JAEA-ISCN Development Programs of Advanced NDA Technologies of Nuclear Material

October 24, 2014

Michio Seya, Naoki Kobayashi, Yosuke NaoiRyoichi Hajima, Kazuhiko Soyama,

Masatoshi Kureta, Hironobu Nakamura, Hideo Harada

Japan Atomic Energy Agency

Introduction

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Diagram for JAEA-ISCN Development Programs of Advanced NDA Technologies of NM

MEXTMinistry of Education, Culture,

Sports, Science and Technology

ISCN

QuBS

R&D: （A）NRF NDA Technology using LCS

Gamma-rays (Intense Mono-energetic Gamma-rays)

NSEC/J-PARC/TRP

R&D: （B）Alternative to 3He Neutron Detection Technology, using

ZnS/B2O3 Ceramic Scintillator

NSEC

R&D: （C）NRD using NRTA and NRCA

JAEA

ISCN: Integrated Support Center for Nuclear Nonproliferation and Nuclear Security

QuBS: Quantum Beam Science Research Center

J-PARC:Japan Proton Accelerator Research Complex

NSEC: Nuclear Science and EngineeringResearch Center

TRP: Tokai Reprocessing Plant

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JAEA-ISCN Development Programs of Advanced NDA Technologies of Nuclear Material

R&&&&D

Order

of

Pres.

Development Programs

（A） 2NRF NDA Technology using LCS Gamma-rays (Intense Mono-energetic Gamma-rays)

（B） 3Alternative to 3He Neutron Detection Technology, using ZnS/B2O3 Ceramic Scintillator

（C） 1 NRD using NRTA and NRCA

1. NRD using NRTA and NRCA(JAEA/JRC-IRMM Collaboration)

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NRD: Neutron Resonance Densitometry

What is NRD?What can be quantified by NRD?

NRD

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NRD: A NDA method to quantify the amount of special nuclear materials(U/Pu) (each of U/Pu isotopes)in sampleswith unknown elemental and isotopic composition, (such as melted fuel debris generated in severe

accidents of nuclear reactors)

NRD : A non-destructive mass spectrometry method

NRD: Neutron Resonance Densitometry

NRCA（（（（NRCA: Neutron Resonance Capture Analysis））））

Quantification of (U/Pu) Isotopes by Analyzing Transmitted Neutrons

with Information of Resonance

Absorptions by Isotopes

NRTA（（（（NRTA: Neutron Resonance Transmission Analysis））））

Concept of NRD

Pulsed Neutron Beams

Measurement Object(NM in thin disk-type

container)

Transmitted Neutrons

Neutron

Detector

Pulsed Neutron Beams

Measurement Object

Gamma-ray emitted from Neutron

Absorption Reaction of Isotopes

mixed with NM

Gamma-ray

Detector

Quantification of Mixed-in Isotopes by Analyzing Emitted Gamma-rays

from Neutron Absorption Reactions（Analysis of NRTA is corrected with

the amount of neutron absorbers.）

NRD

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Areal Isotope Densities(Amount of Isotopes) Fixed by NRTA

NRD

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Measurement Object of NRTANRD

Incident neutron beam

Transmitted neutrons

A thin(~2㎝㎝㎝㎝) disk-type containerwith particle-like melted fuel debris

Particle-like melted fuel debris in a thin (~2㎝㎝㎝㎝) disk-type container

Measurement of NRTA9

Achievable Statistical Uncertainty of NRTA

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Pu238 Pu239 Pu240 Pu241 Pu242 U235 U238

Sta

tist

ical

Un

cert

ain

ty o

f Is

oto

pe

Den

sity

(%

)

0.0

0.2

0.4

0.6

0.8

1.0

Measurement period of 20 min

Neutron source intensity of 1012 n/sec

< 1% for each Pu and U isotopes

NRD

Measurement Object: Spent nuclear fuel (40GWd/t), 56Fe (9 wt%),natB (2.5 wt%)

（Diameter （Φ）：30 cm, Thickness （t） = 1 cm, Weight ~4 kg）

Influence of Thickness and Particle Size on Accuracy of NRTA

NRD

Zero Approximation

Uniform Density Plate

First Approximation

Inhomogeneous Density Parts

（（（（Thickness Effect））））（（（（Particle Size Effect））））

Material density distribution seen from

incident neutrons

A thin(~2㎝㎝㎝㎝) disk-typecontainer with

particle-like MFD

Effects of these factors on precision of NRTA is about 2% in the case of thickness is less than 2㎝㎝㎝㎝.

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NRD

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Uncertainty of Total Pu with10B Concentration and Thickness

Uncertainty of NRD for total Pu with 10% 10B concentration and 2cm thickness Is about 1% .

The quantity of the containing isotopes is determined from a obtained gamma-ray spectrum.

