Role of minor actinides minimization approaches in ... · PDF file1 WATEC Jun 2005 Nawada 1 International Atomic Energy Agency Role of minor actinides minimization approaches in addressing

1

WATEC Jun 2005Nawada

1 International Atomic Energy Agency

Role of minor actinides minimization approaches in addressing eco-friendly

advanced nuclear fuel cycles

H.P. Nawada

Nuclear Fuel Cycle and Materials Section,Division of Nuclear Fuel cycle and Waste Technology

Department of Nuclear Energy



Outline of the presentationOutline of the presentation• Advanced fuel cycles – Partitioning &

Transmutation - MA (MA: Np, Am & Cm) approaches / technologies

• Fuel cycle approach- LMFRFC• Role of Pyro-chemical processes in AFC • Link between process losses and environmental

impact• MA-Fuel / databank

• Fuel cycle approaches o Inert Matrix Fuel, coated particleo Thorium fuel cycle

• Concluding RemarksPu, MA

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Cumulative Spent Fuel Arisings, Storage and Reprocessing, 1990-2020.

0

50100

150

200

250300

350

400450

500

1990 1995 2000 2005 2010 2015 2020

Year

1000 t

on

nes H

M

300

320

340

360

380

400

420

440

GW

e

SF Dis chargedSF StoredSF ReprocessedNuc. P ower

¤¤ Plutonium in spent fuel, presently about 1500 tonne, will increPlutonium in spent fuel, presently about 1500 tonne, will increase over 2500 ase over 2500 tonne in 2050. Separated tonne in 2050. Separated PuPu is increasing steadily.is increasing steadily.

¤¤ MA is about 150 tonnes in spent fuel, and about 35 tonnes in HLWMA is about 150 tonnes in spent fuel, and about 35 tonnes in HLW. In the MAs, . In the MAs, AmAm--241 and 241 and NpNp--237 are predominant237 are predominant..



Advanced Fuel cycleFuel Cycle that incorporate Partitioning and Transmutation to burn transuranic elements is called Advanced Fuel Cycle

• Reduction of long-term radio-toxicity• Determination of a period to terminate the

disposal site (From over million years toless than ≈500-700 years)

• Reduction of repository space requirements• Increased resource utilization • Reduce Proliferation concern• Incorporation of Scientific & technical

innovations

1. Separation of TRUs and LLFPs 2. Fabrication of TRU-rich fuel and

targets3. Transmutation in Thermal &/or Fast

reactors or ADS

CEA Program on Partitioning & Transmutation, D. Warin and H. Safa, International Meeting on Accelerator Driven Transmutation System Technologies, University of Nevada, Las Vegas, April 29, 2003

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Advanced Fuel Cycle consistsa) Reprocessing of LWR-UO2 fuelb) Separation of minor actinides from HLLW resulting

from LWR-UO2 reprocessingc) Fabrication of MA targets for heterogeneous irradiation in LWRsd) Quantitative recycling of U and Pu into LWR-Mixed Oxide (MOX) fuele) Reprocessing of spent LWR-MOX fuel in adequate

facilities (higher Pu inventory)f) Separation of MAs from HLLW & conditioning of individual elements MAsg) Fabrication of FR -fuel (MOX, -metal or -nitride) with limited MA contenth) Irradiation in FRs or dedicated hybrid facilities to very high burnupi) Reprocessing of spent FR-fuel in specially (aqueous and non-aqueous)j) Quantitative separation of all TRUs from the spent FR

fuel processing during multiple recyclingk) Multiple recycling of FR-MOX fuel (and /or ADS) with major TRU

content until significant depletionl) Separation of certain fission products with long half-lives if required

for the disposal step Source: P&T as a Waste Management Option in a Future Nuclear Era, L.H. Baestslé, in Proc. Workshop on Hybrid Nuclear Systems for Energy Production, Utilisation of Actinides & Transmutation of Long-lived Radioactive Waste, IAEA, Sep 3-7, 2001, ICTP, Trieste, Italy, and IAEA, Vienna, Austria, 2001, IAEA/SMR/1326-3



