Nuclear Data Study for Nuclear Transmutation · 2013-12-10 · Nuclear Data Study for Nuclear...
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Nuclear Data Study for Nuclear Transmutation
Research Laboratory for Nuclear Reactors,Tokyo Institute of Technology
Masayuki IGASHIRA
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Contents
1. Introduction2. Present Status of the Accuracy of
Nuclear Databases for MAs and LLFPs3. Cross Section Measurements for MAs and LLFPs4. A Japanese Nuclear Data Project5. Summary
MAs: Minor Actinides (Np-237, Am-241, Am-242m, Am-243,Cm-244, Cm-245, Cm-246, etc)
LLFPs: Long-Lived Fission Products (Se-79, Zr-93, Tc-99,Pd-107, Sn-126, I-129, Cs-135, etc.)
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1. Introduction
# The current national policy in Japan for the managementand disposal of MAs and LLFPs is a sequence of
vitrification,interim storage, and thendepositing
underground together with other nuclear wastes.# If MAs and LLFPs are extracted and transmuted into stable
nuclides, the environmental loading in the geologicalrepository becomes very small.
# The ethical problem that MAs and LLFPs are undesirableproperty for our far descendants will be solved.
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1. Introduction
# The nuclear transmutation of MAs and LLFPs is a very attractive subject.
--> Neutron capture and/or fission reactions are the mostpromising transmutation reactions.
--> Databases on neutron capture and/or fission reactioncross sections for MAs, LLFPs, and related nuclidesare indispensable for developing the transmutationtechnology.
# The accuracy of nuclear databases for those nuclides isquite poor at the present time.--> The improvement of the database accuracy is
an urgent task.
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2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
Nuclear Databases in the World
JENDL-4.0: Japanese Evaluated Nuclear Data Library
ENDF/B-VII.1: Evaluated Nuclear Data File
JEFF-3.1.1: Joint Evaluated Fission and Fusion Library
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Evaluated Error of JENDL-4.0: 4.8%
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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Evaluated Error of JENDL-4.0: 5.7%
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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Evaluated Error of JENDL-4.0: 5.7%
Measurement at GELINA: ND2013
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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243Am
Evaluated Error: 7.0%
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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Capture cross sections of 99Tc
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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Capture cross sections of 107Pd
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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Capture cross sections of 79Se
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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# Accuracy at the present moment:5% - 100%
# Accuracy needed for the development ofNuclear Transmutation Technology: 3% - 5%
2. Present Status of the Accuracy of Nuclear Databases for MAs and LLFPs
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# Problems in Measurements for MAs and LLFPs
- Isotopic and Chemical Impurities in Samples*(Preparation of High-Purity Sample is essential.)--> Impurity identification is necessary.--> Measurements are required for Impurities.
- Radioactivity of Sample--> Small amount of sample--> Intense and Pulsed Neutron Source
*Samples of MAs and LLFPs are chemically extracted fromspent fuel. No isotopic separation is usually performed.
3. Cross Section Measurementsfor MAs and LLFPs
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3. Cross Section Measurementsfor MAs and LLFPs
- Intense and Pulsed neutron sources:# Electron Linear Accelerators: Photo-Neutron Sources
ORELA, GELINA, KURRI-LINAC, etc. (40 - 200 MeV)0.01 - 0.001 neutron/electron
# Proton Linear Accelerators (+ Synchrotron): SpallationNeutron Sources
LANCE, n_TOF, J-PARC/MLF, etc. (0.8 - 20 GeV)20 - 300 neutrons/proton
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3. Cross Section Measurementsfor MAs and LLFPs
Spallation Neutron Sources
- LANSCE: 0.8 GeV protons + W target (80 KW)LANSCE: Los Alamos Neutron Science Center
Lujan Center
- n_TOF at CERN: 20 GeV + Pb target (9 KW)
- MLF at J-PARC: 3 GeV protons + Hg target (>200 KW)J-PARC: Japan Proton Accelerator Research ComplexMLF: Material and Life Sciences Experimental Facilities
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3. Cross Section Measurementsfor MAs and LLFPs
- LANSCE (Lujan)Capture, Fission and Inelastic Cross Sections,DDX
- n_TOFCapture and Fission Cross Sections
- ANNRI* at J-PARC/MLFCapture Cross Sections of MAs, LLFPs, etc.