NRCA (PGA) for Quantification of Impurities

Pulsed Neutron Beams

Measurement Object

Gamma-ray emitted from

Neutron Absorption Reaction

of Isotopes mixed with NM Gamma-ray Detector

NRD

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Nucleus ReactionEnergy of

Prompt γ ray1st Neutron Resonance

Capture,

(n,a)1H 1H(n, g)2H 2223 keV ― 0.332 b

10B 10B(n, ag)7Li 478 keV 170 keV (3839 b)

27Al 27Al (n, g) 28Al 7724 keV 6 keV 0.229 b

28Si 28Si (n, g) 29Si 4934 keV 32 keV 0.169 b

56Fe 56Fe (n, g)57Fe 7646 keV 1 keV 2.59 b

53Cr 53Cr (n, g)54Cr 8885 keV 4 keV 18.4 b

58Ni 58Ni (n, g)59Ni 8999 keV 7 keV 4.62 b

1st Neutron Resonance energy >> 50 eV for contaminated isotopes

Prompt g ray energy >> 661 keV of 137Cs except 478 keV by 10B

Containing Isotopes and Prompt Gamma-ray Energies

NRD

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●●●● High energy resolution●●●● High counting rate●●●● High peak-to-Compton ratio

Detector length

0 mm25 mm50 mm80 mm

100 mm127 mm

High S/N ratio !

Sample(Cs-137)

Main LaBr3(Ce) Detector

Back-catcher Detector

Pulsed Neutron Beam

Backscattering Gamma ray

Detector length

LaBr3 spectrometer with Back-catcher

B-10 (478 keV)

Energy spectra of the detector with a Cs-137 source

Concept of Gamma-ray Spectrometer to quantify 10B

NRD

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Estimated Accuracy of NRD(as a result of collaboration studies)

NRD

About 3% for the amount of U/Pu in particle like Melted Fuel debris

Validation of NRD at GELINA

GELINA at JRC-IRMM

NRD

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0.000

0.005

0.010

Texp

Ttheory

238U 238U238U

235U

Tra

nsm

isso

n

235U

0 5 10 15 20 25 30 35 40-4

0

4

Res

idua

l

Neutron energy / eV

Measurement of the CBNM standard 446

Areal density

NRTA Reference (IDMS)

235U (5.063 ± 0.090) x 10

-4 at/b (5.0326 ± 0.0080) x 10

-4 at/b

238U (1.062 ± 0.010) x 10

-2 at/b (1.0628 ± 0.0015) x 10

-2 at/b

Demonstration of NRD at GELINA

new experimental target hut at 13 m

GELINA at JRC-IRMM

(Demonstration experiments; in the beginning of March 2015 at GELINA)

With Mini Workshop on NRD and active neutron NDA

target (sample)

LaBr3 scintillation detector (JAEA)

NRD

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� Neutron Time-of-Flight (TOF) FacilityInstitute for Reference Materials and Measurements @ Belgium

electron LINAC (aver. 100 MeV)

neutron source

U (target) + water (moderator)

# of neutrons @source

3 x 1013 n/s

neutron TOF technique

- neutron TOF � neutron energy

GELINA （（（（JRC-IRMM））））

ELECTRON LINAC

TARGET HALL

FLIGHT PATHS (SOUTH)

FLIGHT PATHS (NORTH)

NRD

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Mini-Workshop (Tentative) Title: Demonstrations of NRD / Active Neutron NDA Technologies

for Nuclear Material using Pulsed Neutron Beam

Date ： 4 and 5 -March-2015Place： JRC-IRMM (Geel, Belgium)

Agenda (Draft)

Day 1 (PM1:00-PM5:00) Day 2 (AM9:00-PM3:00)

(AM) (AM)4. Demonstration of NRD（Part II）

Stop measurements / Showing the analysis5. Session (2)

NRD and active neutron NDA technologies

(Lunch)

(PM)1. Opening Remarks of the Workshop (JRC / JAEA)2. Introduction of NRD (JRC / JAEA)3. Demonstration of NRD（Part I）

Selection of samples to be measured by NRDStarting of measurement

4. Session (1) NRTA and NRCA(PGA)

(PM)6. Discussion on future prospective of active

neutron NDA7. Closing Remarks

Demonstration / Mini-Workshop(Tentative)

NRD

JAEA/JRC-IRMM welcome your participation. 20

Neutron detector for counting transmitted neutrons

NRTA Measurement container with

particle-like Debris

Gamma-ray detector

Beam dump

Pulsed neutron beams

n ～1012 n/sec

Sample for NRCA

A 30 MeV electron accelerator for pulsed

neutron generation

Target / Moderator

A thin disk-type container for classified particle-like debris for the NRD system

Total Area : 200 m2

1F Machine Room： 15 m × 12 m = 180 m2

2F Control Room： 5 m × 4 m = 20 m2

A Picture of a Practical NRD SystemNRD

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Grinding (Crashing)

Machine

(to be developed)

(Small rock-like debris

into particle-like debris)

a container for classified particle-

like debris

Collection of Particle-like Melted Fuel Debris

Classification of particle-like debris by sizes with sieves

Rock of solidified melted

fuel and fine debris

Particle-like debris will be separated

by particle size in a water.

