HDPE cans 30 Liters, 10 Liters
- Beakers 5 L, 500 mL, 250 mL, 150
mL, 100 mL
- Tributyl phosphate
- Xylene
- Diethyl ether
- Cation Resin Dowex 50W-X8, H+
form (Merck)
- Anion Resin Dowex 1-X8, Cl- form
Project information:
- Code: CS/12/01-02
- Managerial Level: Institute
- Allocated Fund: 80,000,000 VND
- Implementation time: 18 months (Jun 2012- Jan 2014)
- Contact email: [email protected]
- Paper published in related to the project:
Nguyen Thi Huong Lan. Studying the method of preconcentration radium in seawater by manganese
fiber and determination of radium on alpha spectrometer. To be presented in the Youth Conference
on Nuclear Science and Technology, Hanoi, 2014.
VINATOM-AR 13--19
The Annual Report for 2013, VINATOM
139
- Ion exchange columns
- Hydraulic vacuum valve
- Funnels 250 mL, 100 mL
- Standard solution 229
Th
- HNO3 68%
- HCl 36%
- NH4OH 25%
- H2O2
- Ethanol
- 2-Propanol
(Merck)
- KMnO4
- MnCl2
- KOH
- Hydroxylamine
- NaNO2
- NaCl
- FeCl3
- Ammonium citrate
- Ammonium acetate
- Bromocresol green Indicator
- Filter paper.
2.3. Procedures
This subject carried out three procedures to analyzing radium in seawater. Radium in sea
water was co-precipitated with MnO2, Fe(OH)3 and adsorbed on MnO2 fiber before separating
radium by PbSO4.
2.3.1 Co-precipitation with MnO2: 100L seawater is pumped into a bucket, then
acidization before adding tracer 225
Ra. Radium and other isotopes were co-precipitated by the
carrier KMnO4/KOH and MnCl2 solutions at pH 8. The precipitation was carried to the laboratory,
then adding HCl acid with H2O2 to making it completely dissolved. The radium is once again
coprecipitated with Fe(OH)3 and C2H5OH, the pH was adjusted to 8 by NH4OH. The precipitation
of above step was dissolved by conc. HCl acid and then evaporated. Radium was separated from
others isotopes by extracting with TPB/xylene (1:1) solution in two times. The extracted solution
was evaporated, dissolved before had passed through cation exchange column. Radium was finally
separated by 9M HCl solution. The radium solution was evaporated and then dissolved by 0.1M
HCl before deposited NH4OOCH3/HNO3 solution on the stainless steel disk at 600mA in 3 hours.
2.3.2 Co-precipitation with Fe(OH)3: radium in 100L of sea water was precipitated by
adding carrier FeCl3 and Fe(OH)3. The chemical recovery was checked by adding tracer solution 225
Ra. The precipitation was brought to the lab and dissolved with 9M HCl. The radium was
extracted by TPB/xylene (1:1) solution in two times. Then, the radium solution was passed through
two anion exchange columns with different environment. Radium was eluted by 8M HNO3 when
passing through cation exchange column. The eluate with radium was deposited in
NH4OOCH3/HNO3 solution on stainless steel at 600mA in 3 hours.
2.3.3 Co-precipitation with MnO2 fiber: This procedure is collaborated with the pre-
concentration technique by MnO2 fiber. Radium in seawater is absorbed on MnO2 fiber by passing
100L seawater through 30g MnO2 fiber. Ra is eluted from the adsorbed fiber by 5.0 M HCL and a
few drops of H2O2. The radium is extracted from the sample by coprecipitation with carrier
Pb(NO3)2 and K2SO4 and H2SO4 solutions. The precipitation was dissolved by 0.1M EDTA at pH
10 before passed through anion exchange column to separation radium from Th and Ac. The
solution from the anion exchange column step was added 5M CH3COONH4 and 0.5M EDTA and
adjust pH 4-5 by 6M HNO3 before passed through cation exchange column. Th, Ac, Pb was eluted
by CH3COONH4 and HCl. Radium was finally eluted by 6M HNO3. The eluate was deposited with
ethanol solution on stainless steel at 120mA in 2 hours.
VINATOM-AR 13--19
The Annual Report for 2013, VINATOM
140
3. RESULTS AND DISCUSSION
The concentration of radium isotopes in the seawater collected in Phuoc Dinh, Ninh Thuan
province are given in following table:
Table 1: Specific activity of radium isotopes in seawater
- Phuoc Dinh-Ninh Thuan Province.
Sample
code Lat. Long.
Specific activity and error
Ra-226
(mBq/L) Sdv
Ra-224
(mBq/L) Sdv
Ra-223
(mBq/L) Sdv
SW01 11023’10’’ 109
004’15” 0.24 0.09 0.14 0.06 0.006 0.003
SW02 11023’25” 109
003’57” 0.21 0.09 0.12 0.05 0.030 0.010
SW03 11023’40” 109
003’34” 0.14 0.07 0.42 0.21 0.039 0.019
SW04 11023’59” 109
003’07” 0.12 0.06 0.04 0.02 0.009 0.004
SW05 11024’08” 109
002’46” 0.13 0.06 0.07 0.03 0.008 0.004
SW06 11025’09” 109
001’33” 0.39 0.19 0.45 0.21 0.025 0.010
SW07 11025’32” 109
001’36” 0.31 0.15 1.15 0.50 0.018 0.008
SW08 11025’52” 109
001’42” 0.25 0.11 2.19 0.95 0.021 0.010
The results have large errors due to low recovery of radium, a small number of counts
obtained, leading to errors due to large statistical count. Accordingly, the results show that the Ra
concentrations are in the range Ra concentrations in seawater have been published. The samples
SW9, SW10, SW11 have higher levels of Ra concentration because those samples were collected
closely to shore. For samples SW2, SW3, SW4, SW5, SW6 have lower concentrations because of
these samples were taken with increasing distance from the shore. Ra concentrations were
determined by 3 alpha emitters 226
Ra, 223
Ra and 224
Ra.
The procedures by using MnO2, Fe(OH)3 are time-consuming, cumbersome and strenuous
while bad results. The improved technique by adsorbing on MnO2 fiber before separating radium by
PbSO4 is more feasible because of its advantages. With a short time of preparation, all the radium
isotopes can be determined. Within the limits of this subject, the method of analyzing radium by
coprecipitation with PbSO4 has brought quite low recovery yield. Although the radium recovery
yield achieved only 50-60%, the yields were stable by every experiment. Therefore, there is the
need to carry out some more experiments to improve the procedure as well as the chemical yields.
The coprecipitation radium with PbSO4, then separation from other elements by using ion
exchange columns can give good resolution spectra.
4. CONCLUSIONS
Radium preconcentration method in seawater by MnO2 fiber and analyzing radium by
precipitation with PbSO4 are the confidence methods in environmental analyzing techniques. Since
the preconcentration step has not improved in term of this subject, some further experiments should
be carried out to assessing the ability of these methods.
VINATOM-AR 13--19
The Annual Report for 2013, VINATOM
141
REFERENCES
[1] GUOGANG JIA, JING JIA, Determination of radium isotopes in environmental samples
by gamma spectrometry, liquid scintillation counting and alpha spectrometry: A review of
analytical methodology, Journal of Environmental Radioactivity 106 (2012).
[2] H.W.KIRBY, MURRELL L. SALUTSKY, The Radiochemistry of Radium, USA (1964).
[3] International Atomic Energy Agency, Analytical Methodology for the Determination of
Radium Isotopes in Environmental Samples, IAEA Analytical Quality in Nuclear
Application No. IAEA/AQ/19, (2010).
[4] International Atomic Energy Agency, The Environmental Behavior of radium, IAEA
Technical Reports Series 310, Vienna (1990).
[5] J.K. COCHRAN, P.MASQUÉ, Natural radionuclides applied to coastal zone processes,
Marine Radioactivity, (2004).
[6] M. BOURQUIN, Comparison of techniques for pre-concentrating radium from seawater,
Marine Chemistry 109, pp. 226-237, 2008.
[7] M.T. CREAPO, Adsorption of some actinide elements on MnO2, The Science of the Total
Environment, 70, pp. 253-263, Netherlands, 1988.
[8] MARTIN, P., HANCOCK,G.J., Routine analysis of naturally occurring radionuclides in
environmental samples by alpha-particle spectrometry, Supervising Scientist Report 180,
Supervising Scientist Division, Darwin NT, (2004).
[9] NGUYEN THANH BINH, The results of researches in marine radioactive in Vietnam,
period 1999-2003 , Nuclear Research Institute.
[10] NGUYEN TRONG NGO, The surveys and assessments on the marine radioactive at the
expected positions for Nuclear Power Plans in Ninh Thuan Province, (2011).
[11] NGUYEN VAN PHUC, The researches on establishment the scientific and technical basis
to setting up the marine environmental monitoring program in Vietnam, (2011).
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
142
STUDYING, DETERMINING THE RADIONUCLIDE OF TRITUM IN THE
WATER SAMPLES (RAIN, SURFACE WATER) BY USING LIQUID
SCINTILLATION COUNTING (TRi-carb 3180TR/SL)
Nguyen Thi Linh, Nguyen Dinh Tung, Truong Y, Le Nhu Sieu,
Nguyen Van Phuc, Nguyen Van Phu and Nguyen Kim Thanh
Center for Environment Research and Monitoring,
Nuclear Research Insititute, Vietnam Atomic Energy Institute
1- Nguyen Tu Luc, Dalat, Lam Dong
ABSTRACT: Tritium in the environment is of natural or man-made origin. Tritium is a radioactive isotope that
occurs in the environment and is associated with the interaction of cosmic ray in the atmosphere. However, the
most significiant sources of tritium in the environment results from nuclear weapons testing in the atmosphere
carried out during the late 1950s and early 1960s. Today, the most important new sources of tritium in the
environments, such as power stations, processing and using of isotopes released the local tritium. The objective
of this study is the application of the liquid scintillation technique to tritium analysis in water samples (rain,
and surface waters). Following the Eichrom Tritium Column technique, an aliquot of the passed tritium resin
sample (10 mL) is mixed with 10 mL of scintillation cocktail (Ultima Gold LLT, Packard) in 20-mL plastic-
container vials and the sample activity is determined using a liquid scintillation spectrometer, Tri-carb
3180TR/SL. Counting efficiency is evaluated with internal standards. The tritium concentrations of water
samples that were collected from DaLat, Lamdong range between 0 to 36.2 TU.
Keyword: Tritium concentration, liquid scintillation counting, water samples.
1. INTRODUCTION
Now, liquid scintillation counting is the most popular method to measure the tritium
concentration in the low level environmental samples. It takes, however, much time with a lot of
doing to distill off the impurities in the sample before mixing the sample with the liquid scintillation
cocktail.
In the present work, a low background liquid scintillation system detector Tri-carb
3180TR/SL is used to determine tritium concentration in some different types of water: drinking
water, precipitation and surface water. Establishing an appropriate routine procedure for tritium
measurement in water sample was the main goal of our study. In the light of it, we integrated in
investigate optimal procedures such as counting region optimization under variable quench
conditions in order to improve the limit of detection; established the analytical protocol of tritium
concentration in water using EiChrom tritium column method and liquid scintillation spectrometer.
The process would include collection, storage, preparation/extraction of the sample, the preparation
Project information:
- Code: CS/13/01-06
- Managerial Level: Institute
- Allocated Fund: 80,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Nguyen Thi Linh, Nguyen Dinh Tung, Truong Y, Le Nhu Sieu, Nguyen Van Phuc, Nguyen Van Phu,
Nguyen Kim Thanh. Determining the Radionuclide of Titium in the Water Samples in Dalat by Using
Liquid Scintillation Counting (Tri-carb 3180TR/SL). To be published in Journal of Analytical Sciences
No.2/2-2015.
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
143
for counting and the actual sample counting. The goal of the optimization would be to attain an
adequate tritium determination. The investigated method for measurement of tritium concentration
in water is time saving, sensitive, and can be applied for all types of water.
Eichrom's Tritium Column is designed to replace distillation for most routine tritium
analyses of aqueous samples. The column works by removing potential interferences in the LSC
spectrum, just as distillation does. It is not intended to be an enrichment procedure, and as such, it
should be used only in situations where the required detection limit can be achieved by the direct
counting of a 10 mL aliquot of the sample (plus cocktail) processed through the tritium column.
Fig.1 shown the composition of the Tritium Column explains the purpose and capacity of
each component. The Diphonix® Resin removes cations in exchange for hydrogen ions and its
theoretical capacity is 0.8 mEq per column. The anion resin is standard chloride form analytical
grade 1X-8 resin. It exchanges anions in the sample for chloride ions. (It is recommended that the
sample pH be >1.) The polymethacrylate component removes organically bound tritium and
carbon-14 [7,13]. Counting efficiency is evaluated with internal standards. Determining detection
limit of the analytical method at our laboratory is 0.15Bq/lit or 1.3 TU, efficiency of internal
standard of 25% (20 ml –Vial, ratio of coctail and sample 1:1) at Nuclear Research Institute.
2. EXPERIMENTS
2.1. Special Aparatus and Reagents
- Packard Tri-Carb 3180TR/SL spectrometer,
- 20ml plastic scintillation vials
- Background source-sealed 20-mL scintillation vial with cocktail.
- Standardized solutions of 3H water,
- Ultima Gold-LLT cocktail,
- Tritium column-prepacked column
2.2. Sampling
The water samples are collected in 0.5-1L clean, well-sealed polyethylene bottles, and they
are transported to the laboratory in refrigerated containers. Rain water samples were collected at the
Nuclear Research Institute station, 01 Nguyen Tu Luc St.Dalat City, Lamdong Province, at a
latitude 11o57’ N, longtitude 108
o26’ E, 1500m high; Suface water samples were Xuan Huong lake
(at a latitude 11o57’ N, longtitude 108
o26’ E) and Suoi Vang (at a latitude 12
o00’ N, longtitude
108o22’ E).
Accordingly, this study was undertaken in order to analysis of 3H in 18 evironmental
samples collected in Dalat in 2013 (12 surface water, 6 rain and fallout samples); measurment,
calculation and statistics following the method of experimental research established. The results
obtained through this research have been shown in table and figure below.
2.3. Experimental Procedure
We investigated the possibility of an alternative method with Eichrom tritium column for
purification of tritium prior to measurment by Liquid Scintillation counter. Shown in Fig.1 are the
three components in the Tritium Column.
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
144
2.3.1. Preparation of samples
The water samples filtered through a micron filter; for each sample solution, place a tritium
column in the column rack, and a waste tray below the column in the column rack; Add 10 ml of
deionized distilled water into each column to condition resin and allow to drain; Measure 25ml of
sample and add to the top of the column, discard first 5 ml of sample, place a clean, labelled beaker
beneath the column and collect the remaining 20 ml of sample; remove an liquot of sample
collected in the beaker (10 ml) and add to a LSC vials; Add the appropriate amount of Ultima Gold-
LLTcocktail, shake the vial to mix and count vials in Tricarb 3180TR/SL. Peraparation other liquot
of sample and add a small volume of internal standard solution into one of the counting vials.
2.3.2. Counting procedure
After shaking, clean the counting vials, avoid any contact with the light-transmitting parts of
the counting vials. Place the counting vials in a fixed sequence in the liquid scintillation counter:
background, sample 1, sample 1 with internal standard added, sample 1, background, sample 2,…
Before counting, it is advisable to equilibrate the counting vials in the liquid scintillation
counter for light and temperature adaptation, e.g. overnight, thus reducing the interfering
luminescence during counting. Energy regions set for 3H counting: Region A (0.5-4.5 KeV); B (0.5-
5.5 KeV); A (0.5-18.6KeV), using the guidance found in the applicable LS counter manual.
Counting is performed for 10 cycles of 100 min and the tritium activity is calculated for each
sample by averaging the counting values. Low tritium activity concentrations may require a longer
counting period, depending on the desired counting accuracy.
2.3.3. Calculations
The counting efficiency of the sample is calculated using the following expression:
Di
CCE sis
where Cs+i is the count rate of the sample after the addition of the internal standard, Cs is
the count rate of the sample before the addition of the internal standard, and Di is the disintegration
rate of the added aliquot of internal standard. The disintegration rate of the sample, Ds, may then be
calculated as follows:
Ds = Cs/E or
Figure 1: Composition of Tritium Colum.
Prefilter Resin
Anion Resin
Diphonix® Resin
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
145
Calculate isotope activity:
60
VE
CC Bs
AT
where AH-3 is isotope activityof tritium (Bq/lit), Cs is the count rate of the sample, cpm, CB
is the count rate of the blank sample, cpm; V is volumn of analytical sapmple.
3. RESULTS AND DISCUSSION
After sampling, purification of 3H in the water samples collected at Dalat in 2013 (12
surface water, 6 rain and fallout samples); measurment, calculation and statistics following the
method of experimental research established, tritium-specific activities (Bq/L or TU) and counting
efficiency of the samples are presented in Table 1, Fig. 2, and Fig.3.
Table1: The tritium-specific activities in the water samples collected in Dalat City.
TT Sampe Code Efficie
ncy,E
Activity of 3H, Bq/lit
Activity of 3H, TU
1 Xuan Huong lake 02/13 NHXH0213 24.87 0.15 ± 0.10 1.3 ± 0.8
2 Suoi Vang lake 02/13 NHSV0213 26.42 < 0.15 < 1.3
3 Xuan Huong lake 04/13 NHXH0413 25.23 < 0.15 < 1.3
4 Xuan Huong lake 05/13 NHXH0513 25.18 < 0.15 < 1.3
5 Suoi Vang lake 05/13 NHSV0513 24.50 0.63 ± 0.08 5.3 ± 0.6
6 Xuan Huong lake 07/13 NHXH0713 25.45 0.20 ± 0.10 1.7 ± 0.8
7 Xuan Huong lake 08/13 NHXH0813 25.98 0.32 ± 0.06 2.7 ± 0.6
8 Suoi Vang lake 08/13 NHSV0813 24.76 0.61 ± 0.14 5.1 ± 1.2
9 Rain water, Dalat 09/13 MDL0913 24.40 0.17 ± 0.09 1.4 ± 0.8
10 Xuan Huong lake 10/13 NHXH1013 25.96 0.42 ± 0.08 3.5 ± 0.7
11 Xuan Huong lake 10/13 NHXH1013 25.90 0.58 ± 0.18 4.9 ± 1.5
12 Xuan Huong lake 11/13 NHXH1113 25.40 0.22 ± 0.06 1.8 ± 0.5
13 Xuan Huong lake 11/13 NHXH1113 24.70 0.15 ± 0.05 1.3 ± 0.4
14 Suoi Vang lake 11/13 NHSV1113 26.46 0.46 ± 0.09 3.9 ± 0.7
15 Fallout water, Dalat 11/13 RLDL1113 26.47 4.31 ± 0.45 36.2 ± 3.8
16 Rain water, Dalat 25/11/13 MDL1113 22.35 0.29 ± 0.12 2.4 ± 1.0
17 Rain water, Dalat 11/13 RLDL1113 26.47 0.74 ± 0.10 6.2 ± 0.8
18 Xuan Huong lake 01/14 NHXH0114 26.66 0.54 ± 0.12 4.6 ± 1.0
19 Rain water, Dalat 06/01/14 MDL0114 27.33 0.76 ± 0.07 6.4 ± 0.6
20 Rain water, Dalat 06/01/14 MDL0114 24.30 0.78 ± 0.13 6.6 ± 1.1
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
146
Figure 2: Variability of activity of 3H (TU) in the water samples collected in 2013.
Figure 3: Variability of the counting efficiency of 3H evaluated with internal standards.
From the these results we found that establishing an appropriate routine procedure for
tritium measurement in water sample using a low background liquid scintillation system detector
Tricarb 3180 TR/SL.
The results obtained in 2013 shown values of tritium concentration ranging from 1.7 ± 0.0.8
to 6.6 ± 1.1 TU were reported for the water samples collected at Dalat. The setteled procedure can
be applied to determine tritium concentration in different types of water: drinking water,
precipitation, surface water, seawater and wastewater. Even if the uncertainty of the method is high,
and even if tritium levels in the environment continue to decrease, the direct measurement of tritium
concentration in water sample can still be a more rapid and cheaper measurement method for the
radioactivity environmental monitoring program.
4. CONCLUSIONS
Our results show that the LSC methodology applied allows for measuring tritium levels in
water samples from different origins.
TU Activity of Tritium in the water samples collected in Dalat, 2013
E,% Control chart for the counting efficiency of 3H, mean = 25.54 ± 0.91%
VINATOM-AR 13--20
The Annual Report for 2013, VINATOM
147
From the information reported in table 2, it can be concluded that the method presented in
this paper fulfill laboratory requirements as obtained results are optimal. Moreover, this is a simple,
quick and economic technique; the samples were finally measured in a Perkin Elmer Tri-carb
3180TR/SL liquid scintillation equipment. The investigated method for tritium monitoring is time
saving, sensitive, and can be applied for all types of water to contribute to the environmental
monitoring program at Nuclear Research Institute.
5. RECOMMENDATIONS
- It shoud be suitably equipped for The tritium enrichment system using electrolysis
method in order to improve the limit of detection of low level tritium concentration such as sea
water, ground water samples, etc.
- Extend the establishing of the method and analysis of tritium concentration in the
environmental samples (gas, sea water, rain water, fallout) that is collected at Dalat and Ninh
Thuan.
REFERENCES
[1] S.A. Mc Quarrie, C. Ediss, L.I. Wiiebe, Advances in Scintillation Counting, Canada, 1983.
[2] Charles J.Passo, Gordon T.Cook, Handbook of Environmental Liquid Scintillation
Spectrometry: A comparision of Theory and methods, USA, 2006.
[3] Michael F. L’Annunziata (Ed.); “Handbook of RADIOACTIVITY ANALYSIS, Second
Edition” Academic Press, San Diego, (2003).
[4] Donald. L. Horrocks, Applications of Liquid Scintillation Counting, ACADEMIC Press,
1974.
[5] Aleksandra Sawodni, Anna Dazdur and Jacek Pawlyta, Measurments of Tritium
Radioactyvity in Surface Water on The Upper Silesia Region, Journal on Methods and
Applications of Absolute Chronology, Vol.18, 2000.
[6] ISBN. 978-0-662-47497-5: “Standards and Guidelines for Tritium in Drinking Water”;
Published by the Canadian Nuclear Safety Commission (CNSC), 2008.
[7] Stanis. Overview of The Environmental Monitoring Program for Tritium in Spainish River
Waters, Advances in Liquid Scintillation Spectrometry, 2005.
[8] J Eikenberg, M Jäggi, H Beer, H Baehrle, Tritium concentrations in Waters of Ljubljansko
bajie, Slovenia, Advances in Liquid Scintillation Spectrometry, 2008.
[9] S. Forkapic, J. Nikolov, N. Todorovic, D. Mrdja and I. Biki “Tritium Determination in
Danube River Water in Serbia by Liquid Scintillation Counter”, World Academy of Science,
Engineering and Technology 76, 2011.
[10] Trịnh Văn Giáp, Báo cáo tổng kết đề tài cấp bộ về: “Thiết lập quy trình xác định hàm lượng
các đồng vị của Hidro và Oxi trong nước nhằm tiến tới nghiên cứu nước ngầm Hà Nội”, mã
số: BO 02/04-02, Hà Nội, 2003.
[11] Daina riekstina; olgerts Veveris; Anita Skujina; Antra Zalkalne, LSC 2005, Advance in LSC,
pp.355-357, 2005.
[12] Z Tosheva, A Kies, P Letissier, M Langer “Easy and rapid Estimation of Environmental
Tritium with Eichrom Column and LSC measurment” LSC 2005, Advance in LSC, pp. 395-
400, 2005.
[13] Popy IntanTajahaja and Putu Sukmabuana. The Separation of Tritium Radionuclide from
Environmental Samples by Distillation Technique- Advances from Modeling to
Applicaations. 2012.
[14] Ji-Gen Lua,Yan-Jun Huanga, Li-HuaWang, Fang Li, Shu-Zhen Li,Yuan-Fu Hsia.3H and
90Sr
background in water around Tianwan NPP. China; Radiation measurments 42, pp.74-79,
2007.
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
151
STUDY ON PREPARATION OF 177
Lu, LABELING WITH DOTATATE FOR
USING IN DIAGNOSIS AND TREATMENT NEUROENDOCRINE TUMORS
Duong Van Dong, Bui Van Cuong, Pham Ngoc Dien, Chu Van Khoa, Mai Phuoc Tho,
Nguyen Thi Thu and Vo Thi Cam Hoa
Center for Research and Production of Radioisotope,
Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: Due to its physical and chemical characteristics, 177
Lu is a very attractive radionuclide for use in
nuclear medicine. Its main usage is in the treatment of neuroendocrine tumours but its applicability in the
treatment of colon cancer, metastatic bone cancer, non-Hodgkin‘s lymphoma, lung, ovarian, and prostate
cancer, has also been studied. Two alternative production routes are generally applied to obtain 177
Lu, namely
the direct route based on neutron irradiation of lutetium targets and the indirect route based on neutron
irradiation of ytterbium targets followed by radiochemical separation of 177
Lu from ytterbium isotopes. The
comparison of theoretically calculated and experimentally determined yield for 176
Lu(n,)177
Lu reaction is
presented.177
Lu could be produced with a specific activity of 42 mCi/mg by neutron activation using
enriched 176
Lu (2.59%) target when irradiation was carried out at Dalat Nuclear Research Reactor with thermal
neutron flux of 2×1013
n/cm2/s for 100h. The indirect production route as an alternative production route,
177Lu
could be obtained as carrier-free from beta decay of 177
Yb produced by neutron activation of 176
Yb. In this
way, enriched target material was used but it may be the neutron capture cross section is only 2.4 b so resulting
in low activity just enough to study the separation process of 177
Lu from 177
Yb. In the other hand the study on
labeling 177
Lu with DOTATATE is also described the optimization of the reaction conditions to obtain the
complex 177
Lu-DOTA-TATE with a radiochemical purity > 99%, even so the studies of stability in vitro to the
dilution in saline solution during 72 hours. The bio-distribution studies of this product in mice and rabbit are
also investigated.
Key words: Production of 177
Lu, nuclear reactor IVV-9, DOTATATE.
INTRODUCTION
In recent years,177
Lu has emerged as a promising short-range β- emitter for targeted
radiotherapy. It can be employed as an alternative to 131
I or a complement to 90
Y, 177
Lu [T1/2 = 6.73
d, Eβmax = 0.497 MeV, Eγ = 113 keV (6.4%) and 208 keV, (11%)] is being considered as another
viable alternative for the development of new agents for PRRT. The use of 177
Lu provides an
additional advantage of emission of accompanying low-energy, low-abundance gamma photons
suitable for carrying out simultaneous imaging studies. While the high thermal neutron capture
cross-section of 176
Lu (2100 b) makes it quite convenient to produce high specific activity.
177
Lu production could be used moderate flux reactors. The comparatively longer half-life
of 177
Lu provides logistic advantages over the use of PRRT. Moreover, the tissue penetration range
of 177
Lu (maximum range 2 mm) is more favourable than that of 90
Y (maximum range ~12 mm),
especially for smaller metastases
Unlike 90
Y, 177
Lu provides an additional advantage of the possibility to perform
scintigraphic and dosimetric studies with the same agent employed for therapeutic purpose.
Project information:
- Code: ĐTCB/11/01-02
- Managerial Level: Ministry
- Allocated Fund: 800,000,000 VND
- Implementation time: 30 months (Jan 2011- Jun 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
152
Although 90
Y is obtainable in no carrier-added (NCA) from a90
Sr-90
Y generator, but there exists the
stringent requirement of purification from 90
Sr, a natural bone seeker with a long T1/2 of 28.3 years.
On the other hand,177
Lu can be easily obtained in radionuclidically pure form. The excellent
radionuclidic purity of 177
Lu during using of enriched Lu (>60% in 176
Lu) target.
I. EXPERIMENTS
I.1. Equipments
The Dalat Research Reactor of 500kW; HPLC-LCMS, (Shimadzu); Calibrator ISOMED
2000 (Germany); Counter Caprac (Capintec); Heated magnetic stirrer; Micropipette; Thermostat;
Bottles; Glassware…
I.2. Reagents
- DOTATATE was purchased from piCHEM R&D (Austria), (GMP-grade, >95% (HPLC);
Hydrogen peroxide: concentration 35%, residue on evaporation 0.05%, heavy metals 0.0001%;
Hydrochloric acid: concentration 35.0 ~ 37.0%, residue on evaporation 0.001%, heavy metals
0.000005%; Sodium acetate containing 40 mg/mL, 2,5-dihydroxybenzoic acid.
- Pure water: Purified by The PURELAB® Ultra, ultra pure water production system,
conductivity ≤ 18.2 MΩ.cm
- Target specification and preparation: Lu2O3 99.99% (Sigma-Aldrich), Natural and
enriched >60% in176
Lu
Impurity details:
Y2O3 < 5 ppm, CeO3 < 5 ppm, Pr2O3 < 5 ppm, Nd2O3 < 5 ppm, Sm2O3 < 5 ppm, EuO3 < 5
ppm, Gd2O3 14 ppm, Tb2O3 < 5 ppm, Dy2O3 < 5ppm, Ho2O3 < 5 ppm, Er2O3 < 5 ppm, Tm2O3 < 7
ppm, Yb2O3 22 ppm, La2O3 < 5 ppm, CaO < 30ppm, Fe2O3 < 5 ppm, SiO2 30ppm.
II. PROCEDUCES
II.1. 177
Lu production
Target preparation and irradiation
Material target: Lu2O3 99.99%.
+ Target weight: be accurately weighed by analytical balance.
+ Irradiation container: The target is contained in quartz ampoule and placed in dedicated
aluminum containers for irradiation.
- Irradiation
Based on these calculations, the neutron irradiation is established on the basis of ensuring
the general requirements for radiation safety and occupational safety.
+ Irradiation position: neutron trap, thermal neutrons plux: ~ 2.1013
.cm-2
.s-1
.
+ Irradiation time: 100-130 hours.
+ Cooling time: 30-48 hours
Preparation of 177
LuCl3
After cooling, the irradiated target is transferred to the box production, Where irradiated
target was dissolved in 8M hydrochloric acid in 3 neck flask fitted with a reflux condenser and
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
153
heating by Heated magnetic stirrer in the presence of H2O2 30% within 2-4 hours, after the target
have been dissolved completely, the evaporation will be carry out until appear white residue 177
LuCl3, then turn off the heater to cool. After that, cold target will be re-dissolved with 5 ml of
HCl 0,05M, thus the 177
LuCl3 is obtained. The next stage is the quality control and other research
applications.
Radionuclides used in nuclear medicine generally or 177
Lu particularly often mix some kind
of similar radioactive isotopes or same group, they can join in the labeling reaction or to exist in
free state. Evaluation of this impurity is called radionuclide purity. Pharmacopoeia standards define
radionuclide purity must be more than 98%.
The radionuclide purity is checked by diluting the solution, then used a micropipette take 2-
5 (dilution estimated that the maximum activity is less than 107cpm/ml). The measurement
samples are made simultaneously for at least 3 samples for getting the average result, The gamma
spectrometer is used for recording radionuclide purity. The main gamma peaks of 177
Lu are 72, 113,
208, 250 and 321 keV.
II.2. 177
Lu-DOTATATE preparation
Radiolabelling of DOTATATE is carried out by adding 100 μL of 0.4M sodium acetate
containing 40 mg/mL of 2,5-dihydroxybenzoic acid at pH 4.5 (solution A) to 10 μg of DOTATATE
(0.4 mg/mL in 0.4M sodium acetate at pH 4.5) (solution B). The pH of the 177
LuCl3 solution is
adjusted to 3–4, and 25 μL of this solution (containing 0.25 μg of Lu, 20 Ci/mg) (solution C) is
added to the mixture of solutions A and B. The final reaction mixture (solution A + solution B +
solution C) is incubated at 80–90°C for 30 min. A protocol for the preparation of 177
Lu-
DOTATATE is presented in Table 1.
Table 1: Protocol for preparation of 177
Lu-DOTATATE
Reagent Amount/volume
Solution A: CH3COONa buffer (pH=4.5)
containing of 2,5-dihydroxybenzoic acid-
concentration of 40mg/ml
100l
Solution B: CH3COONa buffer (pH=4.5)
containing of 0.4 mg/ml DOTATATE 25l (10g of DOTATATE)
Solution B: 177
LuCl3 solution (pH 3-4) 25l (0.25-0.50 g of Lu, 5mCi
Process: Adding of solution C to a mixture of
solution A and B
Labelling of 177
Lu with DOTATATE by optimization studies
Optimization studies of 177
Lu labelling of DOTATATE various parameters such as ligand
concentration, incubation time and temperature, were varied extensively in order to arrive at the
protocol for maximum complexation. Keeping the reaction volume at 200 μL, the amount of
DOTATATE was varied from 5 to 100 μg in order to determine the optimal ligand concentration
for obtaining maximum complexation. The characterization of the labelled conjugate and the
complexation yield were determined by paper chromatography in 50% aqueous acetonitrile. The
radiochemical purity of the labelled product was estimated by PC, TLC and HPLC analysis using
the gradient elution technique described above.
Stability of the 177
Lu-DOTATATE
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
154
The stability of the radiolabelled peptides prepared under the conditions described above
was studied. The 177
Lu-DOTATATE was found to be adequately stable over a period of 3 d at room
temperature. The addition of free radical scavengers such as 2,5-dihydroxybenzoic acid (40 mg/ml
of the final mixture) was found to be essential for the storage of high specific activity 177
Lu labelled
DOTATATE preparations.
Quality control
- Thin layer chromatography
Thin layer chromatography studies are carried out on silica gel (aluminium sheets, Merck) in
10 cm strips as the stationary phase. Ammonium hydroxide: methanol:water (1:5:10) is used as the
mobile phase. While the free activity remains at the point of origin (Rf = 0), the radiolabelled
peptide migrates to an Rf of 0.4.
- Paper chromatography
The paper chromatography studies are carried out using 10 cm long Whatman 3MM
chromatography papers. For these studies, 5 μl of the test solution is spotted at 1.5 cm from the
lower end of the paper strips, which are developed in 10% ammonium acetate in methanol (30:70
vol./vol.). The strips are subsequently dried and cut into 1 cm segments. The radioactivity
associated with each segment is measured in a well type NaI(Tl) detector. While free activity
remains at the point of origin, the radiolabelled peptide migrates to an Rf of 0.7-0.8. Percent of
labeling efficiency is calculated by using the formula:
A177Lu-DOTATATE
Labeling eficience (%) = x100
A177Lu + A177Lu-DOTATATE
III. RESULTS AND DISCUSSION
III.1. Preparation of 177
Lu
III.1.1. Theoretical calculation results
Radioactivity produced by the reaction of (n, γ) in the irradiation time τ is calculated
from the formula:
1
693.023
1 1.100
....10.023.6)(
Tac eM
gGA
where:
6.023.1023
: Avogadro number
neutron flux: 2.1013
n/cm2.s
ac: activation cross-section: 2050b=2050.1024
cm2
G: isotopic abundance: 2.59% 176
Lu
g: weight of the irradiated sample gram: 1000g
M: atomic weight: 174.97g
T1: half-life: 160h
: irradiated time: 108h
The result after fill all numbers is: 42mCi/mg 176
Lu
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
155
Table 2: The result consult the reference at time of 4,5 day
Table 3: Results calculated using the Excel program
Calculated yields of Lu-177 from enriched Lu-176 (2.59%) target
Irradiated in DNR
Neutron flux(cm2・sec) 2.30E+13
Enrichment of Lu-176 0.0259 0.026
Cross section of formation of Lu-177 2050 2.05E-21
t1/2 (h) Lu-177 161.616h
Number of atoms of 176, in 1mg Lu 176
Lu 8.86192
E+16
=0.001x0.026/176
x6.023E+23
T(hour) A(Lu-177)
Bq/mg
110 1.57151E+09 = 42mCi/mg
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
156
III.1.2. Processing of irradiated target and radioactivity measuring
After cooling, the irradiated target is transferred to the box production, Where it was
dissolved in 8M hydrochloric acid in 3 neck flask fitted with a reflux condenser and heating by
heated magnetic stirrer in the presence of H2O2 30% within 2-4 hours, after the target have been
dissolved completely, the evaporation will be carry out until appear white residue 177
LuCl3, then
turn off the heater to cool. After that, cold target will be re-dissolved with 5 ml of HCl 0,05M.
The stock solution is diluted into 10ml (to mark solution I), then re-dilute one time more by
using 100l solution I dilute into 10ml (to mark solution II).
Get about 1μl -5μl solution II made into 3 samples and qualitative spectrometer on gamma
spectrometer (multi-channel gamma spectrometer system DSPEC ORTEC HPGe detector, the
relative record efficiencies of 58%, energy resolution of 1.9 keV) the collected spectrum as shown
in Figure 2.
Table 4: Measuring results achieved of 3 177
Lu samples
Sample of Lu-177 (1) Measuring time
300sec
starting measure 14h38
208 keV HS position 5 0.003346997
Counter 64231
Activity at measurement time = 581534,3482
5.82E+05 Bq
Sample of Lu-177 (2) Measuring time
300sec
starting measure 14h49
208 KeV HS position 5 0.003346997
Counter 64801
Activity at measurement time = 586695,0117
5.87E+05 Bq
Sample of Lu-177 (3) Measuring time
300sec
starting measure 14h57
208 KeV HS position 5 0.003346997
Counter 648503
Activity at measurement time = 58363,9891
5.85E+05 Bq
A measure of the average: 5.85x105 Bq
- (Amount: 1 µl solution II)
- Cooling time: 136h40, Ended after 30’
- Decay factor of 177
Lu at 136h40’ was 0.5548
- Experimental activity:
5,85x105x10
2x5x10
3 = 14,1 Ci/0,395g Lu = 36mCi/mg Lu
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
157
1x0,5548x3,7x1010
Table 5: The Theoretical and experimental results
Result Activity of
Theoretical
calculation
Activity of
consultation
Activity calculated
using the Excel
program
Experimental
Activity
Activity/mg 42.0mCi 42.0mCi 42.0mCi 36 mCi
III.1.3. Quality control results
Figure 1: The result of Radiochemical purity > 97%
Figure 2: Gamma spectrometry results
of 177
Lu
Figure 3: Beta spectrometry results
of 177
Lu
Comment: The Experimental activity is always lower than the actual activity theory. This is
actually considered appropriate, because theoretical results are calculated under ideal conditions,
while the actual production depends very much experimental parameters. Maybe, because of the
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
158
decrease of neutron flux; and many experimental factors such samples are placed in the irradiation
container as aluminum material, taget density, temperature ...
The Quality control results: The result of Radiochemical purity > 99.9% and The result of
Radionuclides purity >99%.
III.2. Preparetion of 177
Lu-DOTATATE
III.2.1. Radiolabelling optimization
The radiolabelling yield of 177
Lu-DOTATATE as a function of pH, incubation time and
incubation temperature is presented in Fig. 4, 5 and 6, respectively. The results indicate that high
labelling yield of 177
Lu-DOTATATE was obtained at pH 5 with incubation during 25-30 min at a
temperature of 90oC. The effect of varying the molar ratio of Lu to DOTATATE is shown in Fig.7
Figure 4:The influence of pH on
the radiolabeling process
Figure 5: The influence of time on
the radiolabeling process
Figure 6: The influence of temperature on
the radiolabeling process
Figure 7: The influence of concentration on
the radiolabeling process
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
159
Figure 8: The influence of storage time on the radiolabeling process
III.2.2. Bio-distribution control
Rats are the animals most commonly used for testing of 177
Lu -DOTATATE. Using three
Rats are studied at each time point.
The animals are weighed before being injected with the radiopharmaceutical and are kept in
separate numbered cages. The 177
Lu–DOTATATE is prepared by using the lyophilized kit vial to be
tested following the instructions enclosed in the kit. Generally, 0.1-0.5 ml of the preparation is
injected per animal via the tail vein. The injected activity is calculated by taking the difference
between the weight of the loaded syringe and that of the syringe after injection.
At the end time point, the animals are sacrificed and a blood sample is taken by heart
puncture. The organs of interest are carefully dissected, rinsed in saline and placed in individual
disposable plastic tubes or bags and accurately weighed. The tail, which is the site of injection, is
removed and kept separately.
The activity in the organs, tail and carcass is measured either in an isotope dose calibrator or
in a NaI(Tl) crystal scintillation counter. The total retained dose (%TRD) is calculated as follows:
where A is the activity or counts in the organ, and B is the activity or counts in all organs
and the carcass except for the tail. To accurately estimate the activity and to account for decay
corrections in the 99m
Tc activity, standard solutions of the radiophar-maceuticals are prepared.
A typical experiment is given below.
Preparation of standard solution
Draw 0.5 ml of the 177
Lu–DOTATATE in a syringe and estimate its weight by weighing the
empty syringe and the syringe with solution and calculating the difference. Dispense this 177
Lu–
DOTATATE solution into a clean 100 ml glass beaker and add 20 ml of distilled water. This
solution is taken as the standard for estimation of the total activity that is injected into the animals.
The activity retained in the organs is calculated as follows:
If using a NaI(Tl) scintillation counter, the activity retained in the organs
is calculated as:
where Wi is the weight of injection and Ws is the weight of the standard. All the
counts are corrected for background activity.
Rabbits scans
To examine the in-vivo retention, white rabbits (7 week-old) were used. The animals were
kept individual cages at 20 1oC with a relative humidity of 75 10% and 12 h light/dark cycle.
The amimals were allowed free access to food and water, and left to acclimatize for 1 week. 177
Lu–
DOTATATE was administered intraven-ously to the rabbit via an ear vein for the image tests such
as dynamic kinetics and serial images scan using a gamma camera (SPECT-GE).
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
160
The experimental
Seven weeks old white male rabbits (2023.4 100g, n=3), which were anesthe-tized with
Ether, were used for imaging studies. Each rabbit was injected with 177
Lu-DOTATATE via an ear
vein with 111 MBq-/0.5ml. All the rabbit were placed in a posterior position.To confirm the
dynamic kenitics of 177
Lu-DOTATATE, whole body dynamic images for 4h and some static images
at the predeteminated time intervals were obtained using a gamma camera fitted with a low energy
all purpose collimator. Window was centered around 208KeV. Images were scanned by system of
(GE-SPECT).
Order Organ
Time after injected (%)
1 h 4 h 24 h 7 d
1 Blood 0,94±0,35 0,13±0,05 0,15±0,03 0,04±0,005
2 heart 0,26±0,05 0,083±0,02 0,24±0,06 0,05±0,01
3 lungs 4,27±0,37 2,10±0,17 1,14±0,39 0,023±0,02
4 liver 0,29±0,03 4,27±0,033 3,70±0,54 0,046±0,01
5 spleen 0,38±0,06 0,26±0,06 1,90±1,00 0,10±0,04
6 kidney 6,70±0,60 6,05±1,00 1,50±0,30 0,33±0,07
7 stomach 9,00±1,00 5,12±0,71 2,09±0,18 0,28±0,077
8 S. ntestine 1,20±0,30 2,38±0,42 0,41±0,11 0,031±0,01
9 Big intestine 1,23±0,15 2,51±1,20 0,94±0,10 0,13±0,02
10 brain 0,032±0,00 0,028±0,01 0,031±0,01 0,015±0,00
11 pancreas 9,34±3,45 3,18±1,31 0,50±0,05 0,099±0,02
12 muscle 0,12±0,02 0,10±0,11 0,054±0,01 0,03±0,005
13 bone 0,00± 0,00± 0,00± 0,10±0,05
Figure 9: Biodistribution of 177
Lu-DOTATATE
in rat Figure 10: Biodistribution of
177
Lu-DOTATATE
in rabbit
Comment: 177
Lu-DOTATATE was stable than 72 hours after labeling. The results indicate
that high labelling yield of 177
Lu-DOTATATE was obtained at pH=5 with incubation for 25-30 min
at a temperature of 80-90oC. The effect of varying the molar ratio of Lu to DOTATATE is shown in
Fig. 7. The stability of the 177
Lu-DOTA-Tyr3-octreotate was followed by 3 days, and in procedure,
the radiochemical purity was over 99%. Biodistribution studies showed fast blood clearance and the
kidneys were the critical organs.
IV. CONCLUSION
Through the study results can be concluded that the Da Lat Nuclear Reactor in can only be
prepared with carriers 177
Lu using highly enriched target of 176
Lu2O3> 64%. In this study, subject
developed the production processes and institutional standards, ensuring all quality control criteria
of radiopharmaceuticals have met the application requirements.
The radiolabelling procedures for DOTATATE using 177
Lu were optimized, and relevant
quality control parameters were standardized. According to this labeling procedure, the
VINATOM-AR 13--21
The Annual Report for 2013, VINATOM
161
radiochemical purity is more than 99%. In vivo biodistribution studies in normal mice revealed that
the 177
Lu-DOTATATE have suitable pharmacokinetic properties.
REFERENCES
[1] J. Pillai MRA, Chakeraborty, Das T, Venkatesh M, Ramamoorthy N. Production logistics of 177
Lu for radionuclide therapy. Applied Radiation and Isotopes, 59:109-118, 2003.
[2] M. R. McDevitt, D. Ma, L. T. Lai, J. Simon, P. Borchardt, R. K. Frank, K. Wu, V. Pellegrini,
M. J. Curcio, M. Miederer, N. H. Bander and D. A. Scheinberg, Science, 294, 1537, 2001.
[3] IAEA. Quality assurance manual for radiopharmaceuticals. 2002.
[4] P. A. Schubiger, R. Alberto and A. Smith, Bioconjugate Chem., 7, 165, 1996.
[5] IAEA-TECDOC-1340, Manual for reactor produced radioisotopes, January 2003.
[6] G. J. Ehrhardt, A. R. Ketring and L. M. Ayers, Appl. Radiat. Isot., 49, 1998.
[7] F. F. Knapp Jr., S. Mirzadeh, A. L. Beets, M. O’Doherty, P. J. Blower, E. Verdera, J. S.
Gaudiano, J. Kropp, J. Guhlke, H. Palmedo and H. J. Biersack, Appl. Radiat. Isot., 49, 309,
1998.
[8] Technical Reports Series No. 458, Comparative Evaluation of Therapeutic
Radiopharmaceuticals, IAEA, Vienna, 2007.
[9] Technical Reports Series no. 466, Technetium-99m Radiopharmaceuticals Manufacture of
kits, IAEA, Vienna, 2008.
[10] Activation and Decay tables of Radioisotopes, Budapest, 1973.
[11] K. Hashimoto, H. Matsuoka, S. Uchida, Production of no-carrier-added 177
Lu via the 176
Yb(n,
)177
Yb, 177
Lu process, Journal of Radioanalytical and Nuclear Chemistry, Vol. 255, No. 3,
pp. 575–579, 2003.
VINATOM-AR 13--22
The Annual Report for 2013, VINATOM
162
ENVISAGEMENT OF ANALYTICAL PROCESS FOR 13
C/12
C ISOTOPE
RATIO (13
C) IN BENTHIC BIVALVE SAMPLES BY THE ISOTOPE RATIO
MASS SPECTROMETRY (EA-IRMS)
Ha Lan Anh, Vo Tuong Hanh, Vo Thi Anh and Nguyen Hong Thinh
Institue for Nuclear Science and Technology, Vietnam Atomic Energy Institute
ABSTRACT: The procedure for carbon isotope ratio analysis 13
C/12
C (13
C) in benthic bivalve samples was
envisaged. The procedure include: i) chemical processing and ii) carbon isotope ratio analysis
C by the
isotope ratio mass spectrometry (EA-IRMS) with on-line combustion of samples to CO2. The conditions of the
sample processing on temperature, time and preservation are optimizated to avoid the isotope fractionation.
The procedure for carbon isotope analysis 13
C by EA-IRMS consists of the sample combustion at 1030oC
with chromium oxide and silvered cobaltics oxide catalysts. The samples were completely combusted to CO2
by Cu column and the derived CO2 were transported to ion source before separating by following masses in
IRMS. The accuracy of the analysis was made by the comparison with international standards (IAEA CO-8,
IAEA CO-9 and NBS 19) and the precision of the 13
C value obtained was usually better than ± 0.3‰.
1. INTRODUCTION
Stable isotopes are frequently used as tracers in biological systems, and their ability to track
changes and processes over time has made them increasingly important to ecological research. For
ecologists, stable isotopes provide a natural way to directly trace details of element cycling in the
environment (Fry B, 2006).
The use of stable isotopes as tracers requires that the different potential sources have distinct
isotopic values and that stable isotopes do not undergo significant fractionation (Dawson et al.,
2002). In many fields of science, stable isotopes are used as tracers to determine the proportional
contributions of several sources to a mixture. Applications range from water use by plants to the
study of migration and diets in animal ecology. Stable isotope measurements of animal tissues may
give information on the animal diet or location of feeding provided that isotope signatures vary
among potential dietary components and locations of feeding (Bugalho M. N. and et al, 2008).
Stable carbon isotope ratio values (δ13
C) have found increasing use in providing time-
integrated information of feeding relationship and energy flow through food webs. This ratio can
trace the movement and assimilation of nutrient and organic matter soures, such as sewage effluent,
within food chains of coastal systems.
Project information:
- Code: CS/13/04-06
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Ha Lan Anh, Vo Tuong Hanh. Envisagement of analytical process 13
C/12
C isotope ratio (13
C) in
benthic bivalve samples by the isotope ratio mass spectrometry (EA-IRMS). The proceeding of the 10th
national conference on nuclear science and technology, Vung Tau,15-17/8/2013, 5pages (in
Vietnamese).
VINATOM-AR 13--22
The Annual Report for 2013, VINATOM
163
1.1. Measurement notation
Studies examining stable isotopes at or near natural abundance levels are usually reported as
delta, a value given in parts per thousand or per mil (“‰”).
Delta values are not absolute isotope abundances but differences between sample readings
and one or another of the widely used natural abundance standards which are considered delta =
zero (e.g. Pee Dee Belemnite for C, At%13
C=1.1112328). Absolute isotope ratios (R) are measured
for sample and standard, and the relative measure delta is calculated:
δX = ( 1tan
dards
sample
R
R)*1000
where: X is 13
C and R is 13
C/12
C
1.2. Standard materials and calibration
The common reference for δ13
C, the Chicago Pee Dee Belemnite (PDB) Marine Carbonate
Standard, was obtained from a Cretaceous marine fossil, Belemnitella americana, from the PeeDee
formation in South Carolina. This material has a higher 13
C/12
C ratio than nearly all other natural
carbon-based substances; for convenience it is assigned a delta 13
C value of zero, giving almost all
other naturally-occurring samples negative delta values.
All original supplies PDB have been used up and replaced by secondary standards prepared
by the U.S. National Bureau of Standards (for instance NBS-21 graphite, having a carbon isotope
ratio of -28.10‰ compared to PDB).
2. SAMPLING AND METHODS
2.1. Sampling
Benthic (clams and oyster) were individually measured their sizes, i.e. their length, their
height and their width, weighed and recorded. They were kept living 2 days or 3 days in water to
evacuate their gut content after that they were opened. The opened individuals were collected whole
soft tissue. Each sample was collected, separated into 4 parts. Three parts contained in glass bottles,
all samples then transferred to the laboratory and there the samples were dried at 40oC, 60
oC, 105
oC
by oven, 1 part contained in PE plastic bottles, kept in freezer and there the samples were freeze-
dried. Dried samples were powdered and kept in exsiccator until analysis.
2.2. Method of stable isotope analyses
a. Principle analyses
Benthic ((clam: MT) and oyster: MN) samples were weighed into a small tin capsule and
loaded into the Solid AutoSampler of isotope ratio mass spectrometry (EA-IRMS). When the
AutoSampler is triggered, the sample drops into the combustion reactor that is held at 1030°C. The
sample and capsule melt in an atmosphere temporarily enriched with oxygen, where the tin
promotes flash combustion. The combustion products are carried through on oxidation catalyst of
CrO3 by a constant flow of helium used as a carrier gas. The oxidation product CO2 is passed
through a reduction reactor at 650°C containing copper granules then passed through a magnesium
perchlorate filter to remove water. The remaining CO2, then pass through a short chromatographic
column where they are time-separated. They then pass through a Thermal Conductivity Detector,
and out of the vent on the top of the instrument.
The data system converts the output of the ion detector(s) into digital numbers and computes
the isotopic enrichment of the sample. Stable isotope ratios were then determined on an isotope
ratio mass spectrometer (IRMS) and are expressed relative to the conventional standards.
VINATOM-AR 13--22
The Annual Report for 2013, VINATOM
164
b. Standard materials
In this research, the normal working standard for carbon was CO2 produced from Carrara
marble. Internal reference materials used were IAEA CO-8, IAEA CO-9 and NBS-19 for δ13
C.