IAEA coIAEA co--operations in AFC activitiesoperations in AFC activities

Evaluation of actinide Partitioning and Transmutation (1982)Feasibility of separation of noble metals from HLLW (1989)Use of fast reactors for actinide transmutation (1993)Review of nuclear data for ADS related R&D (1998) Utilization of thorium based fuel-cycle for ADS (1998)Non-proliferation and environmental aspects of P&T (2001)Implication of Partitioning and Transmutation in radioactive waste management (2004)Study of process-losses in separation processes in P&T systems in view of minimizing long term environmental impacts(Initiated in 2003)

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Source: Accelerator-driven Systems (ADS) and Fast Reactors (FR) in Advanced Nuclear Fuel Cycles, A Comparative Study,(2002) NUCLEAR ENERGY AGENCY ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT

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TRU- FR burner, multiple recycling fuel cycle scenario

Hydro-metallurgical

PUREX

Hydro-metallurgical

PUREX

Direct oxide

reduction

Direct Direct oxide oxide

reductionreduction

TRU-burning Fast ReactorTRU-burning Fast Reactor

ReprocessedUranium

ReprocessedUranium

Spent fuel

For Waste disposalFor Waste disposal

Pu

FP & U with little

TRU

Electro-refining process

Electro-refining process

TRU

LWRsLWRs

HLLWPyro-

chemical recovery

PyroPyro--chemical chemical recoveryrecovery

Pu

Molten-Salt Extraction

Molten-Salt Extraction

Fresh Fresh UraniumUranium

Spent fuelTRU fuel

TRU

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.

.



USA, Russia, Japan, EU

USA, Russia, Japan, EU

Japan, RussiaUSA, EURussia, Japan, EU

USA, Japan, EU, Korea, India

4. Some of the interested Member States

Laboratory Laboratory Laboratory Laboratory Semi plantSemi-plant3. Scale

High MA loadingDifferent stepsSingle step Fuel fabrication

2. MA loading

Plasma process Li reduction

Link from aqueous methods

Actinide nitrideADS targets & TRISO fuel

Mixed actinide oxides

Zr-based actinide alloys

1. Fuel form

Novel and auxiliary methods

Pyro for HLLW Nitride electro-refining

Chloride / fluoride volatility

Oxide Electro-winning

Metal Electro-refining

Review of pyro-chemical methods

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Review of other aqueous partitioning methods• DIAMEX process to extract Am+Cm • SESAME process for Am/Cm separation• NEXT process for co-recovery of actinides which includes uranium

crystallization step• GANEX Process (Actinide Group Separation method)• UREX process

Fuelrecycling

Solventrecycling

Organicsolvent

F.P.Specific Ancomplexant

HNO3

Fuel

An

LnDiluteacid

Dissolution Crystallization U

U, Pu, M.A.F.P.

(80 %)

Co-Co- Lnstripping

Lnstripping

Anstripping

Anstripping

Anstripping

Fuelrecycling

Solventrecycling

Organicsolvent

F.P.Specific Ancomplexant

HNO3

Fuel

An

Ln Diluteacid

Dissolution U pre-extraction

U

U, Pu, M.A.F.P.

(80 %)

Co-Co-extractionCo-extraction Lnstripping

Lnstripping

Anstripping

Anstripping

Anstripping

Anstripping

The GANEX concept : Group ActiNides EXtraction

Co-recovery of Actinides



HighSingle elements (U, Pu, Np, Am,

Cm)

Continuous

High

Established

Mixture of TRU- Low

Batch

Low

To be established

Product Purity

Process

Throughput

Process losses

Wet processPyro-chemical process

Combination of Pyro-chemical and Wet process

Steps to achieve synergetic combination of both processes

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IMPA

CTRepository

Relation between Process Losses in Nuclear Relation between Process Losses in Nuclear Fuel cycle and Fuel cycle and Environmental ImpactEnvironmental Impact

M

Nuclear fuelmaterial

Fuel cycle

Environment

wasteSeparationProcess

ProcessLosses

ReactorSolidificationMatrix

Fuel Fabrication

Spent fuel storage

?