Small rock-like

debris

Particle-like debris

Debris will be taken

away by breaking,

drilling, cutting etc.

(Just a Possible Idea)

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NRD

Preparation of Precise Measurement of Nuclear Material in Particle-like Debris

A large container for classified

particle-like debris

Thin disk-type containers for classified particle-like

debris for NRTA

Removing of

particle-like debris

Classification of particle-like debris by sizes with sieves

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Making a large batch of

particle-like debris by

mixing

Samples for NRCA to quantify 10B etc.

・

・・

NRD

2. NRF NDA Technology using LCS Gamma-rays (Intense Mono-energetic Gamma-rays)

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ElectronLaser photon

Scattered photon

(X-ray /Gamma-ray)

• Energy depends on energies

of electrons and laser photons.

• Pencil-like beam

• Energy tunable

• Monochromatic X-ray /gamma-ray beam

(dE/E < 1%)

gamma-ray energy (keV)

peak b

rillia

nce (

ph/m

m2/m

rad

2/s/

0.1

%BW

)

0

1e+19

2e+19

3e+19

4e+19

5e+19

1500 1600 1700 1800 1900 2000 2100 2200 2300 2400

εn=0.1mm-mrad

E

dE

Calculated Energy Spectrum

ERL based LCS X-/gamma-ray source has high flux and sharp energy width.

LCS X-ray / Gamma-ray Beamusing ERL （（（（Energy Recovery Linac））））

NRF-NDA

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Electron Gun

Energy Recovery Linac(Super-Conducting Cavity)

(9-cell x 2 cavity)

ExperimentRooms

Laser Enhancement

Cavity

Goals of Basic Technology Demonstration Stage(Electron Beam = 26 MeV, 10 mA)

�LCS Gamma-ray (~ 10keV) Flux ~ 1x1011 ph/s�PE/E < 1%

LCS Gamma -rays

Injector

Demonstration of High Intensity Gamma-rays by an LCS Demo. System

Demonstration in March 2014 at Tsukuba (Japan)

35 MeV electron

s High PowerLaser Oscillator

NRF-NDA

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Next Generation ERL（（（（350 MeV））））

gamma-rays

Laser Enhancement Cavityfor LCS gamma-ray generation

350 MeV electrons

3 loops

A Future LCS Gamma-ray Source with 3-loop ERL

Electron Beam=350 MeV, 10 mALCS Gamma-ray （（（（2-3 MeV））））�Flux ~ 1x1013 ph/s�PE/E < 1%

~ 25 m

High PowerLaser Oscillator

（for Intense Mono-energetic 2-3 MeV Gamma-rays）

NRF-NDA

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LCS Gamma-rays with

Energy 2 - 3 MeV

Next Generation ERL

(350 MeV)

Laser Enhancement Cavity

Cargo

ContainerGamma-ray

Detectors

High Power Laser Oscillator

For detection of NM hidden behind heavy shield in cargo containers

Examples of Possible Applications of NRF NDA System using LCS Gamma-rays （（（（1））））

（Nuclear Security）

Nuclear Material

in Heavy Shield

NRF-NDA

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Examples of Possible Applications of NRF NDA System using LCS Gamma-rays （（（（2））））

（Safeguards: Material Accountancy）

NRF-NDA

Laser Enhancement

Cavity

For precise measurement of NM isotopes in SFA / MFD in a canister

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Transmission NRF Assay of An Isotope （（（（239Pu etc.））））

(For an Example: Assaying 239Pu in Melted Fuel using Witness Plate)

Energy

NRF signal decreases due to

depletion of the gamma-ray

beam.

The amount of decrease of

NRF signal is proportional to

the amount of 239Pu in the

gamma-ray path.

NRF-NDA

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3. Alternative to 3He Neutron DetectionTechnology, using ZnS/B2O3 Ceramic

Scintillator

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ZnS/10B2O3 Ceramic Scintillator Neutron Detector

ZnS/10B2O3 Ceramic Scintillator

Sheet

Signal Processor

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Demonstration Test:

in march 2015

10B2O3/ZnSCeramic Scintillator(Rectangular Area)

An axial sectional view of the designed ASASOverall View

We have been fabricating the alternative HLNCC type NDA system,

ASAS (Alternative Sample Assay System) and preparing a demonstration

test to measure MOX powder or Pu nitrate solution in a sample vial.

Shift Register for IAEA Demonstration (JSR-15)

TTL

ASAS （（（（Alternative INVS））））

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Demonstration （（（（Comparison）））） Test of ASAS with INVS

Demonstration (Comparison) Test: in march 2015

Current INVS ASAS(Alternative INVS)

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Using MOX in TRP

Thank you for your attention.

These R&D programs are sponsored by MEXT (Ministry of Education, Culture, Sports, Science

and Technology) of Japan.

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