Standard deviations on ten aliquots of the same sample were lower than 0.3‰ for δ13
C. For
calculate result of this study, we use the secondary standards for C, including: 1) Community
bureau of reference-BCR: Cod Muscle (lyophilized) with Reference material C stable isotope
compositions-15.64‰ (minus) correlatively with δ13
C; 2) Oyster Tissue (Freeze dried) with the C
stable isotope compositions is -22.35‰ (minus) correlatively with δ13
C.
3. RESULTS AND DISCUSSION
3.1. Results
Time for dry samples (Table 1), δ13
C value of benthic tissues ranged between -33.99‰ and -
20.13‰ (Table 2), (Table 3, Fig.1). There values depend on the conditions dry, weight and kind of
sample.
Table 1: Time for dry sample.
No Sample
name
Time of dry sample (day)
105oC 60
oC 40
oC Freezer-dried
1 MT1 2 4 7 6
2 MT2 2 4 7 6
3 MT3 2 4 6 6
4 MT4 2 4 7 6
5 MT9 2 4 5 6
6 MN 1 3 4 5
Table 2: Result of analysis of clam and oyster.
No Sample
name
Conditions dry samples
13C (‰) 105
oC
13C (‰)
60oC
13C (‰)
40oC
13C (‰)
Freezer-dried
1 MT1 -32.3±0.3 -32.4 ±0.3 -32.3±0.3 -32.3±0.3
2 MT2 -32.5±0.2 -32.5±0.3 -32.3±0.3 -32.4±0.3
3 MT3 -32.4±0.3 -32.4±0.3 -32.2±0.3 -32.6±0.3
4 MT4 -32.3±0.3 -32.4±0.2 -32.2±0.3 -32.2±0.3
5 MT5 -32.3±0.3 -32.6±0.3 -32.4±0.3 -32.3±0.3
6 MN 1 -20.3±0.2 -20.8±0.3 -21.0±0.3 -21.1±0.3
7 MN 2 -21.1±0.3 -20.9±0.3 -21.0±0.3 -20.9±0.3
VINATOM-AR 13--22
The Annual Report for 2013, VINATOM
165
Table 3: δ13
C values depend on weight “age” of benthic on the same condition dry sample
(dry sample by oven at 105oC).
No Sample
name
Weight
(g) Long
(mm)
Wide
(mm)
High
(mm)
13C
(‰)
1 MT4 113.36 11.5 9.5 3.1 -32.21 ± 0.3
2 MT2 114.71 11.5 9.7 2.9 -32.56 ± 0.3
3 MT1 112.78 11.9 9.3 3.1 -32.31 ± 0.3
4 MT3 91.16 10.9 8.5 2.6 -33.66 ± 0.3
5 MT6 90.81 10 8.1 2.7 -33.47 ± 0.3
6 MT5 90.36 10 8.5 2.7 -33.28 ± 0.3
7 MT9 31.12 6.7 4.4 2.5 -33.99 ± 0.3
8 MT10 31.15 6.7 4.2 2.4 -33.85 ± 0.3
9 MT11 31.56 6.9 4.2 2.3 -33.43 ± 0.3
3.2 Discussion
Results dried samples by two methods showed drying time depends on the temperature of
the drying method , with average temperatures of 105oC for 2 days, 4 days and 7 days with 60
oC to
40oC, the higher the temperature the shorter the drying time. In addition, sample drying time by
drying method depends on the “age” (weight ) of the sample, with the big benthics weighing the
sample drying time is longer than the benthic had “old” less than, with dried scallop 105oC
temperature just 24 hours is enough to dry the sample. For freeze-drying process time is 6 days with
dry temperature -50°C, drying time samples by freeze-drying method does not depend much on the
“age” of the organism.
Results δ13
C analysis on mass spectrometer showed no isotope separation phenomenon
occurs due to the drying process templates. For samples were dried at a temperature of 40oC, 60
oC,
105oC and freeze-drying method, δ
13C analysis results showed no difference in outcome analysis,
which showed that the sample drying conditions not occur isotope separation.
The analytical results of samples δ13
C benthics live in freshwater environments and benthic
samples live in saltwater environments showed δ13
C is completely different, reflecting the sharp
differences in habitat conditions related indicators related to δ13
C. For samples that are different
about age, live in the same environment, there is quite clear difference in δ13
C results .
VINATOM-AR 13--22
The Annual Report for 2013, VINATOM
166
4. CONCLUSION
The experimental results show
- Method of drying the sample in different conditions not occur separating isotopes in the
sample. So that temperature is 105oC fit, for shorten the dry sample time.
- Weight of sample for analysis is little.
- The results of the mass spectrometer analyzes have high reliability.
Acknowledgments
The project was completed under the sponsorship of the Institute for Nuclear Science and
Technology, Institute of Atomic Energy, Ministry of Science and Technology, 2013 base level
project.
REFERENCE
[1] Fry B., Scalan R.S. and Parker P.L., 13
C/12
C ratios in marine food webs of the Torres Strait,
Queensland.
[2] Hand book of stable isotope analytical techniques-volume 2-Pie A. de Groot-Elsevier.
[3] Troy F. Gaston, Antionette Kostoglidis.-CSIRO PUBLISHING, The 13
C, 15
N, and 34
S
signatunes of rocky reef planktivorous fish indicate diffirent coastal doscharges of sewage,
Marine and fresh water research 55, pp. 669-689, 2004.
[4] T. B. Coplen, J. A. Hopple, J. K. Böhlke, H. S. Peiser, S. E. Rieder, H. R. Krouse, K. J. R.
Rosman, T. Ding, R. D. Vocke, Jr., K. M. Révész, A. Lamberty, P. Taylor, and P. De Bièvr,
Compilation of Minimum and Maximum Isotope Ratios of Selected Elements in Naturally
Occurring Terrestrial Materials and Reagents, USGS report, 2006.
[5] S. Bouillon, A. V. Raman, P. Dauby and F. Dehairs, Carbon and Nitrogen Stable Isotope
Ratios of Subtidal Benthic Invertebrates in an Estuarine MangroveEcosystem (Andhra
Pradesh, India), Estuarine, Coastal and Shelf Science 54, pp. 901-913, 2002.
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
167
TECHNIQUES FOR INDUCTION OF PREMATURE CHROMOSOME
CONDENSATION (PCC) BY CALYCULIN-A AND MICRONUCLEUS
ASSAY FOR BIODOSIMETRY IN VIETNAM
Pham Ngoc Duy, Tran Que, Hoang Hung Tien, Bui Thi Kim Luyen,
Nguyen Thi Kim Anh and Ha Thi Ngoc Lien
Biotechnology Department, Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: The International Atomic Energy Agency (IAEA) and World Health Organization are interested
in biological dosimetry method for radiation emergency medicine currently. Some cytogenetic techniques such
as premature chromosome condensation (PCC) induced by Calyculin-A and micronucleus (MN) assay are
necessary to develop biodosimetry in Vietnam. In this study, we optimized the condition for MN assay with 6
µg/ml Cytochalasin-B concentration and 72.5 hours for peripheral lymphocyte blood culture. The optimization
for PCC method is 50 nM Calyculin-A concentration for 45 minutes peripheral lymphocyte blood treatment.
For samples exposed to 3.0 Gy gamma 60
Co (dose rate 0.0916 Gy/s), the frequency of MN is 19.02 ± 0.38%,
NBP is 1.95 ± 0.28%, dicentric and ring is 41.43 ± 8.12% and frag and min is 63.33 ± 5.16%. For samples
exposed to 6.0 Gy gamma 60
Co (dose rate 0.0916 Gy/s), the frequency of ring-PCC is 17.73 ± 2.46%, extra
unite is 218.91± 7.58%, dicentric is 83.81 ± 1.09%, ring is 10.75 ± 1.74%, fragment and minute is 193.17 ±
13.10%. MN and ring-PCC are specific marker applying for biodosimetry.
Keywords: Chromosome aberrations, biodosimetry, micronuleus assay, premature chromosome condensation.
Introduction
Chromosome aberration analysis technique has been used for biodosimetry over 40 years
and has become the standards method of radiation dosimetry within the framework of radiation
safety assessment. In the radiation incident, biodosimetry methods combined with physical
dosimetry methods, blood formulars and clinical symptoms of the victims would have been a
comprehensive assessment of the incident. Currently, International Atomic Energy Agency (IAEA),
World Health Organization (WHO) focuses on developing biodosimetry by WHO BioDose
Networks. Many laboratorys have developed cytogenetic techniques such as: conventioning
chromosome aberrations technique, MN technique, PCC technique and FISH technique have
confirmed the strength of the biological dosimetry methods. "Biodosimetry in the 21th century"
Conference organized by the IAEA in 2013 driven for biodosimetry with a combination of
biological markers (multiparameter) from cytogenetic techniques. Thus, establishment of MN and
PCC techniques are very nessesary for developing biological dosimetry in Vietnam.
I. EXPERIMENTS
1. Equipments: Nikon Eclipse 80i microscope, thermostatic bath, Hettich Mikro 120
centrifuge, micropipet, culture cabinet, sterilization autoclaves, incubator.
Project information:
- Code: CS/13/01-04
- Managerial Level: Institute
- Allocated Fund: 75,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
168
2. Reagents: Cytochalasin-B (Sigma), Calyculin-A (Sigma), DMSO, RPMI-1640
medium (Sigma Aldrich), Phytohemaglutinin (Sigma Aldrich), Fetal Bovine Serum (Gibco),
Litium Heparine 400U, Kanamycin Sulfate (Gibco), Colcemid (Gibco), acetic acid, methanol,
toluene (Merck), KCl (0.075M), Citrat natri 1% (Merck), KH2PO4, Na2HPO4, ethnol, Giemsa
(Merck), immersion oil.
3. Subjects: lymphocyte peripheral blood from heathy donors.
4. Experiment designs:
- Experiment 1: optimation of Cytochalasin-B for MN technique. Study on the effect
of Cytochalasin-B at 2; 4; 6; 8 µg/ml concentrations combine with 71; 72; 72.5 cuture times to
the binuclei cell.
- Experiment 2: optimation of Calyculin-A for PCC technique. Study on the effect of
Calyculin-A at 10; 30; 50 nM concentrations combine with 30; 45; 60 minutes treatment to the
PCC index.
- Experiment 3: Study on the cell damaged of gamma ray 60
Co at 3 Gy (0.0916 Gy/s
dose rate) by MN and CA techniques, study on the cell damaged of gamma ray 60
Co at 6 Gy
(0.0916 Gy/s dose rate) by PCC and CA (chromosome aberration Giemsa staining) techniques
II. PROCEDURES
1. Method of culturing lymphocytes and making microscopic slides: Venous blood
was collected and kept in 400U heparin. 0.5 ml of blood were cultured in 9.0 ml RPMI 1640
supplied with 15% Fetal bovine serum (Gibco), 1% Kanamicine, 1% L-glutamine, 5%
Phytohemaglutinin (Sigma). Whole blood was cultured at 37o for 48 hours. Cell harvested and
fixed by Carnoy (3 methanol: 1 acetic acid), make and stain microscopy slides by 10% Giemsa.
2. Analysis of the chromosomal aberrations: Identify the mononuclei, binuclei,
trinuclei and tetranulei cells in MN technique, G1, S and G2/M in PCC technique, chromosome
aberration type in CA technique by the microscope at 1000x.
3. Data analysis: Data was analyzed by SPSS 16.0 and Excel software.
III. RESULTS AND DISCUSSIONS
1. Experiment 1: optimation of Cytochalasin-B for MN technique
All kinds of cell were obtained as in Figure. 1 A, B, C, D.
Figure 1: mononuclei (A), binuclei (B), trinuclei (C) và tetranuclei (D)
The experiment for investigating the effect of Cytochalasin-B concentration and culture time
to the binuclei cells was based on cell culture technique of the IAEA, the culture conditions and
culture medium were optimized in current laboratory condition. Results of proportion of
mononuclei, binuclei, trinuclei, tetranuclei cells obtained in the combination treatment between
Cytochalasin-B at 2, 4, 6, 8 µg/ml and culture time at 71, 72 , 72.5 hours were shown in Table 1 and
Figure 2.
A B C D
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
169
Table 1: The effect of Cytochalasin B concentrations and culture times
to the mononuclei, binuclei, trinuclei and tetranuclei cells.
Treatment Cyt-B (µg/ml) Cuture time
(hours)
Mononuclei
(%) Binuclei (%)
Trinuclei +
tetranuclei (%)
1 2 71 98.51 ± 0.42 1.49 ± 0.42 -
2 2 72 96.52 ± 0.87 3.13 ± 0.92 0.38 ± 0.18
3 2 72.5 92.20 ± 1.55 6.70 ± 0.84 1.10 ± 0.74
4 4 71 89.56 ± 1.85 9.76 ± 1.29 1.03 ± 0.37
5 4 72 87.07 ± 1.89 12.28 ± 2.07 0.65 ± 0.34
6 4 72.5 84.24 ± 2.43 14.66 ± 2.22 1.11 ± 0.27
7 6 71 82.26 ± 1.53 16.60 ± 1.91 1.14 ± 0.42
8 6 72 78.11 ± 3.08 19.58 ± 3.05 2.31 ± 0.27
9 6 72.5 66.75 ± 1.93 30.74 ± 1.36 2.52 ± 0.58
10 8 71 87.49 ± 1.65 16.49 ± 2.07 0.43 ± 0.23
11 8 72 83.74 ± 1.72 15.61 ± 0.85 0.77 ± 0.30
12 8 72.5 83.46 ± 0.52 12.08 ± 1.86 0.93 ± 0.32
0,00
20,00
40,00
60,00
80,00
100,00
1 2 3 4 5 6 7 8 9 101112
Fre
qu
en
cy (
%)
Combinations
Tri + Tetranuclei
Binuclei
Mononuclei
Figure 2: Mononuclei, binuclei, trinuclei and tetranuclei cells.
The percentage of binuclei cells increases from treatment 1 to 9, binuclei cells was highest
(30.74 ± 1.36%) at the treatment 9. While, the percentage of mononuclei cells decreased from
treatment 1 to 9 and in treatment 9 was lowest (66.75 ± 1.93%). The percentage of trinuclei and
tetranuclei cells were not more than 3 % in all treatments. Thus, the treatment 9 was optimized
condition to obtain the highest binuclei cells. Thus, lymphocyte peripheral blood cultured in 72.5
hours at 6 µg/ml concentration of Cytochalasin-B is suitable for MN technique in this study.
2. Experiment 2: optimation of Calyculin-A for PCC technique
All kinds of cell were obtained as in Fig. 3 A, B, C, D.
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
170
Figure 3: lymphocyte (A), G1 cell (B), S cell (C), G2/M cell (D).
Results of proportion of lymphocyte, G1 cell, S cell, G2/M cell obtained in the combination
treatment between Calyculin-A at 10, 30, 50 nM and in 30, 45, 60 minutes were shown in table 2
and Figure 4.
The PCC index increases from treatment 1 to 8 and was highest (24.04 ± 2.64%) at the
treatment 8. The treatment 8 was optimized condition to obtain the highest PCC index. Thus,
lymphocyte peripheral blood cultured in 47 hours, treated at 50 nM concentration of Calyculin-A at
45 minutes is suitable for PCC technique in this study.
Table 2: The effect of Calyculin-A concentration and treatment time the lymphocyte,
G1 cell, S cell, G2/M cell and PCC index.
Treatmet Caly-A
(nM)
Time
(minute)
Lymphocyte
(%) G1 cell (%)
S cell
(%)
G2/M cell
(%)
PCC index
(%)
1 10 30 97.39 ± 1.21 1.01 ± 0.64 0.87 ± 0.35 0.73 ± 0.32 2.61 ± 1.21
2 10 45 96.39 ± 0.06 1.39 ± 0.43 1.35 ± 0.35 0.87 ± 0.26 3.61 ± 0.60
3 10 60 94.10 ± 0.99 0.66 ± 0.28 2.57 ± 0.97 2.67 ± 0.32 5.90 ± 0.98
4 30 30 93.40 ± 1.45 0.99 ± 0.27 2.83 ± 0.53 2.79 ± 1.10 6.60 ± 1.45
5 30 45 87.93 ± 1.56 1.08 ± 0.24 6.64 ± 1.11 4.35 ± 0.38 12.07 ± 1.56
6 30 60 85.65 ± 2.81 1.09 ± 0.60 7.98 ± 1.03 5.28 ± 1.61 14.35 ± 2.81
7 50 30 85.05 ± 1.86 1.60 ± 0.45 7.46 ± 1.28 5.89 ± 1.17 14.95 ± 1.86
8 50 45 75.97 ± 2.64 1.99 ± 0.17 10.52 ± 1.21 11.53 ± 1.71 24.04 ± 2.64
9 50 60 89.32 ± 2.33 1.19 ± 0.47 5.36 ± 1.43 4.13 ± 0.83 10.68 ± 2.33
0
20
40
60
80
100
1 2 3 4 5 6 7 8 9
Fre
qu
en
cy (
%)
Combinations
PCC Index = G1 + S +G2/M
Lympho
Figure 4: The distribution of lymphocyte cell and PCC index.
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
171
3. Experiment 3
Whole blood exposed to gamma 60
Co at 3.0 Gy (dose rate 0.0916 Gy/s). Cell damages were
analysed by MN and CA techniques.
Table 3: Frequency of MN and nu.bridge in lymphocyte exposed to 3.0 Gy gamma 60
Co.
Radiation
dose
Mononuclei
(%)
Binuclei
(%)
Tri +
tetranuclei (%)
Micronuclei
(%)
Nu.bridge
(%)
0 Gy
59.36 38.37 2.26 1.00 -
64.02 32.88 3.09 0.80 -
61.66 34.48 3.86 1.30 -
Mean 61.68 ± 1.90 35.25 ± 2.13 3.07 ± 0.65 1.03 ± 0.21 -
3.0 Gy
51.25 40.39 8.35 19.28 2.27
68.14 30.64 1.23 19.30 2.00
60.22 35.62 4.17 18.48 1.58
Mean 59.87 ± 6.90 35.55 ± 3.98 4.58 ± 2.92 19.02 ± 0.38 1.95 ± 0.28
The frequency of MN in binuclei cell before irradiation was 1.03 ± 0.21%, there were not
any Nu.bridge. After exposed to 3.0 Gy, MN frequency was 19.02 ± 0.38%, Nu.bridge was 1.95 ±
0.28%, MN and Nu.bridge were increased significantly. According to IAEA (2011), using MN
technique in radiation dose range 0.3 to 4.0 Gy.
Table 4: Frequency of chromosome aberrations in lymphocyte
exposed to 3.0 Gy gamma 60
Co.
Radiation dose No. of
metaphase
Dicentric + ring
(%)
Fragment +
minute (%)
0 Gy
1000 - 0.20
1000 - 0.40
1000 - 0.50
Mean - 0.37 ± 0.12
3.0 Gy
211 47.39 62.16
213 46.95 70.15
334 29.94 57.68
Mean 41.43 ± 8.12 63.33 ± 5.16
In 3000 metaphase of samples before irradiation, there were not any dicentric or ring
chromosome, the frequency of minute and fragments was 0.37 ± 0.12%, at the background level.
For the samples irradiated at 3.0 Gy of 60
Co, the frequency of dicentric and ring chromosome was
41.43 ± 8.12%, the frequency of minute and fragment was 63.33 ± 5.16%, these type of
chromosome aberrations originated from DNA double-stranded break. According to IAEA (2011),
the appropriate dose for using CA technique is 0.1 to 5.0 Gy.
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
172
Table 5: Frequency of PCC markers in lymphocyte exposed to 6.0 Gy gamma 60
Co.
Radiation dose G2/M
(%)
PCC index
(%)
Ring
(%)
Extra unit
(%)
0 Gy
13.70 22.37 - 0.20
14.85 25.76 - 0.10
14.04 25.44 - 0.20
Mean 14.19 ± 0.48 24.53 ± 1.53 - 0.17 ± 0.05
6.0 Gy
5.69 10.28 15.15 208.42
5.66 8.36 21.05 226.09
3.54 6.75 17.00 222.22
Mean 4.96 ± 1.01 8.46 ± 1.44 17.73 ± 2.46 218.91± 7.58
PCC index in samples irradiated by 6.0 Gy was lower significantly (p < 0.008), this was due
to high dose irradiation, many lymphocytes could not pass the cell cycle and dead by apoptosis. The
low PCC index also reduced the frequency of G2/M cell (14.19 ± 0.48% before irradiation and 4.96
± 1.01% after irradiation, p < 0.003). Ring chromosomes were not detected in samples before
irradiation, after irradiation, the frequency was 17.73 ± 2.46%. The frequency of extra unit before
irradiation was 0.17 ± 0.05% and after 6.0 Gy irradiation was 218.91 ± 7.58%. Thus, the frequency
of rings and extra units increased very significantly after exposed to 6.0 Gy. However, the
frequency of extra units increased so high, thus this marker was not used for generating the dose
effect calibration curves in biological dosimetry. According to IAEA (2011 ) is the appropriate dose
for using PCC technique is 0.2 to 20.0 Gy .
Table 6: Frequency of chromosome aberrations in lymphocyte exposed to 6.0 Gy gamma 60
Co.
Radiation dose MI index
(%)
Dicentric
(%)
Ring
(%)
Fragment + minute
(%)
0 Gy
7.23 - - 0.2
5.91 - - 0.4
6.74 - - 0.5
Mean 6.63 ± 0.54 - - 0.37 ± 0.12
6.0 Gy
2.20 82.46 9.09 209.09
1.92 85.14 13.16 193.42
4.15 83.84 10.00 177.00
Mean 2.76 ± 0.99 83.81 ± 1.09 10.75 ± 1.74 193.17 ± 13.10
In 6.0 Gy gamma 60
Co, the frequency of dicentric chromosomes was 83.81 ± 1.09%, ring
chromosomes was 10.75 ± 1.74%, fragment and minute was 193.17 ± 13.10%. The frequency of
dicentric, ring, fragment and minute irradiated samples increased significantly compared to control
group.
In this experiment, by the PCC technique, the frequency of ring chromosomes in
lymphocytes after irradiation was 17.73 ± 2.46%, the frequency of fragments and minute was
218.91 ± 7.58%, they are higher than analysing by CA technique (the frequency of ring was 10.75 ±
VINATOM-AR 13--23
The Annual Report for 2013, VINATOM
173
1.74%, fragments and minute was 193.17 ± 13.10%). In PCC technique by Calyculin-A, the ring
chromosomes is very specify for the effects of ionizing radiation, it can be used for building the
dose effect calibration curves at high dose level.
IV. CONCLUSIONS
This study has identified the appropriate conditions for processing MN technique, lymphocytes
cultured with 6 µg/ml Cytochalasin-B and harvested at 72.5 hours. Processing PCC technique,
lymphocytes cultured with 50 nM Calyculin-A in 45 minutes at last culture time. MN and ring-PCC are
suitable for study on biological dosimetry.
REFERENCES
[1] INTERNATIONAL ATOMIC ENERGY AGENCY, Biological Dosimetry: Chromosomal
Aberration Analysis for Dose Assessment, Technical Reports Series No. 260, IAEA, Vienna,
1986.
[2] INTERNATIONAL ATOMIC ENERGY AGENCY, Cytogenetic Analysis for Radiation Dose
Assessment, Technical Reports Series No. 405, IAEA, Vienna, 2001.
[3] INTERNATIONAL ATOMIC ENERGY AGENCY, Cytogenetic Dosimetry: Applications in
Preparedness for and Response to Radiation Emergencies, EPR-Biodosimetry, WHO, IAEA,
Vienna, 2011.
[4] INTERNATIONAL STANDARD ORGANIZATION, Radiation protection-Performance criteria
for service laboratories performing biological dosimetry by cytogenetics, ISO 19238, Switzeland,
2004.
[5] Kanda, R., Hayata, I., Lloyd, Technical Report. Easy biodosimetry for high-dose radiation
exposures using drug-induced, prematurely condensed chromosomes, Int. J. Radiat. Biol.,
75(4): 441-446, 1999.
[6] M. Durante, Y. Furusawa and E. Gotoh, A simple method for simultaneous interphase–
metaphase chromosome analysis in biodosimetry, Int. J. Radiat. Biol, Vol. 74, No. 4, 457 –
462, 1998.
[7] M. Fenech, M. Kirsch-Volders, A. T. Natarajan, J. Surralles, J. W. Crott, J. Parry, H. Norppa,
D. A. Eastmond, J. D. Tucker and P. Thomas, Molecular mechanisms of micronucleus,
nucleoplasmic bridge and nuclear bud formation in mammalian and human cells,
Mutagenesis, Vol. 26 No. 1, pp. 125-132, 2011.
[8] Michael Fenech, Nina Holland, Errol Zeiger, Wushou P. Chang, Sema Burgaz, Philip
Thomas, Claudia Bolognesi, Siegfried Knasmueller, Micheline Kirsch-Volders and Stefano
Bonassi, The HUMN and HUMNxL international collaboration projects on human
micronucleus assays in lymphocytes and buccal cells-past, present and future, Mutagenesis,
Vol. 26, No. 1, pp. 239–245, 2011.
[9] Michael Fenecha, Nina Holland, Wushou P. Chang, Errol Zeiger, Stefano Bonassi, The
HUman MicroNucleus Project-An international collaborative study on the use of the
micronucleus technique for measuring DNA damage in humans, Mutation Research, 428,
271-283, 1999.
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
174
FIELD TEST OF CAPABILITY TO PREVENT CABBAGE CLUBROOT
DISEASE CAUSED BY Plasmodiophora brassicae OF SILVER
NANOPARTICLES SYNTHESIZED BY GAMMA RADIATION
Pham Thi Le Ha, Nguyen Tan Man, Nguyen Duy Hang, Le Hai, Tran Thi Tam,
Pham Thi Sam, Le Huu Tu, Tran Thu Hong, Tran Thi Thuy and Nguyen Tuong Ly Lan
Radiation Technology Department, Dalat Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: The effects of four dose rates 0.27; 0.90; 1.80 and 3.60 kGy/h on the solution of silver (Ag+ 10
-2
M, PVP 2%, ethylenglycol 6%) irradiated at 25 kGy were investigated. The results showed that as the dose
rates increased, the absorption peak shifted to blue wavelengths and also the particles decreased in size. For
field test, nano particles were prepared by irradiation of silver solution at 25 kGy with the dose rate of 3.60
kGy/h. The absorption peaks of the synthesized nanoparticles were obtained at wavelengths of 412 nm and
the average diameter of particles were 14 nm. Using two concentrations of 15 and 20 ppm, silver nanoparticles
had not affected the growth and development of cabbage but showed antifungal activity against
Plasmodiophora brassicae cause club root in cabbage. Using nano particles, the clubroot disease index were 9-
10% compared to 5% of nebijin (fungicide), and 12% of control. The yield of cabbage were 55 tons/ha, 63
tons/ha and 70 tons/ha for the control, nanosilver group, and nebijin group, respectively.
I. INTRODUCTION
Today, nanotechnology is topical question and interested by scientists. Various methods
have been reported for the preparation of silver nanopaticles such as: mechanical grinding, co-
precipitation, spraying, electrolysis sol-gel manufacture, irradiation,…These methods are
disadvantageous because the size of the particles formed is difficult to control or high cost. On the
other hand, γ-irradiation method is advantageous because size, shape and size distribution of
particles are easily controlled and the particles may be prepared at the room temperature,..[1,2] First
time, silver nanoparticles were produced for the antimicrobial aim of health care [3]. Nowadays,
nanoparticles made of silver, have special optical properties that particularly harbour promising
applications for medical technology [4]. In agriculture field, nanosilver have ben used for
preservation and treatment of diseases. Nanosilver solution was used for controlling Septoria leaf
blotch, yellow rust, Fusarium, and powdery mildew on wheat which showed that nanosilver
controls wheat disease. [5]. Plasmodiophora brassicae-the casual agent of club root disease of
crucifers. Plants infected have the low yield. This disease occurs all year in Dalat region of Lam
Dong Province [6,7]. Many ways used to controll this disease include liming the soil, using
chemical,…but the results are still restricted [8-10].
Project Information:
- Code: CS/13/01-02
- Managerial Level: Institute
- Allocated Fund: 75,000,000 VND
- Implementation Time: 12 months (Jan 2013-Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project:
Pham Thi Le Ha, Nguyen Tan Man, Le Hai, Pham Thi Sam, Tran Thu Hong, Tran Thi Tam, Le Huu
Tu, Using silver nano particles prepared by γ irradiation with chitosan as stabilizer to control clubroot
disease on cabbage. The 10th
National Conference on Nuclear Science and Technology, Vung Tau,
8/2013 (in Vietnamese).
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
175
In 2009, the project “Radiation induced synthesis of colloidal silver nanoparticles for control
of clubroot disease of cabbage caused by Plasmodiophora brassicae” was carried out and the
results showed that silver nanoparticles prevent Plasmodiophora brassicae in cabbage in the
laboratory. Based on the good results of the project, we continued to evalue capability to prevent
cabbage clubroot disease of silver nanoparticles in field.
II. MATERIALS AND METHODS
Chemical:AgNO3(PA): Merck, Germany
Facilities: Gamma Co-60 radiation source (Issledavachel-Russia), with the dose rate: 27
kGy/h and gamma Co-60 GC-5000 (BRIT,India), with the dose rate: 3.6 kGy/h.
Plant: Cabbage (Shogun)
Fungicide: Nebijin 0.3DP,
The size of the partocles wree determined by transmsstion electron Microscopy (TEM) and
UV-vis spectrophotometer analysis. The solution of nano particles were tested to prevent cabbage
clubroot disease caused by Plasmodiophora brassicae in the field.
III. RESULTS AND DISCUSSIONS
III.1. The effect of dose rate on silver nanoparticles
III.1.1. The UV absorbance of silver nanoparticles
The results in fig.1 show that when the dose rates increased, absorption peak shifted to the
blue wavelengths.
Figure 1: Uv-visible absorption spectra of silver nanoparticle solutions.
a) Dose rate: 0.27 kGy/h, λmax = 418.0 nm
b) Dose rate: 0.90 kGy/h, λmax = 411.5 nm
c) Dose rate: 1.80 kGy/h, λmax = 411.5 nm
d) Dose rate: 3.60 kGy/h, λmax = 411.0 nm
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
176
III.1.2. TEM image and silver nanopaticle size distribution
0
2
4
6
8
10
12
14
9 11 14 16 18 21 24 26
Size, nm
Fre
qu
ency
, %
a) Dose rate: 0.27 kGy/h (da = 17.85 ± 2.05 nm).
0
2
4
6
8
10
12
14
16
7 9 11 13 20 22 24
Size, nm
Freq
uenc
y, %
b) Dose rate: 0.90 kGy/h (da = 14.74 ± 2.72 nm).
0
4
8
12
16
20
6 9 11 13 17
size, nm
Freq
uenc
y, %
c) Dose rate: 1.80 kGy/h (da = 12.21 ± 1.93 nm).
0
5
10
15
20
25
30
3 5 7 9 11 13 15
Size, nm
Fre
qu
en
cy, %
d) Dose rate: 3.60 kGy/h (da = 7.97 ± 1.85 nm).
Figure 2 (a-d): TEM image and silver nanopaticle size distribution with different dose rates.
The results showed that size of silver nanoparticles decreases with increasing dose rate.
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
177
III.2. Some characteristic of field test silver nanoparticle solution
III.2.1. UV absorbance of field test silver nanoparticle solution
0
0,1
0,2
0,3
0,4
0,5
0,6
300 350 400 450 500 550 600
Wavelength (nm)
Op
tica
l D
ensi
ty (
OD
)
The UV/Vis absorption spectrum of the silver nanoparticle solution is shown in Fig.3. The
absorption peak is obtained at the wavelength of 412 nm.
III.2.2. TEM image and silver nanopaticle size distribution
0
5
10
15
20
5 6 7 9 10 11 12 13 14 16 17 18 20
Kích thước hạt, nm
Tần xuất, (%)
Figure 4: TEM image and silver nanopaticle size distribution.
(da = 13.24 ± 2.25 nm)
The average size of silver nanoparticles of field test solution is 13.24 ± 2.25 nm.
III.2.3. Stability of silver nanoparticles with storage time
The silver nanoparticle solution is observed for 3 months and it shows that the absorption
peak shifted to red wavelengths at first 40 days. From the day of 41st, the λmax kept at the same
wavelength. This indicates that the prepared colloidal gold nanoparticles solution is fairly good
stability in 3 months of storage .
III.3. Field testing results
III.3.1. Toxicity of silver nanoparticles on cabbage
Table 2: Toxicity of silver nanoparticle on cabbage.
Variants Dose Toxicity (level)
1(DAT) 3(DAT) 7(DAT)
1. Nano silver 15 ppm 1 1 1
2. Nano silver 20 ppm 1 1 1
3. Nebijin 0.3 DP 300 kg/ha 1 1 1
Figure 3: Uv-visible absorption
spectrum of field test silver
nanoparticle solution.
(λmax = 412 nm, OD = 0.503)
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
178
DAT: day after treatment.
Using two concentrations of 15 and 20 ppm, silver nanoparticles has not affected the growth
and development of cabbage.
III.3.2. Effect of silver nanoparticles on percentage of infected cabbage
Table 3: Percentage of infected plants.
Variants Dose
Percentage of infected plants (%)1
20 30 40 50 60 70 80
1. Nano silver 15 ppm 0.0a 0.0a 5.00a 6.67b 11.67b 15.00b 15.00b
2. Nano silver 20 ppm 0.0a 0.0a 3.33a 5.00b 10.00b 13.33b 14.33b
3. Nebijin 300 kg/ha 0.0a 0.0a 1.67a 1.67b 5.00b 6.67b 6.67b
4. Control - 0.0a 1.67a 6.67a 16.67a 23.33a 25.00a 25.00a
1: day after treatment.
The results in table 3 showed that, silver nanoparticles had antifungal activity against
Plasmodiophora brassicae cause club root in cabbage.
III.3.3. Effect of silver nanoparticles on the clubroot disease index
Table 4: Effect of silver nanoparticles on the clubroot disease index.
Variants Dose Disease index (%)
1. Nano silver 15 ppm 10.67 ± 4.04
2. Nano silver 20 ppm 9.00 ± 3.46
3. Nebijin 0.3 DP 300 kg/ha 4.67 ± 2.08
4. Control - 21.33 ± 4.51
Using silver nano particles, the clubroot disease index were 9-10% compared to 5% of
nebijin (fungicide), and 12% of control.
III.3.4. Effect of silver nanoparticles on yield of cabbage
Table 5: Effect of silver nanoparticles on yield of cabbage.
Variants Dose Yield (Ton/ha)
1. Nano silver 15 ppm 63.238
2. Nano silver 20 ppm 63.523
3. Nebijin 0.3DP 300 kg/ha 70.810
4. Control - 55.619
The yield of cabbage were 55 tons/ha, 63 tons/ha and 70 tons/ha for the control, nanosilver
group, and nebijin group, respectively.
VINATOM-AR 13--24
The Annual Report for 2013, VINATOM
179
IV. CONCLUSIONS
The effects of four dose rates 0.27; 0.90; 1.80 and 3.60 kGy/h on the solution of silver (Ag+
10-2
M, PVP 2%, ethylenglycol 6%) irradiated at 25 kGy were investigated.
The dose rates increased, the absorption peak shifted to blue wavelengths and also the
particles decreased in size.
For field test, nano particles were prepared by irradiation of silver solution at 25 kGy with
the dose rate of 3.60 kGy/h. The absorption peaks of the synthesized nanoparticles were obtained at
wavelengths of 412 nm and the average diameter of particles were 14 nm.
Using two concentrations of 15 and 20 ppm, silver nanoparticles had not affected the growth
and development of cabbage but showed antifungal activity against Plasmodiophora brassicae
cause club root in cabbage.
Using nano particles, the clubroot disease index were 9-10% compared to 5% of nebijin
(fungicide), and 12% of control.
The yield of cabbage were 55 tons/ha, 63 tons/ha and 70 tons/ha for the control, nanosilver
group, and nebijin group, respectively.
REFERENCES
[1] Kumar M., et al., Radiolytic formation of Ag cluster in aqueous polyvinyl alcohol solution
and hydrogel matrix, Rad. Phys. Chem., 73, p. 21-27, 2005.
[2] Meisel D., Radiation effects on Nanoparticles. Emerging applications of radiation in
nanotechnology, 2005, IAEA-TECDOC-1438, p. 125-136.
[3] Steven J. Oldenburg, Ph.D. (President-nanoComposix, Inc), Silver Nanoparticles: Properties
and Applications.
[4] Sotiriou GA et al.: Non-Toxic Dry-Coated Nanosilver for Plasmonic Biosensors, Advanced
Functional Materials (2010), 20, 4209-4399, DOI: 10.1002/adfm.201000985.
[5] Patent (US 20090075818 A1).
[6] www.cals.ncsu.edu/course/pp728/ Plasmodiophora brassicae html.
[7] Dixon G. R., The biology of Plasmodiophora brassicae Wor.-A review of recent advances.
Acta Hort 706: 271-282, 2006.
[8] Shimotori H., et al., Evaluation of benzenesulfonanilide derivatives for the control of
crucifers clubroot. J. Pestic Sci. 21:31-35, 1996.
[9] Donald E.C., et al., Band incorporation of fluazinam (Shirlan) into soil to control clubroot of
vegetable brassica crops. Aust J ExpAgric 41:1223-1226, 2001.
[10] Murakami H., et al., Reduction of resting spore density of Plasmodiophora brassica and
clubroot disease severity by liming, Soil Sci. Plant Nutr. 48:685-691, 2002.
[11] Báo cáo tổng kết đề tài Khoa học Công nghê cấp Cơ sở năm 2009, “Ứng dụng bức xạ để
chế tạo vật liệu nano bạc, thử nghiệm khả năng điều trị bệnh sưng rễ do nấm
Plasmodiophora brassicae trên cây bắp cải”. 2009.
[12] Xia, Y., Halas N. J. Shape-controlled Synthesis and Surface Plasmonic properties of
Metallic Nanostructures. MRS Bulletin 30, pp. 338-343, 2005.
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
180
STUDY ON IRRADIATED VIETNAM JAVA RAMBUTAN FRUIT
WHICH WAS POSTHARVESTED TREATMENT TO PROLONG
THE SHELFLIFE FOR EXPORT PURPOSES
Nguyen Thuy Khanh1, Nguyen Thi Ly
1, Doan Thi The
1,
Cao Van Chung1 and Nguyen Van Phong
2
1Research and Development Center for Radiation Technology, Vietnam Atomic Energy Institute
202A Street 11, Linh Xuan Ward, Thu Duc District, Ho Chi Minh City
2Southern Horticultural Research Institute
Long Dinh Ward, Chau Thanh District, Tien Giang Province
ABSTRACT: The research:” Study on irradiated Vietnam Java rambutan fruit which was postharvested
treatment to prolong the shelflife for export purposes” was conducted at Research and Development Center for
Radiation Technology and Southern Horticultural Research Institute for 12 months. On the one hand, the
theme was to study the effects of low-dose radiation in the range (200-500 Gy) combined with two types of
packaging: carton boxes and carton boxes + PE perforated cover 0.5% of the area bags. After 13 days
monitoring in 13oC, RH= 85-90% the results showed that Java rambutan fruit which was packed in carton
boxes combined PE bags then irradiated at 300 Gy dose could limit the browning pericarp, dehydration
through the rate of browning, browning level and the percentage of weight loss. Irradiated ramtuban also
remains their pulp quality when testing the soluble solids, the titratable acidity and the ascorbic acid content.
Irradiation did not affect the cell structure of pericarp and pulp by investigating the total ion leakage. On the
other hand, the topics also examined the influence of some postharvest handling and low-dose radiation on
Java rambutan. The results showed that pre-irradiation processing: hot water treatment at 43oC in 6 minuted,
dipping in cloruacalxi 0.4% + citric acid 0.5% solution in 3 minutes, packed in carton boxes + PE bags and
irradiated at 300 Gy dose capable of maintaining the quality which extends the shelflife of Java rambutan more
4 days when kept under conditions of 13oC, RH= 85-90%.
1. INTRODUCTION
Java rambutan (Nephelium lappaceum L) belong to the family Sapindaceae is a tropical fruit
native to Malaysia and Indonesia, which is distributed widely in humid, high rainfall areas of
Southeast Asia. In Vietnam, rambutan is grown in popularity in the province of Dong Nai river
basin or South Central and now Ben Tre, Tien Giang provinces are pioneers in the application
VietGAP and Global GAP for this fruit. Irradiation with an absorbed dose of 400 Gy as quarantine
treatment is approved by U.S. Dept. of Agriculture (USDA/APHIS) for Vietnam rambutan and
dragon fruit [1]. The first Java rambutan treatment was irradiated and export to the United States in
Project information:
- Code: CS/13/07-04
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. Study on effects of low-dose and package treatment to quality and storage capacity of java rambutan,
The 10th
Natioanl Conference on Nuclear Science and Technology, Vung Tau 15-16 August 2013 (in
Vietnamese).
2. Achieved result of training: A master thesis specialized on the Food Technology, Nong Lam University,
HCM City titled “Study on low-dose irradiation combined with other post-harvest treatments in Java
rambutan for export purposes. Student’s name: Ms. Nguyễn Thụy Khanh, Scientific consultants: Dr.
Nguyen Van Phong, Assosiate Professor, Dr. Bui Van Mien, October 2013 (in Vietnamese).
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
181
May 2011 by airport but did not compete with rambutan from other country due to high price. The
problem of competition on the export market have been reviewed and given two solutions: The first
is moving to farming and harvesting Java rambutan in minor season from January to April yearly.
The second is to reduce the costs to sell as well as improve the quality of harvest. The latter solution
is more interested because it can improve the quality and increase the storage time in minor and
major season of rambutan.
The purposes of reasearch were to assess the effects of low-dose radiation combination with
some postharvest treatments to mantain the quality and prolong its shelflife. The outcome of this
research will be a background to improve the quality of rambutan exported to markets approving
irradiation as phytosanitary treatment.
2. EXPERIMENT
2.1. Materials and chemicals
Java rambutan fruits: Were harvested at maturity 90-95 days after blooming from an orchard
in Global GAP model in Phu Phung, Cho Lach district, Ben Tre province during the minor harvest.
Packaging materials: Carton boxes in size of 25×15×5 (cm) and net weight of 2 kg (this is
also the boxes for exporting nowadays in Viet Nam). PE perforated 0.5% bags.
Chemicals: NaOH, phenolphthalein, 2.6 dichlorophenolindophenol, vitamin C, oxalic acid,
CaCl2, manniton, Merk, Germany. 1-MCP, Thailand. Metaphosphoric acid, Chinese.
2.2. Equipment
Irradiation facility: Electron beam accelerator UERL-10-15S2, 10 MeV, supplied by
CORAD Co. Ltd., Russia, at the Research and Development Center for Radiation Technology.
Testing equipment: Handheld refractometer scale 0-320 Brix, Atago, Japan. Colorimeter
Minolta-CR400, Japanese manufactures. Conductivity meter WTW Cond 720 Inlab, Germany.
Other equipments: cold storage, thermor temperature.
2.3. Experimental design and methodology:
a. The effects of packaged treatment and low-dose irradiation to quality and storage
capacity of Java rambutan
Experimental design: The experiment was designed in completely random with two factors:
Factor A was the dose range: 200, 300, 400, 500 Gy and the control (non-irradiated). Factor B was
the type of packing: carton boxes and carton boxes + PE perforated 0.5% bags. The experiment was
repeated two times with 40 fruits of rambutan fruits for each time.
Methodology: The first step, rambutan fruits were taken from Global GAP model farm and
cut the stem leaving 0.5 cm left. The second step, it was packed in carton boxes and carton boxes +
PE perforated 0.5% bags. The last step, rambutan was irradiated by the electron beam facility in a
dose range: 200-500 Gy. Absorbed doses were measured by Fricke dosimeters in each replicate.
b. The effects of post-harvested treatment and low-dose irradiation to quality and
storage capacity of Java rambutan
Experimental design: The experiment was designed in completely random with two factors:
Factor A was the level of radiation: 300 and 400 Gy. Factor B was the postharvest handling that had
done before irradiation. The first was hot water treatment at 43oC in 6 minutes and then steaming 1-
MCP 1.5ppm for 4 hours. The second was hot water treatment at 43oC in 6 minutes and then
dipping in cloruacalxi 0.4% + citric acid 0.5% solution in 3 minutes, and the last was a combination
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
182
of them. Rambutan also was packed in cartons and perforated PE 0.5% bags. The experiment was
repeated three times and 40 fruits of rambutan for each time.
Methodology: The first step, rambutan fruits were taken from Global GAP model farm and
cut the stem leaving 0.5 cm left. The second step, it was post-harvested treatment and packed in
carton boxes and carton boxes + PE perforated 0.5% bags. The last one, rambutan was irradiated at
300 and 400 Gy. Absorbed doses were measured by Fricke dosimeters in each replicate.
Quality determination
The sensory qualities:
- The rate of pericarp browning and disease of the skin fruit (%): By counting the number
browning and diseased rambutan fruits each investigation.
- The degree of pericarp browning and disease of inner and outer surface of the pericarp
(0-5 degree): 0 degree = 0%, 1st degree = 1-5%, 2
nd degree = 6-11%, 3
rd degree = 11-25%, 4
th
degree = 25-50% and 5th
degree means more than 50% surface area are browned or diseased.
- Weight loss: Was determined as percentage of the initial weight by Shimadzu weight
UX8200S-8200g (±0.1g), (Japanese manufactures).
- The external color of the pericarp (including spinterns) (L*, a
*): Color values of 40 fruits
per treatment were recorded at three equidistant locations around the backbone of each fruit (by
Minolta-CR400, Japanese manufactures).
The biochemical qualities of pulp:
- The soluble solids (0Brix): Was directly measured using two to three drops of juice
placed on a handheld refractometer (Atago refractometer-Japan 0Brix 0-32 scale).
- The titratable acidity (%): By the titrimetric method with 0.1N NaOH and
phenolphthalein 1% as indicator (AOAC 942.15).
- The ascorbic acid content (mg/100g): By the 2,6-dichlorophenolindophenol titrimetric
method (AOAC 967.21).
The rate of membrane ion leakage (%) (Jang & Chen, 1995):
The ion leakage in the cell (electrolyte leakage) was determined by conductivity meter
WTW Cond 720 Inlab (by German manufacturers) (EC1). The total leakage of intracellular ions
(electrolyte leakage) (EC2) was determined after the samples were boiled for 15 minutes and cooled
to 25oC.
The total ion leakage (%) = EC1*100/EC2
3. RESULTS AND DISCUSSION
3.1. The effects of packaged treatment and low-dose irradiated to quality and storage
capacity of Java rambutan
3.1.1. The sensory qualities
The rate (%) and degree (score) of pericarp browning:
The Table 1 showed that rambutan fruits after treated, stored at 13oC, RH 85-90% had
begun browning from 5 days. The rate of pericarp browning under 5% on the 5th
day, increased
dramatically around (4.17-62.50)% on the 10th
day and had a strongly increase from 4.25% to 100%
on 13th
day after storage. The degree of pericarp browning under 0.025 on the 5th
day, increased
slightly in the range 0.13 to 2.59 on the 10th
day and had continued from 4 to 0.41 on the last day of
the storage time. Interactions between the method of packaging and irradiation had not significant
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
183
difference at 5% on the 5th
day but there were significantly different from the 10th
day of the storage
time. The rate and degree of pericarp browning of the irradiated rambutan fruit were lower than the
control during the storage time. Among the irradiation treatments, the rate and degree of browning
at 300 Gy and packaging carton boxes + PE perforated 0.5% bags were lowest to compare with the
others. Radiation at low doses (<1 kGy) is not likely to affect the enzyme in the cells but have
capable limiting the activity of the enzyme [4] which is included as phenylalanine ammonia-lyase
(PAL), polyphenol oxidase (PPO) and peroxidase (POD) causes the browning by enzymes [5].
Packaging with PE bags was limited the loss of water in fruits, one of the causes of pericarp
browning [6].
The rate (%) and degree (score) of disease in the skin of rambutan fruits:
The Table 1 showed that the rate of disease under 10% on the 5th
days, increased in range
(34,38-95,84)% and (51,81-100)% of the 10th
and 13th
days of storage time, respectively. The
degree of disease also has the same trend, in the range (0-0,15) score on the 5th
days, (1,29-4,37)
score and (2-4,93) score on the 10th
and 13th
days post-treatment, respectively. Interactions between
the method of packaging and irradiation had not significant differences at the level of 5%.
Rambutan fruits were treated by irradiated at 200-500 Gy could not limit the fungal diseases
because the D10 value which dose can kill 90% pathogens in fruits is 1-3 kGy. The disease in the
skin of fruits increased slightly from 5th
to 10th
days in storage time and dramatically from 10th
to
13th
because of the emergence of disease infected in the former period. The high moisture and
nutrient inside containing bags were convenient conditions for disease growing the latter period.
The external color of the pericarp (including spinterns) (L*, a
*):
The external color of the fruit pericarp was not significant difference between all treatments
and decreased in storage time. External appearance for all treatments was acceptable after 5 and 10
days of storage but unacceptable after 13 days because disease and browning pericarp make
brightness (L* value) and red skin color (a
* value) descending. The obtained results were consistent
with studies in comparing two methods: irradiation and hot forced air treatment in R167 and R134
rambutan cultivars showed that irradiation treatment maintained the color outside of the fruits and
not significant differences with untreated fruits [3].
The weight loss (%):
The weight loss in the range (0.76-8.12)% after 5 days, had an increase in the range (0.85-
14,77)% and (1.42-16.66)% after 10 and 13 days of storage time, respectively. The weight loss
values were significant differences between two types of packaging on 5th,
10th
and 13th
of storage
time. These values for carton boxes + PE 0.5% perforated bags were significantly lower (fruit were
less intensely weight loss) than those of only carton boxes because the PE 0.5% perforated bags
could delay the loss of water by respiration of fruits. At 5 days post-treatment carton + PE treatment
had the weight loss more 7.13 times than PE, this value were 8.21 and 7.55 at 10 and 13 days
respectively. Between all treatments, the irradiated at 500 Gy and packed with carton boxes lost
most weight of 14.77% and 16.66% on 10 and 13d in storage time, respectively. The high dose
level and package in carton boxes without PE bags could make the aging process quickly,
increasing the respiration so that the weight loss had a strongly increase.
3.1.2. The biochemical qualities of pulp
The soluble solids (0Brix):
The soluble solids increased slightly during 1-2 days after harvest and storage in the room
temperature because of the dehydration and then decreased gradually due to the respiration of fruits.
Table 2 shows the soluble solids decrease of storage time, in the range of (15.50-18.60)0Brix on the
5th
day to about (15.50-17.00)0Brix on the 10
thday. As recorded data, there were no significant
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
184
differences of interaction between packaging factors and irradiation factors. Irradiated at doses less
than 900 Gy did not affect to the nutritional composition of the fruit inside [2]. Packaging in carton
+ PE could limit the respiration and weight loss so that decrease the soluble solid value.
The titratable acidity (TA, %):
Total acid content of all treatments decreased slightly, in the range of (0.74-0,97)% and
(0.60-0.81)% on the 5th
and 10th
day during storage time (Table 2). Among irradiation treatments,
after 5 days storage, the highest total acid content was in control samples (1.06%) and the lowest
was at 300 Gy irradiated fruits (0.76%) and had significant differences. On the 10th
day, the highest
value of TA is at dose of 300 Gy (0.73%) but no significant differences compared to the other
treatments. This result is consistent with studies when comparing quarantine by irradiation at 250
Gy and hot forced air treatment showed rambutan irradiated had the total acid concentration
decreased more slowly than the other [3].
The Table 2 shows the vitamin C content tended to decrease during from (7.05-11.68)
mg.100g-1
on 5th
d and (7.04-9.87)mg.100g-1
on 10th
day in post-treatments. There were significant
differences between two methods packaging and no significant differences between five dose levels
of irradiation. Among all treatments, the highest vitamin C contents were at 300 Gy and packaging
carton + PE perforated bags with 11.68 and 9.16 mg.100g-1
, respectively.
3.1.3. The rate of membrane ion leakage (%)
The rate of membrane ion leakage increased in all treatments during time of preservation,
from the 5th
d in the range (52.03-63.76)%, on the 10th
d in the range (60.55-72.64)% and (65.74-
74.37)% on the last of storage time. This result means that the shelf-life of rambutan did not
maintain its quality as the earliest from the 10th
d of storage time. No significant differences
between the total ion leakage of all treatments because irradiation with a low-dose could not affect
the structure of fruit cell wall.
It was concluded that Java rambutan which was irradiated at 300 Gy by electron beams,
packed in carton boxes + PE 0.5% perforated bags had the rate and degree of browning pericarp
lowest among all treatments. In addition, preservation of carton + PE packaging could reduce the
loss of fruits rather than just packed in carton boxes. Irradiation treatment did not effect to the
quality of rambutan by investigating the pulp changes such as the soluble solids, vitamin C, total
acid content and the rate of membrane ion leakage.