.

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Target Values for Target Values for AnAn--Losses to Achieve a Transmutation Rate of about 100Losses to Achieve a Transmutation Rate of about 100

Partitioningand

Fuel Make UpAn input fresh An

fuel

head end losses hulls

shearingresidues

unusuable equipmentcruciblesvessels

molds etc.

- discarded An bearing waste

- recycling of reagents- fission products- degraded chemicals

etc.

100% ≥ 99.5%

≤ X %

≤ Y %≤ Z %



Coordinated Research Project (CRP)Coordinated Research Project (CRP)“Study of Process Losses in Separation Processes in Partitionin“Study of Process Losses in Separation Processes in Partitioning g

and Transmutation (P&T) Systems in view of Minimizing Long Term and Transmutation (P&T) Systems in view of Minimizing Long Term Environmental Impacts”Environmental Impacts”

• 1st Scope Definition Meeting - Oct. 2002, Vienna

• China, Czech Republic, Germany, India, Japan, Republic of Korea,Russian Federation and USA

• 1st Research Coordination Research Meeting -Dec 2003, Vienna

• 2nd Research Coordination Research Meeting - Dec 2004, Czech Republic

• 3rd Research Coordination Research Meeting – Spring 2006, China

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Understanding of losses

Advanced characterization methods for actinides

Separation criteria to minimize environmental impact

List of critical radio-nuclidesDefining environmental impact associated with partitioning and transmutation processesDefining proliferation resistance attributes

CRP Objectives



Minor actinide fuel / target will be the critical link between partitioning and

transmutation

Working Group on Process and property of minor actinide compounds and alloys for nuclear

fuel and target for incineration in thermal and fast neutron spectra

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Issues in MAIssues in MA--based fuel developmentbased fuel development

• MA-based fuel must be fabricableusing remote processes inshildedcells

• The fuel must be compatible with the fuel recycle process

• The fuel form must provide robust containment for fission products

• The technologies of minor actinide-bearing-fuel materials are not well established (although, for dilute minor actinide contents, the properties should not differ substantially from the base U-Pu-

bearing materials).

Americium trapping system for recover and reuse.Alternatively powder metallurgical method viz., mixing, pellet making & sintering

Americium vaporization

Injection-casting of alloy fuels

Metal-alloy

Use of SOL-GEL with direct compact could reduce number of steps

Need for very high temperature and very high affinity of Zr for oxygen

Powder metallurgy by nitration + carbothermicreduction

Nitride

SOL-GEL coprecipitation of TRUs from nitrate solutionAlternative fuel forms such as Vibro-pac

Not easily adaptable to remote handling

Powder metallurgy of pellet fuelOxide



• Minor Actinide Property Database (MADB) Under Preparation

• Bibliographic database on thermodynamic and thermophysical properties of minor actinide (Np, Am, Cm) metals, alloys and compounds

• Access on the internet with some search and filter capabilities (www-nfcis.iaea.org)

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Technical Meeting on

“Current Status and Future Prospects of

Liquid Metal Cooled Reactor Fuel Cycle and Fuels”

(TM-LMFR-2005)

3-7 Oct 2005*at

Central Institute of Improvement of Qualification (TSIPK), Obninsk, Russian Federation

with cooperation fromInstitute of Physics and Power Engineering (IPPE)

Obninsk, Russian Federation

For details: http://www.iaea.org/OurWork/ST/NE/NEFW/nfcms_home.html

* Subject to clearances and approvals



.