# Th, U, Pu and unsealed RI are not usable in MLF* ANNRI: Accurate Neutron-Nucleus Reaction Measurement Instrument
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3. Cross Section Measurementsfor MAs and LLFPs
High Intensity200 kW
80 kW9 kW
K. Kino et al., NIM-A, 626, 58 -66 (2011). 18
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3. Cross Section Measurementsfor MAs and LLFPs
LANSCE(Los Alamos Neutron Science Center), “http://michael.e.gruchalla.org/WebpageImages/Lansce1.jpg”
Lujan Neutron Scattering Center
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3. Cross Section Measurementsfor MAs and LLFPs
LANSCE Activity Report 2010, http://lansce.lanl.gov/news/activityreport/LANSCE%20Activity%20Report%202010.pdf 20
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3. Cross Section Measurementsfor MAs and LLFPs
DANCEDetector for Advanced Capture Experiments
http://lansce.lanl.gov/lujan/instruments/DANCE/pdfs/DANCE.pdf
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3. Cross Section Measurementsfor MAs and LLFPs
EAR-1
EAR-2 under construction
“http://pceet075.cern.ch/ “CERN n_TOF Facility: Performance Report” 22
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3. Cross Section Measurementsfor MAs and LLFPs
TAC: Total AbsorptionCalorimeter
40 BaF2
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3. Cross Section Measurementsfor MAs and LLFPs
ParametersDimensions: 20x20 cm2
Isobutane gas: 7 mbarHigh Voltage: 500-600 VGap between electrodes: 3mmElectrode thickness: 1.5 µm (Mylar+Al)Deposit thickness: 100-300 µg/cm2
Backing thickness: 0.1 µm (Al)1.5 µm (Mylar)
Fission event identification:T1 in coincidence with T2
1 anode: Mylar foil Al-plated2 cathodes with 2mm stripsDelay between strips: 3 ns
Position sensitive 5 channels/detector
Construction by:IN2P3 (IPN Orsay)
Parallel Plate Avalanche Counters PPACs 24
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3. Cross Section Measurementsfor MAs and LLFPs
Nuclear and Particle PhysicsExperimental FacilityMaterials and Life Science
Experimental Facility
Linac(350m) 3 GeV Synchrotron(25 Hz, 1MW)
50 GeV Synchrotron(0.75 MW)
NuclearTransmutation
Neutrinos to SK
J-PARC 25
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Building dimension :Width : 70m Length : 146mHeight : 30mExp. Hall Height : 22m
Target remote handling room
Cooling systems(Basement)
23 neutron beam lines will be Installed in experimental halls under present design.
3. Cross Section Measurementsfor MAs and LLFPs
MLF26
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3. Cross Section Measurementsfor MAs and LLFPs
ANNRI (July, 2009)27
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3. Cross Section Measurementsfor MAs and LLFPs
ANNRI 28
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Large Ge detector array– Two cluster Ge detectors: 7 crystals for each– Eight coaxial Ge detectors– BGO anti-Compton detectors
Shielding– Borated rubber sheet– 6LiH– Lead shields
Data acquisition system– Digital data processing– Pulse height and
TOF are recordedsequentially
– Time resolution= 10 nsec
Ge
Lead shield
3. Cross Section Measurementsfor MAs and LLFPs
4π Ge Spectrometer 29
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Use for:– Complementary use to Ge array– Measurement in the high energy
range Detectors
– 90°detector: 13” diam. × 8” long– 125°detector: 8” diam. × 8” long
Shielding– Borated polyethylene, Pb, 6LiH, Cd
Data acquisition– Multi-stop time digitizer– TOF, pulse height, pulse width are
recorded sequentially
3. Cross Section Measurementsfor MAs and LLFPs
NaI(Tl) Spectrometer 30
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# Title of ProjectSystematic Study on Neutron Capture Reaction CrossSections for the Technological Development of NuclearTransmutation of Long-Lived Nuclear Wastes
# Objective of ProjectTo contribute to the improvement of nuclear databaseaccuracy, by making the precise measurements ofcapture cross sections of Long-Lived Nuclear Wastes(LLNW), analyzing the measured results theoretically,elucidating the capture reaction mechanism of LLNW,and supplying reliable calculated capture cross sectionsfor all LLNW and in the whole neutron energy region.