3.2. The effects of post-harvested treatment and low-dose radiation to quality and
storage capacity of Java rambutan
3.2.1. The sensory qualities
The rate (%) and degree (score) of pericarp browning:
The Table 3 showed that treated rambutan (stored at 13oC, RH 85-90%) had begun
browning after 8 days. The rate of pericarp browning under 2.5% on the 8th
day, increased
dramatically less than 4.67% on the 12th
day and increased strongly from 4.94% to 25% on 16th
day
after storage. The method of postharvest and irradiation as well as interactions between them had
not significant difference at 5% on the 8th
and 12th
day but they had significantly different on the
16th
day of the storage time. The rate of browning at 300Gy combined dipping in hot water and then
Ca/A.C solutions had the lowest: 0% on 8th
day and increased slowly to 4.94% on the 16th
. The
highest in the irradiated treatment at 400 Gy: 2.5% on the 8th
day, 4.67% on the 12th
day and 25%
on the 16th
day, respectively.
The degree of pericarp browning under 0.06 score on the 8th
day, increased to 2.43 score on
the 12th
day and had continued from 0.6 to 4.83 score on the last day of the storage time. Among all
treatments, the degree of pericarp browning of the rambutan which is dipping in Ca/A.C lowered
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
185
than others. Controls through the storage time and among the irradiation treatments, the 300 Gy
irradiation and packaging carton boxes + PE perforated 0.5% bags gave the lowest rate and degree
of browning. The method of postharvest and irradiation as well as interactions between them had
not significant difference at 5% on the 8th
and 12th
day.
The rate (%) and degree (score) of disease in the skin of rambutan fruits:
The Table 3 showed that the rate of disease in the skin rambutan fruits increased during
storage time. The rate was in the range (8.83-18.43)% on the 8th
days, increased in range (13.27-
40.00)% and (74.17-100)% of the 12th
and 16th
days of storage time, respectively. The method of
packaging and irradiation as well as interactions between them had not significant differences at 5%
on the 8th
and 12th
day. The disease in the skin of rambutan fruits increased slightly from 8th
to 12th
days in storage time and increased dramatically from 12th
to 16th
because of the emergence of the
disease infested in the former period.
The degree of disease in the skin of rambutan less than 0.55 score on the 8th
, in the range
(2.34-3.75) on the 12th
and increased (3.88-4.93) on the last day of storage time. Among all
treatments, the rambutan post-harvested by hot water treatment, dipping in Ca/A.C and irradiated at
300Gy had the lowest degree of disease with 0.16, 2.34 and 3.88 score on the time of evaluation,
respectively. Treatment irradiated at doses 400 Gy had the highest level of disease with 0.55, 3.75
and 4.93 score on the 8th
, 12th
and 16th
day in storage, respectively.
The external color of the pericarp (including spinterns) (L*, a
*):
The external appearance for all treatments tended to decrease during storage time. Treated
with hot water and dipping in Ca/A.C could maintain peel color of fruits through L* and a
* value.
Rambutan that treated in Ca/A.C solutions had the brightest color and keeping the original color of
their pericarp.
The weight loss (%):
The percentage weight loss increased with storage time, in the range (0.64-1.18)% after 8
days, had an increase in the range (1.24-2.22)% and (1.96-4.07)% after 12 and 16 days of storage
time, respectively. Rambutan treated by hot water and dipping in Ca/A.C and irradiated at a dose of
300 Gy had the percentage of weight loss at least (1.96)%, while rambutan irradiated at 400 Gy had
the largest weight loss (4.07)% on the 16th
day of storage time. This can be explained by the
conjunction calcium-pectate when fruits dipped in Ca/A.C solutions; and radiation at 400 Gy
increased respiration of fruits resulted in the loss of weight.
3.2.2. The biochemical qualities of pulp
The soluble solids (0Brix):
Table 4 described the soluble solids of rambutan posttreatment decrease of storage time, in
the range of (16.73-17.47)0Brix on the 8
th day to about (16.00-17.00)
0Brix on the 12
thday,
significant differences between two factors experiment. This is explained by nutrients in the pulp
maintained until the 12th
day preservation. Among all treatments, the rambutan which irradiated at
400 Gy had a strongly decrease of the soluble solids.
The titratable acidity (%):
Total acid content of all treatments fruits decreased slowly in the range (0.81-0.85)% and
(0.73-0.83)% on the 8th
and 12th
day during storage time (Table 4). Among irradiation treatments,
there were not significant differences until 12 days after storage because combining between
postharvest handling and irradiation did not increase the aging process of the fruit itself.
Vitamin C content of Java rambutan also decreased with storage time, in the range
(4.36-5.77) mg.100g-1
on the 8th
day and between (3.29-5.07)mg.100g-1
on the 12th
day post-
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
186
treatments. No significant differences between pretreatment methods and their interaction had
significant differences. Among all treatments, the highest vitamin C contents in fruits dipping in
Ca/A.C solutions and irradiated at 300 Gy and packaging carton + PE perforated bags was 5.77 and
5.07 mg.100g-1
on the 12th
and 16th
day, respectively.
3.2.3. The rate of membrane ion leakage (%)
The rate of membrane ion leakage increased in all treatments over time preservation because
of the decrease of cell wall structure. Table 3 showed that this value was in the range (42.50-
48.41)% on the 8th
day, on the 10th
day in the range (53.23-61.50)% and (53.64-64.92)% on the last
of storage time. No significant differences between the total ion leakage of all treatments on the 8th
day but significant difference on others days during storage time. Compared with controls, hot
water treatment and dipping in Ca/A.C solutions were capable of limiting membrane ion leakage
until 16 days.
4. CONCLUSIONS
Combination of post harvested treatments and quarantine irradiation could keep the sensory
and biochemical pulp quality of Java rambutan during storage. Fruits treated by hot water and
dipping in Ca/A.C before irradiated at 300 Gy by electron beams could prolong the its shelf-life
more 4 days in 13oC, RH=85-90% compared to non-treatment.
REFERENCES
[1] [APHIS], Animal and Plant Health Inspection Service, 2008b. Importation of Red
Dragonfruit (redpitaya) (Hylocereus spp.) from Vietnam into the Continental United States.
http://www.regulations.gov/search/Regs/contentSteamerS, 2008.
[2] Fan, X., Niemera, B. A., Mattheis, J. P., Zhuang, H., & Olson, D. W. Quality of fresh-cut
apple slices as affected by low-dose ionizing radiation and calcium ascorbate treatment.
Journal of Food Science, 70(2), 143-148, 2005.
[3] Follet, P. A., and Sanxter, S. Comparison of rambutan quality after hot forced-air and
irridation quarantine treatments. HortScience(7):1315-1318, 2000.
[4] Horak, C. I., Adeil Pietranera, M., Malvicini, M., Narvaiz, P., Gonzalez, M., & Kairiyama,
E. Improvement of hygienic quality of fresh, pre-cut, ready-to-eat vegetables using gamma
irradiation. In Use of irradiation to ensure the hygienic quality of fresh, pre-cut fruits and
vegetables and other minimally processed food of plant origin. Proceedings of a final
research coordination meeting organized by the Joint FAO/IAEA Programme of Nuclear
Techniques in Food and Agriculture and held in Islamabad, Pakistan, 22-30 July 2005 (pp.
23-40). Vienna: International Atomic Energy Agency, 2006.
[5] P. Yingsana, V. Srilaong, S. Kanlayanarat, S. Noichinda, W.B. McGlasson. Relationship
betwwen browning and related enzymes (PAL, PPO and POD) in rambutan fruit
(Nephelium lappaceum Linn,) cv. Rongrien and See-Chompoo. Postharvest Biology and
Technology (50): 164-168, 2008.
[6] T.J. O’Hare. Postharvest physiology and storage of rambutan. Postharvest Biology and
Technology, (6), 189-199, 1995.
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
187
Table 1: The effects of packaged and low-dose irradiated treatment to the rate and degree of pericarp browning, the rate and degree of disease, the
weight loss of rambutan (storaged in 13oC, RH=85-90%).
Packagi
ng (A)
Dose
(B)
The rate of pericarp
browning
(%)
The degree of
pericarp browning
(score)
The rate of disease
(%)
The degree of disease
(score)
The weight loss
(%)
5th
10th
13th
5th
10th
13th
5th
10th
13th
5th
10th
13th
5th
10th
13th
Carton 200 Gy 2.5 37.50 53.13 0.025 0.42 2.56 5 34.38 65.63 c 0.125 1.35 2.66 cd 8.12 12.30 15.63
300 Gy 2.5 11.46 14.59 0.025 0.20 1.88 0 35.42 63.54 c 0 1.29 2.22 d 6.16 10.93 16.26
400 Gy 2.5 16.67 51.05 0.025 1.99 4 2.5 51.05 85.42 ab 0.025 2.26 4.27 ab 6.90 12.29 14.13
500 Gy 2.5 42.71 100 0.025 2.35 4 0 88.54 85.42 ab 0 3.91 4.27 ab 7.61 14.77 16.66
Control 2.5 62.50 100 0.025 2.59 3.90 2.5 75.00 77.08 ab 0.025 2.53 3.24 c 6.54 10.93 15.81
Carton +
PE
200 Gy 0 11.25 11.46 0 0.41 0.41 0 95.84 93.75 a 0 3.70 4.69 a 0.84 2.37 2.71
300 Gy 0 4.17 4.25 0 0.13 0.20 2.5 42.71 51.81 d 0.025 1.66 2.00d 0.76 0.85 1.42
400 Gy 0 7.29 14.58 0 0.25 0.71 10 92.71 100 a 0.15 4.37 4.74 a 1.12 1.05 0.92
500 Gy 0 13.38 19.79 0 0.27 0.66 0 86.63 100 a 0 3.91 4.93 a 0.96 1.40 2.75
Control 0 28.13 54.17 0 2.21 1.41 10 68.75 89.59 ab 0.125 1.61 3.42 bc 1.31 1.82 2.62
CV (%) 27.34 22.22 14.50 23.63 15.26 12.75 33.23 11.12 9.04 37.89 17.77 11.56 29.22 11.57 18.97
A ns * * ns * * ns ns ns ns ns ns * * *
B ns * * ns * * ns ns ns ns ns ns ns * ns
A*B ns * * ns * * ns ns ns ns ns ns ns * ns
ns, *: non significant and significant at p≤ 0.05
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
188
Table 2: The effects of packaged and low-dose irradiated treatment to the soluble solids, the titratable acidity, the ascorbic acid content, the external
color of pericarp (L* and a
*) and the rate of membrane ion leakage of rambutan (storaged in 13
0C, RH=85-90%).
Packaging
(A)
Dose
(B)
The soluble
solids (0Brix)
The titratable
acidity
(%)
The ascorbic
acid content
(mg.100g-1
)
L* a
*
The rate of membrane
ion leakage
(%)
5th
10th
13th
5th
10th
13th
5th
10th
13th
5th
10th
13th
5th
10th
13th
Carton 200 Gy 16.50 16.00 0.62 0.92 bc 7.85 7.74 39.18 34.21 32.32 22.04 19.36 19.85 53.81 57.92 60.55
300 Gy 17.50 17.00 0.66 0.85 cde 8.96 8.66 42.66 34.48 31.12 22.79 19.20 19.36 47.94 59.76 60.77
400 Gy 17.00 16.25 0.64 0.89 bcd 7.05 7.04 37.94 32.38 29.87 22.31 21.26 17.93 51.49 54.87 61.95
500 Gy
18.60 16.50 0.81 0.74 ef 8.96 8.86 38.07 30.34 29.80 22.04 16.54 17.52 54.18
54.38
61,53a
61.53
Control 16.90 17.00 0.78 1.15 a 9.77 8.96 37.86 33.29 33.26 20.70 15.58 18.10 53.76 55.16 65.60
Carton +
PE
200 Gy 15.60 17.00 0.66 0.89 bcd 9.87 8.36 38.58 35.74 29.14 21.23 16.43 16.99 47.60 49.27 53.37
300 Gy 18.60 16.50 0.60 0.73 f 11.68 8.86 39.08 34.03 32.07 24.23 21.28 16.96 56.57 54.64 72.74
400 Gy 16.90 16.25 0.63 0.79 def 10.67 9.16 36.87 28.87 30.64 20.85 18.25 15.95 53.90 54.37 79.43
500 Gy 16.25 15.50 0.65 0.78 ef 10.47 9.87 37.08 31.29 30.47 21.23 19.58 16.42 57.01 59.70 62.75
Control 17.25 16.75 0.64 0.97 b 9.46 8.66 38.35 35.09 32.38 19.70 16.11 17.37 52.02 57.17 60.52
CV (%) 4.26 5.66 15.41 5.47 9.15 11.11 4.94 5.07 6.27 7.26 10.08 7.54 6.05 7.28 17.60
A ns ns ns * * * ns ns * ns * * ns ns ns
B ns ns ns * ns ns ns ns ns ns ns ns ns ns ns
A*B ns ns ns * ns ns ns ns * ns * ns ns ns ns
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
189
Table 3: The effects of pre-irradiated treatment and low-dose irradiation to the rate and degree of pericarp browning, the rate and degree of disease,
the weight loss of rambutan (storaged in 130C, RH 80-85%)
Dose
(A)
Pre-radiated
(B)
The rate of pericarp
browning
(%)
The degree of
pericarp browning
(score)
The rate of disease
(%)
The degree of disease
(score)
The weight loss
(%)
8th
12th
16th
8th
12th
16th
8th
12th
16th
8th
12th
16th
8th
12th
16th
300 Gy Control 2.50 6.67 15.83ab 0.05 0.8ab 2.7ab 18.43 25.83 98.33 0.33 3.63 4.87a 1.10 2.22 2.89bc
T0 + MCP 0.00 4.17 5.00b 0.00 0.5ab 1.8ab 18.07 21.67 95.83 0.25 3.31 4.42ab 1.15 2.20 3.27ab
T0 + Ca/A.C 0.00 0.00 4.94b 0.00 0b 0.6b 8.83 13.27 74.17 0.16 2.34 3.88b 1.09 1.62 1.96d
T0 + Ca/A.C
+ MCP 0.00 1.67 5.00b 0.00 0b 0.7b 9.93 23.33 87.50 0.20 2.75 4.69a 0.64 1.24 2.08cd
400 Gy Control 2.50 4.17 25.00a 0.06a 2.4a 4.8a 20.23 40 100 0.55 3.75 4.93a 0.78 1.95 3.13b
T0 + MCP 0.83 1.67ab 5.83b 0.00 1ab 2.1ab 18.33 25.83 95.83 0.28 3.21 4.55ab 0.98 1.91 3.23ab
T0 + Ca/A.C 0.00 0.00 5.00b 0.00 0.4b 0.7b 10.87 14.19 98.33 0.17 3.34 4.83a 1.18 2.15 4.07a
T0 + Ca/A.C
+ MCP 0.00 0.00 10.00b 0.00 0.5ab 2.2ab 12.42 17.50 90.83 0.27 2.82 4.89a 0.97 1.53 2.87bc
CV (%) 29.97 27.66 34.74 29.73 27.8
6
19.69 17.75 57.97 6.88 33.65 12.90 9.09 38.18 36.34 17.10
A ns ns ns ns ns ns ns ns ns ns ns ns ns ns *
B ns * * ns * * ns * ns ns * ns ns ns *
A*B ns ns * ns ns * ns * ns ns * ns ns ns *
VINATOM-AR 13--25
The Annual Report for 2013, VINATOM
190
Table 4: The effects of pre-radiated treatment and low-dose irradiated to the soluble solids, the titratable acidity, the ascorbic acid content, the
external color of pericarp (L* and a
*) and the rate of membrane ion leakage of rambutan (storaged in 13
0C, RH 80-85%).
Dose
(A)
Pre-radiated
(B)
The soluble
solids (0Brix)
The titratable
acidity (%)
The ascorbic acid
content (mg.100g-1
)
L* a
* The rate of membrane
ion leakage (%)
8th
12th
8th
12th
8th
12th
8th
12th
16th
8th
12th
16th
8th
12th
16th
300 Gy Control 16.73 16.00 0.79 0.85 4.70 2.89 34.23 29.26 26.54 22.54 15.77 14.31 48.37 56.69 64,92
T0 + MCP 17.27 16.67 0.81 0.77 4.43 3.56 36.33 32.73 25.02 21.06 19.62 13.53 43.17 54.77 56,49
T0 + Ca/A.C 17.47 17.00 0.84 0.73 5.77 5.07 37.85 34.09 29.77 26.21 20.25 15.99 42.50 53.23 53,64
T0 + Ca/A.C
+ MCP 17.00 16.80 0.83 0.82 4.43 3.59 37.50 32.16 25.99 24.85 19.95 14.12 44.69 55.96 57,03
400 Gy Control 16.93 16.07 0.83 0.85 4.36 3.39 34.39 29.54 25.13 23.32 20.25 13.91 48.12 61.50 63,09
T0 + MCP 16.93 16.47 0.82 0.82 4.43 3.40 37.37 28.53 26.74 22.53 18.20 13.64 48.41 61.33 63,96
T0 + Ca/A.C 17.00 16.60 0.85 0.77 4.36 4.09 36.49 26.82 25.75 22.03 18.47 13.44 45.45 56.59 57,53
T0 + Ca/A.C
+ MCP 16.90 16.40 0.83 0.83 4.70 3.39 35.38 25.91 25.73 21.09 16.02 11.50 45.22 57.33 62,27
CV(%) 1.31 2.55 4.37 4.55 12.01 18.83 4.00 5.81 6.92 6.96 8.30 12.20 7.07 5.87 6.28
A ns ns ns ns ns ns * * * * ns ns ns * *
B * * ns ns ns * ns * * * * ns ns ns *
A*B ns * ns ns ns * * * * * * ns ns * *
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
191
RESEARCH AND ESTABLISHMENT OF THE ANALYTICAL
PROCEDURE FOR/OF Sr-90 IN MILK SAMPLES
, , Duong Duc Thang, Nguyen Thi Linh and Bui Thi Anh Duong
Center for Radiation Protection and Environmental Monitoring,
Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 - Hoang Quoc Viet, Ha Noi
ABSTRACT: Sr-90 is an indicator for the transfer radionuclides from environment to human. This work was
setup to build a procedure for Sr-90 determination in main popular foodstuff and focus to fresh milk. The deal
of this work was establish procedure for Sr-90, assessment for chemical yield and test sample of Vietnam
fresh milk, also in this work, the QA,QC for the procedure was carried out using standard sample of IAEA.
The work has been completed for the procedure of determination Sr-90 in milk. The chemical yield of recovery
for Y- 90 and Sr-90 were at 46.76 % ±1.25% and 0.78 ± 0.086, respectively. The QA & QC program was
carried out using reference material IAEA -373. The result parse is appropriate equally and well agreement
with the certificate value. Three reference samples were analyses with 15 measurements. The results of Sr-90
concentration after processing statistics given a value at 3.69 Bq/kg with uncertainty of 0.23 Bq/kg. The
certificate of IAEA-154 for Sr-90 (half live 28.8 year) is the 6.9 Bq/kg, with the range 95% Confidence
Interval as (6.0-8.0 ) Bq/kg at 31st August 1987. After Adjusting decay, the radioactivity at this time is 3.67
Bq/kg. It means that such the result of this work was perfect matching the value of stock index IAEA. Five
Vietnam fresh milk samples were analyzed for Sr-90, the specific radioactivity of Sr-90 in milk were in a range
from 0.032 to 0.041 Bq/l.
Keyword: Milk, Sr-90, chemical procedure.
1. INTRODUCTION
Approximately 99% of Sr-90 in the environment is due to the nuclear tests (16.8 million
curies to 1980) and the second largest amount is from the Chernobyl nuclear power plant accident
(216 million curies) had spread in atmosphere. Sr-90 enters the human body through the ingestion
and inhalation. Sr-90 is an indicator for the transfer radionuclides from environment to human.
The nations of the world have the radiation monitoring program regularly Sr-90 in various
subjects, such as soil, vegetables, milk and water over the whole country and especially around the
area nuclear power plants. The Sr-90 activity in every monitoring points and stations had been
reports each year to government.
The principle of Sr-90 analysis is determine the activity of 90
Sr through radioactivity of its
daughter isotopes, 90
Y (β-ray), after separation Sr-90 from the components in the sample,
subsequent samples to accumulate until it reaches equilibrium 90
Sr - 90
Y (about two weeks) and
measurement Y-90 in the form of Y2(C2O4)3 using low level Beta counting.
The Sr-90 radioactivity calculated by following equation:
Project information:
- Code: CS/13/04-04
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 12 months (Jan 2013-Dec 2013)
- Contact email:
- Paper published in related to the project: (None)
Tran Thi Tuyet Mai
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
192
Sr
SrSrYE
nnAA90
100100
60
1)(
2
009090
where: n0 n0 : count rate of 90
Y at the time separation from 90
Y/90
Sr (cpm)
E2: efficiency count compared with standard sources (%).
SrY90 : Efficiency separating of
90Sr (%).
2. SAMPLING AND PROCESS ANALYSIS
2.1. Sampling and sample preparation
Fresh milk samples are often preserved with formaldehyde (HCHO) or sodium azide
(NaN3) and stored to obtain 90
Y in the cases where 90
Sr and 89
Sr must be determined. Samples
were ashes at 450oC temperature of about 12 hours to decompose the organic compounds. Add to
form a carrying amount of Sr2+
stable. Carriers, Strontium in the sample were extracted with
concentrated hydrochloric acid solution. Finally SrCO3 precipitate dried weight to determine the
chemical separation of 90
Sr performance. 90
Sr activity was determined by measuring the isotope
separation and its progeny is 90
Y.
2.2. Procedure
A. Prepare:
Chemicals
Carriers Sr2+
10mg/ml
Carriers Y3+
10mg/ml
HCL Solution 6M, 3M, 0.5M
Crystal H2C2O4
The solution (NH4)2C2O4; solution of (NH4)2C2O4 saturation
NH4OH Solution 25%
NaOH Solution 6M
Solution marks isotope 85
Sr (10 Bq/ml)
CH3COONH4 Solution 2M
Methyl alcohol
Solution (NH4)2CO3 saturation
PH indicator paper
Distilled.
Tools
Electric stove
Flask, heat-resistant glass, glass rod
Filter funnels filter paper
Ceramic cup
Desiccators
Ion exchange column (diameter 20mm, h=190mm)
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
193
Pipet, micropipette.
Equipment
Analytical balance
pH measuring machine
Drying cabinet, centrifuges, and furnaces.
Total beta measuring machine such as PIC Model 9300, designed to fit the measurements of
low level radiation. Solid Geometry sample, sample tray diameter 50mm, range beta radiation
energy of 50 3000 keV, background count rate for 0.5 channel beta counting pulses/min. Relative
performance of about 50%.
Ion exchange resin: type cation exchange resin DOWEX 50 - X8 (100-200 mesh).
Plastic glasses were soaked in distilled water, stir and let stand, decant water.
Add 1 volume of 6M HCl by volume of resin, and stirred for 15 minutes; then decant the
water.
Wash the resin with water, the process is repeated until pH = 7.
Plastic treated with 6M NaOH, then rinsed with distilled water to pH = 7.
Pour the resin into the column (diameter 10 mm 26cm).
Preparing the form of H +: A volume equal to 10 times the volume of heavy plastic over the
column, then rinse with water. After all of the above procedures, the column can be used to analyze
samples.
Recycling with 6M HCl 500ml and 300ml distilled water; reusable plastic column.
B. Principle analyses:
Take about 10 g ash sample into a 500ml beaker.
Add 5 ml carrier solution SR2+
(10mg Sr2+
/ml). Add 20 ml of concentrated nitric acid
(HNO3); heat to dryness; add acid mixture HCL and HNO3 with a 2:1 ratio.
Heat to dryness the solution to about 1/3 then diluted to 700ml by distilled water, heated at
80oC temperature.
Add 10g H2C2O4, then add little NH4OH and adjust the pH from 4 to 4.2. Heat for a few
hours to complete precipitation; cooling the solution (test by giving one by one drop of (NH4)2C2O4
into filtrate, if there precipitate repeat this procedure).
Filtering the precipitate, wash the precipitate three times with a solution of (NH4)2C2O4
0.02M. Transfer precipitate and filter paper into porcelain cup. Furnace at 6000C for 3 hours.
Dissolve the ash with 3M HCl, transfer the filtrate into a 200ml beaker. Heat the filtrate to
dryness on hot plate. Dissolve the residue in 100 to 150ml 0.5M HCl, this is sample solution.
Pour the sample solution into exchange column; add about 30 ml of distilled water with a
flow rate of 2-3 ml/min. Removed the sample solution after through the exchange column.
Desorption Ca2+
by 250ml (CH3COONH4 2M and CH3OH; volume ratio 1:1) solution with
a flow rate of 2-3 ml/min.
Desorption Sr2+
by 200ml (CH3COONH4 2M) solution with a flow rate 2-3 ml/min.
Evaporating eluent solution SR2+
to about half, adjusting pH = 9 by add NH4OH (no CO2).
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
194
Add 10ml saturated (NH4)2CO3 solution, heated on hot plate for a few minutes to form
SrCO3 precipitation.
Filtering the precipitate, record time, washed with a small amount of 0.1M NH4OH solution.
Dissolve the precipitate with 2M HCl. Using Gamma spectrometry to determine the Sr2+
separation
efficiency by measuring 85
Sr . Add 1 ml of Y3+
, and to accumulate for 14 days.
Add NH4OH (no CO2), adjust pH = 8, to form Y(OH)3 precipitate; record time separated Y
from Sr; filter and wash with dilute ammonia.
Add 1ml Sr2+
as a store carrier. Repeat to form Y(OH)3 precipitation.
Dissolve the precipitate with 2M HCl; heat and add H2C2O4 2g (adjust pH = 1-1.5 by
NH4OH to form Y2(C2O4)3 precipitation.
Filter and dry the precipitation.
Measuring and counting on low background beta spectrometry.
3. RESULTS AND DISCUSSION
After equilibrium, the Y-90 of standard sample was separated from Sr-90 in the form of
Y2(C2O4)3 and the decay of Y-90 by the time (haft live 64h) was checked using low level Beta
counting. The count per minute vs. the time was shown in picture 1.
y = 9.4529e-0.0105x
R2 = 0.9914
1
10
0 20 40 60 80 100 120
Thôøi gian, giôø
So
á ñe
ám/p
hu
ùt
Figure 1: Decay of 90
Y maternal separation.
Efficiency Split Y-90 (chemical yield) is the 46.8% with standard deviation is the 1.2%.
And Chemical separation Efficiency of Sr-90 is the average 78.5% ± 2%. The specific
activities of Sr-90 milk samples were calculated and corrected decay time, the results are described
in Table 1. The parameters of chemical procedure were shown in table 2.
Table 1: Results of milk sample activity measured at the time of measurement.
Sample
name
carrier
Y3+
ml
Measurement sample of date
Date
receipt of
samples
Activity Error
Date,
Month Hour Min
BL* SD
M01 10 11/6/13 10 0 6/30/2013 0.0299 0.0038
M01 10 11/6/13 10 0 6/30/2013 0.0427 0.0034
Count p
er min
ute
Time, h
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
195
M02 10 11/6/13 9 29 8/30/2013 0.0428 0.0033
M02 10 11/6/13 9 29 8/30/2013 0.0288 0.0040
M03 10 11/4/13 11 28 6/30/2013 0.0468 0.0034
M03 10 11/4/13 11 28 6/30/2013 0.0359 0.0037
M04 10 11/4/13 13 59 6/30/2013 0.0575 0.0044
M04 10 11/4/13 13 59 6/30/2013 0.0488 0.0035
M05 10 11/6/13 10 4 8/30/2013 0.0349 0.0037
M05 10 11/6/13 10 4 8/30/2013 0.0471 0.0034
* Blank sample.
Table 2: The processing parameters Sr-90 in milk samples.
Sample
name
Volume,
liter
Date
collecting
Mash,
g
Efficiency
of
separation
Error Date
cumulative
The number
of days
accumulated
Equilib
rium
Sr/Y
M01 1.3 30/6/201
3 10.7 0.89 ± 0.02 22/10/2013 129 1
M02 1.35 30/6/201
3 11 0.85 ± 0.02 22/10/2013 68 1
M03 1.35 30/6/201
3 12 0.76 ± 0.02 22/10/2013 127 1
M04 1.5 30/8/201
3 11.5 0.77 ± 0.02 22/10/2013 127 1
M05 1.5 30/8/201
3 13.2 0.66 ± 0.02 22/10/2013 68.00 1
After adjusting the volume of the sample, the measured activity was converted to the
specific activity in Bq/liter with 2σ uncertainties (Table 3).
Table 3: Results of analysis of the average specific activity
of Sr-90 in milk of Vietnam samples.
Sample
name Average activity, Bq Error
Average specific activity
Bq/liter Uncertainty
M01 0.036 0.006 0.032 0.011
M02 0.036 0.007 0.031 0.012
M03 0.041 0.005 0.040 0.011
M04 0.053 0.006 0.046 0.010
M05 0.041 0.006 0.041 0.013
VINATOM-AR 13--26
The Annual Report for 2013, VINATOM
196
4. CONCLUSION
- The work has been completed for the procedure of determination Sr-90 in milk. The
chemical yield of recovery for Y-90 and Sr-90 were at 46.76 % ±1.25% and 0.78 ± 0.086,
respectively.
- The QA & QC program was carried out using reference material IAEA -373. The result
parse is appropriate equally and well agreement with the certificate value.
- Three reference samples were analyses with 15 measurements. The results of Sr-90
concentration after processing statistics given a value at 3.69 Bq/kg with uncertainty of 0.23 Bq/kg.
The certificate of IAEA-154 for Sr-90 (half live 28.8 year) is the 6.9 Bq/kg, with the range 95%
Confidence Interval as (6.0-8.0) Bq/kg at 31st August 1987. After Adjusting decay, the
radioactivity at this time is 3.67 Bq/kg. It means that such the result of this work was perfect
matching the value of stock index IAEA.
- Five Vietnam fresh milk samples were analyzed for Sr-90, the specific radioactivity of
Sr-90 in milk were in a range from 0.032 to 0.041 Bq/l.
Acknowledgments
The project was completed under the sponsorship of the Institute for Nuclear Science and
Technology, Institute of Atomic Energy, Ministry of Science and Technology, 2013 base level
project.
REFERENCES
[1] [1] VANEY, B., FRIEDLI, C., GEERING, J.J., LERCH, P., Rapid trace determination of
radio strontium in milk and drinking water, J. Radioanal. Nucl.Chem, Articles, 134(1), pp.
87-95, 1989.
[2] [2] BARATTA, E.J., Strontium-89 and strontium-90 in milk, in Horwitz W. (Ed.),Official
methods of analysis of AOAC International, 17th edn. AOAC International, Gaithersburg,
Maryland, USA, chapter 13, 3-6, 2000.
[3] [3] MELIN, J., SUOMELA, J., Rapid determination of 89
Sr and 90
Sr in food and
environmental samples by Cerenkov counting: In Rapid Instrumental and Separation
Methods for Monitoring Radionuclides in Food and Environmental Samples, Final Report on
an IAEA Co-ordinated Research Program, International Atomic Energy Agency,
IAEA/AL/088, Vienna, Austria, 1995.
[4] [4] BRUN, S., KERGADALLAN, Y., BOURSIER, B., FREMY, J., JANIN, F.,
Methodology for determination of radio strontium in milk: a review, Lait 83, pp.1-15, 2003.
[5] [5] BRUN, S., BESSAC, S., URIDAT, D., BOURSIER, B., Rapid method for determination
of radio strontium in milk. Radioanal, Nucl. Chem., 253(2), pp.191-197, 2002.
[6] [6] HONG, K.H., CHO, Y.H., LEE, M.H., CHOI, G.S., LEE, C.W., Simultaneous
measurement of 89Sr and 90Sr in aqueous samples by liquid scintilla counting using the
spectrum unfolding method, Appl. Radiat. Iso., 54, pp. 299-305, 2001.
[7] [7] HEILGEIST, M, Use of extraction chromatography, ion chromatography and liquid
scintillation spectrometry for rapid determination of strontium-89 andstrontium-90 in food in
cases of increased release of radionuclides, Radioanal,Nucl. Chem, 245(2), pp. 249-254,
2000.
[8] [8] CHOBOLA, R., MELL, P., DAROCZI, L., VINCZE, A., Rapid determination of radio
strontium isotopes in sampe of NNP origin, J. Radioanal, Nucl. Chem., 267(2), pp.297-304,
2006.
[9] [9] EIKENBERG, J., BEER, H., RÜTHI, M., ZUMSTEG, I., VETTER, A., Precise
determination of 89Sr and 90Sr/90Y in various matrices: The LSC 3-window approach, in:
Chalupnik, S., Schőnhofer, F., Noakes, J. (Eds), LSC2005, Advances in liquid scintillation
spectrometry, Radiocarbon, Arizona, USA, pp.237-249, 2005.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
197
PRELIMINARY ASSESSMENT ABOUT GENETIC DIVERSITY,
THE STABILITY OF POTENTIAL MUTANTS FROM TWO VARIETIES
OF CHRYSANTHEMUM MORIFOLIUM RAMAT. (BRONZE DOA
AND PURPLE FARM) VIA GAMMA IRRADIATION
Nguyen Tuong Mien, Le Ngoc Trieu, Le Tien Thanh,
Pham Van Nhi and Huynh Thi Trung
Center for Applications of Nuclear Technique in Industry, Vietnam Atomic Energy Institute
ABSTRACT: The objects of radiation breeding were chosen, collected and in vitro propagated. The suitable
modalities for acute and chronic irradiation the materials were determined. Two acute and one chronic
irradiation series were executed. Thus, the irradiated materials were achieved to screening for the mutants. In
this study, on farm, through screening 18 phenotypic mutants of both chrysanthemums were recorded and
collected including 6 potential mutants that selected for next research based on their phenotypic differences to
the originals, their aesthetic and low mosaic. These 6 potential mutants together with their original varieties
were micro-propagated to induce the potential mutant lines for estimation on farm of mutant characteristic
segregation rates. Six potential mutant lines of E2a, E2c, E28, E29, I7, I8 are morphologically and genetically
different to their original varieties, possess the identification markers and aestheticism. They were
morphologically stable on farm through 3 series of growing on farm at M1V3, M1V5 and M1V7 generations.
In the genetic respect, they possessed the high stabilities through in vitro generations. All of these criteria show
that, these mutant lines were already to be registered as temporary cultivars/varieties.
I. INTRODUCTION
Chrysanthemum morifolium Ramat is in great demand and widespread in Vietnam as well as
in the world. Most of current cultivated chrysanthemum varieties in Dalat city were imported from
Holland and other neighboring countries. Therefore, it’s necessary to domestically create new
varieties for chrysanthemum cultivation in Dalat to overcome the commercial barriers related to
copyright and local agriculture improvement. Mutation breeding in general and Radiation breeding
in particular allow to obtain new chrysanthemum varieties/lines that differentiated from the
originals in single or multiple phenotypic characteristics such as the color or shape, which
determine their decorative values in relatively short time. The traditional breeding methods like
crossing, screening from nature have been limited in species scope. In most cases of
chrysanthemum, main effect of mutagens on exposed materials were changing color of the
inflorescence, the changes of plant habit or changes in the shape and size of leaves and
inflorescence or the number and of ligulate florets were observed at less frequently. [Banerji and
Datta 1990, Zalewska 2001, Zalewska 2010].
In mutation radiation breeding, both in vivo materials such as shoots, leaves, cutting and/or
whole plants and in vitro materials such as callus, tissue, suspensions of cells, protoplasts etc. have
been used for irradiation treatment. In this study, artificial seeds were used as material for gamma
irradiation to induce mutant base on previous researches of self-authors with the purpose of genetic
diversity and stability estimation of induced mutant lines subsequently.
Project information:
- Code: CS/13/06-03
- Managerial Level: Institute
- Allocated Fund: 80,000,000 VND
- Implementation time: 14 months (May 2013 - Jun 2014)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
198
In the first phase study, on farm, through screening 18 phenotypic mutants of both
chrysanthemums were recorded and collected including 6 potential mutants that selected for next
research based on their phenotypic differences to the originals, their aesthetic and low mosaic.
These 6 potential mutants together with their original varieties were micro-propagated to induce the
potential mutant lines for estimation on farm of mutant characteristic segregation rates.
II. OVERALL GOAL AND MAIN CONTENTS
The aim of this study was to demonstrate the mutant generation effects of gamma rays on
chrysanthemum artificial seeds to establish the scientific base for application this technique in
similar objects.
Three main activities:
+ Micropropagation to induce the potential mutant lines for estimation on farm of mutant
characteristic segregation rates.
+ Genetic diversity estimation in potential mutant lines, determine the genetic differences
among mutant lines and their original cultivars.
+ Outstanding mutant lines genetic stability estimation through in vitro generations.
III. MATERIAL AND METHOD
The objects of investigation are two varieties of chrysanthemum belong to Chrysanthemum
morifolium Ramat species, which one possesses copper and another possesses purple color
inflorescence, these two varieties are different in structure petals (pictures below).
Bronze chrysanthemum. Purple chrysanthemum.
In the first phase study, on farm, through screening 18 phenotypic mutants of both
chrysanthemums were recorded and collected including 6 potential mutants that selected for next
research based on their phenotypic differences to the originals, their aesthetic and low mosaic.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
199
Table 1: Six potential mutants that seclected in the firsrt phase.
These 6 potential mutants together with their original varieties were micro-propagated to
induce the potential mutant lines for estimation on farm of mutant characteristic segregation rates.
In the third generation, after four weeks for growth, the in vitro plants were injected into the fresh
MS medium for 2 weeks for rooting and complete formed plantlets induction.
The completed in vitro plantlets were transferred to ex vitro condition and injected into foam
trays filled with substrate of treated soil, investigate to screen the arisen phenotypic changes if any
during greenhouse stage and record the survival rate of plantlets after 30 days.
Next to the greenhouse stage, the survival plantlets were transplanted into soil-beds in
plastic house with the modified modality of commercial cultivation protocol for chrysanthemum of
CANTI (plants were only exposed to natural photoperiod, without supplementary illumination).
Planted chrysanthemum in plastic house were followed and recorded for criteria of survival
rate, arisen phenotypic mutant characteristics such as color and shape and structure of
inflorescences and leaves, stem’s height etc. compared to the controls (non-irradiated originals)
during the cultivation until completely blooming. The recorded phenotypic mutants will be
collected for micro-propagation.
Potential phenotypic mutants will be selected from all of screened phenotypic mutants if
they possess the obviously different from the controls about color or structure of inflorescences,
good aestheticism and low mosaic.
In the genetic respect, they possessed the high stabilities through in vitro generations. All of
these criteria show that, these mutant lines were already to be registered as temporary
cultivars/varieties.
No Sign
al
Gamma
Dose (Gy)
Charac-
teristic
The first selection
Picture No Signal
Gamma
Dose (Gy)
Charac-
teristic
The first selection
Picture
1 I8 40
Fresh
yellow,
short and
uncurled
petal
4 E2 20 Quill 2
2 I9 40
Yellow,
appear 1or
2 extra petal
5 E28 40 Light purple
3 I7 30 Fresh
yellow
6 E29 40 White with
light purple
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
200
IV. RESULT AND DISCUSSION
1. Micropropagation to induce the potential mutant lines for estimation on farm of
mutant characteristic segregation rates
On the sixth week at thirth generation were done by in vitro microcutting method into the
fresh MS medium. The completed regenerated in vitro plants were planted out into a permanent
place on foam trays filled with substrate of treated soil, estimate the number of survival plantlets
after 30 days. After that, they were transferred into soil-beds, chrysanthemum were growth exposed
to natural photoperiod, applying the standard method.
There was no difference in the development of plants between the mutant/mutant lines and
their original varieties and also no more morphological alteration appeared in the third series of
growing to estimate the mutant morphological stability.
Recorded data indicated that:
- In on farm M1V3 generation, mutant lines of E2a, E2c, E28, E29, I7, I8, E were not
segregated; only 1.2% of individuals in I9 line maintained the mutant forms. Collating to the criteria
to limit the quantity of mutant lines for corresponding to the whole task’s scope, I9 line were not
selected the samples to transfer to in vitro condition for next propagation and breeding. However,
the leaf samples from the individuals that kept mutant morphological characteristic were collected
to extract DNA for genetic analysis.
2. Genetic diversity estimation in potential mutant lines, determine the genetic
differences among mutant lines and their original cultivars
Genomic DNA was isolated from fresh and young leaves of 6 potential mutants with 2
original ones using standard CTAB (Cetyl trimethyl ammonium bromide) method with little
modification. Insoluble polyvinyl polypyrrolidone (PVP) was added to the leaf tissue prior to
grinding. The RNA was removed by giving RNase A (MBI Fermentas, Lithuania) treatment. The
dried DNA was dissolved in minimum amount of dH2O. DNA’s purity degree (OD 260/280) is in
from 1.7 to 2.1 was utilized for RAPD analysis with 22 random decamer oligonucleotide primers as
table below.
Primer Sequence Nu (5’-3’) STT Primer Sequence Nu (5’-3’)
1 BIO27 TGGGCTCGCT 12 OPN6 GAGACGCACA
2 OPC2 GTGAGGCGTG 13 OPN7 CAGCCCAGAG
3 OPA1 CAGGCCCTTC 14 OPN10 ACAACTGGGG
4 OPA2 TGCCGAGCTG 15 OPN13 AGCGTCACTC
5 OPA18 AGGTGACCGT 16 OPM9 GTCTTGCGGA
6 OPA4 AATCGGGCTG 17 S300 AGCCGTGGAA
7 OPA15 TTCCGAACCC 18 S201 GGGCCACTCA
8 OPA6 GGTCCCTGAC 19 UBC728 GTGGGTGGTG
9 OPC10 TGTCTGGGTG 20 OPM9 GTCTTGCGGA
10 OPC11 AAAGTCGCGG 21 OPM18 CACCATCCGT
11 OPC14 TGCGTGCTTG 22 OPN5 ACTGAACGCC
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
201
PCR technique: The reaction is observed with cocktail including: DNA sample 25ng, buffer
solution PCR 1X, MgCl2 2mM, dNTP 10µM, Taq polymerase 1U, primer RAPD 1µM and add
dH2O to 15µl for reaction volume.
PCR Cycle:
Stage Reaction Temp (oC) Time Cycle
1 Denaturation 95 5 minute 1
2 Denaturation 95 1 minute
40 3 Annealing 35 1 minute 30 second
4 Polymerization 72 1 minute 45 second
5 Polymerization Final 72 7 minute 1
6 Final 4 1
After the completion of the PCR, 2.5ul of 6x loading dye (MBI Fermentas, Lithuania) was
added to the amplified product and was resolved in 1.5% agarose gel stained with 0.5 ug/mL
ethidium bromide (Sigma,USA).
As the result showed that 11 primes did not give satisfactory amplification, so were not
considered further. Nine primes resulted in the amplification of distinct and producible bands in the
present investigation. All the primers gave wide range of fragments ranging from 200-2000bp. The
highest number of fragments (11) was amplified by primer S201 and OPA 02, the lowest (03) by
the primer BIO 27.
The research results show that among two original cultivars, among each original cultivar
and potential mutant lines induced from it, among all potential mutant lines together with all two
original cultivars were virtually different in genetic. The highest level of genetic difference among 8
investigated samples was 0.902 and the lowest was 0.443.
Although the mutant lines possessed the genetic differences to their original cultivar, these
genetic variations didn’t exceed the genetic limit of group including the original cultivar and the
induced mutant lines from it.
Figure 1: PCR-RAPD primer BIO 27.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
202
Figure 2: PCR-RAPD primer UBC 728.
Table 2: Homologous genetic coefficient among potential
mutants and original ones.
E2a E2c E28 E29 E I7 I8 I
E2a
1.000
E2c
0.738
1.000
E28
0.770
0.836
1.000
E29
0.689
0.721
0.656
1.000
E
0.672
0.902
0.902
0.689
1.000
I7
0.656
0.557
0.590
0.508
0.557
1.000
I8
0.623
0.492
0.557
0.443
0.525
0.803
1.000
I
0.623
0.557
0.525
0.475
0.525
0.803
0.869
1.000
Analysis by the program NTSys 2.1, this is the dendrogram showing homologous genetic
relationship among in vitro generations of potential mutants with their original ones as below.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
203
Figure 3: Dendrogram showing homologous genetic relationship among
in vitro generations of potential mutants with their original ones.
Analyzing DNA fingerprinting induced by RAPD-PCR not only helped to estimate the level
of difference among original cultivars and the potential mutant lines induced from them but could
be used to identify the mutants lines or groups of each original cultivar and the potential mutant
lines induced from it. These data are necessary for protecting and registering the new cultivars in
the future.
3. Outstanding mutant lines genetic stability estimation through in vitro generations
Genomic DNA was isolated from fresh and young leaves of 6 in vitro potential mutants with
2 original ones at M1V3; M1V5, M1V7. DNA fingerprinting from extracted DNA samples were
induced by RAPD-PCR technique, results of genetic analysis by NTSys software indicate that:
The similarity coefficients among 24 investigated samples fluctuated from 0.55 to 1.00. The
highest similarity coefficients appeared in almost samples that were same lines but different in in
vitro generation.
There is no different so much between the results of similarity coefficient when comparing
the nonhomogeneous samples from one potential mutant with samples belong to two original
chrysanthemum.
In general, the genetic stabilities of all six potential mutant lines and original cultivars were
high. However, with E28 the homology in gene between M1V3 and M1V5 generation is absolute, it
means there is the convulsion in gene at M1V7 but no so much (only 2%).
Figure 4: Dendrogram showing stable genetic relationship
among in vitro.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
204
E2a-
a
E2a-
b
E2a-
c
E2c-
a
E2c-
b
E2c-
c
E28-
a
E28-
b
E28-
c
E29-
a
E29-
b
E29-
c
E-
a
E-
b
E-
c
I7-
a
I7-
b
I7-
c
I8-
a
I8-
b
I8-
c
I-
a
I-
b
I-
c
E2a-a
1.00
E2a-b
1.00
1.00
E2a-c
1.00
1.00
1.00
E2c-a
0.74
0.74
0.74
1.00
E2c-b
0.74
0.74
0.74
1.00
1.00
E2c-c
0.74
0.74
0.74
1.00
1.00
1.00
E28-a
0.77
0.77
0.77
0.84
0.84
0.84
1.00
E28-b
0.77
0.77
0.77
0.84
0.84
0.84
1.00
1.00
E28-c
0.79
0.79
0.79
0.85
0.85
0.85
0.98
0.98
1.00
E29-a
0.69
0.69
0.69
0.72
0.72
0.72
0.66
0.66
0.67
1.00
E29-b
0.69
0.69
0.69
0.72
0.72
0.72
0.66
0.66
0.67
1.00
1.00
E29-c
0.69
0.69
0.69
0.72
0.72
0.72
0.66
0.66
0.67
1.00
1.00
1.00
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
205
E-a
0.67
0.67
0.67
0.90
0.90
0.90
0.90
0.90
0.89
0.69
0.69
0.69
1.00
E-b
0.67
0.67
0.67
0.90
0.90
0.90
0.90
0.90
0.89
0.69
0.69
0.69
1.00
1.00
E-c
0.67
0.67
0.67
0.90
0.90
0.90
0.90
0.90
0.89
0.69
0.69
0.69
1.00
1.00
1.00
I7-a
0.66
0.66
0.66
0.56
0.56
0.56
0.59
0.59
0.61
0.51
0.51
0.51
0.56
0.56
0.56
1.00
I7-b
0.66
0.66
0.66
0.56
0.56
0.56
0.59
0.59
0.61
0.51
0.51
0.51
0.56
0.56
0.56
1.00
1.00
I7-c
0.66
0.66
0.66
0.56
0.56
0.56
0.59
0.59
0.61
0.51
0.51
0.51
0.56
0.56
0.56
1.00
1.00
1.00
I8-a
0.62
0.62
0.62
0.49
0.49
0.49
0.56
0.56
0.57
0.44
0.44
0.44
0.52
0.52
0.52
0.80
0.80
0.80
1.00
I8-b
0.62
0.62
0.62
0.49
0.49
0.49
0.56
0.56
0.57
0.44
0.44
0.44
0.52
0.52
0.52
0.80
0.80
0.80
1.00
1.00
I8-c
0.62
0.62
0.62
0.49
0.49
0.49
0.56
0.56
0.57
0.44
0.44
0.44
0.52
0.52
0.52
0.80
0.80
0.80
1.00
1.00
1.00
I-a
0.62
0.62
0.62
0.56
0.56
0.56
0.52
0.52
0.54
0.48
0.48
0.48
0.52
0.52
0.52
0.80
0.80
0.80
0.87
0.87
0.87
1.00
I-b
0.62
0.62
0.62
0.56
0.56
0.56
0.52
0.52
0.54
0.48
0.48
0.48
0.52
0.52
0.52
0.80
0.80
0.80
0.87
0.87
0.87
1.00
1.00
I-c
0.62
0.62
0.62
0.56
0.56
0.56
0.52
0.52
0.54
0.48
0.48
0.48
0.52
0.52
0.52
0.80
0.80
0.80
0.87
0.87
0.87
1.00
1.00
1.00
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
206
I. CONCLUSION
In this study, on farm, through screening 18 phenotypic mutants of both chrysanthemums
were recorded and collected including 6 potential mutants that selected for next research based on
their phenotypic differences to the originals, their aesthetic and low mosaic. These 6 potential
mutants together with their original varieties were micro-propagated to induce the potential mutant
lines for estimation on farm of mutant characteristic segregation rates. 5/6 potential mutant lines
completely kept the mutant phenotype on farm in M1V3 generation.
Among two original varieties, among each original cultivar and potential mutant lines
induced from it, among all potential mutant lines together with all three original cultivars were
virtually different in genetic. Although the mutant lines possessed the genetic differences to their
original cultivars, these genetic variations didn’t exceed the genetic limit of group including each
original cultivar and the induced mutant lines from it.
The genetic stabilities of four outstanding mutant lines and original cultivars through in
vitro generations of M1V3, M1V5, M1V7.
Six potential mutants are morphologically and genetically different to their original
varieties, possess the identification markers and aestheticism. In the genetic respect, they possessed
the high stabilities through in vitro generations. All of these criteria show that, these mutant lines
were already to be registered as temporary cultivars/varieties.
REFERENCES
[1] Harding J., F.Singh, J.N.M. Mol. “Genetics and breeding of Ornamental Spesies”, Kluwer
Academic Publisher, pp. 135-152, 1991.
[2] Harten A.M.V. Mutation breeding in Vegetatively Propagated Crops, Plant breeding and
Genetics section, joint FAO/IAEA, pp.48-53, 1997.
[3] Hitoshi Nakagawa. “Mutation breeding by Gamma Rays”, Presentation about Institute of
Radiation breeding, 2009.
[4] Hitoshi Nakagawa. “Mutation breeding and Biological researchs by the use of Gamma Rays
irradiation in Japan”, Mutation breeding Workshop of FNCA, 2008.
[5] Keichi Takagi, Masanori, Hitashita, Ngoc Trieu Le. “Internal debudding Effects of proton
beams to variegated Petunia”, Annual report, Wakasa Wan Energy Research Centre, 2008.
[6] Kurt Weising, Hilde Nybom, Kirsten Wolff, Gunter Kahl. “DNA fingerprinting-Principles,
methods, and Applications”, CRC Press-Taylor & Francis Group, second edition, 2005.
[7] Watson D.J, Baker T.A., Bell S.P., Gann A., Levine M., Losick R. “Molecular biology of the
gene”. Benjamin/Cummings, San Francisco, USA, 2004.
[8] Zeeshan Abbas, Naheed Ikram, Shahnaz Dawar and Javed Zaki. “Effect of (60 COBALT)
Gamma rays on Growth and root rot diseases in mungbean (Vigna Radiata.L), Pak. J. Bot.,
42(3): 2165-2170, 2010.
[9] Kim, J.H., M.H. Baek, B.Y. Chung, S.G. Wi and J.S. Kim. “Alterations in the
photosynthetic pigments and antioxidant machineries of red pepper (Capsicum annuum .L)
seedlings from Gamma-irradiated seeds”, J. Plant Biol., 47: 314-321. 2004.
[10] Wi, S.G., B.Y. Chung, J.H. Kim, M.H. Baek, D.H. Yang, J.W. Lee and J.S.
Kim..“Ultrastructural changes of cell organelles in Arabidopsis stem after gamma
irradiation”, J. Plant Biol., 48(2): 195-200, 2005.