Inert Matrix Fuel Fabrication

+ MAs

Objectives of Inert Matrix Fuel (IMF)• Minimizing “proliferation risk” of plutonium by the use of fertile-

free fuel • Minimizing “Minor Actinides” and in turn radiotoxicity in waste

IMF in existing Nuclear Power Plants

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Technical Document on

Viability of Using Inert Matrix Fuel in Reducing Plutonium in Reactors

1. Overview:

2. Potential IMF application; environmental, fuel cycle aspects, economic, non-proliferation aspects, historical before 80’s, current programs

3. R&D activities for IMF qualification

4. Country Specific programs

5. International programs: Irradiations

6. Outlook and Results



Examples of Inert MatrixExamples of Inert Matrix

YyZr1-yO2-y/2, Mg(1-x)Al(2+x)O(4-x)Oxide solid solutionMgAl2O4, Y3Al5O12, ZrSiO4Ternary oxide

MgO, Y2O3, ZrO2, CeO2Binary oxideAlN, TiN, ZrN, CeN,Nitrides

SiC, TiC, ZrCCarbide

Stainless steel, zirconium alloysAlloyAlSi, AlZr, ZrSiInter-metallics

C, Mg, Al, Si, Cr,V, Zr, Mo, WElementInert Matrix formulaInert Matrix type

PuAl4*-AlMetmet

Zr - YyPuxZr1-y-xO2-y/2*Cermet

MgAl2O4 - YyPuxZr1-yO2-y/2*CercerAnzYyPuxZr1-yO2-ψ*Solid solution

CompositionDesign

Examples of Inert Matrix designExamples of Inert Matrix design

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Role of coated particle fuel in realizing Actinide burner Fuel Cycles

•By using a combination of LWRs, HTRs and GCFRs

‡The waste radio-toxicity can be reduced by recycling of both Pu and the MA through symbiotic fuel cycles

Mine LWRU

HTRFg-Pu

MOX

LWR

Sg-Pu

Pu + MAGCFR Waste

Pu, MA



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There were 27 technical presentations from 37 Participants from 17 Member States, EC and 3 IAEA ExpertsTechnical programme: 1.) Countries Overview 2.) Coated Particle Fuel modelling 3.) Coated Particle Fuel Performance and technology and 4.) Novel ideas and application related to Coated Particle FuelPanel Discussion: 1.) Requirements regarding Coated Particle Fuel characteristics for Hydrogen Generation 2.) Desirability of creating a central data-book for coated particle fuel data by the Agency and 3.) Measures for improving international cooperation in Coated Particle Fuel development

Technical meeting onCurrent status and future prospects of Gas-Cooled Reactor fuels

(Jun 2004)



Pu burning with Th in a PWR is more proliferation resistant than with uranium

Proliferation risk of Pu/Th and 233U/Th in FNR and ADS is due to 233U, which is protected by gamma emission from 232 U.

U/Pu MOX (~13% Pu) Th/Pu MOX (~15% Pu)

Pu incineration rate with a burnupof 60 MWd/kgHM

231 kg Pu/GWth.y 395 kg Pu/GWth.y

233U generation rate with a burnupof 60 MWd/kgHM

~0 105 kg 233U/GWth.y

Net fissile material incineration rate 231 kg Pu/GWth.y 290 kg/GWth.y

Thorium fuel cycleThorium fuel cycle

Relative production of minor actinides in diverse cycles

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Technical document on Thorium fuel cycle options:

Potential benefits and challenges

• RATIONALE FOR THORIUM-BASED FUEL CYCLES• IMPLEMENTATION SCENARIOS AND OPTIONS • CURRENT INFORMATION BASE • FRONT-END ISSUES AND CHALLENGES • BACK-END ISSUES AND CHALLENGES• PROLIFERATION RESISTANCE • ECONOMIC ISSUES



• Development of transuranic-based fuel and fuel cycles• Reprocessing of such fuels, in combination with the immobilization of separated

non-reusable radiotoxic nuclides and noble metals for ultimate disposal• Suitable matrixes for 14C and 15N should be developed for the realization of

advanced fuels such as coated particle or nitride fuel etc.,• Methods to recycle and reuse fission products should be addressed • To increase the capacity of repository by separating the heat producing radio-

nuclides and prepare these for cooling storage • Operational exposure: minimize workers’ exposure-limits for such fuel

fabrication and spent fuel treatment.