[11] Barakat M.N., Rania S.A.S. Badr M. and Torky M.G.E. In vitro mutagenesis and
identification of new variants via RAPD markers for improving Chrysanthemum morifolium.
African Journal of Agricultul Research 5 (8): 748-757, 2010.
VINATOM-AR 13--27
The Annual Report for 2013, VINATOM
207
[12] Bhattacharya A. and Teixeira da Silva J.A. Molecular systematics in
Chrysanthemum × grandiflorum (Ramat.) Kitamura. Scientia Horticulturae 109 (4): 379-384,
2006.
[13] Carmen Martín, Uberhuaga E., Pérez C. Application of RAPD markers in characterisation of
Chrysanthemum varieties and the assessment of somaclonal variation. Euphitica 127: 247-
253, 2002.
[14] Nagatomi. S, Miyahira. E. and Degi. K. Induction of flower mutation comparing with
chronic and acute gamma irradiation using tissue culture techniques in Chrysanthemum
Morifolium Ramat. . Acta Hort. (ISHS) 508:69-74, 2000.
[15] Kurt Weising, Hilde Nybom, Kirsten Wolff, Günter Kahl. DNA Fingerprinting in Plants
Principles, Methods, and applications (second Edition). Cpc press taylor & Fancies group,
2005.
[16] Gamma field symposia Number 1-48. Institute of Radiation Breeding-Nias. Hitachi-Ohmiya,
Ibaraki-ken, Japan. (http://www.nias.affrc.go.jp/eng/gfs) 1962-2009.
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
208
ESTABLISHMENT OF ILLUMINATION SYSTEM FOR INVESTIGATION
OF MONOCHROMATIC LIGHTS COMBINATION EFFECTS
ON IN VITRO PLANT GROWTH
Le Tien Thanh, Le Ngoc Trieu, Nguyen Tuong Mien, Huynh Thi Trung and Phan Quoc Minh
Centre for Applications of Nuclear Techniques in Industry, Vietnam Atomic Energy Institute
No.1, DT 723 Street, Da Lat City, Lam Dong Province, Vietnam
ABSTRACT: Super blue and red light LEDs and other electric, electronic components are used to design and
establish 11 independent illumination systems, each system can arbitrarily control to operate at 55 molarities of
illumination which are different from together in monochromatic lights combination and total illumination
intensity based on the microcontrollers. Programs for loading to microcontrollers were created to base on
theoretical calculation and experimental correction. The illumination cycles can be controlled by setting the
timer. These 11 systems and another fluorescent light illumination were used to execute the experiment for
investigation the effects of monochromatic lights combination on in vitro shoot proliferation stage in
Chrysanthemum and Phalaenopsis orchid. Results from this experiment showed that illumination intensity of
400lux is suitable for chrysanthemum, 750lux is suitable for Phalaenopsis orchid and rate of 70% red light –
30% blue light are suitable for both kinds of these plants.
Keyword: Illumination intensity, single wavelength light illumination system, in vitro, LED.
I. INTRODUCTION
Sunlight is the one of most important ecological factors, it supplies the essential energy for
photosynthesis process of natural plants. Artificial light sources are also used in agriculture and
especially in micro-propagation. Up to now, the most popular artificial light sources for plant tissue
culture are fluorescent tubes with light spectrum of 320-380nm, including many unnecessary areas
of plant photosynthesis. Fluorescent tubes posses a short working time, need a large space to set up
and form the high heat in the in vitro incubation room when operating so that a considerable electric
power to regulate the room temperature. Recent studies for other artificial light sources (compact
bulb, LED…) with the goal of electric saving were executed and achieved results are satisfactory.
Combination of monochromatic lights LEDs seems to be the bester one for micro-propagation with
several advantages as small size, high working time, controlled wavelength of emitted lights, low
electric consumption and released heat. In addition, many published studies showed that the single
wavelength illumination system can cause the many positive physiological activations of both ex
vitro and in vitro plants.
With the desire of increasing the quality, reducing the cost of in vitro seedlings and creating
a monochromatic illumination system for research- and application- oriented activities, the task of
“Establishment of Illumination system for investigation of monochromatic lights combination
effects on in vitro plant growth” were promoted. Time for task execution is 2 years (2013 and
2014), contents of the year of 2013 were approve, in this year, it needs to execute the design,
programming, setting up, correcting the LED illumination systems and using the established 11
systems to carry out experiments about investigation the effects of single wavelength lights
combination on in vitro shoot proliferation stage in chrysanthemum and Phalaenopsis orchid.
Project information:
- Code: 36/CS/HĐNV
- Managerial Level: Institute
- Allocated Fund: 100,000,000 VND
- Implementation time: 12 months (May 2013 - Apr 2014)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
209
II. RESULTS FROM THE TASK
1. Design and establish the single wavelength light illumination system
After investigating, task execution team chose two kinds out of current commercial LEDs to
establish the illumination systems. The two chosen kinds of LED possess the compatible light
emitting wavelengths for plant photosynthesis and can be used for arranging together to achieve the
suitable total light density in demanded scope illumination for each system. These are two models
of LEDs from Shenzheng Hanhua Company (China) with basic parameter as below:
Blue LED
Power: 3W, Voltage: 3.6-3.8V
Electric intensity: 700mA
Illumination intensity: 45-50lm
Emitting light wavelength: 470-475nm
Red LED
Power: 3W, Voltage: 2.4-2.6V
Electric intensity: 700mA
Illumination intensity: 80-90lm
Emitting light wavelength: 660-665nm
Figure 1: Images and parameter of chosen blue and red LEDs.
By light intensity experimental measurement, task execution team established a configure to
arrange the LEDs for one of illumination system including two parallel troughs, each trough has a
row of blue LEDs and a row of red LEDs. The distance between each LED on the row is 4cm and
the distance between two same LEDs rows is 24cm. This configure can adapt to relatively
homogeneous and maximum illumination of approximate 1100lux in the demanded surface to be
lighted (36 x 50cm).
Figure 2: Outline of blue and red LEDs arrangement for the monochromatic
lights illumination system.
Task execution team designed and established the electronic control board with two
AT89C51 microcontrollers to control the ON/OFF frequencies of 2N3055/ 2SC5200 power
transistors which supply the electricity to LED system, each microcontroller control the
illumination density of one kind of LEDs. The microcontrollers were loaded with a program that
allows them release different pulses depended on received signals from switch board. The diagram
of electronic control boards and the LED power supply diagram described as below figures:
24cm
7cm
3cm
4cm
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
210
6+5V
Q2
2SC5200
9
1
+5V
R7
0.5 Ohm/5W
14
6
9
R7
0.5 Ohm/5W
1
14
6
R4R
R6
1K
C
R910K
23456789
+
J3
BLUE LED12
13
5
Q1T IP41
Q4
2N3055
15
S1
Reset
-
+ C6
10u
13
5
15
+
Q3
T IP41
13
5
+5V
Cong tac
12345678
161514131211109
R6
560/1W
15
-
12
U2 AT89C52
9
1819
20
2930
31
40
12345678
2122232425262728
1011121314151617
3938373635343332
RST
XTAL2XTAL1
GND
PSENALE/PROG
EA/VPP
VCC
P1.0/T2P1.1/T2-EXP1.2P1.3P1.4P1.5P1.6P1.7
P2.0/A8P2.1/A9
P2.2/A10P2.3/A11P2.4/A12P2.5/A13P2.6/A14P2.7/A15
P3.0/RXDP3.1/TXDP3.2/INT 0P3.3/INT 1P3.4/T0P3.5/T1P3.6/WRP3.7/RD
P0.0/AD0P0.1/AD1P0.2/AD2P0.3/AD3P0.4/AD4P0.5/AD5P0.6/AD6P0.7/AD7
4
+5V
16
R1350K
C
R810K
23456789
12
+24V
4
+24V
16
12
4
+5V
U2 AT89C52
9
1819
20
2930
31
40
12345678
2122232425262728
1011121314151617
3938373635343332
RST
XTAL2XTAL1
GND
PSENALE/PROG
EA/VPP
VCC
P1.0/T2P1.1/T2-EXP1.2P1.3P1.4P1.5P1.6P1.7
P2.0/A8P2.1/A9
P2.2/A10P2.3/A11P2.4/A12P2.5/A13P2.6/A14P2.7/A15
P3.0/RXDP3.1/TXDP3.2/INT 0P3.3/INT 1P3.4/T0P3.5/T1P3.6/WRP3.7/RD
P0.0/AD0P0.1/AD1P0.2/AD2P0.3/AD3P0.4/AD4P0.5/AD5P0.6/AD6P0.7/AD7
16
R5
1K
+5V
Y4
11.059MHz
C
R9
10K
2 3 4 5 6 7 8 9
11
3
+5V
D2
4148
7
+5V
J4
RED LED12
11
R2
10K
3
C7
33p
7
Cong tac
12345678
161514131211109
C8 33p
+5V
D2
4148
11
S1
Reset
3
8
R2
10K
10
Y4
11.059MHz
2
R5
1K
8
C8
33p
+5V
10
C7 33p
2
8
R10
50K
10
2
7
+5V
R6
560/1W
9
C
R910K
23456789
1
+
C6
10u
14
Figure 3: Diagram of electronic control boards for operation
illumination modalities of LED system.
J4
RED LED12
+
R6
560/1W
-
+
R7
0.5 Ohm/5W
-
R1350K
+24V
R6
560/1W
Q2
2SC5200
Q4
2N3055Q1T IP41
R7
0.5 Ohm/5W
Q3
T IP41
+24V
R10
50K
R5
1K
J3
BLUE LED12
R6
1K
Figure 4: Power supply diagram for blue and red LEDs operation.
The programs for microcontroller operation are based on the linear correlation between
illumination intensities and pulse release frequencies from microcontroller, i.e. time for high level
(t1) and low level (t0) of released signal. By theoretical calculation, the task execution team
established two programs to control the operation of red and blue LESs, each program allows the
microcontroller releases pulses at 55 different frequencies based on t0/(t1+t0) rates in
correspondence with 11 illumination intensities in range of 0, 10, 20…90 and 100% at 5 levels of
400, 575, 750, 925 and 1100lux total illumination . These two programs were established in such a
way that when one of 11 switches for red and blue light combination control is turn on together with
one of 5 switches for total illumination intensity, both microcontrollers will simultaneously release
suitable pulses for desired illumination.
After the preliminary Illumination system were established with LEDs, timer, control
system and power supplier, the correction for whole system were executed by experimental
measurement to identify the actual value of light intensity of each illumination modality, adjust the
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
211
impedance of the rheostats and t0/(t1+t0) rates of pulse release from microcontrollers. The system
correction were repeated several times until desire being satisfied. In the result, the suitable two
programs for blue and red LEDs operation control in correspondence with electronic control board
configuration and established LED arrangement were achieved, adapting to the demand for each
light combination rate at each total illumination intensity level.
Figure 5: Control system for LED illumination system.
The corrected preliminary LED illumination system was used as pattern to set up other 10
remains. Each achieved system was operated at each modality of illumination and corrected again
if necessary.
11 LED illumination systems were used to investigate the effect of monochromatic lights on
in vitro plant growth. The demanded illumination space of each system were covered with black
cloth to ensure that it receives the light only from it’s LEDs and avoid the erroneous experiment
results.
Figure 6: 11 LED illumination system were set up on in vitro plant
incubation shelves for experiments.
11 LED illumination systems were set up on 11 shelf blocks and regulated for operation at
11 single wavelength lights combination rates (100% red-0% blue; 90% red-10% blue; …, 10% red
-90% blue and 0% red-100% blue) with highest total illumination intensity level (~1100lux).
Photometer was used to identify the areas that possess the total illumination intensity of ~750lux
and ~ 400lux to arrange the experiments using these two total illumination intensity.
From the top to
bottom:
+ 100% red - 0%
blue;
+ 90% red - 10%
blue;
+ 80% red - 20%
blue;
+ 70% red - 30%
blue;
+ 60% red - 40%
blue;
+ 50% red - 50% blue
From the top to
bottom:
+ 0% red - 100%
blue;
+10% red - 90%
blue;
+ 20% red - 80%
blue;
+ 30% red - 70%
blue;
+ 40% red - 60%
blue
Timer
DC 24V source Electronic control
board
Switches for 5 total
illumination
intensity levels
regulation
Switches for 11
monochromatic
lights combination
rates regulation
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
212
2. Investigation of monochromatic lights combination effects on in vitro shoot
proliferation stage
2.1. Effects of monochromatic lights illumination modalities on in vitro shoot
proliferation stage in chrysanthemum
Stem nodes of in vitro chrysanthemum plants belong to “White Farm” cultivar were grown
in shoot proliferation medium according to the previous protocol of Centre for Application nuclear
techniques in industry (CANTI). Cultured samples were arranged in the incubation conditions of 33
monochromatic lights illumination modalities (integral of the two factors of single wavelength
lights combination rate and total illumination intensity: L1R10, L1R9,…, L1R1, L1R0; L2R10,
L2R9,…, L2R1, L2R0; L3R10, L3R9,…, L3R1, L3R0) with the control experiment lot of
fluorescent tubes. Illumination cycle of 16 hour lighting and 8 hour being dark was used for all
experiment lots.
Four weeks after incubation with experiment conditions, achieved results are presented as
below:
Table 1: Shoot proliferation coefficient, shoot height and morphological characteristics of in vitro
chrysanthemum in different lights illumination modalities after 4 weeks incubation.
Experime
nt lot
Shoot
coefficient
(shoot/cluster)_
)
Shoot height
(cm)
Shoot height and morphological characteristics
Control 2.09 ± 0.28 4.77 ± 0.08 Medium shoot stem; Deep green leaves and stems
L1
R10 2.07 ± 0.20 5.20 ± 0.14 Small shoot stem; pale green leaves and stems (weak
shoots)
R9 2.00 ± 0.13 4.88 ± 0.10 Relatively similar to characteristics from control
R8 2.03 ± 0.17 4.64 ± 0.10
Similar to characteristics from control
R7 2.03 ± 0.23 4.62 ± 0.15
R6 2.07 ± 0.24 4.38 ± 0.13
R5 2.02 ± 0.20 4.26 ± 0.14
R4 2.09 ± 0.24 4.06 ± 0.09
R3 2.04 ± 0.13 3.68 ± 0.08
Plump and dwarf shoot stem; dark green and thick leaves R2 1.98 ± 0.09 3.63± 0.11
R1 2.07 ± 0.15 3.09 ± 0.10
R0 1.98 ± 0.16 2.64 ± 0.07
L2
R10 1.99 ± 0.17 5.21± 0.06 Small shoot stem; pale green leaves and stems (weak
shoots)
R9 2.00 ± 0.16 4.83 ± 0.05 Relatively similar to characteristics from control
R8 2.02 ± 0.22 4.76 ± 0.08
R7 2.04 ± 0.18 4.61 ± 0.10
Similar to characteristics from control R6 2.03 ± 0.23 4.33 ± 0.07
R5 2.04 ± 0.13 4.26 ± 0.10
R4 2.06 ± 0.19 4.05 ± 0.09
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
213
R3 2.04 ± 0.16 3.73 ± 0.09
Plump and dwarf shoot stem; dark green and thick leaves R2 2.03 ± 0.14 3.67 ± 0.10
R1 2.04 ± 0.16 3.15 ± 0.07
R0 1.98 ± 0.13 2.62 ± 0.05
L3
R10 2.07 ± 0.22 5.54 ± 0.11
Small shoot stem; pale green leaves and stems (weak
shoots) R9 1.98 ± 0.11 5.47 ± 0.08
R8 2.06 ± 0.23 5.20 ± 0.09
R7 2.06 ± 0.17 5.15 ± 0.10 Relatively similar to characteristics from control
R6 2.11 ± 0.19 4.50 ± 0.13
Similar to characteristics from control R5 2.07 ± 0.20 4.37 ± 0.09
R4 2.07 ± 0.15 4.12 ± 0.08
R3 2.07 ± 0.13 4.11 ± 0.06
R2 2.09 ± 0.17 3.68 ± 0.14
Plump and dwarf shoot stem; dark green and thick leaves R1 1.98 ± 0.13 3.42 ± 0.07
R0 1.96 ± 0.16 3.14 ± 0.08
Figure 7: Cultured samples were incubated in different monochromatic
lights combination rates.
From above table and graph, it can be recognized that illumination using single wavelength
lights did not influence the shoot proliferation coefficient of in vitro chrysanthemum; in the same
total illumination intensity of monochromatic lights, it is so clear that the shoot height is inversely
Graph 1: Effects of monochromatic
lights combination rates on in vitro
shoot height in Chrysanthemum at
three total illumination intensities of
L1: 1100lux, L2: 750lux and L3:
400lux.
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
214
proportional with blue light rate. The configuration of shoot height and other morphological
characteristics show that the single wavelength lights combination rate of 70% red-30% blue at total
illumination intensity of 400lux is suitable for shoot proliferation of in vitro Chrysanthemum plants.
Figure 8: Morphological characteristics of in vitro Chrysanthemum in different
monochromatic lights combination rates at three total illumination intensities
of L1: 1100lux, L2: 750lux and L3: 400lux.
2.2. Effects of single wavelength lights illumination modalities on in vitro shoot
proliferation stage in Phalaenopsis orchid
Shootlets generated from protocorm like bodies of in vitro Phalaenopsis orchid were
cultured in shoot proliferation medium according to the previous protocol CANTI. Cultured
samples were arranged in the incubation conditions of 33 monochromatic lights illumination
modalities (integral of the two factors of monochromatic lights combination rate and total
illumination intensity: L1R10, L1R9,…, L1R1, L1R0; L2R10, L2R9,…, L2R1, L2R0; L3R10,
L3R9,…, L3R1, L3R0) with the control experiment lot of fluorescent tubes.
9 weeks after incubation with experiment conditions, achieved results are described as
below:
Table 2: Shoot proliferation coefficient and shoot morphological characteristics of in vitro
Phalaenopsis orchid in different lights illumination modalities after 9 weeks incubation.
Experiment lot Shoot coefficient
(shoot/cluster)
Shoot height and morphological
characteristics
Control 3.83 ± 1.06 Deep green leaves and stems
L1
R10 3.77 ± 0.92 Pale green leaves and stems (weak shoots)
R9 3.80 ± 0.88
R8 3.63 ± 0.81
Similar to characteristics from control R7 3.73 ± 0.83
R6 3.77 ± 0.72
R5 3.57 ± 0.77
R4 3.63 ± 0.66
Very deep green and thick leaves R3 3.83 ± 0.75
R2 3.81 ± 0.87
R1 3.67 ± 0.94 Dark green and very thick leaves
R0 3.63 ± 0.84
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
215
L2
R10 3.87 ± 1.04
Pale green leaves and stems (weak shoots) R9 3.80 ± 0.81
R8 3.73 ± 0.94
Similar to characteristics from control R7 3.87 ± 0.88
R6 3.73 ± 0.60
R5 3.63 ± 0.84
R4 3.63 ± 0.86
Very deep green and thick leaves R3 3.63 ± 0.81
R2 3,81 ± 0,81
R1 3.93 ± 0.92
Dark green and very thick leaves R0 3.67 ± 0.83
L3
R10 1.70 ± 0.68
Pale green leaves and stems (weak shoots) R9 1.57 ± 0.63
R8 1.48 ± 0.50
R7 1.67 ± 0.43
Similar to characteristics from control R6 1.43 ± 0.47
R5 1.47 ± 0.50
R4 1.47 ± 0.50
R3 1.42 ± 0.45
Very deep green and thick leaves R2 1.33 ± 0.40
R1 1.46 ± 0.63
R0 1.50 ± 0.54
Graph 2: Effects of
monochromatic lights
combination rates on in
vitro shoot proliferation
coefficient of
Phalaeonopsis orchid at
three total illumination
intensities of L1: 1100lux,
L2: 750lux and L3:
400lux.
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
216
From above table and graph, it can be recognized that illumination using monochromatic
lights significantly influenced the shoot proliferation coefficient of in vitro Phalaeonopsis orchid
when comparing the total illumination intensity of 400lux level to other level and the control.
However, data analysis without the results from the 400lux illumination experiment lots show that
illumination using monochromatic lights did not influence the shoot proliferation coefficient of in
vitro Phalaeonopsis orchid, this is the same case with chrysanthemum.
In the same total illumination intensity of monochromatic lights, shoot proliferation
coefficient is not uneven when comparing within different monochromatic light combination rates
and there was no linear rule for increasing or reducing.
In all of total illumination intensity level, the red light percentage is proportional with the
insipidity of the green of shoots and leaves and inversely with blue light percentage increasing.
In the stage of in vitro shoot proliferation, the shoot proliferation coefficient is the most
important but the quantity of shoots is significant, shoot quantity directly influences the
development and the quantity of ex vitro plantlets established from the shoots. Thus, with
Phaleaonopsis orchid in this case, the execution team estimated the shoot quantity and whole
experiment results based on the color of stems and leaves mainly because the color expresses
chlorophyll accumulation level and the vitality of the in vitro plant and it’s organs. From the results
in the table 9 and graph 2, the task execution team realized that the monochromatic lights
combination rate of 70% red-30% blue at both total illumination intensity of 750 and 1100lux is
suitable for shoot proliferation of in vitro Phaleaonopsis orchid. However, when considering about
the electricity usage effect (750lux illumination is less consumptive than 1100 lux illumination) and
also realizing that the single wavelength lights combination rate of 70% red-30% blue at 750lux is
the only experiment lot gave the shoot proliferation coefficient higher than the control lot but still
kept the leaves possess normal morphological characteristics, the task execution team choose this
illumination modality to be the most suitable for in vitro Phaleaonopsis orchid in the stage of shoot
proliferation.
Figure 9: Shoot morphological characteristics
of in vitro Phalaeonopsis orchid at different
monochromatic lights mixing rates.
Figure 10: Leaf morphological
characteristics of in vitro Phalaeonopsis
orchid shoot at different onochromatic
lighs bombination rates.
III. CONCLUSION
Via the document consulting, investigating the theoretical base and executing the
experiments, the task execution team had established 11 independent monochromatic light
illumination systems using chosen red and blue LEDs. These systems can operate according to
arbitrary control from users at 11 monochromatic lights combination rates with 3 total illumination
intensity levels as conventional requirements.
VINATOM-AR 13--28
The Annual Report for 2013, VINATOM
217
These whole facility including these systems was used to investigate the effects of
monochromatic lights on the shoot proliferation stage of plants. Achieved results show that
illumination intensity of 400lux is suitable for chrysanthemum, 750lux is suitable for Phalaenopsis
orchid and monochromatic lights combination rate of 70% red light-30% blue light are suitable for
both kinds of these plants.
REFERENCE
[1] Briggs W.R., Huala E. Blue – light photoreceptors in highter plants. Annu. Rev. Cell Dev.
Biol., 15, pp.33-62, 1999.
[2] Brown C.S., Shuerger A.C. Growth of pepper, lettuce and cucumber under light-emitting
diodes. Plant Physiol., 102, pp.808-813, 1993.
[3] Bula R.J., Morrow T.W., Tibbitt T.W., Barta D.J., Ignatius R.W., Martin T.S. Light-
emiiting diodes as a radiation source for plants. Hort. Sci., 26, pp.203-205, 1991.
[4] C.D’Onofrio, S. Morini & Bellocchi. Plant Cell, Tissue and Organ Culture, 1998.
[5] Nhut D.T., Takamura T., Watanabe H., Okamoto K., Tanaka M. Responses of strawberry
plantlets cultured in vitro under superbright red and blue light-emitting diodes (LEDs).
Plant Cell Tiss, Org. Cult., 73, pp.43-52, 2003.
[6] Hahn E.J., Kozai T., Peak K.Y. Blue and red light- emitting diodes with or without sucrose
and ventilation affects in vitro growth of Rehmannia glutinose plantlets. Plant biol., 43, pp.
247-250, 2000.
[7] Liu C.Z., Wang Y.C., Kang X.Z., Ouyang F. Investigation of light, temperature and
cultivated modes on growth and artemisinin synthesis of Artemisia annua L. shoots. Acta.
Phytophys. Sin., 25, pp.105-109, 1999.
[8] Miyashita Y., Kitaya Y., Kozai T., Kimura T. Effects of red and far-red light on the growth
and morphology of potato plantlets in vitro: Using light emitting diodes (LEDs) as a light
source for micropropagation”. Acta Hortic., 393, pp.189-194, 1995.
[9] Moreira da Silva M.H., Degergh P.C. The effects of light quality on the morphogenesis of in
vitro cultures of Azoria Vidalii (Wats.) Feer. Plant Cell Tiss. Org. Cult., 51, pp.187-198,
1997.
[10] Tanaka M., Takamura T., Watanabe H., Endo M., Yanagi., Okamoto M. In vitro growth of
Cymbidium plantlets cultured under superbright red and blue light-emitting diodes (LEDs).
J. Hortic. Sci. Biotech., 73, pp.39-44, 1998.
[11] Tennesen D.J. Singsaas E.L., Sharkey T.D. Light-emitting diodes as a light source for
photosynthesis research. Photosynthesis Research, 39, pp.85-92, 1994.
[12] Volmaro C., Pontin M., Luna V., Baraldi R. Blue light control of hypocotyl elongation in
etiolated seedings of Lactuca sativa (L.) cv. Grand Rapids related to exogenous growth
regulators and endogenous IAA, GA3, and abscisic acid. Plant Growth Regul., 26, pp.165-
173, 1998.
[13] Wang W.R., Wang Y.D., Ouyang G.C., Xue Y.L. Effects of light quality on differentiation
and itts related enzymes in callus of cucumber and tomato. Acta. Phytophys. Sin.,17,
pp.118-124, 1991.
[14] Yanagi T., Okamoto K. Utilization of supper light-emitting diodes as artificial light source
for plant growth. Ext. Abstr. Annu. Meet. Jap. Soc. Hort. Sci., pp.374-375, 1993.
VINATOM-AR 13--29
The Annual Report for 2013, VINATOM
218
APPLICATION OF IN VITRO FLOWERING TECHNIQUE
ON EVALUATING OF MUTATION CAPACITY AND COLOR SELECTION
OF TORENIA FOURNIERI L. FOLLOWING IRRADIATION
Le Van Thuc, Le Thi Thuy Linh, Hoang Hung Tien, Dang Thi Dien,
Le Thi Bich Thy and Han Huynh Dien
Department of Biotechnology, Nuclear Research Institute, Vietnam Atomic Energy Institute
ABSTRACT: Gamma irradiation technique combined with tissue culture and in vitro flowering was applied in
this study. The results showed that the frequences of variation in plant regeneration from irradiated leaf
samples were: 0.67% (with 30 Gy dose) and 0.72% (with 40 Gy dose) in MV1 generation; the frequences of
variation in irradiated plantlet samples were: 1.05% (with 30 Gy dose) and 1.15% (with 40 Gy dose) in MV4
generation, the frequences of mosaic were 0.25% and 0.08% in MV3 and MV4 generation, respectively. A total
of 16 mutants were selected based on phenotypic variations going through screening processes of tissue culture
and in vitro flowering. Three promising mutant lines (G40TP1, G40TP2, G30TL1) presented a high genetic
stability through generations cultivated in both in vitro and ex vitro conditions when being compared with the
controls. These mutant lines G40TP1, G40TP2, G30TL1 had a high potential to become new cultivars. This
paper showed that the application of in vitro flowering technique for mutation breeding of Torenia (Torenia
fournieri L.) is a significant complementary and effective model for selecting mutants produced by irradiation.
Introduction
Torenia (Torenia fournieri L.) is Scrophulariaceae dicotyledonous plants, originating from
Southeast Asia, Africa and Madagascar (Yamazaki, 1985). Torenia have sets of chromosomes (2n =
18) and relatively small genome (171 Mbp), it is considered easy to create objects mutation
(Kikuchi et al., 2007). In mutation breeding, the problem in mutation breeding by radiation factors
to consider such as: sample size, selection time, effort, cost, potential mutation miss the big
question posed to the breeders. Therefore, the combination of mutations agent with selective
techniques flowering in vitro is one of the research directions, help us to overcome the weaknesses
of the method traditional selective mutations and mutations found quickly, more efficiently and
thoroughly. In previous studies (2012), in vitro flowering process of Torenia fournieri L. was
completed research. So, use technical coordination gamma irradiation (Co60) with culture
techniques and in vitro flowering to isolate and find the variation in morphology and flower color
Torenia plants even in vitro without taking a lot of time to select on the field.
Project Information:
- Code: CS/13/01-07
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation Time: 12 months (Jan 2013-Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project:
1. Le Van Thuc, Le Huu Tu, Tran Que and Duong Tan Nhut. Study on the effects of gamma ray
irradiation on the morphogenesis of Torenia fournieri L. using in vitro flowering technique. Journal of
Biotechnology, 10(4A), 915-922, 2012.
2. Duong Tan Nhut, Le Van Thuc, Tran Trong Tuan, Truong Thi Dieu Hien, Hoang Xuan Chien, Nguyen
Phuc Huy, Nguyen Ba Nam, Vu Quoc Luan. Affects of some factors on in vitro flowering of Torenia
(Torenia fournieri L.). Journal of Science and Technology, 51(6): 689-702, 2013.
3. Le Van Thuc, Le Thi Bich Thy, Le Thi Thuy Linh, Dang Thi Dien, Han Huynh Dien, Hoang Hung
Tien, Tran Trong Tuan, Truong Thi Dieu Hien, Nguyen Phuc Huy, Duong Tan Nhut. Study on
procedure of in vitro flowering of Torenia (Torenia fournieri L.) to applying on mutation selecting by
irradiation. To be published in J. Nuclear Science and Technology, 2014.
VINATOM-AR 13--29
The Annual Report for 2013, VINATOM
219
I. EXPERIMENTS
1.1. Materials
A population of Torenia fournieri L. (2.000 plants) had been isolated, leaf samples (MV1)
and plantlet samples (MV4), which were made of materials for selected mutations.
1.2. Reagents
Macro minerals, micronutrients, vitamins, hormones are used in all the experiments of Merck;
agar (HaLong Canfoco); sucrose (Bien Hoa Sugar Joint Stock Company).
II. PROCEDURES
Use technical coordination gamma irradiation (Co60) with tissue culture techniques and in
vitro flowering to isolate and find the variation in morphology and flower color Torenia plants even
in vitro.
III. RESULTS AND DISCUSSION
3.1. Determining the ability of the mutant plant regenerated from leaf samples (MV1) by in
vitro flowering technique
The type of mutation Gamma dose (Gy)
Control 30 Gy 40 Gy
Flower colors 0 16 15
Structural variation 0 3 4
Flower size 2 9 12
Branchers on the plant 0 3 4
Chlorophyl mutations 0 1 3
Irregular shape buds (stunted, slow-growing, multi-body) 0 10 6
Leaf shape (elongated leaves and small leaves) 0 1 2
* Data were recorded in a total of 6,418 (30 Gy) and 6,389 (40 Gy) individuals.
Frequency mutation (MV1) in the dose of 30 Gy and 40 Gy was 0.67% and 0.72%.
3.2. Determining the ability of the mutant plants (MV4) by in vitro flowering technique
The type of mutation Gamma dose (Gy)
Control 30 Gy 40 Gy
Flower colors 0 20 14
Structural variation 0 5 10
Flower size 3 15 12
Branchers on the plant 0 3 4
Chlorophyll mutations 0 5 7
Irregular shape buds (stunted, slow-growing, multi-body) 0 6 11
Leaf shape (elongated leaves and small leaves) 0 4 7
* Data were recorded in a total of 5,742 (30 Gy) and 5,652 (40 Gy) individuals.
VINATOM-AR 13--29
The Annual Report for 2013, VINATOM
220
Frequency mutation (MV4) in the dose of 30 Gy and 40 Gy was 1.05% and 1.15%.
3.3. Determining the stability of genetic mutations in M1V1 to M1V4 generation
Line of white flower has a very low dissociation rate of only about 1% in M1V4 generation,
while flowers with 4 lips gold-purple dissociation rate is 12.73%. Flowers with 4 lips purple
dissociation rate is very low 0.85% (M1V4), this shows lines flowers with 4 lips purple have a high
genetic stability.
Figure 3.1: Mutation spectrum of flower colors isolated
M1V1 generation (irradiation plantlets).
3.4. Determining the stability of genetic mutations in M1V1 to M1V4 generation
Code Color and structure
of the flower
Dissociation
rate of M1V5
(%)
Dissociation
rate of M1V6
(%)
Dissociation
rate of M1V7
(%)
Dissociation
rate of M1V8
(%)
Control Purple flowers 0 0 0 0
G40TP1 White flowers 0 0 0 0
G40TP2 Purple flowers 0.47 0.20 0 0
G30TP3 Flowers with 4 lips purple 10.25 7.69 5.20 3.06
G40TP4 Yellow body plants 1.9 0.5 0 0
G30TL1 White flower yellow dots 0.50 0.35 0 0
G30TL2 Pale purple flowers 12.60 5.20 3.47 2.00
G30TL3 Flowers with separate
stamen 50.60
35.32 25.09 13.51
Figure 3.2: These mutant line purebred developed into new breeds.
VINATOM-AR 13--29
The Annual Report for 2013, VINATOM
221
3.5. Comparison of the genetic stability of the mutant lines in in vitro and ex vitro
Code of the mutant lines
Control G40TP1 G40TP2 G30TL1 The monitoring
indicators Conditions
Survival rate (%) In vitro 100±0.0 100±0.0 100±0.0 100±0.0
Ex vitro 87.47 ±1.5a
* 86.41±2.1a 85.31±1.8a 81.15±1.3b
Plant height (cm) In vitro 8.92±1.3a 8.73±1.5
a 6.47±1.3b 8.65±1.8a
Ex vitro 12.35±1.9 a 11.98±2.3
a 9.50±2.1b 12.49±1.6
a
Number of
root/explant
In vitro 18.67±0.7ns
17.23±1.2 ns
19.11±0.9 ns
18.35 ±1.2
ns
Ex vitro 14.25±1.6a 11.79±1.8b 13.08±2.1a 12.73±1.5b
Diameter of leaf
(mm)
In vitro 13.50±0.6a 8.35±0.8a 12.07±0.5b 13.75±0.6a
Ex vitro 15.26±0.7a 11.33±1.4c 14.09±0.9b 15.35±0.9a
Length of leaf (mm) In vitro 24.59±1.4b 27.41±1.3a 23.15±1.5b 25.33±1.8b
Ex vitro 26.19± 1.7b 27.89±1.3a 24.30±1.5c 26.83b ±1.3b
Length of stem (mm) In vitro 10.07±0.2a 11.30±0.5a 5.49±0.1b 10.33±0.6a
Ex vitro 14.58±0.7 16.29±0.5 7.34±0.9c 14.87±0.7b
Number of flower
buds/explant
In vitro 2.76±0.4b 2.50±0.1 3.30±0.1a 2.65±0.4b
Ex vitro 3.48±0.3b 3.65±0.6b 4.29±0.8a 3.19±0.8bc
Flower size (mm) In vitro 19.80±0.3
ns 20.03±0.5
ns 19.69±0.5
ns 19.80±0.7
ns
Ex vitro 20.15±0.6ns
20.46 ±0.7
ns 21.05±0.7
ns 21.11±0.5
ns
Dissociation rate of
flower color (%)
In vitro 0 0 0 0
Ex vitro 0 0 0 0.15
*Different letters within a row indicate significant differences at P = 0.05 by Duncan’s
multiple range test; after ± is the standard deviation of the iteration; G40TP1: white flowers;
G40TP2: purple flowers; G30TL1: white flower yellow dots; ns: non-significant difference. Data
recorded after 45 days of cultivation.
IV. CONCLUSIONS
Total number of individual variation occurs when irradiation leaf samples were 43 plants
(30 Gy) and 46 plants (40 Gy); frequency mutation (MV1) in the dose of 30 Gy and 40 Gy was
0.67% and 0.72%.
Total number of individual variation occurs when irradiation plantlet samples were 58 plants
(30 Gy) and 65 plants (40 Gy); frequency mutation (MV4) in the dose of 30 Gy and 40 Gy was
1.05% and 1.15%, mosaic frequency in MV3 and MV4 respectively 0.25% and 0.08%.
A total of 16 mutants were selected through a screening process in vitro flowering
technique. The genetic stability of three elite breeds (G40TP1, G40TP2, G30TL1) have high genetic
stability through generations in vitro and ex vitro cultivation. The lines G40TP1, G40TP2, G30TL1
mutation are eligible to develop new breeds.
VINATOM-AR 13--29
The Annual Report for 2013, VINATOM
222
The results showed that the feasibility of the application of in vitro flowering technique for
mutation breeding is really effective, creating the basis for investment and development sectors
mutation breeding in Lam Dong.
REFERENCES
[1] Duncan, D. B. Multiple range and multiple F test. Biometrics, 11, 1-42, 1995.
[2] Kikuchi, S., Kino, H., Tanaka, H., Tsujimoto, H. Pollen tube growth in cross combinations
between Torenia fournieri and fourteen related species. Breed Scinece, 57, 117-122, 2007.
[3] Murashige, T., Skoog, F.A. Revised medium for rapid growth and bioassays with tobacco
tissue culture. Plant Physiology, 15, 473-497, 1962.
[4] Yamazaki, T. A. Revision of the Genera Limnophila and Torenia from Indochina. Journal
Factor Science the University of Tokyo 3(13), 575-624, 1985.
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
225
ESTABLISHING THE STANDARD X-RAY BEAM QUALITIES
FOR CALIBRATION OF DOSIMETERS USED IN DIAGNOSTIC
RADIOLOGY FOLLOWING IAEA-TRS457
Duong Van Trieu, Ho Quang Tuan and Bui Duc Ky
Institute for Nuclear Science and Technology, Vietnam Atomic Energy Institute
179 - Hoang Quoc Viet, Ha Noi
ABSTRACT: The determination of the patient dose needs to provide a reference dose for the patient that
reference dose levels to assess the relative risk during X- ray diagnostic. This mission, We had established a
number of standard beam qualities to perform calibrations of diagnostic dosimeters and methods of measuring
patient dose in X-ray diagnostic. At radiation dosimetry room, we had establish RQR2, RQR3, RQR4, RQR5,
RQR6 beam qualities based on IAEA-TRS457 documentation with homogeneity coefficient (h) for each beam
quality in the range 0.7-0.8, and haft-value layers HVL1, HVL2 of experimental and IAEA is different about
10%. Established calibration method for diagnostic dosimeters as KAP meters, UNFORS dosimeters, and the
TLD dosimeters, practical measurements of entrance surface air kerma on Shimadzu X-ray machines used
phantom.
1. INTRODUCTION
The patient dosimetry equipments as dose meter, TLD dosimeters, semiconductor detector
are used to determine patient doses in diagnostic radiology. The standard ionization chambers in X-
rays diagnostic are used to calibrate the patient dosimetry equipment. Standard rooms of the
Institure Nuclear of Sciences and Technology are performed calibration dosemeter equipments. To
meet the requirements of the Atomic Energy Law of radiation protection for patients during
diagnostic radiology, standard room are conducting setting cablibration methods in diagnostic X-
rays according to the IAEA TRS-457 (guidelines, standards and practices to measure the patient
dosimetry in X-ray diagnostic by Agency international Atomic energy Agency launched).
2. ESTABLISHMENT TO PERFORM CALIBRATIONS OF DIAGNOSTIC
DOSIMETERS
Determine of the HVL.
The first HVL (HVL1), is defined as the thickness of the specified material which attenuates
the air kerma or air kerma rate in the beam to one half of its original value measured without any
absorber.
The second HVL (HVL2) is equal to the difference between the thickness of an absorber
necessary to reduce the air kerma (air kerma rate) to one quarter, d1/4, and the value of HVL1:
HVL2 = d1/4 - HVL1. The ratio between HVL1 and HVL2 is termed the homogeneity coefficient, h:
h=HVL1/HVL2.
Project information:
- Code: 06 /CS/HĐNV
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
226
D1
M
A
D2
F
S
Pb house
Detector
25cm
25cm 50cm
X-ray tube
Figure 1: Schematic drawing of the HVL measurement set-up, where: Fo is the focal spot;
S is the shutter; D1, D2 are apertures; F is added filtration; A is the HVL absorber;
M is the monitor chamber; D is the detector.
Table 1: Table practice results measured with the IAEA TRS-457.
Beam
qualities kV
addition
al filter
(mmAl)
HVL
1
HVL
2 h
HVL1
(Practic
e)/HVL1
(IAEA)
HVL2
(Practice)
/HVL1
(IAEA)
h
Practice
/IAEA
RQR2 IAEA 40 2.424 1.411 1.76 0.80
1.05 1.06 0.99 Practice 40 2.4 1.483 1.869 0.79
RQR3 IAEA 50 2.424 1.765 2.328 0.76
1.04 1.06 0.98 Practice 50 2.4 1.835 2.474 0.74
RQR4 IAEA 60 2.67 2.162 3.61 0.60
1.06 0.89 1.20 Practice 60 2.7 2.29 3.197 0.72
RQR5 IAEA 70 2.851 2.553 3.61 0.71
1.02 1.02 1.00 Practice 70 2.55 2.605 3.687 0.71
RQR6 IAEA 80 3.132 3.02 4.369 0.69
1.01 1.03 0.98 Practice 80 2.75 3.06 4.499 0.68
Table 1 shows the values of homogeneity coefficient h in the range of 0.68 to 0.79 and haft-
value layers HVL1, HVL2 of experimental and IAEA is different about 10%.
3. PRACTICE FOR DIAGNOSTIC CALIBRATIONS FOR KAP METER
Calibration of KAP meters in terms of the air kerma–area product for radiation transmitted
through the chamber (96035B ion chamber).
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
227
Figure 2: Set-up for KAP meter calibration.
Table 2: The calibration coefficient of KAP meter for radiation
quality DV60, DV70, DV80.
Beam qualities Nk (without MCh) Nk with MCh Different
DV60 1.788 1.792 0.228%
DV70 1.737 1.742 0.281%
DV80 1.713 1.718 0.267%
Nk is the calibration coefficient of the KAP meter
Table 2 shows the calibration factor of KAP meter for beam qualities DV60, DV70, DV80
using monitor chamber different without monitor chamber about 0.5%. Specifically, the beam
quality DV60 is 0.228%, DV70 and DV80 is 0.281%, 0.267%.
4. PRACTICE FOR DIAGNOSTIC CALIBRATIONS FOR UNFORS DOSE METER
The calibration coefficient of the UNFORS dose meter ef
ef ef
70 70
rUN UN UN r rDVDV DV DV DV DVUN
DV
MN N k N k
M
where UN
DVM and efr
DVM are the mean values measured with UNFORS dose meter and the reference
chamber for beam qualities DV. efr
DVk the factor correcting for the difference in response between
beam qualities DV70 and DV. ef
70
r
DVN is calibration factor of reference chamber with beam quality
DV70.
Figure 3: Set-up for UNFORS dose meter calibration.
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
228
DET
Phantom tp
d1
dFTD
Table or w all bucky
d2
Table 3: The calibration coefficient of UNFORS dose meter for radiation quality DV60,
DV70, DV80.
Beam qualities Nk (without MCh) Nk with MCh Different
DV60 1.287 1.290 -0.249%
DV70 1.312 1.299 0.975%
DV80 1.329 1.314 1.072%
Table 3 shows the calibration factor of UNFORS dose meter for beam qualities DV60,
DV70, DV80 using monitor chamber different without monitor chamber about 1.0%. Specifically,
the beam quality DV60 is-0.249%, DV70 and DV80 is 0.975%, 1.072%.
5. PRACTICE FOR INCIDENT AIR KERMA AND ENTRANCE SURFACE AIR
KERMA MEASUREMENT
5.1 Incident air kerma and entrance surface air kerma measurement using ion
chamber VICTOREEN (Model: 635; Seri No: 971) and phantom
A detector of the diagnostic dosimeter is positioned at a sufficient distance from the entrance
surface of the phantom to avoid backscatter and the incident air kerma is calculated from the
measurement at the detector position using the inverse square law.
Figure 4: Geometry used for the calculation of incident air kerma and
entrance surface air kerma
for general radio-graphy,
where dFTD=100cm is the
distance between the tube
focus and the patient
support, d1=56cm is the
distance between detector
and the tube focus,
d2=85cm the distance
between detector and the
patient support and tp=15cm
the thickness of the
phantom (30cm x 30cm x
15cm).
Incident air kerma 2
1
2
( )i
dK K d
d
where K(d) is air kerma at the measurement point (at a
distance, d1, from the X ray focus) from the mean value of ion chamber readings.
Entrance surface air kerma Ke=KiB where B is backscatter factor.
Table 4: Results of incident air kerma and entrance surface air kerma measurement using
ion chamber + phantom and KAP.
Filter Field size kV mA ms Backscatter
factor (B)
Ki
mGy
Ke
mGy
KAP
cGy.cm2
2.5mmAl 10cmx10cm 80 200 250 1.41 3.28 4.62 41.0
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
229
70 200 250 1.39 2.51 3.49 31.3
60 200 250 1.36 1.74 2.36 21.5
20cmx20cm
80 200 250 1.48 3.58 5.30 171.0
70 200 250 1.41 2.54 3.59 132.2
60 200 250 1.36 1.82 2.48 93.1
25cmx25cm
80 200 250 1.5 3.54 5.31 258.2
70 200 250 1.46 2.69 3.93 198.4
60 200 250 1.36 1.85 2.52 139.6
5.2 Incident air kerma and entrance surface air kerma measurement using UNFORS
dose meter and phantom
Figure 5: Geometry used for the calculation of
incident air kerma and entrance surface air kerma for
general radio-graphy, where dFTD=100cm is the
distance between the tube focus and the patient support
and tp=15cm the thickness of the phantom (30cm x
30cm x 15cm). DET will be attached to the phantom.
Table 5: Results of incident air kerma and entrance surface air kerma measurement using
UNFORS dose meter + phantom and KAP.
Filter Field size kV mA ms Ke UNFORS
(mGy)
KAP
cGy.cm2
2.5 mm Al
10cm x 10cm
80 200 250 5.505 41.0
70 200 250 3.847 31.3
60 200 250 2.844 21.5
20cm x 20cm
80 200 250 5.818 171.0
70 200 250 4.332 132.2
60 200 250 2.983 93.1
25cm x 25cm
80 200 250 5.788 258.2
70 200 250 4.402 198.4
60 200 250 3.001 139.6
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
230
Table 6: The comparison of air kerma entrance surface of the IC VICTOREEN, UNFORS.
Figure 6: The graph compares the entrance surface air kerma
of ion chamber Victoreen and UNFORS doser meter.
The graph 6 and table 6 shows, the entrance surface air kerma change depending on field
size and kV, mA and time parameters of the X-ray machine.
- With the same kV, mA and time parameters set on the X-ray, field size increases, the
entrance surface air kerma increases.
- When changing the kV with the same field size, air kerma change respectively.
- The results of air kerma entrance surface measurements of ion chamber VICTOREEN
and UNFORS dose meter difference about 19%.
Field size kV mA ms Ion chamber
VICTOREEN mGy
UNFORS
mGy
10cm x 10cm
80 200 250 4.62 5.505
70 200 250 3.49 3.847
60 200 250 2.36 2.844
20cm x 20cm
80 200 250 5.30 5.818
70 200 250 3.59 4.332
60 200 250 2.48 2.983
25cm x 25cm
80 200 250 5.31 5.788
70 200 250 3.93 4.402
60 200 250 2.52 3.001
VINATOM-AR 13--30
The Annual Report for 2013, VINATOM
231
6. CONCLUSION
The mission, we had build RQR2 ÷ RQR6 beam qualities in X-ray diagnostic. Established
calibration method for diagnostic dosimeters as KAP meters, UNFORS dosimeters, and the TLD
dosimeters, practical measurements of entrance surface air kerma on Shimadzu X-ray machines
used phantom.
REFERENCES
[1] Technical Reports Series No. 457. Dosimetry in Diagnostic Radiology: An international
code of practice, International Atomic Energy Agency, Vienna, Austria, 2007.
[2] Implementation of the International Code of Practice on Dosimetry in Diagnostic
Dadiology (TRS 457): Review of Test Results, Austria, February 2011.
VINATOM-AR 13--31
The Annual Report for 2013, VINATOM
232
RESEARCH ON STABILIZATION OF RADIOACTIVE WASTE
BY METHOD OF SYNROCK CERAMIC
Nguyen Hoang Lan, Nguyen Ba Tien, Vuong Huu Anh and Nguyen An Thai
Center for Radioactive Waste Management and Environmental Treatment,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48-Lang Ha, Dong Da, Ha Noi
- Tên chủ nhiệm đề tài: Nguyễn Hoàng Lân
- Đơn vị: Trung tâm xử lý chất thải phóng xạ và môi trường – VCNXH
ABSTRACT: Separate phases from synroc polyphases ceramic were investigated to fabricate completely
synroc and the distribution of stable isotopes (Sr) in synroc matrix was surveyed simultaneously with leaching
test. The experimental conditions: 13.5 x 11mm pressed pellet synroc with pressure of 2.5-3tons/cm2, sintering
temperature ttk = 1250oC, thermal lifting velocity vt = 20
oC/min with 2 hours prolongation in 1250
oC, Sr
loading amount was 7 % mole, the results showed that pellets contain 3 phases perovskite CaTiO3, zirconolite
CaZr Ti2O7, hollandite BaAl2Ti6O16 with average density of 4.1 g/cm3, leaching rate R (g/m
2.d) of 10
-6, 10
-5 for
Ti, Sr respectively.
I. REQUIREMENTS AND TARGET
- Determining of synroc formular, fabricating of synroc ceramic, evaluating of waste load
and stability of product.
- Investigation on application capacity of synroc to immobilization of radioactive waste.
- Issuing of research results on factors affecting to synthesis of synroc and chemical
stability of synroc by Sr leaching test.
- Fabricate of synroc ceramic comprised 3 phase perovskite CaTiO3, zirconolite
CaZrTi2O7, hollandite CaZrTi2O7.
- Propose the synthesis procedure of synroc ceramic to immobilization of radioactive
waste.
II. METHODOLOGY AND EXPERIMENTAL
Synroc ceramic fabrication techniques: fine powder was mixed with oxides material
composition of 75% (CaO-TiO2-ZrO2 : 25%-65%-10% mole)-25% (15 % Al2O3-10% BaO) then
grinded in agate mortar, fine powder sample was added 3 % PVA as binder agent, then cold pressed
to form pellets with size of 11x13.5 mm, using high hardness mold, the mold diameter of 15mm,
zinc stearate was added as mold lubricant and pellets pressed under pressure about 2.5-3tons/cm2 by
one-dimensional hydraulic pressing machine. Green pellets were placed in high heat resistant boat
and sintered at 1250oC in air, heat rate of 20
oC/min and prolongation at 1250
oC for 2h after
Project Information:
- Code: CS/13/03-03
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation Time: 12 months (Jan 2013-Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project:
Nguyen Hoang Lan, Nguyen Ba Tien, Vuong Huu Anh, Nguyen An Thai. Research on immobilization
of radioactive waste by method of synroc ceramic synthesis. To be published in Journal of Nuclear
Science and Technology, VINATOM, 2014.
VINATOM-AR 13--31
The Annual Report for 2013, VINATOM
233
finishing sintering sample was cooled in furnace to room temperature, analysis results examined by
ICP - MS, SEM, XRD, EDS.
Sr/synroc matrix loading and leaching test: Synroc ceramic pellet loaded 7% Sr was
fabricated similarly, ANSI / ANS 16.1-1986 standard utilized for leaching test.
III. RESULTS AND DISCUSSION
The tables, graphs and images.
Table 1: Optimal technological parameters for fabrication of synroc loading Sr.
No Parameters Unit Value
1 Material composition of synroc % mole 75% (CaO-TiO2-ZrO2:
25%-65%-10%)-25%
(15% Al2O3-10% BaO)
2 Loading percent of Sr % mole 7
3 Binder (PVA) % weight 3
4 Mold lubricant (zinc stearat/aceton) % weight 0.2-0.3
5 Cylinder size of pellet (DxH) mm 13.5x11
6 Pressure ton /cm2
2.5-3
7 Sintering temperature oC 1250
8 Prolongation at sintering temperature h 2
9 Heat rate oC/min 20
10 Sintering environment -
Air
11 Cooling rate to room temperature -
Turn off furnace and wait
to room temperature
Table 2: Properties of synroc ceramic loaded Sr product.
No Properties Unit Result
1 Loading percent Sr % mole 7
2 Cylinder size of green pellet (DxH) mm 13.5x11
3 Cylinder size of sintered pellet (DxH) mm 12.31x10.55
4 Phases identified by X-ray - Perovskit, zirconolite,
hollandite
5 Average water adsorption % weight 3.26
6 Average density g/cm3
4.1
7 Leaching rate of Sr g/m2.d 10
-5
8 Leaching rate of Ti g/m2.d
10
-6
VINATOM-AR 13--31
The Annual Report for 2013, VINATOM
234
Figure 1: Sr/synroc ceramic pellet product.
Figure 2: X-ray diffraction of 25% CaO-
65% TiO2-10% ZrO2 system.
Figure 3: SEM image of 25% CaO-65%
TiO2-10% ZrO2 system
Figure 4: X-ray diffraction of complete.
3- phases synroc.
Figure 5: SEM image of complete.
3- phases synroc.
VINATOM-AR 13--31
The Annual Report for 2013, VINATOM
235
Figure 6: SEM image of synroc
loaded 7% Sr.
Figure 7: Selected areas for EDS analysis
of synroc loaded 7% Sr.
a
b
Figure 9: Relation of leaching rate
with time.
Figure 8: EDS results of synroc loaded
7% Sr (a-area 1, b-area 2).
In this work, we have investigated and fabricated ceramic synroc material application for
stabilization of radioactive isotopes in radioactive waste, this research has determined mole
composition of oxides to form synroc of 75% (CaO-TiO2-ZrO2: 25%-65%-10%, respectively)-25%
(15% Al2O3-10% BaO) and appropriate sintering temperature at 1250oC with 2h prolongation.
Synroc ceramic was fabricated with complete three crystal phases perovskit, zirconolite, hollandite
with high density and homogeneous. The distribution and immobilization of Sr in synroc matrix
was also investigated and examined by ICP-MS, SEM, XRD, EDS as images, tables above showed
high chemical stability of sample. The low leaching rate of synroc had a good ability to immobilize
Sr (10-5
g/m2.d).
IV. CONCLUSION
1. During the experimental section, studying on CaO-TiO2-ZrO2 system of synroc was
established and conducted to evaluate composition in equilibrium formation of perovskite,
zirconolite.The result obtained was sample of (CaO-TiO2-ZrO2: 25%-65%-10% mole, respectively).
2. The results of investigation of complete 3 phases synroc formation was launched. An
appropriate proportion of oxides component in the forming of three-phases synroc perovskite,
VINATOM-AR 13--31
The Annual Report for 2013, VINATOM
236
zirconolite and hollandite has determined by experiment, the result surveyed was sample of (75%
(CaO-TiO2-ZrO2: 25%-65%-10% mole, respectively) -15% Al2O3-10% BaO).
4. The survey results of loading stable isotope strontrium showed compatibility Sr/synroc
matrix and can be loaded up to 7% mole.
5. Leaching test aimed to survey separation of strontrium from synroc by water to assess
chemical stability of synroc. The results showed that leaching rate decreases over time with very
little separated concentration of elements showing high chemical stability of synroc.
6. Synthesis procedure of synroc ceramic to stabilize radioactive waste has been proposed.
V. RECOMMENDATION
Based on some of results archived of project, respectfully request that the agency is allowed
to invest in more extensive research on project to assessment and application of synroc more
holistically.
REFERENCES
[1] Ringwood, A. E., Kesson, S. E., Ware, N. G., Hibeberson, W.O. and MAJOR, A.
“Immobilization of high level nuclear reactor wastes in SYNROC”. Nature 278, 219-
223.
[2] H. J. Rossell, J. Solid State Chem. 99, pp.38-51, 1992.
[3] ]. I.w. Donald, B.L. Metcalfe, R.N.J. Taylor “The immobilization of high level radioactive
wastes using ceramics and glasses”, Journal of materials science 32, 5851-5887, 1997.
[4] L. W. Coughanour, R S. Roth, S. Marzullo and F. E. Sennett, J. Res. Nat, Bur. Stand. 54,
pp. 191-199, 1955.
[5] J. M. McHale, N. V. Coppa, “Instantaneous Formation of Synroc-B Phases at Ambient
Pressure” Scientific Basis for Nuclear Waste Management XIX, eds.
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
237
CALCULATION AND MEASUREMENT DOSE RATE AT THE CONTROL
AREA OF ELECTRON BEAM ACCELERATOR UELR-10-15S2
AT RESEARCH AND DEVELOPMENT CENTER
FOR RADIATION TECHNOLOGY
Nguyen Anh Tuan, Tran Van Hung, Cao Van Chung and Nguyen Hoang Hai
Research and Development Center for Radiation Technology, Vietnam Atomic Energy Institute
202 A Sreet 11., Linh Xuan Ward, Thu Duc Dist., HCM City, Vietnam
ABSTRACT: In order to provide data on the dose rate at the control area of electron beam accelerator UELR-
10-15S2 for assessing radiation safety, the approximation method and MCNP simulation were used to
calculate, and then were compared with Fricke dosimetry at high dose area and TLD dosimetry at low dose
area. At the high dose area, inside the irradiation room, accelerator room and along the conveyor, the results of
the calculation methods are good agreed with the results of Fricke dosimeters. At the low dose rate, they were
calculated for the most extreme cases (10 MeV bremsstrahlung energy) by approximation method; the results
are 6.0 Sv/h at the control room and 1.0 Sv/h at the product loading – unloading. MCNP code was applied to
calculation dose rate without natural radioactive background, and the results outside irradiation room are 10-3
Sv/h. TLD dosimeters were used to accumulated measure in a month (including background) and the results
obtained from 0.3 to 0.7 Sv/h, these values are equal to radioactive background.
1. INTRODUCTION
Accelerator UELR-10-15S2 is linear accelerator generation (LINAC) using RF wave [1] to
accelerate the electron beam energy 10 MeV, 15 kW maximum power. The scanning and bending
magnet systems were specifically designed to enable double-sided scanning irradiation products.
The dose rate in areas outside the control room when scanning double-sided irradiation is much
higher than on the upper scan only. In addition, under the scan can cause skyshine effects for the
surrounding area, so the shielding concrete was calculated, designed and built to the best shielding
both transmission and scattering of the bremsstrahlung. The structure of radiation shielding concrete
is shown in Fig.1.
Project information:
- Code: CS/13/07-02
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
4
1
2
3 5
6
(1): Loading –
unloading
area
(2): Control
room
(3): Modulator
room
(4):
Irradiation
room
(5):
Accelerator
room
(6): Concrete
Figure 1: the
structure of
radiation shielding
concrete [2].
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
238
2. CALCULATION METHOD AND DOSIMETRY
2.1. Approximation theory
Assuming anisotropic photon source, energy of 10 (MeV) is placed in the irradiated head of
the accelerator UELR-10-15S2 with a dose of 1.5 x 109 (Sv/h) at the source position, received
dose rate outside irradiation room by photon transmission and multiple scattering photon along the
conveyor.
2.1.1. Transmission calculation
The dose rate outside irradiation room is calculated by inverse-square law and shielding
material thickness. The dose rate at the target, P0 [Sv.m2kW
-1h
-1], is calculated for electron beam
power of 15 kW:
P0 = 15x104x10
4 = 1.5x10
9 [Sv.m
2/h], with = 90
0 (2.1)
P0 = 15x2,8x105x10
4 = 4.2x10
10 [Sv.m
2/h], with = 0
0 (2.2)
The inverse-square law is applied to calculation dose rate outside irradiation room:
2
0
1 R
P=P (2.3)
Outside irradiation room, the dose rate is also calculated by attenuation factor K:
P2 = P1.K (2.4)
and
TVL
X-
10=K (2.5)
where X is a barrier of thickness;
TVL is tenth-value layer.
The tenth-value layer, TVL, depends on the radiation energy, thickness and characteristic of
shielding materials [3].
2.1.2. Scattering calculation
After the first scattering onto concrete, the energy of photon reduced up to 0.5 MeV and the
second up to 0.3 MeV. The photon scattering schema is shown in Fig. 2.
Figure 2: The multiple scattering schema [4].
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
239
After the first scattering, dose rate PS1 [Sv] is calculated by:
PS1 = P(R, ). )E,θ,θ(αs1
.2
1
1
SR
S [Sv/h] (2.6)
where RS1 [m] is distance from scattering surface S1 to S2;
P(R, ) is average dose rate on the scattering surface S1 and is calculated by inverse-square
law;
R [m] is distance from source to the scattering surface;
)E,θ,θ(αs1
is scattering coefficient.
After the second scattering, dose rate PS2 [Sv/h] is calculated by:
PS2 = P(R1, 1θ ).
2
2S22
2
1S11R/S.α.R/S.α [Sv/h] (2.7)
where RS2 [m] is distance from scattering surface S2 to S3;
P(R1, 1θ ) [Sv/h] is average dose rate on the scattering surface S2;
2 = ),,( 22 Es is the second scattering coefficient.
2.2. MCNP simulation [5]
The MCNP origin of coordinates was selected at vertical position of the electron beam on
the floor. The surfaces and the cells are defined by the coordinates of Oxyz axes to escribe the
shielding concrete of the irradiation room. Cross section perpendicular to the axis Oz on the first
and the second floor are shown in Fig. 3.
The error reduction tools which using MCNP code include: increased importance (imp) for
the points calculation, optimization of detector radius which around point calculation and
optimization of physical space.
Figure 3: Perpendicular to Oz cross section of shielding concrete by MCNP.
0,0,120
0,0,300
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
240
2.3. Experimental dosimetry
According to the calculation results, the dose rate is very high at the irradiation room (from
10610
8 Sv/h) and very low outside (equal to radioactive background), so dose rate at the
irradiation room was measured by Fricke dosimeters and TLD dosimeters measured at the outside.
2.3.1. Dosimetry at the irradiation room
* Experimental equipment:
- Fricke dosimeter: Solution of (NH4)2 Fe (SO4)2 x 6 H2O, NaCl, H2SO4 and distillated
water was prepared according to ASTM standard [6];
Dose range: 20400 Gy;
Error: 3%.
- Measuring system: JACCO V-630 spectrometer [7]
* Experimental steps:
- Calculation data analysis;
- Setting position and time dosimetry.
2.3.2. Dosimetry outside the irradiation room
* Experimental equipment:
- TLD dosimeter: LiF: MCF crystal, range energy: 410000 keV;
- Model: RE-2000S, serial number: 1502050010;
- Made in Germany;
- Error: 7%
- Lower threshold: 50 nGy
* Experimental steps:
- Calculation data analysis;
- Setting position and time dosimetry.
3. THE RESULTS AND RADIATION SAFETY ASSESSMENT
3.1. Calculation and dosimetry results at the first floor
Dose rate distribution at the first floor of accelerator UELR-10-15S2 is shown in Fig.4.
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
241
Figure 4: Distribution dose rate at the first floor.
Calculation and dosimetry results are shown in Table 1.
Table 1: The results of dose rate distribution at the first floor.
Points Theory MCNP calculation Dosimetry
D (Sv/h) D (Sv/h) D (Sv/h)
1 2.6E+08 4.2E+08 0.004 1.3E+08 0.03
2 5.5E+06 6.9E+06 0.050 2.2E+06 0.03
3 1.5E+04 3.2E+04 0.080 3.2E+04 0.03
4 6.4E+00 1.4E-03 0.150 4.9E-01 0.07
5 4.2E+06 4.4E+06 0.020 9.0E+05 0.03
6 2.0E+00 1.3E-03 0.180 4.5E-01 0.07
7 4.3E-03 2.5E-04 0.240 3.5E-01 0.07
In Table 1, dose rate was calculated for photon energy of 10 MeV by equation theory; the
results were calculated by MCNP code without radioactive background; dose rate at points 5, 6 and
7 was measured by TLD dosimeter, other points by Fricke dosimeter.
3.2. Calculation and dosimetry results at the second floor
Distribution dose rate at the second floor is shown in Fig. 5.
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
242
Figure 5: Distribution dose rate at the second floor.
The calcultion and dosimetry results at the second floor are shown in Table 2.
Table 2: The calcultion and dosimetry results at the second floor
Points Theory MCNP calculation Dosimetry
D (Sv/h) D (Sv/h) D (Sv/h)
8 4.3E+07 4.6E+07 0.03 1.1E+07 0.03
9 8.6E+06 6.4E+06 0.04 1.6E+06 0.03
10 2.3E+04 9.4E+03 0.12 2.8E+04 0.03
11 2.5E+00 2.6E-03 0.12 3.5E-01 0.07
12 1.0E+00 5.3E+00 0.06 1.5E+00 0.07
13 - 6.8E-01 0.09 6.2E-01 0.07
At the high dose area (point 8, 9 and 10), the results of calculation methods are good agreed
with the measured. At the low dose area, the outside accelerator room, dose rate was calculated for
photon energy of 10 MeV by equation theory; the results were calculated by MCNP code without
radioactive background; the results were measured by TLD dosimeter including background.
3.3. Calculation and dosimetry results on the top of the irradiation room
On the top of the irradiation room, dose rate was calculated and measured at the ventilation
channel (point 15) and reference position player directly to the electron beam (point 14). The
calculation and dosimetry results were shown in Table 3.
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
243
Table 3: The calcultion and dosimetry results on the top of the irradiation room.
Points Theory MCNP calculation Dosimetry
D (Sv/h) D (Sv/h) D (Sv/h)
14 4.3E+01 8.3E+01 0.10 1.8E+01 0.07
15 6.1E+02 4.2E+02 0.06 2.47E+02 0.07
At points 14 and 15, dose rate is very high so it generates skyshine effect, however, the
calculated dose rate caused by skyshine is very low (10-3
Sv/h).
3.4. The radiation safety assessment
In order to assess radiation safety for groups working outside the irradiation room, it
necessary to compare dose rate at workplaces with dose limit according to ICRP standards.
Table 4: Comparing dose rate with ICRP standards.
Groups Point Dose rate,
Sv/h
ICRP standard,
Sv/h
Occupational exposure 4 0.49 0.07 6.0
6 0.45 0.07 6.0
11 0.35 0.07 6.0
12 1.50 0.07 6.0
13 0.62 0.07 6.0
Public exposure 7 0.35 0.07 0.12
In Table 4, dose rate was accumulate measured including radioactive background by TLD
dosimeter. At the workplaces of radiation workforce, dose rate is less than ICRP standard so
workplaces are safety for radiation workforce. At the public area, dose rate was measured by TLD
dosimeter equals to background and calculated by MCNP code without background 10-3
Sv/h.
3.5. Warning radiation area
On the top of the irradiation room, dose rate is very high; distribution dose and limit
working time are shown in Table 5.
Table 5: Dose and limit working time on the top of the irradiation room.
Point Dose rate
(Sv/h)
Limit working time
(h)
14 18.0 2.7
15 247.0 0.2
Because of very high dose rate on the top of the irradiation room, there should be warning
radiation symbol at the stars to the top. During irradiation, if there is a problem independent of the
control system, the operator must switch off accelerator before troubleshooting.
VINATOM-AR 13--32
The Annual Report for 2013, VINATOM
244
4. CONCLUSIONS
Dose rate was calculated for the most extreme cases (10 MeV bremsstrahlung energy) by
approximation method, and the results obtained at the control room 6.0 (Sv/h) and 1.0 at the
loading-unloading product.
MCNP code simulated the concrete shielding then was applied to calculation dose rate at the
control area without radioactive background. The results were calculated by MCNP code outside
the irradiation room of 10-4
(Sv/h); these results were less than four levels natural radioactive
background.
In order to assess radiation safety, dose rate was accumulate measured outside the irradiation
room by TLD dosimeter. The results show that dose rate equal to radioactive background (0.4
Sv/h) at the control room and loading - unloading area, so these values are less than ICRP standard
during irradiation.
In addition, dose rate was calculated and measured at the high dose area (inside irradiation
room, along conveyor) so that comparing between calculation and dosimetry results. The
calculation results are good agreed with dosimetry (less than 10 %) at the high dose rate. Dose rate
also was calculated and measured at the top of the irradiation room where radiation can scatter
along ventilation channel to establish radiation warning and recommend working time in the
particularly dangerous area.
REFERENCES
[1] Jean-Luc Biarrotte, RF Cavities for Particle Acceleration, CNRS/IPN Orsay, 2009.
[2] Corad service, Preliminary Calculation of Radiation Shielding for Electron Beam System
Deliverred Under Contract No. 01/12-08-2, St. Petertburg, Russia, 2009.
[3] Philip M.K. Leung, The Physical Basis of Radiotherapy, The Ontario Cancer Institute, 1990.
[4] IAEA, Radiological Safety Aspects of the Operation of Electron Linear Accelerators,
Technical Reports Series 188, 1979.
[5] NCRP, Radiation Protection Design Guidelines for 0.1-100 MeV Particle Accelerator
Facilities, National Council on Radiation and Measurements No.51, 1997.
[6] Los Alamos National Laboratory, Monte Carlo N-Partical Code System, Los Alamos, New
Mexico, 2000.
[7] ASTM, Standards practice for using the Fricke Reference-Standard dosimetry system,
Standards on dosimetry for radiation processing, ASTM (2nd
edition), pp. 261-268, 2004.
[8] www.jascoint.co.jp
[9] ICRP, The 2007 Recommendations of the International Commission on Radiological
Protection, Annals of the ICRP Publication 103, 2007.
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
247
STUDY ON IMPROVING ANTIOXYDANT AND ANTIBACTERIAL
ACTIVITIES OF SILK FIBROIN BY IRRADIATION TREATMENT
Tran Bang Diep, Nguyen Van Binh, Hoang Phuong Thao, Pham Duy Duong,
Hoang Dang Sang and Nguyen Thuy Huong Trang
Hanoi Irradiation Centre,Vietnam Atomic Energy Institute
No.5-Minh Khai, Tu Liem, Ha Noi
ABSTRACT: Silk fibroin at dry state and the solution of 3% were irradiated by Co-60 source at dose ranges
0÷1000 kGy and 0÷50 kGy respectively. The results showed that irradiation treatment for fibroin solution have
higher effectiveness for improvement of some bio-activities of silk fibroin compared with dry state irradiation
treatment due to remarkably reducing of irradiation doses. The antioxidant activity of fibroin was significantly
increase by irradiation. The maximum value of DPPH radical scavenging activity was 70.4% when fibroin
solution was irradiated at dose of 10 kGy. Irradiated fibroin solution also shown antibacterial activity against
tested bacteria strains (E. coli, and S. aureus). In order to estimate the applicability of our irradiated fibroin, the
silk fibroin solutions were lyophilized to obtain a pure fibroin powder, then their bio-activities were compared
with those of commercial silk fibroin (Proteines De Soie/ Zijdeproteine, Bioflore, Canada). Our fibroin powder
revealed higher antioxidant and antibacterial activities. The amino acid compositions of our irradiated fibroin
were also higher than that of the commercial product. Thus, the irradiated silk fibroin can be used for further
application in cosmetic and other related fields.
Keyword: Silk, Fibroin Solution, Radiation Treatment, Antioxidant Activity, Antibacterial Activity.
1. INTRODUCTION
Silk derived from the silkworm Bombyx mori is a natural protein that is made mainly of
fibroin and Sericin. The fibroin is a major component of silk fiber (75%), serving as the core. It
contains at least two fibroin protein, light-chain (25 kDa) and heavy-chain (325 kDa). The sericin is
a minor component (25% of the silk fiber), serving as a glue-like protein coated on the two fibroin
cores to conceal a unique luster of fibroin. Both fibroin and sericin contain the same 18 amino
acids, although in different amounts. Another difference between these two proteins is crystalline
repetitive amino acids (-Gly-Ala-Gly-Ala-Gly-Ser-) along its sequence, forming a large number of
β-sheet microcrystallines. This reinforcement contributes the strength and stiffness to the silk fiber
[1].
Silk fibroin has been used as a textile material for thousands years because it has excellent
natures such as lightness and warmth on wearing, beautiful gloss, etc... Recently silk fibroin is also
considered to be natural protein with interesting characters and applications in new diversified
fields, especially medical, cosmetic and pharmaceutical materials [8]. On practical application, it is
necessary to change form of silk fiber in many cases. For example, skin film and block are studied
for artificial skin and for contact lens respectively. Powder has been already used as additions for
food, cosmetic or pharmaceutical materials [4].
Project information:
- Code: CS/13/08-02
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
248
In fact, it is difficult to degrade or dissolve silk fibroin in water because of its crystal
structure. This limitation influenced on the use of silk fibroin, especially for cosmetic and
pharmaceutical applications. The radiation technique has been increasingly used for structural
modification of organic compounds. Gamma radiation can cause the macromolecule chains to
cross-link, graft and degrade. Recently, some authors reported that the conversion efficiency from
fiber to powder of silk fibroin improved by EB treatment, that the solubility in water of silk fibroin
improved while the mechanical properties weakened after treatment with gamma radiation [4, 7, 9].
Despite the mechanisms by which gamma irradiation produce several biological effects on
peptide/protein are still clearly unknown but the latest studies showed the antioxidant and anti-
tumor activities, tyrosinase inhibitory ability, … of silk fibroin were enhanced by gamma irradiation
[2, 3].
In our previous report of 2011, the irradiated fibroin with better degradation and higher
water solubility compared with natural fibroin was produced. Accordingly, this study was
undertaken in order to investigate the effective of gamma irradiation for enhancement of antioxidant
and antibacterial activities of silk fibroin which are among important properties of variety of
cosmetic and pharmaceutical. Process for production of water-soluble silk fibroin powder by
irradiation treatment had been proposed. In the future, the results of this study may be a prerequisite
to expand the applications of radiation technology for using abundant silk fibroin of country as
cosmetic and pharmaceutical materials.
2. EXPERIMENTAL
2.1. Materials
Silk fibroin fiber was purchased from My Duc Commune, Ha Noi. The medium for the
cultivation of microorganism such as Nutrient Broth and Nutrient Agar was supplied by Difco,
USA. The chemicals such as Na2CO3,CaCl2, KBr, DPPH (2, 2-diphenyl-1-picrylhydrazin), CH3OH,
ascorbic acid at analytical grade were supplied by Merck chemical company, Germany, while
C2H5OH was bought from a domestic company.
2.2. Silk fibroin extraction preparation
The raw silk fibers were subjected to removal of the sericin by the method described by
Byun et al. [2].
10g of silk fibroin was dissolved in 100 ml of calcium chloride solution
(CaCl2/C2H5OH/H2O=1:2:8 in mole ratio) at 70 ± 2oC for 1 h. The mixed solution was dialyzed in
distilled water with a molecular weight cutoff of 12-14 kDa for 72 h. The final concentration of the
silk fibroin aqueous solution was 3% (w/v).
2. 3. Irradiation
Silk fibroin at dry state and the solution of 3% were irradiated by Co-60 source of Hanoi
Irradiation Center at dose ranges 0÷1000 kGy and 0÷50 kGy respectively.
2.4. Antioxidant activity
To evaluate the antioxidant of silk fibroin, a radical oxygen species (ROS) scavenging
method (DPPH) was used, according to Lucconi [6]. In particular, silk fibroin solutions were tested
at different concentrations (0.005, 0.0075, 0.01 mg/ml). One milliliter of aqueous silk fibroin
solutions were mixed with 2 milliliter of methanol solution containing DPPH 10 μg/ml. Samples
were incubated in the dark for 1 hour at 25oC and absorbance was measured at 517 nm with UV-
VIS spectrophotometer AV-2450 Shimadzu, Japan. Reaction mixture without fibroin sample was
used as negative control, while ascorbic acid was used as positive control at the same concentration
of fibroin samples.
Radical scavenging activity was calculated by the following formula:
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
249
% activity = (A-B)/Ax100
where A is the absorbance of negative control and B is the absorbance of tested solution.
The analyses were performed in three replicates.
2.5. Antibacterial activity
Three kinds of bacteria strains E. coli, B. subtillis and S. aureus were used for antibacterial
activity testing of silk fibroin.
The antimicrobial activities of irradiated fibroin solutions were investigated and compared
with antimicrobial activities of non-irradiated fibroin solution as control. The procedure for testing
was performed as the modified methods of agar disk diffusion and agar dilution methods (AOAC
2000).
2.6. Determination amino acid composition of irradiated silk fibroin
The amino acid components existing in the irradiated silk fibroin was determined using a
high performance liquid chromatography (HPLC, National Institute for Food Control). The results
were also compared to a commercial product in order to estimate the applicability of irradiated silk
fibroin in practice.
3. RESULTS AND DISCUSSION
3.1. Effects of irradiation conditions and irradiation doses on antioxidant activity of
silk fibroin
The powder and 3% solution of silk fibroin was irradiated at different doses and its DPPH
radical scavenging activity was evaluated and compared with that of ascorbic acid and the
commercialized fibroin powder.
3.1.1. Effect of irradiation treatment at dry state on antioxidant activity of silk fibroin
Antioxidant activity of fibroin irradiated at different doses from 0 to 1000 kGy at dry state
was shown in Table 1 and Fig. 1 presences the UV spectra of the mixed solutions of the irradiated
fibroin in methanol containing DPPH. In the dose range of investigation, the ROS-radical
scavenging activity (%) of irradiated fibroin increases when increasing of irradiation doses. This
value is 50.6% when fibroin was irradiated at dose of 1000 kGy.
Table 1: Antioxidant effect of fibroin irradiated at dry state.
Irradiation dose (kGy) ROS- radical scavenging activity (%)
0.005 mg/ml 0.0075 mg/ml 0.01 mg/ml
0 5.55 ± 0.18 8.43± 0.26 12.05± 0.18
50 5.02 ± 0.16 8.87 ± 0.27 11.08 ± 0.36
100 8.20 ± 0.22 11.46 ± 0.46 14.61 ± 0.41
200 14.40 ± 0.42 17.60 ± 0.43 17.06 ± 0.43
500 15.47 ± 0.39 22.22 ± 0.38 26.14 ± 0.65
750 17.30 ± 0.24 28.90 ± 0.51 36.40 ± 0.54
1000 28.12 ± 0.14 36.20 ± 0.61 50.60 ± 0.36
Commercialized Fibroin 6.20 ± 0.21 7.60 ± 0.35 12.76 ± 0.41
Ascorbic acid 91.07 ± 0.42 - -
(-) No investigated
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
250
0
0,02
0,04
0,06
0,08
0,1
0,12
0,14
0,16
0,18
400 450 500 550 600 650 700
Op
tica
l d
en
sity
Wavelenght (nm)
Figure 1: UV absorbency of fibroin (0.01 mg/ml) irradiated at dry state in DPPH solution.
( Negative control, 0 kGy, 50 kGy, 100 kGy, 200 kGy,
500 kGy, 750 kGy and 1000 kGy)
3.1.2. Effect of irradiation doses on antioxidant activity of 3% solution of silk fibroin
A 3% solution of silk fibroin was irradiated at dose range from 0 to 50 kGy and Table 2
shows the antioxidant activity of the fibroin solutions irradiated at different doses. Figure 2
presences the UV spectra of the mixed solutions of the irradiated fibroin in methanol containing
DPPH.
From the these results, we found that 70.04% is maximum value of DPPH radical
scavenging activity obtained with the fibroin solution irradiated at dose of 10 kGy. The antioxidant
activity of the irradiated fibroin solutions also reduced gradually to 32.2% when doses increased
continuously to 50 kGy.
Table 2: Effect of irradiation doses on antioxidant activity of 3% solution of silk fibroin.
Irradiation dose
(kGy)
ROS- radical scavenging activity (%)
0.005 mg/ml 0.0075 mg/ml 0.01 mg/ml
0 5.55 ± 0.18 8.43 ± 0.26 12.05 ± 0.18
5 7.95 ± 0.21 8.65 ± 0.25 32.20 ± 0.63
10 23.80 ± 0.38 27.8 ± 0.66 70.04 ± 0.18
20 14.45 ± 0.18 21.40 ± 0.56 53.60 ± 0.79
30 11.30 ± 0.44 15.38 ± 0.41 48.05 ± 0.74
40 8.30 ± 0.26 12.20 ± 0.45 35.80 ± 0.62
50 5.60 ± 0.17 10.10 ± 0.12 32.20 ± 0.65
Commercialized
Fibroin 6.20 ± 0.21 7.60 ± 0.35 12.76 ± 0.41
Ascorbic acid 91.07± 0.42 - -
(-) No investigated.
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
251
0
0.02
0.04
0.06
0.08
0.1
0.12
0.14
0.16
0.18
450 500 550 600 650 700
Op
tica
l d
en
sity
Wavelength (nm)
Figure 2: UV absorbency of fibroin (0.01 mg/ml) derived from 3% irradiated fibroin
solutions in DPPH solution ( Negative control, 0 kGy, 5 kGy, 10 kGy,
20 kGy and 30 kGy).
Similar effect also was observed by some Korean authors when they studied on some
physiological activities of fibroin solution (1 mg/ml). They reported that DPPH radical scavenging
activity of fibroin solution increased to more 80% at irradiation dose of 5 kGy compared with 9% of
unirradiated fibroin solution. DPPH radical scavenging activity slightly reduced to about 53% at
dose of 50 kGy. The authors suggested that the changes of molecular weight of fibroin by
irradiation treatment induced the enhancement of its antioxidant activity [3].
From the these results we found that irradiation treatment for fibroin solution have higher
effectiveness for improvement antioxidant activity of silk fibroin compared with dry state
irradiation treatment due to remarkably reducing of irradiation doses. The dose of 10 kGy is optimal
dose for highest antioxidant activity of silk fibroin.
3.2. Effects of irradiation doses on antibacterial activity of silk fibroin
The antibacterial activity of 3% solution of irradiated silk fibroin against 3 tested bacteria
strains (E. coli, S. aureus , B. subtillis) were investigated through the parameters as width of clear
zone of growth inhibition (Table 3 and Fig. 3) and minimum inhibitory concentration (MIC) (Table
4).
Table 3: Width of clear zone of growth inhibition
of the irradiated fibroin solution for 3 tested bacteria strains.
Irradiation dose
(kGy)
Width of clear zone of growth inhibition (mm)
E.coli S. aureus B. subtillis
0 – – –
5 – – –
10 5.4 ± 0.09 3.6 ± 0.10 –
20 5.6 ± 0.25 3.6 ± 0.12 –
40 5.4 ± 0.11 3.5 ± 0.08 –
* Concentration of fibroin solution using for tested was 1%.
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
252
(–) No observed
The results show that, antibacterial activity of fibroin solution had been improved by gamma
irradiation. However, there were no significant differences in antibacterial activity against E. coli
and S. aureus of all samples in dose ranges from 10 to 40 kGy. The 30 mg/ml solution of fibroin
was not enough to inhibit growth of B. subtillis for all investigated doses.
Figure 3: Clear zone of growth inhibition of the irradiated fibroin solution at different
concentrations treated at dose of 10 kGy for (a)-E. coli and (b)-S. aureus.
Table 4: Minimum inhibitory concentration of irradiated silk
fibroin solution at diffident doses.
Irradiation dose
(kGy)
MIC (mg/ml)
E. coli S. aureus B. subtillis
0 30 30 >30
10 4.2 6.5 >30
20 4.5 6.5 >30
40 4.5 7.0 >30
The antibacterial activity of fibroin powder treated at dose of 500 kGy was also reported by
Jindaron [5]. The authors found that the MICs of fibroin powder for E. coli B/r and S. aureus K
were 2.4 mg/l and this concentration was also not enough to inhibit growth of Bacillus subtillis. In
this study, similar activity was obtained for silk fibroin solution irradiated at doses from 10 to 40
kGy.
3.3. Amino acid composition of irradiated silk fibroin
Table 5: Amino acid profile of irradiated fibroin powder and commercial product.
Amino acid Irradiated fibroin
(mg/g)
Commercial fibroin -
bioflore (mg/g)
Aspartic
Serine
Glutamic
9.99
104.96
No observed
No observed
No observed
No observed
b
t
e
s
t
e
d
b
a
c
t
e
r
i
a
s
t
r
a
i
n
s
a
t
e
s
t
e
d
b
a
c
t
e
r
i
a
s
t
r
a
i
n
s
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
253
Glycine
Histidine
Threonine
Arginine
Alanine
Proline
Cystine
Tyrosine
Valine
Methionine
Lysine
Isoleucine
Leucine
Phenyalanine
247.24
No observed
3.23
No observed
No observed
No observed
1.40
75.06
42.47
No observed
2.13
6.47
5.19
7.71
0.19
No observed
0.70
No observed
No observed
No observed
0.37
4.03
7.55
3.72
10.61
7.49
11.65
8.46
From the results above, it is evident that the water-soluble yellowish silk fibroin powder can
be prepared by lyophilization of the irradiated silk fibroin solution. The amino acid components of
the irradiated silk fibroin were also analyzed and presented in Table 5. As one can see, the amounts
of some amino acid exsisting in the irradiated fibroin such as serine, glycine, tyrosine and valine
were much higher than those in the commercial product. This might be because the amino acid
compositions of raw materials for silk fibroin production were effected by species of silk. In
addition, the silk protein may be degraded into amino acid during gamma irradiation. The result was
consistent with the experiment done by Vaithanomsat [10] that the chemical compositions of silk
protein could be influenced by silk species and feed and this, therefore would be able to indicate the
amino acid pattern of silk products.
4. CONCLUSIONS
Our results show that gamma irradiation could improved some bioactivity of silk fibroin.
Irradiation treatment for fibroin solution have higher effectiveness for enhancement antioxidant and
antibacterial activities of silk fibroin compared with dry state irradiation treatment.The maximum
antioxidant activity was 70.4% obtained for the fibroin solution that irradiated at dose of 10 kGy.
These irradiated fibroin solution also shown antibacterial activity against the tested bacteria strains
(E. coli and S. aureus).
The water-soluble silk fibroin powder can be prepared by lyophilization of irradiated silk
fibroin solution. The irradiated silk fibroin powder revealed the higher antioxidant and antibacterial
activities in comparision with a commercial silk fibroin (Proteines De Soie/Zijdeproteine, Bioflore,
Canada). The amino acid components of the irradiated fibroin were also higher than those of
commercial product. Thus, the irradiated silk fibroin may potential be used for cosmetic and other
related applications.
REFERENCES
[1] G.H. Altman, F. Diaz , C. Jakuba, T. Calabro, R.L. Horan, J.S. Chen, H. Lu, J. Richmond,
D.L. Kaplan, Biomaterials 24, pp. 40-416, 2003.
[2] E.B. Byun, N.Y. Sung, J.H. Kim, J.I. Choi, T. Matsui, M.W. Byun, J.W. Lee, Chemico-
Biological Interactions 186, pp. 90-95, 2010.
[3] http://www.faqs.org/patents/app/20090286959
VINATOM-AR 13--33
The Annual Report for 2013, VINATOM
254
[4] K. Ishida, H. Takeshita, Y. Kamiishi, F. Yoshii, T. Kume, JAERI-Conf. 2001-005, pp. 130-
138, 2001.
[5] J. Chvajarernpun, C. Siri-Upathum, JAERI-Conf. 2002-003, pp. 76-81, 2002.
[6] G. Lucconi, Scientifica Acta 6, pp. 3-6, 2012.
[7] W. Pewlong, B. Sudatis, H. Takeshita, F. Yoshii, T. Kume, JAERI-Conf. 2000-003, pp. 146-
152, 2000.
[8] R. M. Reddy, Academic Journal of Entomology 2, pp. 71-75, 2009.
[9] B. Sudatis, S. Pongpat, JAERI-Conf. 2002-003, pp.101-104, 2002.
[10] P. Vaithanomsat, Kasetsart J. (Nat.Sci) 40, pp.152-158, 2006.
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
255
STUDY ON PREPARING CARBOXYMETHYL STARCH HYDROGEL
RADIATION-CROSSLINKED ON THE ELECTRON BEAM CCELERATOR
TO DO THE MOISTURIZING MATERIAL IN COSMETIC
Nguyen Thanh Duoc, Doan Binh, Pham Thi Thu Hong and Nguyen Anh Tuan
Research and Develepment Center for Radiation Technology,
Vietnam Atomic Energy Institute
202 A Sreet 11., Linh Xuan Ward, Thu Duc Dist., HCM City, Vietnam
ABSTRACT: Hydrogel of carboxymethyl starch (CMS) matrix was prepared by crosslinking of electron beam
(EB) radiation on the EB linear accelerator UERL-10-15S2 (energy of 10 MeV, capacity of 15 kW, Russia)
with support substances such as polyvinyl pyrrolidon (PVP), Kappa-Carragenan and Montmorillonit (MMT).
The characteristic properties of hydrogel membrane such as gel content, degree of swelling, mechanical
strength, adhesion force, water vapor transmission rate (WVTR) and skin allergy were experimented. This
research will be firstly oriented in applications of CMS hydrogel material in cosmetic and personal care field
such as facial mask for skin care, moisturizing membrane for skin and so on.
1. INTRODUCTION
Nowadays, people’s demands of beauty and personal care are very necessary. The more
modern and developed life is, the more necessary demands of cosmetic are. Many developed
countries in this field such as Dutch, Korea, Japan have done a lot of researches [5,6,7,8] and
prepared many kinds of product in the market. In Dutch, O.S Lewal and et prepared CMS hydrogel
crossed by chemical activator axit carboxylic as glutaric, suberic, pimelic and butanetetracarboxylic
[5]. In Japan, group of Nagasawa had a result in radiation crosslinking of carboxymethyl starch [6];
Yoshii and et researched crosslinking CMS at high concentration by irradiation method without
chemical initiator [7]. In Korea, group of Hoon Song resulted in CMS hydrogel used for removing
iron in aqueous Solution [8]. And the products have many different puposes of use such as: facial
mask, moisturizing membrane or scream for skin and so on.
Materials applied in this filed such as gel, hydrgel, nanoparticle and so on have
characteristic properties that satisfy some standard requirements about skin allergy, asepsis,
nontoxic property with people and ability of biodegradation in the environment after used [9].
Radiation crosslinking is the best way to process the products like hydrogel membrane applying to
the cosmetic field.
This research is the basic step of preparation the hydrogel membrane on the CMS matrix by
the method of EB crosslinking. And it will be firstly oriented in applications of CMS hydrogel
material in cosmetic and personal care.
Project information:
- Code: CS/13/07-03
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
256
2. EXPERIMENT
Raw chemical materials
PVP, BASF Kollidone 90, Mw: 1000.000 Da (Dutch); CMS, Emsize CMS 150, MW = 600
kDa, DS=0.85, Emsland-Stärke (Dutch); Kappa-Carragenan, Marcel (Phillipine); Montmorillonite,
Merk (Dutch) and pure water.
Instrument, equipment:
Electron beam accelerator UERL-10-15S2, 10 MeV, CORAD Ser. Ltd, Russia.
DTA, TA-60WS, Shimadzu, Japan
Mechanical analysis, Stograph V10-C, Toyoseiki, Japan
Mechanical analysis QCTech, Taiwan
And other laboratory equipments
Preparation method of sample and irradiation
Weigh 5g CMS, 10g PVP, 1g κ-Carrageenan and 100mg reinforcing phase MMT. Mix the
blend in the glass erlen containing 100g pure water in 4 hours and kept steady over night at the
room temperature. Boil the compound in a bain-marie at 80oC in 3 hours, then decrease the
temperature and keep it at 70oC in 1 hour to remove the bubbles. Pour the blend into the PET mould
with the shape 10cm x 10 cm x 0.3cm at 45oC. Finally, pack it in the PE plastic membrane and then
irradiated on Electron beam accelerator UERL-10-15S2, 10 MeV, Russia.
Analysing the WVTR of hydrogel membrane
Determine the water vapor transmission rate by weighing the lost weight of the cylinder
vase with the diameter 35mm and the height 50mm containing 25ml water that was covered the
hydrogel membrane with diameter 40mm on the its head. The vase was kept in the incubator at
35oC in 24 hours [3,4].
WVTR (g/m2/h) =
24
106
10
Ax
xmm bb
where: mb0: weight of the vase before incubating (g);
mb1: weight of the vase after incubating in 24 hours (g);
A: square of the vase’s surface (mm2).
Analysing the adhesive properties of hydrogel membrane
Sample with the shape 150mm x 20mm covered and rolled with a force about 5N on the
plastic’s surface made of nonwoven PE fiber at the room temperature in 3 hours. Peeling force was
determined in the tensile machine QCTech (Taiwan) and moved at an angle to the direction of the
plastic surface with the peeling velocity 50mm/minute [1,2].
Analysing the degradation of hydrogel membrane in the environment of α-amylase
enzyme
Dry the sample at 65oC until its weight had no change, then grind it into small pieces.
Balance 50mg and put in the glass vases having 4ml buffer solution acetate (pH = 4.6) and 1ml
CaCl2 0.1% and 1ml enzyme -amylaza 0.1%, then keep the vase in the incubator at 400C in 24
hours. After 1 hour, sample was filtered by the filter-paper and cleaned by the pure water
sometimes. Sample was dried at 65oC until its weight had no change again.
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
257
3. RESULT AND DISCUSSION
Preparation of the hydrogel membrane with the best ratio of components
From the result of basic experiments, the best ratio of components PVP:CMS:
Kappacarragen = 10g:5g:1g in 100ml pure water with (MT2) and without the reinforcing phase
MMT (MT0) was chosen to determine characteristic properties of sample in the following
experiments in a range of absorbed dose 10-25 kGy.
Characteristic properties
Effect of the absorbed dose on the gel content
50
52.5
55
57.5
60
62.5
65
67.5
70
5 10 15 20 25 30
Absorbed dose (kGy)
Gel
con
ten
t (%
)
3
4
5
6
7
8
9
Deg
ree
of w
ater
sw
ellin
g
(g/g
)
MT0
MT2
Figure 1: Effect of the absorbed doses on the gel content and degree
of water swelling of hydrogel membrane.
In the result of scheme 1, gel content of MT2 is lower than MT0 in range of absorbed doses
10-25 kGy. Both of them increase with the increasing absorbed dose and saturated at the dose 20
kGy. In the opposite, the water swelling of MT2 is higher than MT0 and both of them descrease
with the increasing of absorbed doses. All components are hydrophilic, so in the hightly
crosslinking stage, it prevents the hydration of polymer chains in membrane.
Effect of absorbed dose on the tensile strength and elongation at break
In the studied range of abosorbed doses, tensile force at break of MT2 is higher than MT0
(Figure 2). It show that tensile strength was improved with the reinforcing MMT. Both of samples
increase linearly and get maximum values at dose 20 kGy. In another way, elongation at break of
MT0 and MT2 decrease with the increasing of absorbed doses.
0.07
0.08
0.09
0.10
0.11
0.12
5 10 15 20 25 30
Absorbed dose (kGy)
Ten
sile
fo
rce
at
bre
ak
(MP
a)
120
140
160
180
200
220
240
Elo
ng
ati
on
at
bre
ak
(%
)
MT0
MT2
Figure 2: Effect of the absorbed doses on the tensile force
and elongation at breake of hydrogel membrane.
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
258
Adhesive property
0.03
0.04
0.05
0.06
0.07
0.08
0.09
10 12.5 15 17.5 20 22.5Absorbed dose (kGy)
Ad
hesi
ve f
orce (
N/c
m)
.
Figure 3: Effect of the absorbed doses on the the adhesive property
of hydrogel membrane MT2.
Testing the effect of the absorbed doses on the the adhesive property of hydrogel membrane
MT2 shows that adhesive force decreases with the increasing of absorbed doses. It demonstrates
that the adhesive force is opppsite in the gel content or degree of crosslinking. At the optimus
absorbed dose 20 kGy, adhesive force of membrane gets the saturated value and has no change in
over 20 kGy. Comparing the adhesive property of MT0 and MT2 at the absorbed dose 20 kGy
(Figure 4), the result shows that MMT component does not affect to adhesion ability of membrane
because their values of adhesive force have difference in deviation of calculation, alternately 0.04
and 0.043 N/m for MT0 and MT2.
Figure 4: Effect of MMT on the
adhesive property of hydrogel
membrane at the absorbed dose 20
kGy.
Result of thermo gravimetric analysis
Figure 5: Represending
thermogravimetric analysis of
sample.
MT0
MT2
0
0.01
0.02
0.03
0.04
0.05
1
Ad
hes
ive
forc
e (N
/cm
)
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
259
In the result, sample MT2 with MMT component has the higher temperature beginning the
decomposition than the control sample MT0 in the same experimented condition. (286oC so với
275oC). At 360
oC, appear a small peak that determined effect of MMT on the change of weight.
Result of the WTVR
Test the WVTR of hydrogel membrane with and without the reinforcer MMT at the
absorbed dose 20 kGy. From the table 1, their WVTR have difference in deviation of calculation
and at low values 23.60 for and MT0 and 24.97 for MT2. The result shows that moisturizing ability
of MT0 and MT2 are the same whether the sample has MMT component or not.
Table 1: WVTR of hydrogel membrane with and without the reinforcer MMT
at the absorbed dose 20 kGy.
WVTR (g/m2/hour)
Control 57.54 ± 4.54
MT0 23.60 ± 3.12
MT2 24.97 ± 2.95
Result of the degradation in the environment of α-amylase enzyme
Test the degradation of sample MT0 and MT2 irradiated at the dose 20 kGy in the
environment of α-amylase enzyme during 24 hours. The result shows that transmission rate of MT2
is lower than MMT. MMT is an inorganic substance, maybe it prevent and moderate the hydrolytic
degradation of enzyme on the CMS polymer chains .
72
74
76
78
80
82
84
86
88
0 2 4 6 8 10 12 14 16 18 20 22 24
Time (hour)
Per
cen
t o
f sa
mp
le's
wei
gh
t a
fter
deg
rad
ati
on
(%
)
MT0
MT2
Figure 6: Velocity of sample’s degradation at absorbed dose 20 kGy
in the environment of enzyme following the time.
4. CONCLUSION AND RECOMMENDATIONS
- Hydrogel membrane on the CMS matrix prepared from the compound PVP/CMS/Kappa-
Carragenan with the best ratio 10g/5g/1g/100 ml water and reinforcer MMT about 50-100mg has
good characteristic properties to make the moisturizing membrane for skin in the cosmetic:
+ The optimal range of absorbed doses: 20-25 kGy.
+ Water swelling: 5-6 g/g.
+ Tesile force at break: 0.09-0.10 MPa.
VINATOM-AR 13--34
The Annual Report for 2013, VINATOM
260
+ Elongation at break: 130-150 %
+ WVTR: 20-25 g/m2/hour.
- Hydrogel membrane on the CMS matrix irradiated in a range dose 20-25 kGy on the EB
accelerator has some restriction such as:
+ Because of the high dose rate, irradiated membrane appears a lot of bubbles and amount
of bubles increases with increasing of absorbed doses.
+ Making shape of product may be processed on the gamma system with the low dose rate,
then step of crosslinking and making asepsis on the EB accelerator.
REFERENCES
[1] Razzak M. T. et al., “Irradiation of polyvinyl alcohol and polyvinyl pyrrolidone blended
hydrogel for wound dressing”, Radiat. Phys. Chem., Vol. 62, pp.101-113, 2001.
[2] Murat Şen*, Esra Nazan Avcı, “Radiation synthesis of poly (N-vinyl-2-pyrrolidone)-κ-
carrageenan hydrogels and their use in wound dressing applications.I. Preliminary laboratory
tests”, Journal of Biomedical Materials Research Part A, Vol. 74A, pp.187-196, 2005.
[3] Jian Ping Gong et at., “Formation of a strong hydrogel-porous solid interface via the double-
network principle”, Acta Biomaterialia, Vol. 6, pp.1353-1359, 2010.
[4] Liudmila Korkina, Vladimir Kostyuk and Liliana Guerra, “Biohydrogels for the In Vitro Re-
construction and Insitu regeneration of human skin”, Hydrogels, Biological Properties and
Applications, pp. 97-109,2009.
[5] Olayide S. Lawal et al., “Hydrogels based on carboxymethyl cassava starch cross-linked with
di- or polyfunctional carboxylic acids: Synthesis, water absorbent behavior and rheological
characterizations, European Polymer Journal, 45, pp.3399-3408, 2009.
[6] Naotsugu Nagasawa*, Toshiaki Yagi, Tamikazu Kume, Fumio Yoshii, “Radiation
crosslinking of carboxymethyl starch”, Carbohydrate Polymers, 58, pp.109-113, 2004.
[7] Fumio Yoshiia,*
, Long Zhaob, Radoslaw A. Wach
b, Naotsugu Nagasawa
a, Hiroshi Mitomo
b,
Tamikazu Kumea, “Hydrogels of polysaccharide derivatives crosslinked with irradiation at
paste-like condition”, Nuclear Instruments and Methods in Physics Research B, 208, pp.320-
324, 2003.
[8] Bhoj Raj Pant†, Hye-Jin Jeon, and Hyun Hoon Song*, “Radiation Cross-linked
Carboxymethylated Starch and Iron Removal Capacity in Aqueous Solution”,
Macromolecular Research, Vol. 19, No. 3, pp.307-312, 2011.
[9] Rafael M. Ottenbrite, Kinam Park, Teruo Okano, Biomedical Applications of Hydrogels
Handbook, Springer, pp.1-15, 2010.
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
261
RESEARCH ON DEGRADATION OF SILK FIBROIN
BY COMBINATION OF ELECTRON BEAM IRRADIATION
AND HYDROTHERMAL PROCESSING
Nguyen Thi Kim Lan, Dang Van Phu, Le Anh Quoc and Nguyen Quoc Hien
Research and Development Center for Radiation Technology, Vietnam Atomic Energy Institute
202 A Sreet 11., Linh Xuan Ward, Thu Duc Dist., HCM City, Vietnam
ABSTRACT: Silk fibers and silk proteins have been demonstrated to be useful to apply in the textile industry,
biomedical, cosmetics, pharmaceuticals. In this study, the effects of electron beam (EB) irradiation combined
with hydrothermal processing to the solubility of silk fibroin and generation of soluble silk protein were
investigated. The solubility of unirradiated and irradiated fibroin were greater than 80% when hydrothermal
degradation was performed in the sodium hydroxide solution at appropriate concentration of 0.05 M. However,
the solubility of irradiated fibroin was greater than that of unirradiated sample. The protein content increased
from 0.4617 to 0.6530 mg/mg when irradiation doses increased from 0 to 200 kGy, respectively. The
molecular weight of protein was determined by SDS-PAGE method. The characteristics of silk protein were
confirmed by scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FT-IR),
thermogravimetric analysis (TGA) and X-ray diffraction (XRD).
Keywords: Silk fibroin, silk protein, electron beam irradiation.
I. INTRODUCTION
Silkworm (Bombyx mori) silk is a natural protein consisting of sericin and fibroin protein.
Fibroin has a long history of use as textiles and surgical sutures because of the remarkable
properties such as mechanical strength, elasticity, biocompatibility and controlled biodegradation.
In addition to, fibroin has been potential material for biomedical applications such as enzyme
immobilizing membranes, an oral dosage gel form, scaffolds for tissue engineering and materials
with anti-HIV activity or reducing blood glucose and cholesterol levels [1-4]. Proteins and amino
acids extracted from silk fibroin have been used as additives in soap production, hair conditioners
and body care products because of good moisturizing properties and compatibility with human skin
[2-8]. Many studies have been realized to segment fibroin using proteolytic enzymes. However, the
high cost of enzymes themselve has limited industrial production [9-10]. Another method which has
been used to recover the silk proteins and amino acids is hydrothermal treatment [11]. The results
showed that the use of only water at high temperature and pressure without addition of acid or alkali
catalyst would not get products effectively [8]. Research and application of irradiation technology
for degradation of silk fibroin have attracted considerable interest. Some of research results showed
that gamma or EB irradiation can affect the structures of the fibroin fibers. For example, the high
irradiation doses from 500 to 1000 kGy directly affect the solubility of silk fibroin [6, 12]. Every
year, the silk industry produces tons of silk wastes from broken down or unreeled cocoons. So, the
Project information:
- Code: CS/13/07-01
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Nguyen Thi Kim Lan, Dang Van Phu, Le Anh Quoc, Nguyen Quoc Hien, Research on degradation of
silk fibroin by combination of electron beam irradiation and hydrothermal process, Journal of Nuclear
Science and Technology, VINATOM, 2013.
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
262
application of electron beam irradiation method combined with hydrothermal processing to increase
the solubility of fibroin and to create soluble silk proteins from silk wastes is of great interest.
II. EXPERIMENTAL
II.1. Degumming of silk cocoon
Silkworm cocoon was obtained from local silk farm (Di Linh, Vietnam) and degummed
using the hydrothemal degumming method adopted by Yamada et al. [13]. The removal of sericin
by hydrothermal reaction was carried out in a SM200 autoclave (Yamato, Japan) at the temperature
of 120oC in 30 minutes. The reaction products consisted of aqueous solution and remaining fibroin
residue, which was separated from the soluble product using a filter paper (Satorius, Germany). The
fibroin residue was then dried in a forced air oven at 60oC.
II.2. Electron beam irradiation
The irradiation processing of fibroin was done at Research and Development Center for
Radiation Technology using the electron beam accelerator (UERL-10-15S2). The doses delivered to
different samples were measured by Radiochromic film B3000 (GEX) dosimeter. The samples were
subjected to various doses at 0, 50, 100 and 200 kGy.