Some Potential Challenges in Addressing Environmentally Benign Some Potential Challenges in Addressing Environmentally Benign Advanced Fuel CyclesAdvanced Fuel Cycles

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Conclusions

• Identification of sources of loss (e.g. of long living radiotoxic waste)• Understanding of chemical processes (e.g. of actinides)• Understanding of the physical processes (e.g. actinides and FP taking part in volatilization,

precipitation, etc.,)• Adaptation of the processes to suppress losses

• Development of advanced characterization methods for P&T;• Group separation of all Actinides• Integration of treatment and re-fabrication processes and technologies• Innovative fuel cycles such as thorium fuel cycle • Establishing a knowledge database for development of partitioning and transmutation

technology matured towards environment friendly fuel cycles. • Development of Regional and International approach



Thank you for your kind attention

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Provisional programme

• Role of LMFRs in sustainable nuclear energy development • General LMFRs developments / new concepts • Current status of LMFR fuel cycles • Economics of LMFBR fuel cycles and its comparison with the other fast reactor fuel

cycles • Current status of liquid metal-cooled reactors fuels • Advanced fuel fabrication, design including conventional one/new concepts • Development of fuel fabrication technology including QA and QC • Irradiation testing, fuel performance in normal and transient conditions and fuel

modelling • Existing and planned facilities and experimental programs • Advances in materials development for fuel cycle application • Trends in innovative fuel cycle concepts including partitioning and transmutation

pertinent to LMFR fuel cycle development specially encompassing the subject areas: o Theory, Design, Development, irradiation testing and performance o Status and innovations in partitioning as well as transmutation methods Waste

reduction, proliferation-resistance and environmental improvement through LMFR fuel cycles

o Challenges and R&D needs in LMFR fuel cycle o Cross-cutting and infrastructure issues

• Knowledge conservation on LMR fuel cycle • Prospects for international collaboration and co-ordination of R&D activities • IAEA’s role in meeting the needs for information exchange and collaborative R&D.



Plutonium inventory as a function of Plutonium inventory as a function of IMF irradiation time in PWRIMF irradiation time in PWR

0 200 400 600 800 1000 1200 14000

10

20

30

40

50

60

70

80

90

100

0

10

20

30

40

50

60

70

80

90

100

Pu-240 + 242

Pu-239 + 241

Standard MOX

Uranium free matrix

Plut

oniu

m in

vent

ory

[%, o

f ini

tial l

oadi

ng]

Full power days

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[1] PLUTONIUM AND MINOR ACTINIDE DESTRUCTION IN (PLUTONIUM/ACTINIDE)–SiC BUNDLES for 229 MW·d.

Civilian (plutonium/actinide)–SiC fuel content Isotope Fresh

(g/bundle)Discharge(g/bundle)

Destruction(%)

238Pu 5.9 5.5 6.8239Pu 205.0 6.2 97.0240Pu 95.6 57.5 39.9241Pu 31.0 15.8 49.0242Pu 18.5 41.5 -

Total Pu 356.0 126.5 64.5

237Np 29.96 14.76 49.3241Am 30.73 3.69 88.0243Am 5.30 9.94 -242Cm - 8.58 -244Cm - 3.96 -

Total MA 65.99 40.93 38.0

Documents

Role of minor actinides minimization approaches in ... · PDF file1 WATEC Jun 2005 Nawada 1 International Atomic Energy Agency Role of minor actinides minimization approaches in addressing