II.3. Hydrothermal degradation in NaOH solution of irradiated fibroin
II.3.1. Effect of NaOH concentration
In each experiment, the irradiated fibroin and 0-0.1 M NaOH solution (weight ratio = 1:100)
were loaded into the autoclave (and) operated at 120oC for 1 hour. The solution and the remaining
insoluble residue were separated using a filter paper. The insolube residue was then washed with
water until pH=7, dried to get its net weight. The content of soluble fibroin was calculated
following equation (1). The protein content in solution was assayed by Lowry’s method [14] using
bovine serum albumin (BSA) as a standard and from that the protein content obtained per one
weight unit of initial fibroin (mg/mg) was calculated.
The content of soluble fibroin (%) = 100 (mo – mr) / mo (1)
where mo and mr are the weight of initial fibroin and the remaining insoluble fibroin residue,
respectively.
II.3.2. Effect of hydrothemal reaction time
The effect of hydrothemal reaction time of the fibroin samples was determined in the same
manner that described as effect of NaOH concentration. However, the experiments were conducted
in a reaction time interval of 10-30 minutes and NaOH concentration of 0.05 M. The protein
solutions were neutralized to pH = 6-7 by HCl and then dialyzed against deionized water using
cellulose tubings (molecular weight cut off 12 kDa) for 18 h with several changes of water to
remove salts. Protein powders were obtained by a Modullyo free-dryer (Thermo Electron
Corporation) with operating temperature -50oC or a ADL311 spray-dryer (Yamato, Japan) with
inlet and outlet air temperature of 120 and 60oC respectively, and liquid flow rate of 5 ml/minute.
II.4. Analysis of protein characterization
Molecular weight of the protein was determined by sodium dodecyl sulfate polyacrylamide
gel electrophoresis (SDS-PAGE) with 10% acrylamide gel using the Mini-PROTEANR 3-cell
system. A broad range marker (Bio-rad) was run as a molecular weight marker (7.1-209 kDa). Gels
were stained by G250 Coomassie Blue stain and the proteins were detected by dark blue traces on
transparent gel background.
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
263
The morphology of particles of the protein powders were observed by SEM images using
S4800 scanning electron microscope, Hitachi, Japan.
The protein powder samples were pelleted with KBr and recorded Fourier Transform
Infrared Spectroscopy (FT-IR) by a FTIR-8400S spectrometer (Shimadzu, Japan).
The protein powder samples were put into aluminum pans. Thermogravimetric analysis
(TGA) of these samples was done by DTG-60 system (Shimadzu, Japan). The temperature range
was scanned from 25oC to 600
oC at a predetermined rate of 10
oC/min.
The X-ray diffraction (XRD) analysis of the protein powders were recorded on D8 Advance
(Brucker) diffractometer using CuK radiation. These samples were scanned in the 2 range of 10-
30o with scan rate of 0.4
o/minute.
III. RESULTS AND DISCUSSION
III.1. Hydrothermal degradation of irradiated fibroin
Table 1: Effect of NaOH concentration on the solubility and protein content of irradiated
and hydrothermal degraded fibroin.
Irradiation dose
(kGy)
NaOH concentration (M) NaOH concentration (M)
0.025 0.05 0.075 0.025 0.05 0.075
Solubility (%) Protein content (mg/mg)
0 44.5 81.0 89.4 0.2339 0.4617 0.4705
50 51.3 84.6 92.1 0.3297 0.5409 0.5492
100 52.1 86.5 93.0 0.3644 0.5723 0.5760
200 53.9 88.9 94.6 0.4457 0.6530 0.6609
The solubility and protein content of irradiated fibroin that was degraded by hydrothermal
treatment in NaOH solution of 0.025-0.075 M were indicated in table 1. The results showed that the
unirradiated and irradiated fibroin had the solubility more than 80% when NaOH concentration was
0.05 M. The solubility of unirradiated fibroin was 81% while those of fibroin irradiated 50, 100 and
200 kGy were 84.6, 86.5 and 88.9%, respectively. The solubility of 50-200 kGy irradiated fibroin
was larger than that of the unirradiation sample from 2-8%. On the other hand, the solubility of
fibroin at the concentration of 0.075 M NaOH increased in comparison with concentration of 0.05
M NaOH, but protein content did not increase significantly. The protein content of 0-200 kGy
irradiated fibroins obtained from 0.4617 to 0.6530 mg/mg at the concentration of 0.05 M NaOH
while protein content was from 0.4705 to 0.6609 at 0.075 M NaOH. So, the concentration of 0.05
M NaOH was effective to dissolve 1% irradiated fibroin in the hydrothermal degradation reaction.
Table 2: Effect of time of hydrothermal reaction on solubility, protein content of irradiated
fibroin before and after dialysis.
Dose
(kGy)
Time (min.) Time (min.) Time (min.)
10 20 30 10 20 30 10 20 30
Solubility (%) Protein content Before
dialysis (mg/mg)
Protein content After
dialysis (mg/mg)
0 53.8
3.2
62.6
2.8
67.3
2.0
0.390
0.020
0.427
0.030
0.436
0.013
0.233
0.012
0.244
0.011
0.227
0.023
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
264
50 56.9
4.0
64.5
2.2
69.2
3.1
0.425
0.028
0.494
0.027
0.533
0.032
0.237
0.010
0.247
0.018
0.231
0.017
100 60.6
2.5
67.3
2.7
71.7
4.5
0.452
0.031
0.539
0.034
0.564
0.015
0.242
0.016
0.254
0.020
0.238
0.017
200 66.4
2.3
72.3
4.1
76.9
4.5
0.498
0.040
0.585
0.093
0.622
0.056
0.251
0.010
0.263
0.008
0.249
0.032
The solubility and the protein content before and after dialysis of irradiated fibroin
according to time of hydrothermal degradation reaction in 0.05 M NaOH solution were presented in
table II. The solubility of unirradiated and irradiated fibroin increased when hydrothermal reaction
time increased. The analysis results of the protein content showed that the protein content obtained
before dialysis also increased with the increase of reaction time. However, after the protein
solutions were dialysed by cellulose membranes with Mw cut off 12 kDa, the remaining protein
content at hydrothemal reaction time of 30 minutes was less than those at reaction time of 10 and 20
minutes. This might be due to lost of protein fragments whose molecular weight was less than 12
kDa were created during the reaction time of 30 minutes and so these fragments were exchanged
against in dialysis process.
III.2. Characteristics of silk protein
III.2.1. Molecular weight measurment
The results of gel electrophoresis analysis of silk protein were showed in Fig.1. The
molecular weight of protein was in range from 13 to 200 kDa and the sizes dominant lied between
34 and 50 Da that indicated the dagradation of peptide linkage. The result here is consistent with
other studies. In the research of effects of gamma irradiation on biodegradation of silk fibroin [6],
the fibroin fibers irradiated in range 0-1000 kGy were hydrolyzed by enzymatic methods in 7 days
to prepare proteins whose molecular sizes were about 33-37 kDa. Meanwhile, the research results of
Lamoolphak et al. [11] showed that the protein obtained after hydrothermal decomposition of
fibroin at temperature over 140oC had molecular weight less than 10 kDa.
Figure 1: SDS-PAGE of the marker (lane TC); spray dried sample: 50 kGy - (lane 1);
free-dried samples: 0 kGy (lane 2), 50 kGy (lane 3), 100 kGy (lane 4), 200 kGy (lane 5).
5 4 3 2 1 TC Da
209,000 124,000 80.000 49.100 34,800 28,900 20,600 7,100
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
265
III.2.2. Observation of SEM
(a) (b)
Figure 2: SEM image of protein powder (a) freeze drying, (b) spray drying.
The results on figure 2 showed that the freeze drying process of protein solution created the
protein powder with long flake-like particles while spray drying process formed protein powder
with circular particles whose size was in range between 2 and 5 m.
III.2.3. FTIR characterization
Figure 3: Infrared spectrum (FTIR) of protein powders from 0-200 kGy
irradiated fibroin.
The results of infrared spectra of the protein powders from unirradiated and irradiated
fibroin were indicated in fig. 3. The results showed that, the infrared spectra of irradiated samples
presented characteristic absorption peaks were similar that of unirradiated sample. The absorption
peak of C=O stretching mainly occured at the wavelength of 1652-1654 cm-1
. The vibration of N-H
bonding was at position of 1539-1542 cm-1
. And the phase combinations of C-N stretching and
C=O bending vibration fell in wavelength of about 1242 cm-1
[3, 15]. It was found that there was no
difference in the FT-IR spectral results of the protein powders obtained from fibroin irradiated and
unirradiated.
4000 3750 3500 3250 3000 2750 2500 2250 2000 1750 1500 1250 1000 750 500 (1/cm)
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
266
III.2.4. TGA Characterization
The thermogravimetric analysis (TGA) results of the protein powders from fibroin
unirradiated and irradiated 50-200 kGy were presented in fig. 4. The thermogram of all samples
indicated the division into four distinct sections. From room temperature to 100oC, the weight loss
was due to water evaporation of about 9%. In the second, from 100 to 280oC, the samples began to
decompose in range from 20 to 30%. In the third, there was a difference in thermal decomposition
of the irradiated fibroin samples and the original sample. The protein powder of unirradiated fibroin
decomposed 60% at temperature of 520oC. While the protein powder of irradiated samples lost
weight over 70% at the same temperature. At the end, about 70% weight of the protein powder of
unirradiated fibroin and 90% weight of the protein powders of 50-200 kGy irradiated fibroin were
decomposed to volatiles at 600oC. These results showed that the thermal stability of the protein
powders decreased with increasing irradiation dose for silk fibroin. According to the study of
Nogueira et al [16], the thermal decomposition of fibroin membranes is influenced by the internal
structure and physical properties of the sample with the degree of molecular orientation being one
of the most important parameters. Well-oriented silk materials will have decomposition temperature
of above 300oC, no oriented silk fibers with -sheet structure usually decompose in about 290-
295oC and amorphous silk fibroin occurs at a temperature lower than 290
oC. The thermal stability
of the protein powder obtained from the spray drying process was less than that of the free dried
protein powders. The results of TGA in this study showed that the protein powders had dominant
amorphous structure.
Figure 4: TGA thermograms of protein powders.
III.2.5. X-ray diffraction analysis
As well know that, silk fibroin has two regions of structure that are crystalline and
amophous. Tree types of crystal structure are -helix (silk I), -sheet (silk II) and helical structure
(silk III) [2, 11]. The main diffraction peaks of silk I are present at 2 = 12.2o, 19.7
o , 24.3
o and
28.2o while that of silk II are present at about 2 = 9.1
o , 18.9
o , 20.7
o [2]. In addition to, the
amorphous structure displays a broad diffraction peak [11]. XRD spectra of protein powders of
fibroin irradiated 0-200 kGy were recorded in the 2 range of 0o to 30
o (fig. 5 ). A sharp peak at 2
= 13o and a broad peak at 2 = 28
o-31
o were displayed on the XRD spectra of the protein powder
from unirradiated fibroin. This result indicated that there was presence of both crystal and
amorphous structure in the protein powders. On the other hand, XRD of protein powders prepared
of fibroin irradiated 100 and 200 kGy showed two broad peaks which shifted to position of 2 =
19o-22
o and 2 = 28
o-30
o. This could be a result of essential presence of amorphous structure. In
the same condition of irradiation, protein obtained from spray dried solution showed the XRD result
being the same as that of free dried samples.
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
267
Figure 5: XRD spectra of protein powders of fibroin unirradiated
and irradiated 100 and 200 kGy.
IV. CONCLUSIONS
Research on degradation of silk fibroin by electron beam irradiation combined with
hydrothermal processing to prepare silk protein were carried out. The solubility of unirradiated and
irradiated fibroin were greater than 80% when hydrothermal reaction was performed in NaOH
solution of 0.05 M. The solubility of irradiated fibroin was higher than that of unirradiated sample.
The protein content increased from 0.4617 to 0.6530 mg/mg when irradiation doses increased from
0 to 200 kGy, respectively. The molecular weight of protein was mainly in the range from 34-50
kDa. The process of freeze-drying or spray-drying formed protein powders whose particle size was
2-5m. It was found that the protein powder had essential amorphous structure and the EB
irradiation process affected the structure of silk fibroin.
REFERENCES
[1] EB. Byun et al.,“Enhancement of anti-tumor activity of gamma-irradiated silk fibroin via
immunomodulatory effects”, Chemico-Biological Interactions, 186, 90-95, 2010.
[2] J. Kundu et al.,“Silk fibroin nanoparticles for cellular uptake and control release”,
International Journal of Pharmaceutics, 388, 242-250, 2010.
[3] A. Sionkowska et al., “The influence of UV radiation on silk fibroin”, Polymer Degradation
and Stability, 96, 523-528, 2011.
[4] R. Rajkhowa et al.,“Ultra-fine silk powder preparation through rotary and ball milling”,
Powder Technology, 185, 87-95, 2008.
[5] GH. Altman et al.,“Silk-based biomaterials”, Biomaterials, 24, 401-416, 2003.
[6] A. Kojthung et al., “Effects of gamma radiation on biodegradation of Bombyx mori silk
fibroin”, International Biodeterioration & Biodegradation, 62, 487-490, 2008.
[7] Q. Lu et al., “Degradation Mechanism and Control of Silk Fibroin”, Biomacromolecules, 12,
1080-1086, 2011.
[8] K. Kang et al.,“Behavior of hydrothermal decomposition of silk fibroin to amino acids in
near-critical water”, Korean Journal of Chemical Engineering, 21 (3), 654-659, 2004.
[9] Y. Suzuki et al.,“Enzymatic degradation of fibroin fiber by a fibroinolytic enzyme of
Brevibacillus thermoruber YAS-1”, Journal of Bioscience and Bioengineering, 108 (3), 211-
215, 2009.
2o
10 20 30
Counts 4000
3000
2000
1000
0
VINATOM-AR 13--35
The Annual Report for 2013, VINATOM
268
[10] RL. Horan et al., “In vitro degradation of silk fibroin”, Biomaterials, 26, 3385-3393, 2005.
[11] W. Lamoolphak et al., “Hydrothermal production and characterization of protein and amino
acids from silk waste”, Bioresource Technology, 99, 7678-7685, 2008.
[12] H. Takeshita et al.,“Production of fine powder from silk by radiation”, Macromolecular
Materials and Engineering, 283 (1), 126-131, 2000.
[13] H. Yamada et al.,“Preparation of undegraded native molecular fibroin solution from
silkworm cocoons”, Materials Science and Engineering, C 14, 41-46, 2001.
[14] OH. Lowry et al.,“Protein measurement with the folin phenol reagent”, Journal of
Biological Chemistry, 193(1), 265-275, 1951.
[15] S. Halabhavi et al.,“Interaction of 8 MeV Electron Beam with P31 Bombyx mori Silk
Fibers”, Materials Sciences and Application, 2, 827-833, 2011.
[16] GM. Nogueira et al.,“Preparation and characterization of ethanol-treated silk fibroin dense
membranes for biomaterials application using waste silk fibers as raw material”, Bioresource
Technology, 101, 8446-8451, 2010.
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
269
SYNTHESIS OF Fe3O4-CHITOSAN MAGNETIC NANOCOMPOSITES
BY GAMMA IRRADIATION FOR ABSORBING OF HEAVY METALS
IN AQUEOUS SOLUTIONS
Tran Minh Quynh, Nguyen Van Binh, Nguyen Quang Long and Hoang Dang Sang
Hanoi Irradiation Center, Vietnam Atomic Energy Institute,
No.5-Minh Khai, Tu Liem, Ha Noi
ABSTRACT: Studies on adsorption capacity of the obtained Fe3O4-chitosan nanoparticles for metal ions in
aqueous solutions showed that initial amount of adsorbent and pH have much influenced on their adsorption
capacity. Adsorption rate was quite fast at first, then slower. Maximum adsorption capacity were measured at
25C are 71, 41.4 and 26 mg/g obtained at pH 5, 6 and 7 for Cu(CH3COO)2.H2O, Pb(CH3COO)2.3H2O and
NaH2AsO4.7H2O, respectively. The adsorption capacity increased with adsorbent amount to a certain value,
then leveled off. These results suggested that the Fe3O4-chitosan nanoparticles can be applied as a potential
adsorbent for removal of heavy metals from aqueous solution, but it required further studies including of
adsorption kinetics and desorption in order to control the process in practice.
1. INTRODUCTION
Magnetic nanoparticles (Fe3O4) have been studied and applied in many various fields due to
their superparamagnetic properties as well as their responsibility to surrouding fields [1-3]. Their
application was further improved by incorporating with multi-functional polymers such as chitin,
chitosan, alginate or other bio-polymers [1,4]. Recently, magnetic Fe3O4-chitosan nanoparticles
were prepared by using chitosan as stabilized agent for coating Fe3O4 [5,6]. These magnetic
nanoparticles can be used as adsorbent for removal of some pollutants in the aqueous solutions via
their covalent bonding of chitosan with metal ions or organic compounds. In addition, chitosan can
be modified in order to adsorb certain substance, especially for preparation of the targeted drug
delivery systems, adsorbents, enzymatic or microbial immobilizers, etc.
Several methods have been developed for preparation of magnetic and Fe3O4-chitosan
nanoparticles such as blending, polymerization, co-precipitation, suspension crosslinking... [6-11].
However, the nanoparticles are rather large and inhomogeneous in size, limited their application in
practice. In this study, gamma irradiation treatment has been applied for preparation of the
ferrimagnetic and Fe3O4-chitosan nanoparticles from FeCl3 solutions and the solutions containing
chitosan and Fe3O4, respectively. During irradiation, chitosan can crosslink resulting in the stable
nanoparticles [12].
Project information:
- Code: CS/13/08-01
- Managerial Level: Institute
- Allocated Fund: 70,000,000 VND
- Implementation time: 10 months (Mar 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Tran Minh Quynh, Nguyen Van Binh, Nguyen Quang Long, Hoang Dang Sang. Characterization of
the magnetic Fe3O4 nanoparticles prepared by gamma irradiation. Nuclear Science and Technology.
2014, xx-xx (Accepted).
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
270
The size, structure and magnetic properties of the obtained magnetite and Fe3O4-chitosan
nanoparticles were characterized by SEM, TEM, XRD and vibrating sample magnetometer (VSM).
The Fe3O4-chitosan nanoparticles were applied as an efective absorbents for removal of some metal
ions from aqueous solutions. Their adsorption capacity for heavy metal ions were determined by
UV spectrometer.
2. MATERIALS AND METHODS
2.1. Materials
FeCl2.4H2O, FeCl3.6H2O, Cu(CH3COO)2.H2O, Pb(CH3COO)2.3H2O, AgNO3 were bought
from Xilong Chemical Co. Ltd., China. Zinc in pellet, triallyl isocyanurate (TAIC), sodium
diethyldithiocarbamat (NaDDC) were purchased from Wako Pure Chemical Inc., Japan.
NaH2AsO4.7H2O from BDH Chemical, England. Chloroform, isopropanol, acetic acid, parafin and
other organic solvents from Dae Jung Chemicals and Metals.Co., Ltd. Korea. NaOH, NH3OH, HCl,
and other popular chemicals were bought from Merck, or Guangdong Guanghua Sci-Tech. Co., Ltd.
China.
2.2. Radiation preparation of magnetite and Fe3O4-chitosan nanoparticles.
Gamma irradiation has been used to preparation of magnetite nanoparticles as reported by
Wang et al [11]. Firstly, FeOOH.H2O was precipitated by dropping NH3OH into FeCl3 solution to
the molar ratio about 1.8 for NH3 compared to Fe3+
, the precipitant was collected, washed and dried
at 60C under vacuum for a hour. 20 mL isopropanol was added to each 100 mL of FeOOH 1% for
OH scavenger and differnt mixtures were irradiated at various radiation dose ranging from 10-50
kGy under gamma source of about 60 kCi at Hanoi Irradiation Center. After that, alkaline solution
(NaOH 10%) was added to the irradiated solution for precipitation. The precipitant was separated,
washed and dried under vacuum at 60C for 2 hours. Finally, the obtained products were ground
into small size, the obtained black magnetite nanoparticles were storaged in desiccator in order to
avoid oxidation.
For preparation of Fe3O4-chitosan nanoparticles, magnetite nanoparticles were regularly
dispersed in parafin into 100 mL homogenous emulsion, then 20 mL chitosan solution, 2 mL TAIC
were added, the obtained emulsion were iradiated at various radiation dose. The resulting products
after pricipitation with alkaline solution were ground into fine particles and the effects of radiation
dose and chitosan concentration on the particle size and their structures were determined by
scanning electron microscope SEM), transition electron microscope (TEM), X-ray diffraction
(XRD), and vibrating sample magnetometer (VSM).
2.3. Measurements
Adsorption capacitis of Fe3O4-chitosan nanoparticles for Cu(II), Pb(II) and As(V) ions were
investigated with the Cu(CH3COO)2.H2O, Pb(CH3COO)2.3H2O and NaH2AsO4 solutions. 100 mL
of salt solution was put into each 250 mL flask, a predetermined amount of Fe3O4-chitosan was
added and the solution was shaken in a thermostat at 25C at 120 rpm. The adsorption capacity in
mg of metal ions adsorbed on 1 g of the adsorbent at equilibrium in mg/g (Qe) was calculated as
follow:
Qe = (C0 - Ce) V / m (1)
where C0 and Ce (mg/L) were the metal concentrations at initial and the time of equilibrium,
respectively. V is the volume of solution containing metal ion (in this case 100 mL), and m is
adsorbent mass in gram. The effects of pH, contact time, and initial amount of Fe3O4-chitosan on
the adsorption capacity for metal ion at equilibrium were studied at the same conditions.
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
271
3. RESULTS AND DISCUSSIONS
3.1. Radiation preparation of magnetite and Fe3O4-chitosan nanoparticles
The results showed both magnetite Fe3O4 and Fe3O4-chitosan nanoparticles can be prepared
by precipitating the irradiated solutions in alkaline solution. Figure1 shows the SEM and TEM
images of these products. From that, average size of the resulting particles can be estimated.
Average diameter of the obtained nanoparticles reduced from 46 to 19 nm with irradiation dose.
Table 1: Preparation of magnetite nanoparticlesby gamma radiation.
Sample Radiation dose (kGy) Reaction yield (%) Average size (nm)
1 10 10.5 46
2 20 27.6 35
3 30 38.9 27
4 40 46.3 21
5 50 42.4 19
However, these reaction yield quickly increased with radiation dose to 40 kGy, then slightly
reduced. These values are much smaller than those compared with copricipitation method, but
similar to the nanoparticles prepared by gamma radiation as reported elsewhere [11]. Therefore, the
dose of 40 kGy was selected as optimal dose for radiation preparation of magnetite nanoparticles.
3.2. Characterization of Fe3O4-chitosan and the effect of chitosan concentration
Table 2: Typical properties of magnetic Fe3O4-chitosan nanoparticles.
Sample Weight ratio of
Fe3O4/Chitosan
Particle size (nm) (s) (emu/g)
1 10/1 25 30.52
2 5/1 26 30.37
3 2/1 31 12.37
4 1/1 35 1.25
Figure 1: SEM microscope of magnetite nanoparticles (a) and
TEM image of Fe3O4-chitosan nanoparticles (b) prepared by gamma radiation.
a b
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
272
Typical properties of magnetic Fe3O4-chitosan have been investigated with chitosan
concentration in the emulsion for radiation preparation. In order to investigate the influences of
chitosan solution on the properties of the resulting magnetic Fe3O4-chitosan nanoparticles, the same
amount of Fe3O4 dispersed in parafin were mixed with the chitosan solutions of different
concentration and iraidated at 40 kGy. The results were presented in Table 2.
Figure 2: TEM images of different magnetic Fe3O4-chitosan nanoparticles.
-60
-40
-20
0
20
40
60
-10000 -5000 0 5000 10000
Magnetic Field (Oe)
Mag
ne
tiza
tio
n (
em
u/g
)
Fe3O410:1/Fe3O4-chitosan
5:1/Fe3O4-chitosan2:1/Fe3O4-chitosan1:1/Fe3O4-chitosan
Figure 3: Hysteresis loop of magnetic Fe3O4 and Fe3O4-chitosan nanoparticles.
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
273
As one can see, average diameter of the nanoparticles, which were calculated from their
TEM images increased with chitosan amount in the initial emulsions. The results suggested that the
molar ratio of chitosan and Fe3O4 much influenced on the resulting particles. Average size of the
nanoparticles increased with chitosan content while their saturation magnetization (s) quickly
decreased. The value of (s much reduced with the ratio of chitosan and Fe3O4 higher than 1:2, this
may due to the excessivie chitosan would be absorbed onto the surface of polymer magnetic
nanostructures. Low saturation magnetization may reduced the responsibility of magnetic materials
with surrounding field, then the Fe3O4/chitosan ratio of 5:1 were chosen for further experiments.
The structural properties of Fe3O4 and Fe3O4-chitosan were also analysed by X-ray
difraction. Figure 4 shows XRD patterns of these nanoparticles by compared with the data of
magnetite standard pattern. The diffraction peaks at 2q = 30.2, 35.6, 43.1, 53.4, 57 and 62.6,
correspond to (220), (311), (400), (422), (511) and (440), respectively. There are no impurity peak
suggested that the products contain Fe3O4 with a tiny amount of -Fe2O3.
3.3. Adsorption equilibrium of some metal ions onto the magnetic Fe3O4-chitosan
In this experiment, the magnetic Fe3O4-chitosan nanoparticles were used as absorbent
materials for removel some heavy metal ions in aqueous solutions. Figure 4 showed the equilibrium
adsorption capacity of the material for Cu(II), Pb(II) and As(V) in the aqueous solutions at diferent
pH.
Figure 5 showed the dependance of adsorption capacities of Fe3O4-chitosan for Pb(II) in
aqueous solution of Pb(CH3COO)2 at equilibrium state (Qe). It was obviously that, adsorption
capacity of magnetic Fe3O4-chitosan nanoparticles depended on the pH and initial amount of the
absorbent. Maximum efficiency for removal of Pb(II) was about 41.4 mg/g, which can be observed
at pH 6. The adsorption efficiency increased with the initial amount of the absorbent, it reached to
maximum with 0.05 g of magnetic material for solution containing 100 ppm Pb(II), then leveled off
with further increasing of absorbent content.
Inte
nsity (
a.u
)
2
(deg)
20
30
40
50
60
70
311
440 51
1 400
220
422
XRD patterns of magnetite standard sample,
Magnetic Fe3O4 nanoparticles and
Fe3O4-chitosan nano composites prepared by gamma radiation
Figure 4: XRD patterns of various magnetic nanoparticles with and without chitosan.
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
274
4. CONCLUSION
Gamma irradiation treatment has been applied for preparation of the ferrimagnetic and
Fe3O4-chitosan nanoparticles from solutions of FeCl3 and chitosan containing Fe3O4, respectively.
The results showed that the Fe3O4-chitosan nanoparticles can be prepared by precipitating the
irradiated solutions in alkaline solution, but the yield of this reaction was much lower than
compared with preparation of ferromagnetic nanoparticles. Average diameter of the obtained
nanoparticles ranging from 10 to 25 nm depended on the irradiation dose, and it quickly increased
with radiation dose to 40 kGy dose, then slightly decreased. These values also increased with
chitosan amount in solution. Therefore, the 5:1 ratio of Fe3O4 and chitosan, and the dose of 40 kGy
were chosen as the optimal conditions for preparation of Fe3O4 and Fe3O4-chitosan nanoparticles.
Studies on adsorption capacity of the obtained Fe3O4-chitosan nanoparticles for metal ions
in aqueous solutions revealed that the initial amount of the adsorbent and pH have much influenced
on adsorption process. Adsorption rate was quite fast at first, then gradualy slow. Maximum
adsorption capacity were measured at 25C are 71, 57 and 26 mg/g obtained at pH 5, 6 and 7 for
Cu(CH3COO)2.H2O, Pb(CH3COO)2.3H2O and NaH2AsO4.7H2O, respectively. The adsorption
capacity increased with adsorbent amount to a certain value, then leveled off. These results
suggested that the Fe3O4-chitosan nanoparticles can be applied as a potential adsorbent for removal
of heavy metals from aqueous solution, but it required further studies including of adsorption
kinetics and desorption in order to control the process in practice.
REFERENCES
[1] Bin Kang et al. Radiation synthesis and megnetic properties of novel Fe3O4-chitosan
compound nano particles for targeted drug carrier. Radidation Physics and Chemistry 76,
968-973, 2007.
[2] Nhung NT, Thuong NTK. Separation and removal of Pb2+
from aqueous solutions using
Fe3O4 nanopartilces. VNU Journal of Science, Natural Sciences and Technology, Hanoi
National University 24, 305-309, 2008.
[3] M.Faraji et al. Cetytrimethylammonium Bromide-Coated Megnetite Nanoprticles as Highly
Efficient Adsorbent for Rapid Removal of Reactive Dyes from the Textile Companies
Wastewaters. Journal of the Iranian Chemical Society.
[4] Duc NH, Danh TM, Dung TT. Preparation and study on magnetic properties of nanoparticles
Fe3O4 for biomedical applications. VNU Journal of Science, Natural Sciences and
Technology, Hanoi National University 23, 231-237, 2007.
0
10
20
30
40
50
2 3 4 5 6 7 8
pH
Adsorp
tion c
apacity (
mg/g
)
Figure 5: Adsorption capacity of Fe3O4-chitosan for heavy metal ions at equilibrium.
60
65
70
75
80
0 0.05 0.1 0.15 0.2 0.25
Weight of Fe3O4-chitosan material (g)
Adsorp
tion e
ffic
iency (
%)
VINATOM-AR 13--36
The Annual Report for 2013, VINATOM
275
[5] Lian-ying Zang et al. Control synthesis of magnetic Fe3O4-chitosan nanoparticles under UV
irradiation in aqueous system. Current Applied Physics 10, 828-833, 2010.
[6] Gui-yin Li et al. Preparation and properties of megnetic Fe3O4-chitosan nanoparticles.
Journal of Alloys and compounds 466, 451-456, 2008.
[7] Tomohiro Iwasaki, et al. Mechanochemical preparation of magnetite nanoprarticle by
coprecipitation. Material Letters 62, 4155-4157, 2008.
[8] Jing Xu, et al. Preparation and magnetic properties of magnetite nanopracticles by sol-gel
method. Journal of Magnetism and Magnetic Materials 309, 307-311, 2007.
[9] R.Y.Hong et al. Synthesis of Fe3O4 nanoparticles without inert gas protection used as
precursors of magnetic fluids. Journal of Magnetism and Magnetic Materials 320, 1605-
1614, 2008.
[10] Don Keun Lee et al. Preparation and characterization of megnetic nanoparticle by γ-
irradiation. Materials Science Engineering C24, 107-111, 2004.
[11] Wang S, Xin H, Qian Y. Preparation of nanocrystalline Fe3O4 by -ray radiation. Materials
Letters 33; 113-116, 1997.
[12] Jinhua Du et al. Preparation of superparamagnetic γ- Fe2O3 nanoparticles in nanoqueous
medium by γ-irradiation. Journal of Megnetic Materials 302, 263-266, 2006.
VINATOM-AR 13--37
The Annual Report for 2013, VINATOM
276
STUDIES ON STERILIZATION PROCESS FOR SOMETRADITIONAL
PRODUCTS OF HERBAL MEDICINE BY GAMMA RADIATION
Hoang Phuong Thao, Nguyen Van Binh, Tran Bang Diep, Hoang Dang Sang,
Nguyen Thuy Huong Trang, Pham Duy Duong and Tran Minh Quynh
Hanoi Irradiation Center, Vietnam Atomic Energy Institute
No.5-Minh Khai, Tu Liem, Ha Noi
ABSTRACT: Herbal eyebright products and their raw materials have been irradiated with 1, 2, 3 and 5 kGy by
Co-60 gamma radiation source at Hanoi Irradiation Center (VINATOM) for sterilization. Initial bioburdens
were under the limitation levels established for the traditional medicines according to the decree of
16/2011/TT-BYT issued by Vietnam Health Ministry. These values for both bacteria and fungus slightly
increased during storage to three months, reach to about 103 and 10
2 CFU/g for bacteria and mold,
respectively. However, there are no microbial colony could be observed in the samples irradiated with dose
higher than 3 kGy, suggested that the radiation dose of 3 kGy was enough for sterilization of eyebright raw
powders and products. At higher radiation dose of 5 kGy, the moisture and vitamin A content of the samples
were insignificantly changed. These mean the radiation treatment with lower dose did not influenced on the
quality of eyebright products, and radiation treatment can be applied to prolong the storage of not only
eyebright, but also other traditional medicines.
1. INTRODUCTION
The use of eyebright in cultural and traditional settings may differ from concepts accepted
by current Western medicine. Considering the use of herbal supplements, consultation with a
primary health care professional is advisable. Additionally, consultation with a practitioner trained
in the uses of herbal/health supplements may be beneficial, and coordination of treatment among all
health care providers involved may be advantageous.
Food irradiation is a modern technology applied to assure the quality and sanitary safety of
foods. At present, there are more than 30 countries worldwide applied food irradiation technology
for processing of more than 40 different kind of food from fresh fruits, cereals, meat and other
agricultural and seafood products to dehydrated spices. Due to wholesomeness as well as economic
benefit of irradiated food, World Health Organization (WHO), Food and Agriculture Organization
(FAO) and International Atomic Energy Agency (IAEA) approved irradiation as an effective
quarantine method for food similar to the hot and cold temperature treatment [1]. Irradiation is
effective method for quarantine control and prevention of foodborn diseases as well as reducing
economic loss. The herbal medicines have been used in many countries but in Vietnam there is no
adequate scientific and technological base for application development methods on an industrial
scale. So there should be more research applications of radiation technology on medicinal products
for traditional medicine development, while enhancing the applications of nuclear energy in the
economic field.
Project information:
- Code: CS/13/08-03
- Managerial Level: Institute
- Allocated Fund: 60,000,000 VND
- Implementation time: 12 months (Jan 2013- Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
Quynh TM et al. Studies on decontamination for herbal eyebright raw material and product by
gamma radiation. To be published in Journal of Nuclear Science and Technology, VINATOM, 2014.
VINATOM-AR 13--37
The Annual Report for 2013, VINATOM
277
In this project, both eyebright raw materials and commercial products were collected as
samples from Traphaco joint stock company, which has grown into the second largest
pharmaceutical firm in Vietnam. Their initial bioburden as well as their contamination levels during
storage were investigated with radiation dose in order to verify the advantages of radiation
treatment for sterilization and prolong the storage period for the herbal medicine.
2. MATERIALS AND METHODS
2.1. Materials
The eyebright raw materials and commercial products were kindly supported from Traphaco
joint stock company, Vietnam. These samples were divided and packaged into PE bags of about 20
g for each. Meat-pepton agar (MPA) and Sabouraud dextrose agar were purchased from Nihon
Seiyaku, Japan. Other chemicals were bought from Wako Pure Company, Japan.
2.2. Determination of microorganism contamination
Microbial contamination levels in both eyebright raw material and commercial product were
investigated based on number of count forming unit per 1g sample (CFU/g), which can be
developed in MPA and Sauboraud media for bacteria and fungfus, respectively according to TCVN
5165-90 [2,3].
2.3. Radiation treatment and measurements
The samples were irradiated by gamma Co-60 radiation at dose of 0, 1, 2, 3 and 5 kGy as
respective symbol of M1-5 under Co-60 source of Hanoi Irradiation Center with dose rate of about
~1 kGy per hour. Moisture and vitamin A content in the samples were determined by drying and
HPLC [4].
3. RESULTS AND DISCUSSIONS
3.1. Microbial contamination levels of eyebright samples during storage
Table 1: Bioburden of the eyebright samples during storage.
Sample Storage period
(month)
Total number of colony forming unit (CFU/g)
Aerobic bacteria Fungi and molds
Raw materials
0 590 ± 0.22 46 ± 0.21
1 150 ± 0.08 23 ± 0.11
3 600 ± 0.30 13 ± 0.04
Commercial
products
0 26 ± 0.15 13 ± 0.05
1 33 ± 0.20 6 ± 0.01
3 250 ± 0.090 13 ± 0.06
The total number of bacteria and fungi (CFU) observed from the eyebright samples during
storage were presented in Table 1. From the data, we can concluded that contamination levels of
aerobic bacteria in both raw material and commercial products of eyebright increased, but fungal
levels slightly decreased with storage period. These may due to recontamination of bacteria into the
samples during storage. It was very interesting that the contamination level of fungi reduced. It
required further studies for clearify this phenomena. However, we should applied some method to
control the recontamination for eyebright samples during storage, especially for eyebright raw
materials. In this study, gamma radiation has been used to sterilization eyebright and prolong their
VINATOM-AR 13--37
The Annual Report for 2013, VINATOM
278
storage periods. And the contamination levels of eyebright samples were investigated with radiation
dose.
3.2. Radiation effects on the microbial level of eyebright during storage
Table 2: Total number of microorganisms contaminated
on the eyebright samles with radiation dose after three months storage.
Sample Dose (kGy) Total number of colony forming unit (CFU/g)
Aerobic bacteria Fungi and molds
Raw materials
0 590 ± 0.22 46 ± 0.21
1 66 ± 0.26 (N)
2 12 ± 0.01 (N)
3 (N) (N)
5 (N) (N)
Commercial
products
0 26 ± 0.15 13 ± 0.05
1 21 ± 0.13 6 ± 0.01
2 (N) (N)
3 (N) (N)
5 (N) (N)
None: can not observed
Table 2 showed the existing of aerobic bacteria and fungi on the eyebright storage. The
results suggested that radiation treatment can be used as an effective tool for reduction of total
microorganisms existing in both eyebright raw material and commercial products. The radiation
dose of 3 kGy was enough for prolong the storage period of the eyebright products over three
months without microbial contamination.
3.3. Radiation effect on the quality of eyebright powders and products
0.0
2.0
4.0
6.0
8.0
10.0
0 1 2 3 5Radiation Dose (kGy)
Mo
istu
re c
on
ten
t (%
)
0.0
2.0
4.0
6.0
8.0
10.0
0 1 2 3 5
Radiation Dose (kGy)
Mo
istu
re c
on
ten
t (%
)
Figure 1: Effects of gamma irradiation and storage period on the moisture content
of eyebright powder (a) and products (b).
just after irradiation;; aafftteerr oonnee mmoonntthh aanndd tthhrreeee mmoonntthhss
aa bb
VINATOM-AR 13--37
The Annual Report for 2013, VINATOM
279
As presented in Figure 1, the mosture content in both eyebright material and product slightly
reduced by radiation, then quickly recovered during storage. For each sample, there are no
significant changes in moisture content during stogare. It may due to the hydrolysis of water during
gamma irradiation, but the sample can absorb the moisture to the saturated content during storage.
Table 3: Vitamin A content (µg/1000g) in the eyebright samples with radiation dose.
Radiation dose
(kGy)
Eyebright Samples
Raw powder
after irradiate
Raw powder
after 1 month
Capsule after
irradiate
Capsule after 1
month storage
0 127.13 113.21 116.1 119.13
1 125.07 116.15 114.08 120.11
2 124.01 111.2 112.05 125.07
3 120.18 115.3 118.08 128.22
5 127.13 118.3 113.09 116.1
Vitamin A was detected with high performance liquid chromatography (HPLC) by
procedure of H.HD.QT.145 at National institute for Food Control. As one can see from the Table 3,
all eyebright samples containing vitamin A. However, the content of vitamin A in powder samples
higher than that in commercial samples (eyebright capsule). It may due to the presence of other
additives in the commercial products, or the degradation of vitamin A during processing. Vitamin A
seemed not to be affected by radiation treatment, and storage in laboratory condition. According to
some studies, radiation treatment did not effected to beta-caroten of herbs or other compounds at
lower radiation dose of 10 kGy [5]. However, other ingredients of the eyebright raw material and
commercial products should be determined for understanding the influence of radiation treatment
on the quality criteria of these oriental drugs.
4. CONCLUSION
Microbial contamination level of eyebright raw powder and commercial product increased
with storage period, but it can be easily controlled by radiation treatment. Radiation dose of 3kGy is
enough for elimination the growth of aerobic bacteria as well as fungi and molds existing on the
eyebright samples. Radiation treatment at higher dose of 5 kGy does not influence on the quality of
eyebright materials. Therefore, gamma irradiation should be considered as an effective method for
sterilization for not only eyebright raw materials and products, but also for other herbal medicines.
REFERENCES
[1] IAEA (International Atomic Energy Agency) Irradiation to ensure the safety and quality of
prepared meals, Vienna, Austria, p.375, 2009.
[2] Dung NL et al. Study methods of microorganisms. Vol 2. Science and technology Publisher,
Hanoi, pp. 7-15, 1982.
[3] Standards of Vietnam TCVN 5104-90, Food and spices products, National Committee of
Science, Hanoi, 1990.
[4] J. Farkas, “Chapter 11 radiation decontami-nation of spices, herbs, condiments and other
dried food ingredients”, Szent Istvan University, Budapest, Hungary, 2000.
[5] Paula M. Koseki, et al. Effects of irradiation in medicinal and eatable herbs. Radiation Physis
and Chemistry; 63: 681-684, 2002.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
283
STUDY ON BENEFICIATION TECHNOLOGY OF DONG PAO RARE-
EARTH-BARITE-FLUORITE WITH TWO PRODUCT PLANS ABOUT
CONTENT AND RECOVERY OF RARE-EARTH FINE ORES
Duong Van Su, Truong Thi Ai, Bui Ba Duy, Bui Thi Bay, Nguyen Hong Ha,
Le Thi Hong Ha, Doan Thi Mo, Doan Dac Ban and Nguyen Hoang Son
Center for Radioactive Ore processing Technology,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48- Lang Ha, Dong Da, Ha Noi
ABSTRACT : The ore sample used in the research was taken from the F3 ore bodies and the sample of the F7,
F9 and F16 ore bodies which contain the average of 5.98% TR2O3; they are multi-metals ore which is difficult
to enrich, highly weather with very complex ingredients. The process of the experiment is the ore is crushed,
grinded, screened and classified reasonably to-0.1mm and divided into 3 particle size with the following
technique: (1)-0.020mm is primary sludge and the rare-earth fine ore; (2) 0.075-1mm is gotten through the
sludge concentrating table with the output is the 2 parts: the heavy part which is dried magnetic separator with
high magnetism to get the rare-earth fine ore and the light one; (3) Light minerals, non-magnetic and
ferromagnetic minerals group are grinded together to 85% of them get size within-0.075 mm then mix it with
0.020-0.075 mm group. Using flotation separator, get barite-rare earth mixture and fluorite. After that, we
separate this mixture by secondary flotation and get refined rare earth, barite and fluorite mineral.
The result of the theme: (1) product plan A-rare-earth fine ore has TR2O3 content archive 42.07% with
recovery is 69.70%; (2) product plan B-rare-earth fine ore has TR2O3 content archive 29.64% with recovery is
80.01%.
1. THE PROJECT OBJECTIVE
The suggestion toward the procedure of the Dong Pao rare-earth enrichment technique to
obtain the fine ore with the quality and the quantity is:
(1) Refined barite with βBaSO4 90% and BaSO4 75% acquired is 50 kg.
(2) Refined fluorite with βCaF2 85% and CaF2 60% acquired is 50 kg.
(3) Refined rare earth minerals we get follow two option:
+ Plan A: Refined rare earth with βTR2O3 42% and TR2O3 75 % acquired is 50 kg.
+ Plan B: Refined rare earth with βTR2O3 30 % and TR2O3 90 % acquired is 50 kg.
Project Information:
- Code: 01/11/VCNXH
- Managerial Level: Ministry
- Allocated Fund: 700,000,000 VND
- Implementation Time: 24 months (Jan 2012 – Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project:
1. Duong Van Su, Truong Thi Ai, Bui Ba Duy, Le Quang Thai, Trinh Nguyen Quynh, Vu Khac Tuan, Bui
Thi Bay, Nguyen Hong Ha. Summarize some of the results of the research about Lai Chau rare earth's
beneficiation technology was published. 4th
National conference on mineral processing science and
technology, Ha Noi 2014.(in Vietnamese).
2. Duong Van Su, Truong Thi Ai, Bui Ba Duy, Le Quang Thai, Trinh Nguyen Quynh, Vu Khac Tuan, Bui
Thi Bay, Nguyen Hong Ha. Difficults in technology for rare earths milling process on Lai Chau’s ore. 4th
National conference on mineral processing science and technology, Ha Noi 2014. 26th
National
conference on milling science and technology, Vung Tau 2014. (in Vietnamese).
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
284
2. THE INTRODUCTION OF THE RESEARCH SAMPLE AND THE PROCESSING
EQUIPMENT, THE MAIN ENRICHMENT METHOD USED IN THE STUDY
2.1. The research sample
The research sample is taken from the F3 ore bodies and the technical sample from the F7,
F9 and F16 ore bodies of “The further probing the Dong Pao fluorite -barite rare-earth project in
Ban Hon, Tam Duong, Lai Chau” in 2010 of Lai Chau rare-earth joint stock. The total of the mixed
sample used to do the research is blended with the weight proportion of F3/F7/F9/F16=1.5/1/1/1,
added up into 1 sample with the weight of 1650kg.
2.2. The processing equipment and the main enrichment method used in the research.
The main equipment of the project is introduced from Fig. 1 to Fig. 6.
Figure 1: Trammel screen, shaking -
spiral classifier-vibrating screen.
Figure 2: Sludge concentration table
BxL = 1.8x4.5 m (Chinese).
Figure 3: Hydrocyclone D = 25.0 mm. Figure 4: Dry magnetic separator 138 T
СЭМ (USSR).
Figure 5: Wet magnetic separator with
high intensity (USA).
Figure 6: Floatation machine DENVER
(USA).
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
285
2.3. Reasons for milling methods and equipment selection.
With all the characteristics of ore's material composition, minerals in Dong Pao rare earth
ores; we've chosen milling methods and equipment base on several reasons as follow:
1. Dong Pao rare earth ores are weathered, especially for rare earth minerals. Their form
usually is friable powder, sometime clutching to each other by hydroxide iron gel. Rare earth
minerals have strong bond and well mixed with most of accompany minerals, therefore smashing,
grinding, screening step must be adequate to help release all minerals from stick together. It's
suggested that ore should be smashed to below 1 mm particle size.
2. Rare earth content in primary sludge (with 0.020 mm particle size) is considerably rich;
reach 24.77% TR2O3, so hydrocyclone separator is selected for primary sludge removal to refined
ore. It's also advantage for following milling step.
Rare earths are mostly concentrated in 0.075 mm particle size (Table 13-76.27% and Table
14-78.10%), so smashed ore to 1.0 mm size is separated to 3 smaller size groups: (1) 0.075-1.0 mm;
(2) 0.020-0.075 mm and (3) below 0.020 mm (primary sludge) in order to help later milling
processes.
3. Density of minerals in this ore from heavy to light as follow: hematite 5.0-5.2 >
magnetite 4.9-5.2 > bastnaesite 4.7-5.0 > barite 4.3-4.5 > goethite 4.0-4.4 > limonite 3.3-4.0 >
fluorite 3.0-3.2 > felspate 3.0 > crystal 2.5-2.8 >… dirt. It's realized that bastnaesite belong to group
with very high density, therefore, we can use gravity separator to separate them to 2 groups base on
their density: (1) heavy minerals group contain hematite, magnetite, bastnaesite and barite; (2) light
minerals group contain fluorite, crystal and dirt. The analysis result show that rare earth content in
light group is still high, so we can only use gravity separator right before dry magnetic separator to
save energy for drying step.
4. Magnetism characteristic of minerals fin this ore from strong to weak as follow:
magnetite (very strong) > hematite (strong) > Goethite (weak) > limonite (very weak) > bastnaesite
(very weak) > … > barite (non magnetic) > fluorite (non magnetic) > crystal (non magnetic) > dirt
(non magnetic). With the difference a bout magnetism, we can use magnetic separator to separate
ore to 4 groups: (1) strong magnetic minerals; (2) weak magnetic minerals, (3) very weak magnetic
minerals and (4) non magnetic minerals.
On site experiments of Dong Pao rare earth ore milling reveal that bastnaesite mineral has
very weak magnetism, so we have to use very strong magnetic separator with very high magnetism
flux density, up to 1.5-1.8 millions Tesla. Ore with particle size from 0.075-1 mm is very
susceptible with dry magnetic separator. Particle size of 0.075 mm and below can't be used with dry
magnetic separator at any flux density, wet magnetic separator (American ERIEZ) also ineffective
on this particle size.
5. Water repellency of minerals: Ore sample has 3 useful minerals; among them, barite has
highest natural floatability compare to fluorite and bastnaesite on any collector in the market.
Fluorite and bastnaesite has similar floatability, depent on collector. As a result, in the flotation
separate step, we must figure out most effective reagent with high selective on each minerals and
optimum condition of flotation separate.
2.4. Suggest an enrichment technological layout for Dong Pao rare earth ore.
Base on the research off content, result collected from experiment of each enrichment
method, model and actual condition, we have presented technological layout for enrichment of
Dong Pao rare earth ore, combine several enrichment methods such as,classification, gravity
concentration, magnetic separation with strong magnetic field, selective floation or collective
floation, as shown in figure 7. Enrichment steps in this layout are listed as follow:
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
286
1. Properly prepare ore, avoid grind it too fine. Trammel screen, shaking, grinding balls,
vibrating screen and spiral classifier are used together to bring all ore particle below 1.0 mm size.
2. Using particle size classification methods (hydrocyclone, spiral classifier) to separate
processed ore to 3 groups base on their particle size: (1) 0.075-1.0 mm; (2) 0.02-0.075 mm; (3)
below 0.02 mm (primary sludge). Particle size below 0.02 mm are separated will bring advantages
for later steps because it's already very fine rare earth refined ore.
3. Using gravity concentration (sludge concentrating table and multi gravitational separator)
separate ore group with particle size 0.075-1.0 mm to two minor groups: (1) heavy minerals group
and (2) light minerals group.
4. Dry magnetic separator with high magnetic field is use on dried heavy minerals group to
separate it to 3 minor groups: (1) ferromagnetic minerals group (has strong and medium
magnetism); (2) rare earth minerals group (has weak magnetism) and (3) non magnetic minerals
group-contain mostly barite).
5. Light mineral group and non magnetic minerals group and some of ferromagnetic group
are grinded together to 0.075 mm particle size (at least 85%) and mix with 0.02 – 0.075 mm particle
size group. After all, flotation separators are used to separate this mixture to refined rare earth ore,
fluorite ore and barite ore.
Figure 7: Technological layout for enrichment of Dong Pao rare earth
ore in laboratory scale.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
287
3. DONG PAO RARE EARTH MILLING PROCESS WITH TWO PRODUCTS
Base on process has described in figure 7 and probe experiments' result, we has conclude it
to two processes, which lead to two products as described in figure 8 and 9. There're some
differences between these process as listed below:
1. Hydrocyclone separate step: Particle size need to separate are 0.015 mm and 0.020 mm
respectively.
2. Dry magnetic separate under strong magnetic field step: differences between separate
times.
3. Flotation separate step: collector, depressor expenditures, time use on froth skimming,
amount of cleaner circuit step.
3.1. Dong Pao rare earth milling process follow product A.
Dong Pao rare earth milling process follow product A is demonstrate in figure 8. All the
steps of this process are described in table 1 and listed below:
- Run of mine (ROM) is dry screened on screens with 2 aperture size d1 = 5.0 mm and d2
= 10.0 mm to 3 particle size + 10.0 mm; 5.0-10.0 mm; -5.0 mm. Ore with 10.0 mm size are crushed
in smooth-roll crusher to-5.0 mm size. 5.0-10.0 mm particle size ore will go through trammel
screen, shaking and grinding machine, the mix with-5.0 mm particle and proceed through primary
spiral classifier combine with vibrating screen with aperture size = 1 mm. Final product will be ore
with particle size < 1.0 mm. circulation spigot product with size > 1.0 mm will go back to trammel
screen, shaking again.
- The product with particle size < 1.0 mm will go to secondary spiral classifier with
topping threshold particle size 0.075 mm, we'll get 2 products in < 0.075 mm and 0.075-1.0 mm
particle size. 0.075-1.0 mm size is separated on sludge concentration table to 2 groups: heavy and
light.
- Heavy group from concentration table is dried and go through dry magnetic separator
138 T СЭМ (USSR) with field indensity H = 1.000-5.000 gauss and 15.000 gauss. We'll get 3
products after this step as ferromagnetic minerals, refined rare earth minerals 1A and non-magnetic
minerals A.
- -0.075 mm size ore is separated by hydrocyclone with D = 25.0 mm (sand tube diameter
dc = 6 mm and sludge flow pressure H = 2.5-2.8 kg/cm2) to 2 products with particle size-0.015 mm
and 0.015-0.075 mm. Product with-0.015 mm particle size, also called as primary sludge has high
rare earth content and named as refined rare earth minerals 2A.
- Ferromagnetic, non-magnetic minerals and light group products from concentration
tables are grinded to 85%-0.075 mm and mixed together with 0.015-0.075 mm size ore from
cyclone to form a product named assorted product-0.075 mm.
- Assorted product-0.075 mm, barite and rare earth are fed together in primary flotation
separator with reagent’s ingredients as follow: depressor is liquid glass with dosage 2.500 g/t, pH
modifier is sodium bicarbonate with dosage 1.200 g/t to get pH = 10.5, collector S-SDS with dosage
650 g/t with froth skimming time 7 minutes.
- Floating products from flotation separator also go to secondary flotation separate to get
barite with reagent's ingredients as follow: depressor is liquid glass with dosage 2.000 g/t, collector
BEROL 2014 with dosage 650 g/t. Primary refined barite minerals will go through 2-3 milling
process to get refined barite and middlings. Sinking products from process above are separated by
selective flotation one more time to get rare earth minerals with 2.000 g/t liquid glass as depressor
and 550 g/t sodium oleate as collector. Primary refined rare earth mineral will go through 3 milling
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
288
processes to get refined rare earth and middlings. All middlings are send back to the primary
flotation separator.
- Sinking products from primary flotation separator will go through secondary flotation
process with 2.000 g/t liquid glass as depressor and 900 g/t acid oleic as collector to get fluorite.
Primary refined fluorite mineral will go through 3 milling process to get refined fluorite and
middlings. Middlings will be sent back to the beginning of this process.
Table 1: Milling process follow product A.
Separate step Milling process and products
Magnetic
separate step
Field intensity, gauss Products
1000-5000 Ferromagnetic ore
15000 Refined rare earth ore 1A
Hydrocyclone
separate step
D = 25.0mm
Sand tube
diameter
db,mm
Sand tube
diameter
dc,mm
Sludge flow
pressure H,
kg/cm2
Products
4.0 6.0 2.5-2.8 - 0.015mm
(refined rare
earth ore 2A)
0.015-
0.075mm
Flotation
separate step
Reagent’s ingredients, Time use on froth
skimming, amount of cleaner circuit.
Reagent
expenditures, g/t
Time,
minute
Collective
flotation step
on barite and
fluorite
- Sodium bicarbonate
- Liquid glass
- S-SDS
- Time use on froth skimming
1200
2500
650
-
4
4
4
7
Flotation
separate step
on barite
- Liquid glass
- BEROL 2014
- Time use on froth skimming
- Amount of cleaner circuit.
2000
650
-
-
4
4
6
2-3
Flotation
separate step
on rareearth
- Liquid glass
- Sodium oleate
- Time use on froth skimming
- Amount of cleaner circuit.
2000
550
-
-
4
4
4
3
Flotation
separate step
on fluorite
- Liquid glass
- Acid oleic
- Time use on froth skimming
- Amount of cleaner circuit.
2000
900
-
-
4
4
4
3
The result of milling process follow product A (figure 8) on mixed ore is describe in table 2
and on F3 ore is describe in table 3.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
289
Quality of refined product A (DH-A) is evaluated by multi-element analysis at Geology
Analysis and Experiments Center and presented in table 4. Total acquired quantity of DH-A from
project is 50.0 kg.
Figure 8: Dong Pao rare earth milling process follow product A.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
290
Table 2: Result of Dong Pao rare earth ore enrichment follow
product A on mixed ore.
No Products Yield % Content,% Recovery,%
TR2O3 BaSO4 CaF2 TR2O3 BaSO4 CaF2
1 Rare earth
fine ore 1A 0.69 59.21 1.98 1.17 6.83 0.05 0.07
2 Rare earth
fine ore 2A 3.25 25.96 9.28 4.15 14.11 1.17 1.09
3 Rareearth
fine ore 3A 5.97 48.86 18.66 3.22 48.76 4.31 1.55
4
Total Rare
earth fine
ore DH-A
9.91 42.07 14.42 3.38 69.70 5.54 2.71
5 Barite fine
ore 20.25 2.53 92.35 2.63 8.57 72.45 4.31
6 Fluorite
fine ore 8.51 1.59 2.38 85.23 2.26 0.78 58.73
7 Tailings A 61.33 1.90 8.93 6.90 19.47 21.23 34.25
ROM 100.00 5.98 25.81 12.35 100.00 100.00 100.00
Table 3: Result of Dong Pao rareearth ore enrichment follow
product A on F3 ore.
No Products Yield % Content,% Recovery,%
TR2O3 BaSO4 CaF2 TR2O3 BaSO4 CaF2
1 Rare earth
fine ore 1A 1.38 51.13 3.65 0.82 5.61 0.09 0.09
2 Rareearth
fine ore 2A 9.92 38.69 22.44 3.08 30.53 4.16 2.54
3 Rareearth
fine ore 3A 10.51 44.24 34.20 5.20 37.00 6.72 4.55
4
Total Rare
earth fine
ore SS-96
21.81 42.15 26.92 3.96 73.15 10.98 7.18
5 Barite fine
ore 43.50 2.96 92.55 5.57 10.24 75.27 20.14
6 Fluorite
fine ore 8.12 4.43 4.33 87.54 2.86 0.66 59.08
7 Tailings A 26.56 6.50 26.37 6.16 13.74 13.09 13.60
ROM 100.00 12.57 53.49 12.03 100.00 100.00 100.00
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
291
Table 4: Result of multi-element analysis of rareearth fine ore DH-A and DH-B.
No Value,
concentration
Barite fine
ore
Fluorite fine
ore
Rare earth
fine ore DH-A
Rare earth
fine ore DH-B
1 TR2O3; % 2.53 1.59 42.07 29.64
2 BaSO4; % 92.35 2.38 14.42 15.56
3 CaF2; % 2.63 85.23 3.38 6.41
4 CaO; % 0.41 1.97 1.30 2.29
5 SiO2; % 1.86 1.38 1.23 4.97
6 Fe; % 0.25 0.36 0.61 2.64
7 U; ppm 3.0 5.0 2.0 5.0
8 Th; ppm 5.0 7.0 5.0 4.0
3.2. Dong Pao rare earth milling process follow product B.
Dong Pao rare earth milling process follow product B is demonstrate in figure 9. All the
steps of this process are described in table 5 and listed below:
- COM is dry screened on screens with 2 aperture size d1 = 5.0 mm and d2 = 10.0 mm to
3 particle size + 10.0 mm; 5.0-10.0 mm; -5.0 mm. Ore with 10.0 mm size are crushed in smooth-
roll crusher to -5.0 mm size. 5.0-10.0 mm particle size ore will go through trammel screen, shaking
and grinding machine, the mix with -5.0 mm particle and proceed through primary spiral classifier
combine with vibrating screen with aperture size = 1 mm. Final product will be ore with particle
size < 1.0 mm. Circulation spigot product with size > 1.0 mm will go back to trammel screen,
shaking again.
- The product with particle size < 1.0 mm will go to secondary spiral classifier with
topping threshold particle size 0.075 mm, we'll get 2 products in < 0.075 mm and 0.075-1.0 mm
particle size. 0.075-1.0 mm size is separated on sludge concentration table to 2 groups: heavy and
light.
- Heavy group from concentration table is dried and go through dry magnetic separator
138 T СЭМ (USSR) with field intensity H = 1.000-5.000 gauss, 14.000 gauss and 15.000 gauss.
We'll get 3 products after this step as ferromagnetic minerals and non-magnetic minerals B. Two
magnetic products acquired from 14.000 and 15.000 gauss condition are mixed together to form
refined rare earth minerals 1B.
- - 0.075 mm size ore is separated by hydrocyclone with D = 25.0 mm (sand tube
diameter dc = 4.0 mm and sludge flow pressure H = 1.5-1.8 kg/cm2) to 2 products with particle size
-0.020 mm and 0.020-0.075 mm. Product with-0.020 mm particle size, also called as primary sludge
has high rare earth content and named as refined rare earth minerals 2B.
- Ferromagnetic, non-magnetic minerals and light group products from concentration
tables are grinded to 85%-0.075 mm and mixed together with 0.020-0.075 mm size ore from
cyclone to form a product named assorted product-0.075 mm.
- Assorted product-0.075 mm, barite and rare earth are fed together in primary flotation
separator with reagent’s ingredients as follow: depressor is liquid glass with dosage 2.500 g/t, pH
modifier is sodium bicarbonate with dosage 1.200 g/t to get pH = 10.5, collector S-SDS with dosage
650 g/t with forth skimming time 8 minutes.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
292
- Floating products from flotation separator also go to secondary flotation separate to get
barite with agent's ingredients as follow: depressor is liquid glass with dosage 2.000 g/t, collective
BEROL 2014 with dosage 650 g/t. Primary refined barite minerals will go through 2-3 milling
process to get refined barite and middlings. Sinking products from process above are separated by
selective flotation one more time to get rare earth minerals with 2.000 g/t liquid glass as depressor
and 650 g/t sodium oleate as colector. Primary refined rare earth mineral will go through 3 milling
process to get refined rare earth and middlings. All middlings products are send back to the primary
flotation separator.
- Sinking products from primary flotation separator will go through secondary flotation
process with 2.000 g/t liquid glass as depressor and 900 g/t acid oleic as collector to get fluorite.
Primary refined fluorite mineral will go through 3 milling process to get refined fluorite and
middlings. Middlings will be sent back to the beginning of this process.
The result of milling process follow product B (figure 9) on mixed ore is describe in table 6
and on F3 ore is describe in table 7.
Quality of refined product B (DH-B) is evaluated by multi-element analysis at Geology
Analysis and Experiments Center and presented in table 4. Total acquired quantity of DH-B from
project is 50.0 kg.
Figure 9: Dong Pao rare earth milling process follow product B.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
293
Table 5: Milling process follow product B.
Separate step Milling process and products
Magnetic separate
step
Field intensity, gauss Products
1000-5000 Ferromagnetic ore
14000 Magnetic 2 Refined rare
earth ore 1B 15000 Magnetic 3
Hydrocyclone
separate step
D = 25.0mm
Sand tube
diameter
db,mm
Sand
tube
diameter
dc,mm
Sludge flow
pressure H,
kg/cm2
Products
4.0 4.0 1.5-1.8 -0.020mm
(refined rare
earth ore 2B)
0.020-
0.075mm
Flotation separate
step
Reagent’s ingredients, Time use on
froth skimming, amount of cleaner
circuit
Reagent
expenditures,
g/t
Time,
minute
Collective
flotation
step on
barite and
fluorite
- Sodium bicarbonate,
pH =10,5
- Liquid glass
- S-SDS
- Time use on froth
skimming
1200
2500
650
-
4
4
4
8
Flotation
separate
step on
barite
- Liquid glass
- BEROL 2014
- Time use on froth
skimming
- Amount of cleaner
circuit.
2000
650
-
-
4
4
6
2-3
Flotation
separate
step on
rare earth
- Liquid glass
- Sodium oleate
- Time use on froth
skimming
- Amount of cleaner
circuit.
2000
650
-
-
4
4
6
2
Flotation
separate
step on
fluorite
- Liquid glass
- Acid oleic
- Time use on froth
skimming
- Amount of cleaner
circuit.
2000
900
-
-
4
4
4
3
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
294
Table 6: Result of Dong Pao rare earth ore enrichment follow product B on mixed ore.
No Products Yield
%
Content,% Recovery,%
TR2O3 BaSO4 CaF2 TR2O3 BaSO4 CaF2
1 Rareearth fine
ore 1B 1.18 47.73 2.12 1.67 9.42 0.10 0.16
2 Rareearth fine
ore 2B 5.66 23.31 9.31 4.33 22.06 2.04 1.98
3 Rareearth fine
ore 3B 9.30 31.20 21.07 8.28 48.53 7.59 6.23
4 Total Rareearth
fine ore DH-B 16.14 29.64 15.56 6.41 80.01 9.73 8.38
5 Barite fine ore 20.25 2.53 92.35 2.63 8.57 72.45 4.31
6 Fluorite fine
ore 8.51 1.59 2.38 85.23 2.26 0.78 58.73
7 Tailings B 55.10 0.99 7.98 6.41 9.16 17.03 28.58
ROM 100.00 5.98 25.81 12.35 100.00 100.00 100.00
Table 7: Result of Dong Pao rareearth ore enrichment follow product B on F3 ore.
No Products Yield
%
Content,% Recovery,%
TR2O3 BaSO4 CaF2 TR2O3 BaSO4 CaF2
1 Rareearth fine
ore 1B 1.89 46.21 4.53 1.07 6.95 0.16 0.17
2 Rareearth fine
ore 2B 16.17 31.59 25.61 3.22 40.64 7.74 4.33
3 Rareearth fine
ore 3B 14.91 29.27 35.80 5.33 34.72 9.98 6.60
4 Total Rareearth
fine ore SS-98 32.97 31.38 29.01 4.05 82.31 17.88 11.10
5 Barite fine ore 43.50 2.96 92.55 5.57 10.24 75.27 20.14
6 Fluorite fine
ore 8.12 4.43 4.33 87.54 2.86 0.66 59.08
7 Tailings B 15.41 3.74 21.49 7.56 4.58 6.19 9.68
ROM 100.00 12.57 53.49 12.03 100.00 100.00 100.00
4. RESULTS, CONCLUSIONS AND SUGGESTION
4.1. Results and conclusions about material composition of Dong Pao rare earth ore.
1. Research samples had very complex material composition, belong to group of "multi-
metals" ore and the ore itself is very hard for milling. Total rare earth oxide is not too high, only
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
295
5.98% Tr2O3. However, barite and fluorite take a large part, for detail: 25.81% BaSO4, 12.35%
CaF2. There're many miscellaneous minerals come together with rare earth with high content of Ca,
Al, Fe, Si, S, Mn, Pb, Mg,... In the samples also contain radioactive elements like uranium and
thorium in low proportion, 18 ppm and 3 ppm respectively. Rare-earth minerals mostly exist in
bastnaesite form. In this kind of ore, barite take a large contain, 4 to 5 times when compare to all of
other rare-earth oxide contain together. Moreover, some of rare-earth element exist in Yttrofuorite
form (Ca,Y)F2-3 and fluorite form CaF2[(CaF2)0.75(YF3)0.25].
2. Dong Pao ore is highly weathered carbonate deposit, mostly rare earth minerals. Their
primary structure mostly destroyed to friable powder, sometime clutching to each other by
hydroxide iron gel. It has strong bond and well mixed with most of accompany minerals.
3. Minerals in Dong Pao ore are diluted or separated in fine and very fine grain.
Orientation and distribution of rare earth and two other assimilate minerals barite and fluorite is
very sharp. The finer grain, the higher content of rare earth and it goes opposite with barite and
fluorite. Rare earth concentrate in fine particle size-0.075 mm. Rare earth content in primary sludge
-0.020 mm is pretty high: 24.77% TR2O3.
4.2. Results and conclusions about material composition of Dong Pao rare earth ore.
We have selected milling technology of Dong Pao rare earth ore as a combination of many
enrichment methods.
- Crude ore is handled properly to grain size-1.0 mm by hydrocyclone and spiral classifier
and separate to 3 sizes: (1) 0.075-1.0 mm; (2) 0.020-0.075 mm and (3)-0.020 mm. Particle size-
0.020 mm is primary sludge, has high content of rare earth elements and can be considered refined
rare earth minerals.
- Separate Dong Pao rare earth ore which sizes 0.075-1.0 mm to 2 sub groups (1) heavy
minerals and (2) light minerals using sludge concentration table. Follow this step, using dry
magnetic enrichment to separate heavy minerals group to 3 sub groups: (1) ferromagnetic minerals,
(2) rare earth minerals (weak magnetism) and (3) non-magnetic minerals.
- Light minerals, non-magnetic and ferromagnetic minerals group are grinded together to
85% of them get size within-0.075 mm then mix it with 0.020-0.075 mm group. Using flotation
separator, get barite-rare earth mixture and fluorite. After that, we separate this mixture by
secondary flotation and get refined rare earth, barite and fluorite mineral.
- Refined minerals have met the follow quality requirements and quantity as follow:
Refined barite with βBaSO4 content = 92.35% and the recovery of BaSO4 72.45% acquired is 50 kg.
Refined fluorite with βCaF2 = 85.23% and the recovery of CaF2 58.73% acquired is 50 kg. Refined
rare earth minerals we get follow two option:
+ Plan A: Refined rare earth with βTR2O3 = 42.07% and the recovery of TR2O3 69.70%
acquired is 50 kg.
+ Plan B: Refined rare earth with βTR2O3 = 29.64% and the recovery of TR2O3 80.01%
acquired is 50 kg.
- Technology diagram for Dong Pao rare earth minerals in laboratory scale has chosen as
figure 9 and technological quality acquired as follow this technology introduced in table 6.
4.3. Suggestions
1. In order to avoid unnecessary risk when design an build a rare earth milling factory in
Lai Chau, it is imperative to run experiments in larger scale (semi-industrial scale) for testing this
technology diagram and collect all the technological and economical parameters which are closest
to real scale operation. It'll serve well for technological design and project initiate of the factory.
VINATOM-AR 13--38
The Annual Report for 2013, VINATOM
296
2. Lai Chau rare earth milling technology is “flexible” and “open”; it can adapt to material
composition of various ore bodies.
3. In real industrial scale, in order to has it reasonable from all aspect of technology,
economy and especially guarantee using precious resources in most effective way; it should be
round up the rare earth elements oxide in refined minerals from 30.0-35.0 %.
REFERENCES
[1] Hoàng Trọng Mai, Giáo trình “Khoáng vật học đại cương”, Đại học Mỏ-Địa chất, Hà Nội
năm 1997.
[2] Nguyễn Văn Hạnh, Luận án tiến sỹ kỹ thuật “Nghiên cứu khả năng tuyển tách đất hiếm,
fluorit và barit từ quặng hỗn hợp đất hiếm phong hóa Đông Pao”, Hà Nội năm 2006.
[3] Báo cáo “Nghiên cứu khả thi thân quặng F3 Đông Pao, Lai Châu”, Công ty Toyota Tsusho và
Sojitz Nhật Bản năm 2009.
[4] Nguyễn Thị Hồng Hà, Báo cáo tổng kết đề tài “Nghiên cứu công nghệ tuyển quặng đất hiếm
phong hóa thân quặng F7 Đông Pao, Lai Châu”, Hà Nội năm 2010.
[5] Nguyễn Duy Pháp, Báo cáo tổng kết “Nghiên cứu mẫu công nghệ Đề án thăm dò bổ sung mỏ
đất hiếm-fluorit-barit Đông Pao thuộc xã Bản Hon, xã Bản Giang, huyện Tam Đường, tỉnh
Lai Châu”, Hà Nội năm 2011.
[6] Trần Thị Hiến, Báo cáo sơ bộ “Thí nghiệm mẫu công nghệ quặng đất hiếm mỏ đất hiếm Bắc
Nậm Xe, xã Nậm Xe, huyện Phong Thổ, tỉnh Lai Châu”, Hà Nội năm 2013.
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
297
IMPROVING TECHNOLOGY AND SETTING-UP A PRODUCTION
LINE FOR HIGH QUALITY ZINC OXIDE (99.5%) WITH A CAPACITY
OF 150 TON/YEAR BY REDUCTION-OXIDATION PROCESS
Pham Minh Tuan, Tran The Dinh, Tran Ngoc Vuong, Tuong Duy Nhan, Tran Trung Son,
Le Huu Thiep, Nguyen Trung Dung, Le Thi Hong, Luong Manh Hung and Bui Huy Cuong
Center for Technology Development,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48- Lang Ha, Dong Da, Ha Noi
ABSTRACT: Zinc oxide is used not only for the rubber industry, but also in many other industries such as
pigments, ceramics, cosmetics etc. On the basis of references on international scientific researches and
practical activities for the production of zinc oxide in our country, we have carried out additional research and
testing to establish a zinc oxide production line for preparation of high quality (99.5%) product by treating the
industrial zinc containing waste to obtain required composition materials [Zn] >50%; [Pb] < 0.3%; [Cl]/[PbO]
< 0.2 for reduction-oxidation processes using reverberatory furnace.
Keywords: Zinc oxide; reduction oxidation method; american process; direct zinc oxide.
1. OVERVIEW
Reduction-oxidation method (American process) is the most important method for the
highest capacity production of zinc oxide at present. Most industries are using ZnO produced by
this method.
The resulting product by this method is often not of high quality, depending on the type of
raw materials, which can be obtained with a concentration of ZnO 70% to 99%. Along with the
advancement of science and technology today, ZnO produced by this method can reach the higher
quality zinc oxide of 99.5%.
Basically, the method consists of following stages: 1)materials processing; 2)reduction of
zinc oxide in the materials into metallic zinc by using coal, coke; 3) then zinc metal at high
temperature will be evaporated and react with oxygen in the air to form zinc oxide.
Reduction oxidation method is carried out by means of two basic types of devices: the rotary
kiln and reverberatory furnace.
The reverberatory furnace method is currently most commonly used to produce ZnO thanks
to its high quality products. This method has the advantage of a favorable investment due to low
cost, simple device, easily to fabricate. The downside of this method is its rather low recovery
performance compared to the method using a rotary kiln: typical recovery efficiency of zinc is
around 90%.
Technology fundamentals
The chemistry of the production process by reduction-oxidation method can be represented
by the following reaction equation:
Project Information:
- Code: HĐDA. 06/2010/NLNT
- Managerial Level: Ministry
- Allocated Fund: 1,700,000,000 VND
- Implementation Time: 42 months (Mar 2010-Aug 2013)
- Contact Email: [email protected]
- Papers published in relation to the project: (None)
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
298
ZnO (solid ) + CO = Zn vapor + CO2 (1)
Zn vapor + O2 = ZnO (solid) (2)
During the reduction-oxidation of zinc, lead (Pb) content in the raw material will have a
similar behavior to zinc. Pb content in ZnO product by this method highly depends on the Pb
content in raw materials. In addition, quality of the resulting ZnO product obtained by reduction-
oxidation process depends mainly on two other factors: temperature of reverberatory furnace and
chloride salt content in raw materials.
2. TECHNOLOGY IMPROVEMENT
We have implemented this project with the following specific measures:
1. Research a method of Lead separation, while minimizing Pb and chloride salt
concentrations in raw materials.
2. Change reverberatory furnace design to increase impurity removals efficiency and
improve the furnace performance.
3. Use material pressed pellets instead of powder materials, and design, set-up a dust
handling systems for reduction-oxidation furnace to improve efficiency of reduction-oxidatition
process.
2.1. Lead removal
The reaction of Pb separation process is represented by the following reaction equation :
2NaCl + PbO + 2SiO2 + Al2O3 = PbCl2↑ + 2NaAlSiO4 (1)
2NaCl + PbO + CO2 = PbCl2↑ + Na2CO3 (2)
2NaCl + ZnO + CO2 = ZnCl2↑ + Na2CO3 (3)
According to [19] , the reaction (1) occurs at temperatures of 900-10000C, the reaction time
of about 90 minutes, the activation energy for reaction (1) is 175 kJ/mol, the reactions (2) and (3)
can occur at lower temperatures (800-10000C).
Figure 1: Schema of Lead removal experiment.
The experiment results have been shown in the table 1.
Table 1: Pb removal study by chlorination method.
Sample Con.,% Reaction
temp.,oC
Reaction time, min.
15 30 45 60 75 90 105 120
M1 Zn 67.5
Pb 2.70
850 2.65 2.5 2.2 1.7 1.3 1.1 0.7 0.55
900 2.6 2.4 2.05 1.5 1.1 0.9 0.65 0.55
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
299
Cl 6.1
950 2.6 2.2 1.85 1.2 0.85 0.7 0.55 0.4
1000 2.55 2.15 1.75 1.05 0.7 0.55 0.5 0.4
M2
Pb 3.6
Cl 6.2
Zn 67.0
850 3.55 3.3 2.7 2.35 1.55 1.05 0.9 0.85
900 3.55 3.25 2.55 2.2 1.55 1 0.8 0.8
950 3.5 3.2 2.5 2.0 1.4 0.9 0.8 0.7
1000 3.5 3.1 2.4 1.9 0.95 0.85 0.75 0.7
M3
Pb 3.6
Cl 6.2
Zn 67.0
3%NaCl
850 3.55 3.3 2.7 2.35 1.55 0.8 0.55 0.5
900 3.55 3.25 2.55 2.2 1.55 0.8 0.55 0.5
950 3.5 3.2 2.5 2 1.4 0.7 0.5 0.45
1000 3.5 3.1 2.4 1.9 0.95 0.7 0.45 0.45
When the concentration of Pb in raw material is lower (experiment 1), Pb removal process
showed its good efficiency. In the case of high Pb concentrations, although the reaction time
extended to 120 minutes, even at temperatures of 10500C (the highest temperature in the
temperature range survey), amount of Pb remained in the reaction mass was still higher than the
value required (experiment 2).
This phenomenon can be explained that, chlorides containing in the reaction mass was
disintegrated so chloride amount remained could not be enough to transform all Pb containing in the
raw material to lead chloride, therefore chloride salt should be added to the reaction mass to suply
additional chloride for the chlorination reaction (experiment 3, fig.2).
From the experimental results, we could see that, when chloride is added in the form of
sodium chloride, Pb separation efficiency increases even though the amount of chlorine in the
starting material is very large compared with the Pb content in the material.
The additional amount of sodium chloride is calculated according to [19,25]. The
verification experiment showed that NaCl salt should be added so that the total amount of chloride
in the reaction mass was about 3 times larger (in stoichiometric) compared with Pb content in raw
materials.
Figure 2: Lead removal test (Sample tested No.3).
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
300
Through empirical data survey of Pb separation process, following conclusions can be
made:
1) Pb removal process will achieve good efficiency at temperatures in the range 800-
10000C, the time needed to maintain the reaction temperature is 90 minutes.
2) Pb contain in the zinc slag can be reduced to the value of 0.4%.
3) When the concentration of Pb in the zinc slag is high, chloride in the form of sodium
chloride should be added to provide reacting agent for chlorination reaction.
4) This method can simultaneously solve both the most important issues: removal of Pb and
reduction of chloride contained in the raw material.
2.2. Reduction-oxidation furnace set-up
We have changed the design, creating two separate zones in the furnace: Reduction Zone
and oxidation Zone. Air supply for oxidation process is fed into the oxidation chamber through the
intake air (see Fig.3).
Figure 3: Reverberatory Furnace Design Improvement.
Based on additional research, a system of devices are listed below.
1 Reverberatory furnace for Reduction-Oxidation of Zinc: Productivity 600kg/batch;
02 blower power 4 kW; 18000 -20000m3 /h, pressure 250 mmH2O;
Drain system of 10 chambers deposition system made of SUS304 stainless steel.
2 Dust collection system with bag house, filter surface area: 300m2; dust collection
fan of 350mmH2O pressure, flow 12.000m3/h. Working temperature: <100°
3 Ball press machine, Model YBM430: Rolls diameter 430 mm.Capacity: 6-8 t/h.
Motor power: 11 kW.
4 Grinding machine Model ZC-800: Grinding Barrel Diameter: 800 mm.Capacity of
10 ton/h. Motor 30 kW.
5 Mixing Machine, Model YZM-300: Length 3000 mm; Mixing tank 2500x550mm;
Mixing velocity: 40 v/ph.
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
301
3. TRIAL PRODUCTION
Five trials with different composition materials have been done. Each test is carried out by
using 20 tons of zinc slag processed. It has been confirmed:
- The measures applied to improve the quality of materials is a suitable solution to
produce zinc oxide of desired quality.
- The reduction-oxidation furnace system has ability to produce high quality zinc oxide
with the appropriate material.
- Standard input for the production of high quality zinc oxide by reduction-oxidation
method : [Zn]> 50%; [Pb] <0.3%; [Cl] / [PbO] <0.2.
Table 3 below discribes the composition of pretreated material (to reduce Pb and Chloride).
Table 3: Pretreated material composition.
Zn Pb Cl Mass remained,%
X1 76.0 0.36 0.23 100
X2 75.4 0.48 0.22 94
Table 4: Raw (untreated) material composition.
Procedure for high quality inc oxide production.
The production procedure and technical parametters required for each stage have been
shown in the fig.5 below.
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
302
Figure 5: Technology schema for high quality zinc oxide(99.5%) production line.
Table 5: Analysis and assessment of product quality.
No. Species Analysis method Results Examiner
1 ZnO ISO13658(E) 99.52% Analytical Center,
Lab Vilas 143-
Istitute for Mining
and Metallurgy.
2 Pb ISO5889(E) 0.15%
3 Fe ISO5889(E) 0.003%
4 Particles Size LSPSDistribution Analyser
LA-950
5-10µm ITRRE.
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
303
4. CONCLUSIONS
- The Project “Improving technology and setting up a production line for high quality
zinc oxide (99.5%) with a capacity of 150 ton/year by reduction-oxidation method” has been
implemented as registered in the Project Notes. Specifically:
- Technology improvement: The Projects completed all technology items, aimed at the
stages of production of zinc oxide, especially focused on the process of the raw material heat
treatment in a rotary kiln. By using pretreated zinc containing materials, ZnO product meet all
requirements of rubber grade high quality zinc oxide even quality of zinc slag material is not high.
The main technological parameters have been established and a new zinc oxide production line by
reduction-oxidation process has been built.
- Technology equipment: A new Production line equipment mainly focused on the
enhancing process efficiency and increasing product quality. The material pelleting technology is a
key solution in production technology. Dust collection system, gas treatment combined with
material pelleting technology have brought about economic efficiency: increasing product revenue
performance and meeting environmental protection requirements.
- Production: The total amount of product produced during the time of implementing the
project was 455 tons. Zinc oxide products met all the requirements of vulcanized rubber technology.
In fact, the production cost will be reduced at a larger production scale by the depreciation of
equipment and less labor consumption.
REFERENCES
[1] PHẠM QUANG TRUNG, Nghiên cứu quy trình nung phân huỷ ZnCO3 thành ZnO trên
thiết bị nung động, Báo cáo tổng kết đề tài CS-99-13, Viện Công nghệ Xạ-Hiếm, Viện Năng
lượng Nguyên tử Việt Nam, Hà Nội 4/2000.
[2] YUREN JIANG, ET AL, Preparation of High Purity Zinc Oxide from Zinc Metal Scrap,
Akita University and the University of Tokyo-Japan.
[3] G. HEIDEMAN, Reduced zinc oxide levels in sulphur vulcanization of rubber compounds.
Ph.D. Thesis, University of Twente, Enschede, the Netherlands, 2004.
[4] BERGENDORFF O., PERSSON C., HANSSON C., Chemical changes in rubber allergens
during vulcanization.
Department of Dermatology, University Hospital, Lund University, Sweden.
[5] DANIEL L. HERTZ, JR., Theory & Practice Of Vulcanization, Seals Eastern Inc., Red
Bank, NJ 07701.
[6] LUTAO LI, ET AL, Formation of ZnO-containing Dust from Zn-bearing Steel Melts,
Technical University of Claustahl-Germany, July 25, 1994.
[7] HIROYUKI MATSUURA, ET AL, Removal of Zn and Pb from Fe2O3-ZnFe2O4-ZnO- PbO
Mixture by Selective Chlorination and Evaporation Reactions, The University of Tokyo-
Japan, January 30, 2006
[8] www.omnexus.com, Review of vulcanization chemistry.
[9] J.G.KREINER, Method for improving rubber curing rates, US Pat. 4882394, 11/1989.
[10] CHSSR KUMAR, AVINASH M NIJASURE, Vulcanization of rubber, ICI Research and
Technology Center, Thane, India..
[11] Treatment of polyvinylchloride, US patent 5698759.
[12] Treating Lead and Zinc-containing steelmaking by-products, US patent 4765829.
[13] Chloride melt process for the separation and recovery of Zinc, US patent 6931474.
[14] JAE-MIN YOO, BYUNG-SOO KIM, MIN-SEUK KIM AND JINKI JEONG, Separation of
Lead and chlorine from electric arc furnace dust to recover Zinc, Korea Institute of
VINATOM-AR 13--39
The Annual Report for 2013, VINATOM
304
Geoscience and Mineral Resouces, 3/2007.
[15] JOHN HENRY CALBECK. Production of Zinc oxide, US patent 2 603 554.
[16] BECKMANN ET AL. Treating Lead and Zinc containing stellmaking byproducts, US
patent 4 765 829.
[17] SHUGARMAN, Lead removal method, US patent 4 704 260, 11/1987.
[18] FRANK G. BREYER, EARL C. GASKILL ET AL. Manufacture of Zinc Oxide, US patent
1522097.
[19] M.P. KIRK. Apparatus for Producing Zinc oxide, US patent 1566103.
[20] DA02/2005. Hoàn thiện công nghệ sản xuất kẽm cacbonat. Viện Công nghệ Xạ-Hiếm, Viện
Năng lượng Nguyên tử Việtnam, 6/2007.
[21] A.M.LASTOTSEV, E.I. GORODNICHEVA, Calcualting power consumption for mixing
high-viscosity newtonian liquids with blade mixers, UDC 66.063.
[22] DAT-NLNT/06-04, Hoàn thiện công nghệ và dây chuyền thiết bị cho sản xuất ZnO 98,5%
quy mô 150tấn/năm, Hà nội 12/2008.
VINATOM-AR 13--40
The Annual Report for 2013, VINATOM
305
DETERMINATION OF RARE EARTH AND OTHER ELEMENTS
IN YEN-PHU RARE EARTH ORE AND OTHER INTERMEDIATE
PRODUCTS FROM THE FLOATATION AND HYDROMETALLURGICAL
PROCESS ON PORTABLE XRF Si-PIN DETECTOR
Doan Thanh Son, Phung Vu Phong and Nguyen Hanh Phuc
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48- Lang Ha, Dong Da, Ha Noi
ABSTRACT: The concentration of rare earths elements such as La, Ce, Pr, Nd, Gd... and other elements as Ca,
Fe, U, Th in Yen Phu rare earth ore and other intermediate products from the flotation and hydrometallurgical
process was determined by using Si-PIN detector fluorescence spectrometry. The precision and accuracy of
quantitative analysis was tested by standard reference materials and comparative analysis with different
analytical methods. The analytical procedures were set-up and applied for the determination of rare earth and
other elements in Yen Phu rare earth ore and other intermediate products from the flotation and
hydrometallurgical process with high precision and accuracy.
I. INTRODUCTION
Previously ICP methods were often used to analyze the rare earth elements, however the
disadvantage of this method of analysis was time-consuming because it needed to digest the solid
samples. In published articles written about the identification of rare earth elements by X-ray
fluorescence method, the wavelength dispersion fluorescence systems (WD-XRF) were almost
applied. In ITRRE, there was a report concerning energy dispersion fluorescence system (ED-XRF)
from the year of 2000, in which some rare earth elements belonged to the “light group” was
determined. However, the detector of that (ED-XRF) system was semiconductive Si(Li), and the
number of rare earth elements determined has been limited. The energy dispersion fluorescence
system (ED-XRF) with Si-PIN detector for direct analysis of individual rare earth elements was
thus employed for the study of La, Ce, Pr, Nd, Ca, Fe, Th, U determination in Yen Phu rare earth
ores with the aiming supplying the demands of rare earth ore beneficiation. The procedure was
established with the low error and high precision.
II. EXPERIMENTAL
1. Investigation of the current, voltage of X ray generator to obtain the characteristic X-ray
with highest intensity of elements La, Ce, Pr, Nd, Ca, Fe, Th, U in Yen Phu rare earth ore.
Project Information:
- Code: 23/CS/HĐNV
- Managerial Level: Institute
- Allocated Fund: 75,000,000 VND
- Implementation Time: 12 months (Jan 2013 – Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project: (None)
VINATOM-AR 13--40
The Annual Report for 2013, VINATOM
306
Table 1: Dependence of characteristic X line intensity on X-ray tube current.
No Elements
Characteristic X-ray intensity at the voltage U = 30 kV
and different X-ray tube current
I=5 μA I=10 μA I=15 μA I=20 μA I=25 μA
1 Ca 4096 5054 5389 4903 4260
2 Fe 336524 461749 471320 434574 384631
3 La 5863 7733 7992 7245 6630
4 Ce 14343 18395 19217 17423 15003
7 Ag-IN 7300 11152 14597 17780 19480
8 Ag-CO 1446 2215 2966 3717 3917
(Dead time )% 16.88 30.56 41.98 51.69 59.29
The voltage of X ray generator by 30 kV and X-ray tube current by 10 μA was chosen when
analyzed of rare earths and other elements in Yen Phu rare earth ore and other intermediate products
from the flotation and hydrometallurgical process on the portable XRF Si-PIN detector.
2. Quantitatively analysis methods for the determination of rare earth and other elements in
Yen Phu rare earth ore and other intermediate products from the flotation and hydrometallurgical
process on the portable XRF Si-PIN detector.
Fundamental parameter method
Fundamental parameter method in QXAS software
Fundamental parameter is the most versatile method for quantification in the QXAS package
and suited even for completely unknown samples. Practically all modes of excitation with
electromagnetic radiation in the range of X-rays can be covered and many more parameters can be
selected to match the assumptions needed for the calculations with the experiment.
The sample self-absorption was corrected by the use of scatter peaks such as Compton and
Rayleigh. The specially characteristic when calculating using fundamental parameters method are
some factors such as absorption and enhancement correction are taken into consideration.
3. Analysis in the comparison with Standard Reference Materials and other methods.
Results received when analyses of the Yen Phu Rare earths ore by X-ray fluorescence Si-
PIN detector using fundamental parameter method compare with the one when analyses by ICP-
MS method.
Table 2: Analysis of Yen Phu Rare earth Ore by XRF and ICP-MS method.
No Element Unit
Results (%)
YA-
XRF
YA-
ICPMS
Relative
Error
(%)
YB-
XRF
YB-
ICPMS
Relative
Error
(%)
YC-
XRF
YC-
ICPMS
Relative
Error
(%)
1 Ca % 0.8 0.77 3.90 0.56 0.51 9.80 0.47 0.43 9.30
VINATOM-AR 13--40
The Annual Report for 2013, VINATOM
307
2 Fe % 9.72 9.54 1.89 8.78 9.1 3,52 8.08 7.57 6.74
3 Y % 5.794 5.31 9.11 5.94 5.57 6.70 6.834 6.40 6.78
4 La % 1.212 1.13 7.26 1.24 1.13 9.65 1.342 1.23 9.11
5 Ce % 2.468 2.35 5.02 2.57 2.37 8.57 2.824 2.61 8.20
6 Pr % 0.467 0.47 0.64 0.46 0.47 2.34 0.499 0.51 2.16
7 Nd % 2.324 2.12 9.62 2.05 2.10 2.43 2.487 2.26 10.04
8 Sm % 0.577 0.54 6.85 0.61 0.54 12.96 0.616 0.58 6.21
9 Gd % 0.736 0.66 11.52 0.74 0.67 13.28 0.715 0.76 5.92
10 Dy % 0.867 0.84 3.21 0.84 0.87 2.99 1.043 1.01 3.27
11 Er % 0.58 0.54 7.41 0.61 0.55 10.91 0.725 0.66 9.85
12 Yb % 0.48 0.42 14.29 0.47 0.44 6.82 0.565 0.52 8.65
13 Th % 0.286 0.27 5.93 0.41 0.39 5.13 0.37 0.40 7.50
14 U % 0.044 0.04 10.00 0.05 0.04 6.82 0.048 0.044 9.09
From the table, it can be found that resulted analysis is reliable compare with reference
material standard. The Relative Error bethwen compared methods are less then 10%.
Table 3: Analysis of a rare earth samples (M1) by Si-PIN fluorescence
in comparison with results received from Japan laboratory (ICP-OES).
Elements Unit Results (%)
XRF Japan Relative Error (%)
Ca % 4.49 4.4 2.00
Mn % 1.10 1.18 7.27
Fe % 3.04 3.54 9.26
Y % 0.23 0.22 4.35
Ba % 6.18 6.55 5.99
La % 11.20 11.53 2.95
Ce % 14.94 15.8 5.76
Pr % 1.32 1.58 7.48
Nd % 4.50 4.59 2.00
Sm % 0.48 0.47 2.08
Th % 0.1066 0.114 6.94
U % 0.061 0.059 3.28
From the table 3, it can be found that the diffence between analytical result of M1 rare earth
sample, which was done by Si-PIN X-ray fluorescence and that obtained in Japan laboratory (ICP-
MS) are less then 10%.
VINATOM-AR 13--40
The Annual Report for 2013, VINATOM
308
III. CONCLUSION
Project has solved the following issues
1. The technical parameter of Si-PIN spectrometry was investigated. The studies found
that when the voltage of X ray generator by 30kV and X-ray tube current by 10 μA was chosen
will give the characteristic X-ray with the highest intensity.
2. The selection of X-ray line fluorescence and the fitting of spectrum was performed
when analyzed of rare earths and other elements in Yen Phu rare earth ore and other intermediate
products from the flotation and hydrometallurgical process on the portable XRF Si-PIN detector.
3. Some quantitatively analysis methods used in X-ray fluorescence such as calibration
curve and fundamental parameter was studied. The detection limit of rare earth elements such as La,
Ce, Pr, Nd... was received.
REFERENCES
[1] Ron Jenkins, X-ray Fluorescence Spectrometry.John Wiley and Son, Ed 1988.
[2] IAEA-TECDOC-950, Sampling, storage and sample preparation procedures for X-ray
fluorescence analysis of environmental material. IAEA June 1997.
[3] IAEA-QXAS Quantitative X-ray Analysis System. Ver 1.2 (1995-1996).
[4] Rafal Sitko, Quantification in X-ray Fluorescence analysis theoretical background.
VINATOM-AR 13--41
The Annual Report for 2013, VINATOM
309
STUDYING OF PREPARATION SILVER NANO-PARTICLES
USING SPINNING DISC REACTOR
Hoang Van Duc, Nguyen Thanh Chung, Tran Ngoc Ha,
Ho Minh Quang and Nguyen Thi Thuc Phuong
Center for Material Science Technology,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48-Lang Ha, Dong Da, Ha Noi
ABSTRACT: Preparation of silver nano-particles using spinning disc reactor has been investigated. The effects
of technological factors and experimental conditions such as: concentrations of AgNO3, glucose, PVP,
spinning speed, ect. on quality of nano-silver particles have been studied. With experimental conditions:
rotation speed of 2000 rpm, weight rate of mPVP:mAgNO3=1, AgNO3 concentration of 0.01 M, glucose
concentration of 0.02 M, silver particles of about 12 nm were obtained and the nano-silver solution were stable
for more than 40 days.
Keywords: Spinning disc reactor, silver nano-particles.
1. INTRODUCTION
Based on recently published documentary, nano-silver prevents many kinds of bacterial
from development, destruction of cell membrane of about 650 kinds of dangerous single-celled
bacterial, especially Staphylococcus aureus (Gram+) and Escherichia coli (Gram-). The impact of
nano-silver on baterium is not similar to that of anti-biotic medicine. While anti-biotic medicine
affects on baterium in a long time, nano-silver destroys baterium in a very short time [1].
Nowaday, nano-silver product has many potential applications in many daily fields such as
aquaculture, breeding, farming fields and daily demands.... However, applications of nano-silver are
still limited due to high cost of the product.
Recently, investigation of general nano-sized materials, specially nano-Ag has been paid
much attention in Vietnam. Some initial results has been obtained, especially in applications of
nano-product. However, reported investigations almost use costly resources and are based on
conventional methods, so the product price is high, that limited wide applications of nano-silver [2].
In this work, spinning disc reaction method has been used to prepare nano-silver, in which
reactions take place on the surface of spinning disc, not only causing significantly improved micro-
mixing effection, but also intensifying mass-transfering rate and shortening reaction time [3, 4].
2. EXPERIMENTAL
In this work, the technology applied for preparation nano-silver is precipitation method on
the surface of spinning disc reactor.
Project Information:
- Code: CS/13/03-02
- Managerial Level: Institute
- Allocated Fund: 80,000,000 VND
- Implementation Time: 12 months (Jan 2013 – Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project:
Hoang Van Duc, Ngyen Thi Thuc Phuong. Preparation of nano-silver by reaction method on surface of
spinning disc reactor. (Submitted to Journal of Nuclear Science and Technology, VINATOM).
VINATOM-AR 13--41
The Annual Report for 2013, VINATOM
310
A schematic diagram of the experimental set-up is shown in Fig.1 in which tank A contained
AgNO3 and protecting reagents (PVP, PVA, PEG...) solution, tank B contained alkali solution
(NaOH, NH4OH, Na2CO3...) and reducing agent (glucose, starch, HCHO, NaBH4....).
The reaction between Ag cations and glucose in NaOH solution is as follows:
2Ag+ + C6H12O6 + H2O 2Ag
0 + C6H11O7
- + 3H
+
At first, tank A contained AgNO3 and protecting agent solutions, tank B contained NaOH
and reducing agent solutions with certain rates. The solutions in tank A and tank B were pumped by
pump C at a specific flow ratio onto the center of the spinning disc with a rotation speed ranging
from 0 to 3000 rpm. The liquid was accelerated due to centrifugal force, causing it to spread over
the disc surface and forming a thin film where the reducing reaction took place. After that, the
slurry of reaction products was shooted out to wall of spinning disc F and then flowed into tank A
to mix with AgNO3 solution. After the solution in tank B was exhausted, solution in tank A was
continuously pumped for a certain time. The recycle operation was adopted to give a high yield
because the retention time on the spinning disc was too short.
Figure 1: Experimental scheme for preparation nano-silver
using spinning disc reactor.
A: Solution of AgNO3 and protecting agent; B: Solution of NaOH and reducing agent;
C: Pump; D: Flowmeter; E: Liquid distributor; F: Spinning disc.
3. RESULTS DISCUSSION
List of tables, graphs and images
Table 1: Optimal technological parameters for preparation of nano-silver.
Rotation speed (rpm) 2000
Liquid flow rate LA (mL/min) 800
Liquid flow rate LB (mL/min) 200
[glucose] (mol/l) 0.02
[NaOH] (mol/l) 0.05
Weight rate: PVP/AgNO3 1
[AgNO3] (mol/l) 0.01
VINATOM-AR 13--41
The Annual Report for 2013, VINATOM
311
Table 2: Properties of nano-silver solution product.
N0. Property Nano-silver solution
1 Appearace Dark brown
2 Medium Distilled water
3 Mean particle size 12 nm
4 Distribution of particle size 9 – 15 nm
5 Protecting agent PVP K30
6 Concentration 500 ppm
Figure 2: UV-vis absorbtion spectrum of
nano-Ag colloid using protecting agent PVP.
0
10
20
30
40
50
60
0 0.25 0.5 0.75 1 1.25 1.5 1.75 2
Tỷ lệ khối lượng PVP/AgNO3
Kíc
h t
hư
ớc h
ạt
(nm
)
Figure 3: Correlation of nano-Ag particle
size and rate PVP/AgNO3.
10
12
14
16
18
20
22
24
26
28
0.005 0.01 0.015 0.02 0.025 0.03 0.035 0.04 0.045
Nồng độ gluco (mol/l)
Kíc
h t
hư
ớc h
ạt
(nm
)
Figure 4: Correlation of nano-Ag particle
size and glucose concentration.
10
15
20
25
30
35
0 0.005 0.01 0.015 0.02 0.025 0.03 0.035
Nồng độ AgNO3 (mol/l)
Kíc
h t
hư
ớc
hạ
t (n
m)
Figure 5: Correlation of nano-Ag particle
size and AgNO3 concentration.
.
10
12
14
16
18
20
500 1000 1500 2000 2500 3000
Tốc độ quay (v/p)
Kíc
h t
hư
ớc h
ạt
(nm
)
Figure 6: Effect of rotation speed on
nano-Ag particle size.
Figure 7: UV-vis absorbtion spectrum of
sample 16 after reaction and after 42 days.
VINATOM-AR 13--41
The Annual Report for 2013, VINATOM
312
Figure 8: TEM image of nano-silver colloid
after reaction (M16).
Figure 9: TEM image of nano-silver colloid
after 42 days (M16).
In this work, we have investigated and synthesized sucessfully nano-silver solution with
mean particle size of 12nm, narrow particle size distribution using spinning disc reaction system.
Furthermore, factors such as: selecting protecting agent, effect of initial material concentration,
rotation speed.... on quality of nano-silver product have been studied. The optimal experimental
conditions for preparation of nano-silver particles were: AgNO3 concentration = 0.01M, glucose
concentration = 0.02M, rate of mPVP/mAgNO3 = 1, rotation speed = 2000rpm. Figure 2 is UV-vis
spectrum of nano-silver colloid protected by PVP. Figures 3, 4, 5 and 6 are diagrams of correlation
of technological factors and silver particle size. Figure 7 is UV-vis spectrum of sample 16 (sample
of silver was prepared with optimal experimental conditions) after reaction and after 42 days.
Figures 8 and 9 are TEM images of sample 16 after reaction and after 42 days.
4. CONCLUSION
1. Designed and manufactured sucessfully spinning disc reaction system and employed
this system for preparation of silver nano-particles.
2. Investigated technological factors that affect on particle size of nano-silver product.
3. Suggested optimal experimental conditions for preparation of nano-silver by spinning
disc reaction method.
4. Prepared 5 litres of 500 ppm nano-silver solution with mean size of 12 nm and narrow
size distribution. Stabilized time for nano-silver solution is more than 40 days.
5. Based on researching data, this work released technological process for preparation of
silver nano-particle at experimental scale.
6. The scientific paper “Preparation of nano-silver by reaction method on surface of
spinning disc reactor” has been approved for publishment on VINATOM magazine.
5. PROPOSAL
This work has investigated and released process for preparation of high-quality nano-silver
solution. However, due to limit of investigation time and research grant, the technological process
suggested by this project just reached experimental discontinued scale with small amount of
reactants for each batch run. In order to improve and apply satisfactory results of this project in
daily life, research group give some suggestions as follows:
VINATOM-AR 13--41
The Annual Report for 2013, VINATOM
313
1. Vietnam Atomic Energy Institute (VINATOM) and Institute for Technology of Rare
Earth and Radioactive Elements (ITRRE) pay attention to allow this project to continue investigate
optimization of technological process and preparation reaction system.
2. Nano-silver particles have potentiality in applications for aquaculture, breeding and
cultivating fields... Therefore, we hope that this project will be scaled up to Ministry-level project in
order to investigate more deeply and comprehensively applications and properties of nano-silver
product.
REFERENCES
[1] Clifford Y. Tai, Yao-Hsuan Wang, Hwai-Shen Liu, “A green process for preparing silver
nanoparticles using spinning disk reactor” Published online December 28, 2007 in Wiley
InterScience Vol. 54, No. 2.
[2] Clifford Y. Tai,* Yao-Hsuan Wang, Chia-Te Tai, and Hwai-Shen Liu “Preparation of Silver
Nanoparticles Using a Spinning Disk Reactor in a Continuous Mode” Ind. Eng. Chem. Res.
2009, 48, 10104-10109.
[3] P. Silvert et al, Preparation of colloidal silver dispersions by the polyol process, J. Mater.
Chem, 1996, 6(4), 573-577.
[4] Hoàng Văn Đức, Nghiên cứu khả năng điều chế canxi cacbonat kích thước nanomet. Luận
văn thạc sỹ khoa học. Hà Nội 2009.
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
314
RESEARCH ON TECHNOLOGY OF MAKING RARE EARTH ALLOY
HAVING RARE EARTH CONTENT ≥ 30% FROM ORE ( ≥ 40% REO)
USING ALUMINUM THERMAL TECHNOLOGY IN ARC FURNACE
Ngo Xuan Hung, Ngo Trong Hiep, Tran Duy Hai and Nguyen Huu Phuc
Material Technology Center,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48-Lang Ha, Dong Da, Ha Noi
ABSTRACT: Arc furnace was used to smelt materials consisting of rare earth ore having rare earth content of
≥ 40% REO, aluminum as the reducing agent and additives. Rare earth alloy was obtained with rare earth metal
content of more than 30%.
I. INTRODUCTION
Rare earth alloys (FeRE) have been used as an agent to modify physical and mechanical
characteristics of the steel. Rare-earth metals in the molten steel, will reduce the amounts of
phosphor, sulfur, nitrogen, oxygen that are harmful to the properties of steel and have adversely
affect to mechanical properties of steel.
The research team of institutional level scientific project coded CS/13/03-04 proposed one
scientific task that was technology for making rare earth alloy having rare earth content ≥ 30% by
reducing rare earth ore through aluminum thermal technology in arc furnace.
Investigated technological parameters in the arc furnace include: reaction temperature,
reaction time and the actual mass ratio of reducing aluminum to theoretical calculation. From
obtained results, the research team proposes the optimal technical parameters as follows:
- The mass ratio Al(p)/Al(t) =140%.
- Temperature of the reduction: 16000C.
- Time of the reduction: 80 minute.
- The obtained products are FeRE alloys having chemical composition as following: 30-
32% RE, 40%Si, 1-2%Al and remain Fe.
II. EXPERIMENTAL
2.1. Raw materials
Chemicals: REO 40.0%, Al 99.5%, Si 99.0%, CaF2, CaCO3 with exact chemical
compositions. Some of them given in the following pictures.
Project Information:
- Code: CS/13/03-04
- Managerial Level: Institute
- Allocated Fund: 85,000,000 VND
- Implementation Time: 12 months (Jan 2013-Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project: (None)
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
315
Figure 1: Rare earth ore
(40%REO).
Figure 2: Metalic Silicon. Figure 3: Al granules, powder.
2.2. Equipments and product quality assessment method
1. Arc smelting furnace with conditions (15kVA).
2. Spectrum analyzer ICP-MS.
3. Molecular structure analyzer by X-ray diffraction Bruker-D5005.
4. Images of equipments.
Figure 4: The arc smelting furnace (15kVA).
III. RESULTS AND DISCUSSION
3.1. Study the influence of the mass aluminum ratio on rare earth ore recovery and
product quality
Base on reaction equation: RE2O3 + 2Al + 4Si = 2RESi2 + Al2O3, we will receive 392g
RESi2 + 102g Al2O3 from 328g RE2O3 + 54g Al + 112g Si.
With experimental conditions as follows: 328g rare earth ore (contains ≥40% REO), the
reaction temperature t = 1.600oC and time for reaction = 80 minutes, the obtained results are
showed in table 1.
Table 1: Influence of mass aluminum ratio to the rare earth ore on product quality.
N0
Ratio Al, % Experiment result
RE, % Productivity (RE), %
1 110 4.12 64.0
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
316
2 120 31.6 79.5
3 130 32.28 83.3
4 140 32.0 86.5
5 150 26.5 76.9
The optimal reducing Al ratio is chosen: 140%.
3.2. Study the effect of reducing temperature on product recovery efficiency
- Reducing temperature varies from 15000C to 1700
oC.
- Raw material is rare earth ore (containing ≥40% REO) = 328g;
MAl (140%) = 63.18 g; Reaction time: = 80 minutes.
Experiment results are presented in table 2.
Table 2: Effect of reducing temperature on the product recovery.
N0 Temperature,
0C
Experiment results
RE, % Productivity (RE), %
1 1500 4.12 64.0
2 1550 31.6 79.5
3 1600 32.2 86.5
4 1650 30.0 82.0
5 1700 24.2 77.6
Graphical presentation of the results is showed in Fig. 5:
Figure 5: Influence of reducing temperature on product recovery.
- The maximal recovery of % = 86.5% is achieved at reducing temperature of 1600oC.
- The reducing temperature t = 1600oC is chosen.
Pro
du
cti
vit
y,
%
0 1500 1550 1600 1650 1700 1750
40
50
60
70
80
90
100
Temperature
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
317
3.3. Study effects of reducing time on product recovery
Reducing time varies from 60 minutes to 100 minutes.
Experiment results are presented in the table 3.
Table 3: Effects reducing time on product recovery.
N0
, minutes Experiment results
RE, % Productivity (RE), %
1 60 18.7 66.0
2 70 28.6 76.4
3 80 32.0 86.0
4 90 32.1 86.2
5 100 28.0 76.0
- Maximal product recovery of % = 86.5% is achieved at reducing time of 80 minutes.
- Reducing time of 80 minutes is chosen.
3.4.Product quality assessment
The composition of rare earth alloys obtained from thermal reducing reaction are presented
in the following table.
N0 Sample
Experiment results
RE, % Al, % Si, % Fe, %
1 FeRE.01 4.12 - 67.8 Remain
2 FeRE.02 31.6 - - Remain
3 FeRE.03 32.2 - - Remain
4 FeRE.04 32.0 2.0 35.2 Remain
5 FeRE.05 24.2 3.2 - Remain
6 FeRE.06 18.7 - - Remain
7 FeRE.07 28.6 - - Remain
8 FeRE.08 26.5 - - Remain
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
318
3.5. Manufacturing process of rare earth alloys
Based on the above experiment results, the research team proposes a manufacturing process
of rare earth alloy (containing RE≥30%):
Figure 6: Diagram of making rare earth alloys containing ≥ 30% RE.
* Preparation for manufacturing rare earth alloys containing ≥ 30% RE as follows:
- CaF2 and CaCO3 are selected as additives because they are good for adjusting the
fluidity of the slag.
- The reducing process is carried out at temperature of 16000C.
- Reaction time is 80.
- Experiments are conducted in arc furnace 15KVA with volume of 600g for each
experiment.
IV. CONCLUSION
The institutional level project coded CS/13/03-04 has been implemented in more than one
year. Some important preliminary results have been achieved as follows:
- Research team proposed one optimal process for manufacturing rare earth alloy having
content of RE ≥ 30%.
Rare earth ore silicon Alumium
Arc melting method
Molten
Themal reaction
Filling the mold, cooled
Casting, pull out product
Rare alloy (30%RE)
product
Waste slag Recovering
product
Additives
VINATOM-AR 13--42
The Annual Report for 2013, VINATOM
319
- The process is conducted in arc furnace 15 kVA with reaction time of 80 minutes. Raw
materials consist of rare earth ore having content of ≥ 40% REO, aluminum, silicon and additives
that are mixed together and smelted in arc furnace. Melted product is filled into mold and allowed
to cool. Rare earth alloy having content of RE ≥ 30% is recovered after removing slag.
REFERENCES
[1] Bui Van Muu, Nguyen Van Hien, Nguyen Ke Binh, Truong Ngoc Than. Theory of
metallurgical processes. Fire training. Hanoi, 1997.
[2] X-Kh Nguyen Khac Xuong. "Material metal."
[3] Phung Viet Ngu, Pham Kim Dinh, Nguyen Kim Thiet. Theory of metallurgical processes.
Fire practiced 2. Hanoi, 1997
[4] USGS Mineral Commodities Summaries 2011.
[5] Z.L.K. Yasuda et al J alloys and Comp. Vol 193, pp. 26-28, 1993.
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
320
A TEST STUDY ON THE RECOVERY OF ZINC OXIDE FROM BAC-KAN
LOW GRADE ZINC ORE
Tran Ngoc Vuong, Pham Minh Tuan, Luong Manh Hung and Bui Huy Cuong
Center for Technology Development,
Institute for Technology of Radioactive and Rare Elements, Vietnam Atomic Energy Institute
48-Lang Ha, Dong Da, Ha Noi
ABSTRACT: A leaching process of the zinc ore has been carried out by a mixtures of ammonia and
ammonium carbonate under different conditions, then zinc was recovered from the leach liquors in the form of
zinc oxide. Experimental conditions were as the following: A leaching solution containing 80g/l of NH3 and
60g/l of CO2, solid-liquid ratio being 1:1 (200gs of ore and 200ml of solution), crushed zinc ore of particle size
below 0.1 mm, 2 hours of digestion under agitation with a stirring speed of 60-80 rpm/min at room temperature
or at 50°C. The recovery efficiency of zinc could thus be reached 80 to 85%. Purity of obtained product was up
to 99% of ZnO, while Pb content was lower than 0.2% .
I. INTRODUCTION
Zinc ore hydrometallurgy using diluted sulfuric acid is a primary method for zinc recovery
but in this process, many impurities such as Fe, Cu, As, etc. [1, 5] will be dissolved into the leach
solution along with zinc. Zinc ores, especialy Bac Kan low-grade zinc ore contains a large amounts
of impurities (Fe, Pb, Si, etc.) Accordingly, this method is a chemicals consuming and moreover,
the impurities removal from the leach liquors is generally costly and complicated.
Hydrometallurgy method using ammonia and additive reagents such as ammonium
carbonate, sulfate, chloride is based on zinc amphoteric property. In contacting with solutions
containing amonia/amonium salts, zinc oxide or zinc salts will be selectively extracted into solution,
while most of undesirable impurities such as Fe, Pb, etc. generaly retained as precipitate, which can
be removed as insoluble residue. From the obtained leach solution, zinc can be recovered in the
form of 2.ZnCO3 , 3.Zn(OH)2 or ZnCO3.3Zn(OH)2, which is easy to transform to zinc oxide or other
zinc compounds and the recovery of ammonia for its recycling also facilitate [3, 4, 6].
Zinc leaching process and recovery using amonia/amonium salts method can be discribed by
the following reaction equation:
Dissolution step:
ZnO + (NH4)2CO3 + 2NH4OH = Zn(NH3)4CO3 + 3H2O
Solution purification:
Me2+
+ Zn = Me + Zn2+
Hydrolysis and precipitation:
5Zn(NH3)4CO3 + 4H2O = 2ZnCO3.3Zn(OH)2.H2O ↓ + 3CO2 + 20NH3↑
Project Information:
- Code: CS/13/03-01
- Managerial Level: Institute
- Allocated Fund: 80,000,000 VND
- Implementation Time: 12 months (Jan 2013-Dec 2013)
- Contact Email: [email protected]
- Papers published in relation to the project: (None)
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
321
4Zn(NH3)4CO3 + 4H2O = ZnCO3.3Zn(OH)2.H2O ↓ + 3CO2 + 16NH3↑
Calcination (at 650-700°C)
ZnCO3.3Zn(OH)2.H2O → 4ZnO + CO2 + 7H2O
According to this method, ammonia generaly is used in combination with other reagents
such as ammonium carbonate, or sulphate or chloride. However ammonium carbonate is more
favourable due to creating intermediate compounds such as salts of zinc basic carbonate, which is
easily converted into zinc oxide with a specific surface area of 15-110 m2/g. This value very much
depends on the conditions of calcination (in the atmospheric environment or in a vacuum,
temperature and duration of calcination, etc.)[1, 2, 6].
II. EXPERIMENTAL
Zn content and impurities in the ore samples was determined by chemical method and
Inductively Coupled Plasma Mass Spectrometry (ICP-MS), respectively.
Minerals in the ore sample are determined by XRD at the Testing Center, Institute of
Building Materials.
Zn, Pb in the leach solutions and in ZnO products are determined by titration.
First experimental survey was conducted in the reaction conditions as follows:
Leaching temperature: at room.
Stirring speed: 60-80 r/min.
Concentration of reagents: NH3 80g/l, CO2 60g/l
Time of reaction: 120min.
Weight of ore: 200g.
Volume of reating agents solution: 200ml.
The experiment was then conducted in different reaction conditions by changing the ratio of
raw materials and reagents, reagent concentration, temperature and time of reaction, agitation
condition, etc. to point out the most suitable conditions in terms of maximium for zinc recovery
efficiency.
Zinc in the solution was precipitated in the form of ZnCO3.2Zn(OH)2 by removing NH3
from leach solution at temperature of 70-90°C with air flow contacting. Time of heating and air
contact was 180 minutes. Basic zinc carbonate precipitate was filtered, washed with distilled water
and then dried at a temperature of 100°C. Basic zinc carbonate precipitate ZnCO3.2Zn(OH)2 was
sintered at temperatures of 650-700°C for 120 minutes. The resulting product was analyzed by
chemical analysis and by inductively coupled plasma mass spectrometry (ICP-MS), particle sizes of
ZnO was determined by Lazer Scattering method using Particle Size Analyzer LA-950.
III. RESULTS AND DISCUSSION
Bac-Kan zinc ore contained about 7.0% of Zn and main impurities as Fe (41.8%), Pb
(5.77%).
X-ray diffraction diagram (Fig. 1) showed that zinc in ore existes in the form of mineral
Zn(ClO3)2.6H2O, Na4Zn2Si3O10/2Na2O.2ZnO.3SiO2. It was also found zinc in the form of
hydroxide Zn(OH)2, ZnCO3. Iron existed mostly in the form of magnetite Fe3O4. Other remaining
substances were mainly in the amorphous phase.
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
322
Figure 1: X-ray diffraction diagram of Bac-Kan Zinc Ore.
The experimental results proved that the selection of ammonia and ammonium carbonate as
reaction agents for zinc recovery fitted perfectly to Bac-Kan zinc ore because of a large amount of
the impurities such as Fe, Pb were retained insoluble. A schematic diagram for zinc oxide recovery
technology from zinc ores by hydro-metallurgical method using ammonia and ammonium
carbonate was shown below.
From the study, it was concluded that the most suitable experimental conditions for Zinc
recovery efficiency up to 85% was as the following.
Leaching temperature: 50°C.
Stirring speed: 60-80 r/min
Concentration of reagents: NH3 80 g/l , CO2 60g/l
Time of reaction: 120min.
Weight of ore: 200g.
Volume of reating agents solution: 200ml.
Crushed ore size: < 0.1mm.
From obtained leach solution, zinc was recovered in the form of basic zinc carbonate
precipitate by hydrolysis reactions. Basic zinc carbonate salts obtained then undergo filtration,
washing and drying. Dried basic zinc carbonate is calcinated in a furnace at 650-700oC for 120
minutes to obtaine ZnO products.
The composition of resulting product was shown in table 1, ZnO purity was up to 99%, and
impurities such as Pb, Fe were very low (<0.1%).
X-ray diffraction diagram confirmed that the formation of ZnO is mainly in obtained
product.
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
323
Table 1:. Chemical composition of zinc oxide product.
No. Species Unit Content
1 ZnO % 99.20
2 Mg % 0.004
3 K % 0.002
4 Ca % 0.006
5 Fe % 0.005
6 Cu % 0.006
7 As % 0.015
8 Cd % 0.002
9 Sn % 0.001
10 Sb % 0.160
11 Ba % 0.002
12 Pb % 0.160
13 Li ppm 0.15
14 Na ppm < 0.001
15 Al ppm 0.53
16 Si ppm 1.14
17 Mn ppm 1.17
The results of particle size determination shows that median size of ZnO particles is 6.9µm
(Figure 2).
Figure 2: Particle size distribution of Zinc Oxide Product.
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
324
SEM images of the obtainned zinc
oxide confirmed this product is very fine with
nanoparticles. It is can be seen by using SEM
image that the median size of particles
increased due to agglomeration of zinc oxide
particles.
Figure 3: SEM image of Zinc Oxide Product.
After the experimental study, we propose a technological process shown below
Figure 4: Technology Schematic Diagram for zinc oxide recovery using reagent
mixture of amonia and amonium carbonate.
Zinc oxide Ore Zn<8%
Leaching (120 min.)
Filtration
Hydrolysis (t0 70-
80oC); 180 min.
Insoluble
residue
Filtration
Basic Zinc Cacbonate
Calcination 650-700oC (120 min.)
ZnO 99%
Solution of NH3 80g/l and
CO2 60g/l
VINATOM-AR 13--43
The Annual Report for 2013, VINATOM
325
IV. CONCLUSIONS
Although Bac-Kan zinc oxide ore contained low grade of zinc and very high levels of
impurities, a method using a mixture of amonia and ammonium carbonate shows a great promise in
the recovery of zinc from this ore. Zinc recovery efficiency was up-to 85%. From the leach
solution, a high quality product of ZnO 99% could be obtained.
REFERENCES
[1] Daniel A. D. Boateng, “Method for the solvent extraction of Zinc”, US patent 5135652,
2/1992.
[2] Raymond Lee Nip, “Method for preparing of zinc carbonate”, US patent 6555 075, 4/2003.
[3] W.Herbert Burrows, “Zinc oxide recovery process”, US patent 3849121, 12/1974.
[4] Frank H. Murphy, Matt W. Oleksy, “Recovery of Zinc and ammonium chloride”, US patent
4865831, 09/1989.
[5] Yeonuk Choi, Serge Payant, Joo Kim, “Product of zinc oxide from acid soluble ore using
precipitation method”, US patent 6726889 B2, 04/2004.
[6] Nicholas J. Welham, Garry M. Johnston, Matthew L. Sutclife, “Method for ammoniacal
leaching”, US patent 8388729 B2, 03/2013.
VINATOM-AR 13--44
The Annual Report for 2013, VINATOM
329
RESEARCH TO BUILD THE ADVANCED TRAINING PROGRAMS
FOR NUCLEAR POWER PLAN
Nguyen Manh Hung
Nuclear Training Center, Vietnam Atomic Energy Institute
Le Van Hong and Cao Dinh Thanh
Vietnam Atomic Energy Institute
Nguyen Ba Tien
Institute for Technology of Radioactive and Elements, Vietnam Atomic Energy Institute
ABSTRACT: The documents use for training of field Nuclear Power at Nuclear Training Center (NTC) is
necessary .On the based analysis, research the current situation and material authors has been to building
specialized Training Programs for Nuclear Training Center (NTC) and to compilation documents use for
training includes is 05 topics: 1. Assessment nuclear power plant technology in the world, 2. Safety analysis of
nuclear reactors, 3.Nuclear fuel cycle, 4. Management technology uses radioactive waste in nuclear power
plants and 5.Nuclear Power Plan.
1. INTRODUCTION
On August 20th
, 2010 the Prime Minister Nguyen Tan ZDung has signed a decree related to
the developing of the education and training programme in the frame of the NPP project in
Vietnam. Several universities in Vietnam are encouraged to participate to such a programme. To
2020, the expected number of experts working in different nuclear field would be around 3000
persons. So that, the Documents about Nuclear Power Plan use for training in NTC is necessary.
The development of a highly skilled human resource is an essential element in the
infrastructure required by a country planning to introduce nuclear power (figure: HRS Development
for NPP Project). As IAEA points out /68/, the principle involved is to identify the human resource
knowledge, skills and abilities needed to implement the nuclear project and to develop the
educational and training institutions to prepare the human resources necessary for the discharge of
their function. This paper describes some of the skills needed, gives some quantitative estimates of
the numbers of experts needed, identifies some possible education and training resources and
concludes with some suggestions for getting started on this important infrastructure element in
Vietnam with regard to the decree just signed by the Prime Minister Nguyen Tan Dung mentioned
Project information:
- Code: 04/2012/HD-NVCB
- Managerial Level: Ministry
- Allocated Fund: 500,000,000 VND
- Implementation time: 24 months (Jan 2012-Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project:
1. Strategy and Challenges of Nuclear HRD for Introduction of the 1st Nuclear Power Plant in VIETNAM
Nguyen Manh HUNG NTC-VINATOM-Meeting Coordinator FNCA Tokyo 2013.
2. Challenges in developing HR for Nuclear Education Programmes in Vietnam.
Nguyen Manh HUNG NTC-VINATOM-Meeting Coordinator FNCA 2012.
3. Nuclear Human Resource development in Vietnam Atomic Energy Institute Nguyen Manh Hung NTC-
VINATOM-International Conference on Nuclear Human Resource 29-31 October 2013,Hanoi,Vietnam.
VINATOM-AR 13--44
The Annual Report for 2013, VINATOM
330
above. The problem preparation Human resource for MOST (VINATOM, VARANS and VAEA) is
importance also; because MOST is organization have function: Radiation protection, nuclear safety,
State management of nuclear Energy, Program R/D in nuclear Energy and Consulting for NPP plan.
Figure: HRS Development for NPP Project.
2. RESULTS AND DISCUSSION
The project “Research to build the advanced training programs for nuclear power plan”
during from 2012 to 2013 with purpose to compile 05 textbooks (1000 pages) and 05 E- learning
lesion (800 slices) is:
1. Assessment nuclear power plant technology in the world;
2. Safety analysis of nuclear reactors;
3. Nuclear fuel cycle;
4. Management technology uses radioactive waste in nuclear power plants;
5. Nuclear Power Plan.
And organize training course “To improve knowledge on Nuclear power Plan for managers
of state agencies”. The report is including 02 parts:
A. To compile Curriculum about Nuclear Power;
B. Organize Training course.
On the part A, the author has to compile Curriculum about:
- The knowledge of nuclear reactors, fabrication technology, the basis of the hydrothermal
reactor and system safety analysis is presented in 02 textbooks and 02 E- learning lesion is
Assessment nuclear power plant technology in the world and Safety analysis of nuclear reactors is
include some problems as:
1. Overview of nuclear reactor technology and nuclear power plants;
2. The basic principles of neutron physics and nuclear fission;
VINATOM-AR 13--44
The Annual Report for 2013, VINATOM
331
3. Hydrothermal basis of nuclear reactor;
4. Pressurized water reactor technology-PWR;
5. Boiling water reactor technology-BWR;
6. Heavy water reactor technology pressure-PHWR;
7. Safety design and related issues;
8. Generation nuclear reactors and advanced design;
9. Practical part: Analysis, assessment, technology selection NPP.
and
1. Identify potential risk of radiation in NPP;
2. Design perspective NPP safety;
3. The system safety engineering;
4. Safety Analysis;
5. Analysis of a large number of incidents have occurred;
6. Some orientations enhance safety NPP;
7. The preventive measures and troubleshooting;
8. Introduction of safety analysis calculations RELAP.
- The knowledge of the Nuclear fuel cycle and radioactive waste treatment in nuclear
power plants (NPP) is presented in 02 textbooks and 02 E-learning lesion is Nuclear Fuel Cycle and
Management, technology use radioactive waste in nuclear power plants, so that the contents of the
textbooks should be supply for participants the knowledge about Nuclear fuel cycle and how to
management and technology use radioactive waste in NPP Plan.
1. Fuel for nuclear reactors.
2. System Reactors and corresponding fuel types.
3. Nuclear fuel cycle of the reactor.
4. Technology production Nuclear fuel.
5. Marketing of Nuclear fuel.
and
1. Introduction of radioactive waste.
2. Radioactive Waste.
3. Decontamination of radioactive materials.
4. Assessment safety in the management of radioactive waste.
5. The exercises.
- In addition, the energy problems in the world such as energy demand, energy resources,
environmental issues, as well as issues related to nuclear power development and international
cooperation was the introductory textbook Nuclear Power Plant and E- learning lesion. Its cover
some problems as:
1. Sources of Energy;
VINATOM-AR 13--44
The Annual Report for 2013, VINATOM
332
2. Electrical energy today and future;
3. Nuclear Power;
4. Nuclear fuel cycle;
5. Nuclear Waste;
6. Other uses of atomic energy Environmental issues, health and safety;
7. No nuclear proliferation;
8. History Nuclear Energy.
On the part B, Nuclear Training Centre organized a training course to improve knowledge
on nuclear power for managers of state agencies from 6-8 Nov 2013. More than 30 participants
come from the Department of International Cooperation belong the Ministry of Science and
Technology, the Safety Board, the cultural community of the Group electricity of Vietnam;
Department of fire police , College of electricity HCM city, Joint Stock Construction Company,
Consultancy Electrical 1, 2 and 3; and College of Central Power have attend the training course.
3. CONCLUSION
Finally, the authors proposed commendations and measures to promote the Human Resource
Development as:
Continuing the compilation of textbooks on nuclear power technology, radiation safety,
nuclear safety, and system control equipment in nuclear power plants as well as exercises for the
reactor, radiation measurements recorded for documents teaching resources.
Acknowledgements
The authors would like to express their thanks to the Ministry of Science and Technology
and Vietnam Atomic Energy Institute for their great encouragement and financial support for this
work. We also want to express our gratitude to colleagues, which are participation and contribution
on this work.
REFERENCES
[1] “Nuclear Energy in the 21st Century” Ian Hore Lacy-World Nuclear.
[2] TrÞnh Xuân BÒn, Nguyễn Quang Hưng-Cơ sở chọn vùng và đề xuất kế hoạch thăm dò uran
phục vụ chương trình phát triển điện nguyên tử ở nước ta. Hội thảo nguyên nhiên vật liệu hạt
nhân-Hà nội 1999.
[3] Thái Bá Cầu và cs, Báo cáo khoa học đề tài KHCN.09.04/04, Luận cứ và khả năng nội địa
hoá từng phần công nghệ sản xuất nhiên liệu hạt nhân.Hà Nội-1998.
[4] IAEA Technical Document: Minimum Infrastructure for a Nuclear Power Project, Final
draft, 12 January 2006.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
333
COLLECT, ANALYZE AND DATA BASE FOR BUILDING UP
THE INVESTMENT REPORTS OF CENTER FOR NUCLEAR SCIENCE
AND TECHNOLOGY CONSTRUCTION PROJECT
Pham Quang Minh, Tran Chi Thanh, Cao Dinh Thanh, Mai Dinh Trung,
Hoang Sy Than, Nguyen Nhi Dien, Trinh Van Giap, Le Ba Thuan and Vu Tien Ha
Vietnam Atomic Energy Institute
ABSTRACT: Following the Contract No.19/HĐ/NVCB dated July 10, 2013 signed by the President of
Vietnam Atomic Energy Institute (VINATOM), an additional ministerial Project was approval by the Decision
No. 526/QĐ-VNLNT dated July 8, 2013 by the VINATOM’ President in order to implement an important task
for VINATOM. This project was implemented by the Institute for Nuclear Science and Technology (INST) in
Hanoi as management organization and VINATOM as the owner of project’s results. Main objectives of this
Project are to support national budget for implementing to collected the general report from previous projects
which are relevant to CNEST and new research reactor, IAEA guidance documents, documents provided by
ROSATOM in seminars in 2010, 2012 and 2013, report from expert visits of Ministry of Science and
Technology and completed the general report about the construction project of CNEST.
I. INTRODUCTION
The intention for building up the Center of Nuclear Science and Technology (CNEST) was
formed right after the Government Prime Minister of Vietnam had an agreement with Russia
Federation about the construction of the first Nuclear Power Plant of Vietnam (Ninh Thuan 1 NPP)
during the official visit to Russia Federation in 12/2009. The purpose of CNEST is to support the
nuclear power project and nuclear power program of Vietnam. The funding for CNEST will be
provided by Russia Federation to Vietnam through priority credit.
To have the official information for CNEST and to prepare the funds for the project,
Vietnam Atomic Energy Institute (VINATOM) has established the Ministry level project about:
“Collect, Analyze and data base for building up the investment reports of Center for Nuclear
Science and Technology construction project”, and submit to Ministry of Science and
Technology for approvement, and further submit to the Government. This report will be the basis
for Ministry of Finance of Vietnam to start the negotiation with Ministry of Finance of Russia
Federation.
II. CONTENTS
II.1. Data resources for reviewing and analyzing
The investment for CNEST has the purpose of acclerate the research in application of
atomic energy, enhance the abilities of high level human resources in Nuclear science and
Project information:
- Code: 19/2013/HD-NVCB
- Managerial Level: Ministry
- Allocated Fund: 350,000,000 VND
- Implementation time: 6 months (Jun 2013-Dec 2013)
- Contact email: [email protected]
- Paper published in related to the project: (None)
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
334
technology and support the nuclear power program as well as application of atomic energy for the
development of the socio-economic.
To prepare for the CNEST project, VINATOM has established some following projects:
- 2010 Ministry level project: “Survey, collect and research the initial data for site
selection of Center for Nuclear Science and Technology”.
- 2011 Ministry level project: “Research and determine design requirement of Center for
Nuclear Science and Technology”.
- 2012 Ministry level: “Research and buildup the criteria set for site selection of new
research reactor and create the initial report for site selection of Center for Nuclear Science and
Technology”.
- B-Branch sub-project: “Building up the argument for new research reactor project of
Vietnam” under the independent National level project: “Builind up the R&D capacity for
supporting the Nuclear power program” Code name: DTDL 2002/17, 2002-2004 period.
- Ministry level project: “Research the plan of building up new research reactor and
perform some calculation about neutron physics and thermal hydraulic to classify research reactor”
Code: BO/06/01-04, 2006-2007 period.
- 2007 Organization level project “Determine the technical mission for new research
reactor and necessary infrastructure investment for this mission as well as human resources
requirement for managing, operating and ultilizing new researc reactor”.
Besides these project reports, a lot of documents from IEAE guidance, technical documents
provided from ROSATOM at the seminars about CNEST in 2010, 2012 and 2013;
recommendations and opinions of scientist during the seminars, results of the discussion between
ROSATOM and experts group of Ministry of Science and Technology during the visit to research
facilities of Russia Federation in 04/2013 are also the documents sources for project establisher to
perform the contents of these project and building up General reports for CNEST.
II.2. Analyzing and reviewing methodology
Inquiring the results of all listed project, guidance documents from IAEA, technical
documents about research reactor, auxiliary system for Nuclear safety research complex, and
Material science complex that ROSATOM provide through all the seminars about CNEST in 2010,
2012 and 2013.
Research, exchange and unify about technical information requirements of the research
reactor, auxiliary system and devices for Nuclear safety research complex, structure of Material
Science complex’s laboratory between ROSATOM’s organizations and send experts group of
Ministry of Science and Technology to visit the research facilities of Russia in 04/2013.
Ultilize the results, design requirement (TOR) for CNEST.
About site selection for the new research reactor: progress the build process of the site
selection review criterial; perform reviewing, analyzing and comparing activites candidate sites by
grading system follow the criteria with the support of Expert Choice software as well as progress
the basic survey for candidate sites.
Establish conference, seminar to gather opinions from senior experts about technical
requirements of research reactor, auxiliary system and devices for Nuclear safety research complex,
structure of Material Science complex.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
335
III. GENERAL REPORT OF CONSTRUCTION PROJECT OF CNEST
This general report include the following main contents: The need for investment of
CNEST; The progress of of CNEST project; Structure and main sub-division of CNEST;
Construction sites for new research reactor and other research facilities under CNEST; Funding and
funding phases of CNEST; Project establishment plan; and Some recommendation, conclusion.
III.1. The need for investment of CNEST
With the 35 years history of development, VINATOM has played an important role in
forming and developing the atomic energy field in Vietnam, contribute to bring the application of
Nuclear techniques, radiation technology to socio-economic of the country. After the southern
Vietnam was brought back to freedom, the staffs of VINATOM have immediately started to recover
the Dalat Research reactor, and the construction and operation of this research reactor has
contribute largely to acclerate the development of science and technology, application of nuclear
techniques, radiation technology as well as developing the human resources for the atomic energy
field of Vietnam. In this period, when Vietnam is establishing the Nuclear power development
program, acclerating the R&D, technical consultant in nuclear power filed had became a new and
very essential mission of VINATOM.
On 5st March 2012, according to decision No 265/ QD-TTg, the govermental Prime Minister
has approved the project “Enhancing the R&D and technical support capabilities for supporting the
application of atomic energy and ensuring the safety, security” in order to build up and develop
Vietnam Atomic Energy Institute (VINATOM) to an advance level in the region, take role as an
organization for R&D of science and technology; as well as a national technical support
organization, independent in quality assurance and quality control, ensure safety, security and
environment protection for nuclear power development.
With the aim of developing science, technical capabilities and human resources; and in the
framework of collaboration between The social republic of Vietnam and Russia Federation about
nuclear power; establishing Center for Nuclear Science and Technology (CNEST) is well suited
with the collaboration between two countries. In short term, CNEST will support the Ninh Thuan 1
Nuclear power plant process, and for long term CNEST will support the technology receive and
adaptation, moving forward to master the design, technical, operation techniques, maintenance of
the nuclear power plant, make sure that the nuclear power plant will be operated safely and have
good efficient. Beside that, CNEST will create a good condition to establish the modern research,
enhance the application of atomic energy in other socio-economic field and step by step increase the
science and technology capabilities of the country.
III.2. Site selection for new research reactor
The site selection process of the new research reactor will be established by 3 following
phases:
Phase 1: Creation of review criteria to compare sites candidate, from that, determine the
potential region and sites that may be selected and construction location.
Phase 2: Base on the review criteria and basis data collected, perform the the review and
comparison between the potential region and sites to chose 1 or 2 most suited sites that can sastify
all the technical and socio-economic requirements, as well as many advantage as possible to submitt
to te Governmental Prime Minister for approvement.
Phase 3: Perform the detail survey about the location which has been approved by
Governmental Prime Minister to establish investment preparation profile and submitt according to
legal framework.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
336
Base on the ranking comparison criteria for potential site for new research reactor which has
been approved by Minstry of Science and Technology, Power Consulting Engineering Company I
had cooperate with VINATOM to anlazye, review and ranking 5 potential sites to chose the most
appropriate location that meet the criteria.
And the most potential location is Sub-section 151A (Lam Vien forest management board,
belong to ward 12, Dalat city, Lam Dong Province), on the ground of Center for High level Nuclear
techniques application project.
III.3. Structure of CNEST
According to international experiences, to acclerate and support Nuclear power development
program, VINATOM has determined 15 necessary speciality orientations. VINATOM has
collaborated with ROSATOM scientist to discuss, research the possibility, efficiency of the project
and delivered structurize methodology of CNEST to be 2 part of following components:
a) Construct a new and modern nuclear research facility, gather in one location, include
research reactor with capacity of about 10-20MWt, research laboratories and devices related to
research and application from ultilizing the research reactor.
This nuclear research facility is the main component of CNEST, and its location is expected
to be placed in Dalat city, with the following mission and function: Research and application in
fields of neutron technology, material science, radioisotopes, application of radiation techniques in
healthcare, agriculture and support the nuclear power related field like reactor physics, radioactive
waste management, Instrumentation and Control, environment protection, technical services.
b) Investment for equipages into one of the existing research facility under VINATOM in
Hanoi city, in which are performing research about speciality orientations that is not related to the
new research reactor.
Mission and function of these facilities is to support nuclear power program, including :
Nuclear power safety and technology (mechanical and thermal hydraulic), Material science,
Chemical technology, Nuclear and radiation technology, Radiation protection and environment
monitoring, radioactive waste management, human resources development (simulation devices),
nuclear services (Non-destructive evaluation,..) Center for simulation and calculation, as well as
basic science like Nuclear physics.
After CNEST would be constructed and operated, all the research complex of Northern
Vietnam will be the place for establishing research, human resources development, directly support
for nuclear power. The collaboration between Universities, Research institution (including Vietnam
Academic of Science and Technology) in the Northern Vietnam is necessary to acclerate R&D
activities, creating many research group with high level abilities with fully support to nuclear power
project, and this shall be the basis for education of new generation of experts, human resources for
Nuclear power program.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
337
Figure 1: Roles and positions of CNEST in Nuclear Power Program of Vietnam.
III.4. Location of the components of CNEST
1) Location of Dalat Nuclear Research Center (DNRC)
The selected construction site of DNRC including new Research reactor and relevant
devices and systems will be at Ward 12, Dalat city, lie inside the 107 Ha project which has been
approved and licensed the document for ultilization of real estate by local goverment of Lam Dong
Province for building the new nuclear research faclity of VINATOM.
This location has sastified almost every criteria to build the CNEST with the new research
reactor with capacity of about 10-20 MWt.
2) Construction location of the Nuclear power safety research Complex (Hanoi city)
The process of selecting the site for the Nuclear power safety research has been established
based on the human resources, research experience and existed space in Institute for Nuclear
Science and Technology. Beside that, the integrity of infrastructure with the project of Center for
environment radiation monitoring of the country will decrease the initial investment and preparation
time related to construction procedure.
3) Construction location of Material science complex (Hanoi city)
The Material sience complex in Hanoi city can be placed at the research facility of Institute
of Radioactive and Rare Earth Elements at 140 Nguyen Tuan street, Thanh Xuan distr, Hanoi. This
location is also the place where Center of Non-destructive Evaluation lie.
4) Construction option for research facility in Hoa Lac high-tech zone
The difficulties of selecting location for 2 center components in Hanoi are very troublesome,
because of the features of individual components. Establishing the project with 2 components in 2
different research units is very challenging.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
338
Because of that, VINATOM has submitted the option for construct all the components in the
Northern of Vietnam into only one location, appropriate for short term mission and long term
development, we can gather research staff not only from VINATOM but also other research
institution and universities in Northern Vietnam. The most optimum location is inside Hoa Lac
high-tech zone. This zone has a 50000 m2 area.
III.5. Funding and Funding phases of CNEST
1) Total credit funding from Russia Federation
The investment for the construction is from the credit funding of Russia Federation
according to Bilateral government agreement which was signed on 21/11/2012.
Table 1: General description of total investment according to job contents.
Category Borrowed funds (Thousands of USD)
Hanoi Dalat Project
Management
General expense
Construction 91 940
Installation 1 190 29 333
Devices 32 554 165 333
Others 4 286 75 964 49 954 60 965
Back up 4 458 36 718
Total 42 489 399 288 110 919
Total funds 552 696
2) Parallel funding from Vietnam
Investment for facility construction of 2 research components at Hanoi, as well as funding
for all relevant work to the infrastructure are all responsibility of Vietnam.
Table 2: Parallel funding from Vietnam to Northern infrastructure.
No. Categories Expected fund
1 Investment for construction of the facility and
installation research devices and control room for
Nuclear power safety research Complex
41 Billion VND
2 Investment for auxilary construction and technical
infrastructure for Nuclear power safety research
Complex
51 Billion VND
3 Investment for new construction and completion of
the building and infrastructure of the Material
science Complex
90 Billion VND
Total 182 Billion VND
(equal to 9 Millions USD)
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
339
III.6. Human resources development for CNEST
A general human resources development program for entire CNEST has been built in the
feasibility study of CNEST.
Human resources solution for CNEST:
- Consider Dalat Nuclear research institute to be the mini version of CNEST in the future,
and Dalat NRI will be “transition step” to educate and provide human resources for this field;
- Send student abroad for further education (send to Russia Federation);
- Recruit new engineer with good potential and send them for further education abroad
and also on-job training in research organization like GIDROPRESS, VNIIAES or SNITTMASH
institute when experts of these organization perform the design and construction process for
CNEST;
- Educate through research work, mission and projects of VINATOM, collaboration with
universities in Hanoi;
- Educate through performing establishment project inside the framework of CNEST
project (with Russia partners), and may be send experts to research institute in Russia to work with
this project.
IV. CONCLUSION
The main results of this project can be summarize as following:
1. The project has collected the general report from previous projects which are relevant to
CNEST and new research reactor, IAEA guidance documents, documents provided by ROSATOM
in seminars in 2010, 2012 and 2013, report from expert visits of Ministry of Science and
Technology;
2. The project has completed the general report about the construction project of CNEST;
3. Reports about the project which has been approved by Ministry of Science and
Technology in 8/2013. This report will be the supportive material for financial negotiation of
Ministry of Finance and the basis for application for government investment to prepare for the next
stage of the CNEST project in 2014.
REFERENCES
[1] Nguyễn Việt Hùng, Báo cáo tổng kết Nhiệm vụ cấp Bộ năm 2010” Khảo sát, thu thập,
nghiên cứu dữ liệu ban đầu phục vụ cho lựa chọn địa điểm xây dựng Trung tâm Khoa học và
Công nghệ hạt nhân”.
[2] Lê Văn Hồng, Báo cáo tổng kết nhiệm vụ cấp Bộ năm 2011” Nghiên cứu xác lập các yêu cầu
thiết kế (TOR) cho Trung tâm Khoa học và Công nghệ hạt nhân”.
[3] Mai Đình Trung, Báo cáo tổng kết nhiệm vụ cấp Bộ năm 2012 “Nghiên cứu xây dựng bộ tiêu
chí lựa chọn địa điểm xây dựng lò phản ứng nghiên cứu và lập báo cáo sơ bộ lựa chọn địa
điểm dự án Trung tâm Khoa học và Công nghệ hạt nhân”.
[4] Nguyễn Nhị Điền, Báo cáo tổng kết đề tài nhánh B “Xây dựng luận cứ cho đề án Lò phản
ứng nghiên cứu mới ở Việt Nam” thuộc đề tài độc lập cấp Nhà nước “Xây dựng tiềm lực
R&D phục vụ chương trình phát triển Điện hạt nhân” mã số ĐTĐL-2002/17 giai đoạn 2002-
2004.
[5] Nguyễn Nhị Điền, Báo cáo tổng kết đề tài cấp Bộ “Nghiên cứu phương án xây dựng lò phản
ứng nghiên cứu mới và thực hiện một số tính toán neutron và thủy nhiệt để nhân dạng lò
phản ứng” mã số BO/06/01-04 giai đoạn 2006-2007.
VINATOM-AR 13--45
The Annual Report for 2013, VINATOM
340
[6] Nguyễn Nhị Điền, Báo cáo tổng kết nhiệm vụ cấp cơ sở năm 2007 ” Xác định các nhiệm vụ
kỹ thuật cho LPUNC mới và các đầu tư cơ sở vật chất kỹ thuật cần thiết phục vụ nhiệm vụ
này và nhu cầu nhân lực cho quản lý, vận hành và khai thác sử dụng LPUNC”.
[7] IAEA TEC-DOC-1234, The Applications of Research Reactors, Report of an Advisory
Group Meeting held in Vienna, 4-7 October 1999.
[8] Radioisotope Production in Nuclear Research Reactors. IAEA-TECDOC-2000.
[9] Report of the IAEA Regional Management Workshop on Strategies to Enhance Utilisation of
Local Radiopharmaceuticals, RAS/2/009, Korea, 22-26 October 2001.
[10] Các tài liệu do các đoàn chuyên gia của ROSATOM cung cấp qua các hội thảo, chuyến thăm
và làm việc tại Việt Nam liên quan đến dự án Trung tâm KH&CNHN năm 2010, 2012 và
2013.
VINATOM-AR--13
The Annual Report for 2013, VINATOM
343
2.1. LIST OF VIE PROJECTS 2013
(implemented by VINATOM)
Code Project Title Start
Year
Budget
(USD)
Field
code Project
Counterpart
Institution
VIE2011
Enhancing the Capability
of Uranium and Related
Atomic Mineral
Exploration for Nuclear
Energy
2012 76,913.00 7 Le Ba Thuan
ITRRE
VIE6025
Upgrading the Standard
Dosimetry and Nuclear
Safety Laboratories of the
Institute for Nuclear
Science and Technology
(INST)
2012 76,174.00 29 Vu Manh Khoi
INST
VIE9011
Improving the Capability
for Site Characterization
and Evaluation of New
Nuclear Installations
2009 230,865.59 9F Truong Y
NRI
VINATOM-AR--13
The Annual Report for 2013, VINATOM
344
2.2 LIST OF FNCA PROJECTS 2013
(Implemented by VINATOM and Vietnam other organizations)
Fields Project Tittle Project Coordinators
Radiation
Utilization
Development
Mutation Breeding Dr. Le Huy Ham
Director General
Institute of Agricultural Genetics (AGI)
Ministry of Agriculture and Rural Development (MARD)
Biofertilizer Dr. Pham Van Toan
Director, Postgraduated Department, Vietnam Academy of
Agricultural Sciences (VAAS)
Ministry of Agriculture & Rural Development (MARD)
Electron Accelerator
Application
Dr. Quoc Hien NGUYEN
Principal Scientist
Research and Development Center for Radiation
Technology (VINAGAMMA)
Vietnam Atomic Energy Institute (VINATOM)
Radiation Oncology Dr. Bui Cong Toan
Head of General Radiotherapy Department,
National Cancer Institute (K Hospital)
Research Reactor
Utilization
Developemnt
Research Reactor
Network
Mr.Duong Van Dong Director,
Center for Research and Production of Radioisotope,
Nuclear Research Institute(NRI),
Vietnam Atomic Energy Institute (VINATOM)
Neutron Activation
Analysis
Mr. Cao Dong Vu Deputy director of Center for Analytical Techniques
(CATech)
Nuclear Research Institute (NRI)
Vietnam Atomic Energy Institute (VINATOM)
Nuclear Safety
Strengthening
Safety Management
Systems for Nuclear
Facilities Project
Dr. Nguyen Nhi Dien
Director, Nuclear Research Institute,
Vietnam Atomic Energy Institute (VINATOM)
Radiation Safety and
Radioactive Waste
Management
Dr. Le Ba Thuan
Director
Institute for Technology of Radioactive and rare Elements
Vietnam Atomic Energy Institute (VINATOM)
Nucclear
Infrastructure
Stecnthening
Human Resources
Development
Ms. CAO Hong Lan Deputy Director
Department of Administration and Personnel
Vietnam Atomic Energy Institute (VINATOM)
Nuclear Security and
Safeguards
Dr. NGUYEN Nu Hoai Vi Director of Nuclear Control Division
Vietnam Agency for Radiation and Nuclear
Safety(VARANS)
VINATOM-AR 13
The Annual Report for 2013, VINATOM
345
2. 3 List of INT\RAS\ Non RCA Projects 2013
(Implemented by VINATOM)
Code Title Year of
approval
Budget
(USD)
Project
Type Project
Coordinators
INT2014
Supporting Member States to
Evaluate Nuclear Reactor
Technology for Near-Term
Deployment 2012 INT
Tran Chi
Thanh
RAS0060
Enhancing Capacity for Effective
Use and Maintenance of Nuclear
Instrumentation 2012
Footnot A
(FA) Non-RCA
Dang quang
Thieu
RAS0065
Supporting Sustainability and
Networking of National Nuclear
Institutions in Asia and the Pacific
Region 2012 361,418.00 Non-RCA
Nguyen Manh
Hung
RAS0066
Contingency Project for
Institutional Development 2012 188,235.06 Non-RCA
Cao Dinh
Thanh
RAS1012
Characterizing and Optimizing
Process Dynamics in Complex
Industrial Systems Using
Radiotracer and Sealed Source
Techniques 2012 291,348.00 RCA
Nguyen Huu
Quang
RAS1013
Supporting Advanced Non-
Destructive Examination for
Enhanced Industrial Safety,
Product Quality and Productivity 2012 195,000.00 RCA Vu Tien Ha
RAS1014
Supporting Radiation Processing
for the Development of Advanced
Grafted Materials for Industrial
Applications and Environmental
Preservation 2012 262,500.00 RCA Doan Binh
RAS1019
Enhancing Safety and Utilization
of Research Reactors 2012 FA Non-RCA Luong Ba Vien
RAS5055
Improving Soil Fertility, Land
Productivity and Land
Degradation Mitigation 2012 390,211.00 RCA Phan Son Hai
RAS5056
Supporting Mutation Breeding
Approaches to Develop New Crop
Varieties Adaptable to Climate
Change 2012 354,000.00 RCA
Le Quang
Luan
RAS5057
Implementing Best Practices of
Food Irradiation for Sanitary and
Phytosanitary Purposes 2012 268,500.03 RCA
Tran Minh
Quynh
RAS6070
Supporting Quality Assurance
Team for Radiation Oncology
(QUATRO) Training 2012 181,248.01 Non-RCA
Tran Ngoc
Toan
VINATOM-AR 13
The Annual Report for 2013, VINATOM
346
RAS7021
Marine benchmark study on the
possible impact of the Fukushima
radioactive releases in the Asia-
Pacific Region 2011 763,710.11 RCA Le Nhu Sieu
RAS7022
Applying Isotope Techniques to
Investigate Groundwater
Dynamics and Recharge Rate for
Sustainable Groundwater
Resource Management 2012 236,760.01 RCA
Nguyen Kien
Chinh
RAS7023
Supporting Sustainable Air
Pollution Monitoring Using
Nuclear Analytical Technology 2012 337,388.00 RCA
Vuong Thu
Bac
RAS7024
Supporting Nuclear and Isotopic
Techniques to Assess Climate
Change for Sustainable Marine
Ecosystem Management 2012 240,751.00 RCA
Trinh Van
Giap
RAS8109
Supporting Radiation Processing
of Polymeric Materials for
Agricultural Applications and
Environmental Remediation
(RCA) 2009 410,582.83 RCA Doan Binh
RAS9064
Strengthening the Transfer of
Experience Related to
Occupational Radiation Protection
in the Nuclear Industry and Other
Applications Involving Ionizing
Radiation 2012 119,743.35 Non-RCA Vu Manh Khoi
RAS9065
Strengthening Radiation
Protection of Patients in Medical
Exposure 2012 191,848.96 Non-RCA Ng Huu Quyet
RAS9068
Strengthening and Harmonizing
National Capabilities for
Response to Nuclear and
Radiological Emergencies 2012 236,032.48 Non-RCA
Le Ngoc
Thiem
RAS9071
Establishing a Radioactive Waste
Management Infrastructure 2012 506,948.02 Non-RCA
Nguyen Ba
Tien
VINATOM-AR 13
The Annual Report for 2013, VINATOM
347
2.4 LIST OF RESEARCH CONTRACTS 2013
(Implemented by VINATOM and Vietnam other organizations)
No CRP
Code Title Programme Start Date
Expected
End Date Closing date
1 D12011 Integrated Isotopic
Approaches for an
Area-wide Precision
Conservation to
Control the Impacts of
Agricultural Practices
on Land Degradation
and Soil Erosion
Food and
Agriculture
2008-12-08 2013-12-07
2 E13031 Role of Nuclear
Cardiology
Techniques in
Ischemia Assessment
with Exercise Imaging
in Asymptomatic
Diabetes
Human Health 2006-03-15 2012-12-31
3 E13037 The Use of Sentinel
Lymph Node in
Breast, Melanoma,
Head & Neck and
Pelvic Cancers
Human Health 2010-10-12 2013-12-31
4 F22046 Development of
Radiation-Processed
Products of Natural
Polymers for
Application in
Agriculture,
Healthcare, Industry
and Environment
Radioisotope
Production and
Radiation
Technology
2007-12-01 2012-12-31
5 F33017 Use of Environmental
Isotope Tracer
Techniques to Improve
Basin-scale Recharge
Estimation
Water
Resources
2009-03-26 2013-03-26
6 I11008 Financing Nuclear
Investments
Capacity
Building and
Nuclear
Knowledge
Maintenance
for Sustainable
Energy
Development
2013-09-05 2016-09-05
VINATOM-AR 13
The Annual Report for 2013, VINATOM
348
7 F31004 Stable Isotopes in
Precipitation and
Paleoclimatic Archives
in Tropical Areas to
Improve Regional
Hydrological and
Climatic Impact
Models
Water
Resources
2013-07-04 2016-07-03
8 F22060 Radiometric Methods
for Measuring and
Modelling Multiphase
Systems Towards
Process Management
Radioisotope
Production and
Radiation
Technology
2012-07-09 2016-07-09
9 F22051 Radiation Curing of
Composites for
Enhancing their
Features and Utility in
Health Care and
Industry
Radioisotope
Production and
Radiation
Technology
2011-03-14 2015-03-14
10 F12024 Utilisation of
Accelerator-Based
Real-time Methods in
the Investigation of
Materials with High
Technological
Importance
Nuclear
Science
2012-03-28 2016-03-28
11 E43023 Stable Isotope
Techniques in the
Development and
Monitoring of
Nutritional
Interventions for
Infants and Children
with Malaria, TB and
other Infectious
Diseases
Human Health 2009-09-08 2014-02-28
12 E35008 Strengthening of
“Biological dosimetry”
in IAEA Member
States: Improvement
of current techniques
and intensification of
collaboration and
networking among the
different institutes.
Human Health 2012-02-10 2016-02-09
13 E13041 Nuclear Cardiology in
Congestive Heart
Failure Value of
intraventricular
synchronism
assessment by gated-
Human Health 2013-09-13 2016-09-13
VINATOM-AR 13
The Annual Report for 2013, VINATOM
349
SPECT myocardial
perfusion imaging in
the management of
heart failure patients
submitted to cardiac
resynchronization
therapy (IAEA-
VISION CRT)
14 D62008 Development of
Generic Irradiation
Doses for Quarantine
Treatments
Food and
Agriculture
2009-06-11 2014-06-11
15 D24012 Enhancing the
Efficiency of Induced
Mutagenesis through
an Integrated
Biotechnology
Pipeline
Food and
Agriculture
2009-02-04 2014-05-20
16 D15013 Approaches to
Improvement of Crop
Genotypes with High
Water and Nutrient use
Efficiency for Water
Scarce Environments
Food and
Agriculture
2011-11-01 2015-11-01
17 D12013 Landscape Salinity
and Water
Management for
Improving
Agricultural
Productivity
Food and
Agriculture
2013-06-04 2018-06-03
VIETNAM ATOMIC ENERGY INSTITUTE
THE ANNUAL REPORT FOR 2013
Responsible for publishing
Publishing editor
Cover designer
: Pham Ngoc Khoi
: Nguyen Quynh Anh
: Nguyen Hoang Anh
SCIENCE AND TECHNICS PUBLISHING HOUSE
70 Tran Hung Dao, Hoan Kiem, Ha Noi, Vietnam
Publishing registration No: 2247-2014/CXB/6-134/KHKT.
Publishing decision No: 182/QĐXB-NXBKHKT dated November 11, 2014
Quantity: 100, size: 21x29.5 cm.
Printed at: Truong Xuan Commercial and Printing Joint Stock Company.
Printing finished and copyright deposited in the 4th
quarter of 2014.
VIỆN NĂNG LƯỢNG NGUYÊN TỬ VIỆT NAM
The ANNUAL REPORT for 2013
Ban biên tập:
TS. Trần Chí Thành, Tổng biên tập
TS. Cao Đình Thanh, Phó tổng biên tập
KS. Nguyễn Hoàng Anh, Ủy viên, Thư ký Ban biên tập
TS. Nguyễn Thị Kim Dung, Ủy viên
ThS. Nguyễn Thị Định, Ủy viên
CN. Nguyễn Thị Phương Lan, Ủy viên.