# Term of ProjectFrom June, 2010 to March, 2015
4. A Japanese Nuclear Data Project
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4. A Japanese Nuclear Data Project
Project Representative
Measurement @ J-PARC/MLF/ANNRI
Measurement @Tokyo Tech
Measurement @Kyoto U
TheoreticalAnalysis
Improvement ofNeutron Beam
Measurementusing NaI(Tl)
Measurementusing Ge Array
Structure of Project
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Radioactive samples of MAs and LLFPs were prepared.
All samples are sealed in Al or Ti containers.
Half Life DecayMode
Activity(Bq)
Net Weight(mg)
Np-237 2.1 ×106 y α 26M5.2M1M
100020038
Am-241 4.3 ×102 y α 0.95G 7.5
Am-243 7.4 ×103 y α 0.95G 128
Cm-244 1.8 ×10 y α 1.8G×6 0.6×6
Cm-246 4.4 ×103 y α 1.8G×4 1.1×4
Half Life DecayMode
Activity(Bq)
Net Weight(mg)
Zr-93 1.5 ×106 y β− 47M 472
Tc-99 2.1 ×105 y β− 50M 78
Pd-107 6.5 ×106 y β− 380k 20
I-129 1.6 ×103 y β− 3M 404
MA
LLFP
Radioactive Samples
4. A Japanese Nuclear Data Project
Samples of important stableisotopes were also prepared.
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Experiments of 244,246Cm- Samples and Measurement Conditions -
Samples:Cm-244 (T1/2=18.1y: MA)
Net weight = 0.6 mgActivity = 1.8 GBqMeasurement Periods: 64 hours
Cm-246 (T1/2=4753y: MA)Net weight = 2.1 mgActivity = 12.1 MBq (244Cm: 1.7GBq)Measurement Periods: 94 hours
Both of the samplesChemical form = CmO2Container = Al capsule
Outside9mmΦ 1.5mmt
Inside5mmΦ 0.5mmt
For the background estimation, a dummy case (Al 278mg) and a blank sample was measured for 48 and 44 hours.
Table 1 The isotopic composition of the 244Cm sample or the 246Cm sample.
244Cm sample 246Cm sample TIMS (mole%) TIMS (mole%)
244Cm 90.1±1.7 27.5±0.5245Cm 2.71±0.34 1.06±0.28246Cm 7.22±0.34 59.4±1.3247Cm N.D. 2.9±0.4248Cm N.D. 9.10±0.24
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Capture Cross Sections of 244CmA. Kimura et al., J. Nucl. Sci. Technol., 49, 708-724 (2012)
The results of the resonance peaks under 20-eV are also the first experimental results in the world.
[1]M. S. Moore et.al. , Physical Review C, 3, 1656 (1971).
Only one set of cross section data for 244Cm (n,γ) was reported in 1971[1].
First DATA
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First DATA
[1]M. S. Moore et.al. , Physical Review C, 3, 1656 (1971).
Only one set of cross-section data of 246Cm (n,γ) was reported in 1971[1].
The results of the resonance peaks under 50-eV are the first experimental results in the world.
Capture Cross Sections of 246CmA. Kimura et al., J. Nucl. Sci. Technol., 49, 708-724 (2012)
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Capture Cross Sections of 237NpK. Hirose et al., J. Nucl. Sci. Technol., 50, 188-200 (2013)
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665 [b] at 25.3 meV (DANCE) was normalized as 684.87 [b]
Neutron Energy (eV)0.1 1
Cro
ss S
ectio
n (b
)
0
2000
4000
6000
8000eng (eV) vs sigma/G E, LAS vs Sig, LAS *1.03
Capture Cross Sections of 241AmH. Harada et al., ND2013
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Capture Cross Sections of 107PdS. Nakamura et al., ND2013
3.9-eV Res. --> 105Pd5.2-eV Res. --> 109Ag
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5. Summary
# It was explained that databases on neutron capture and/orfission reaction cross sections for MAs, LLFPs, and related nuclides were indispensable for developing thenuclear transmutation technology.
# The present status of the accuracy of nuclear databasesfor MAs and LLFPs was briefly reviewed.
# A general view of cross section measurements for MAsand LLFPs using SNSs was taken.
# A Japanese nuclear data project was explained.
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Thank you for your attention
CollaboratorsHokkaido Univ.: Y. Kiyanagi (moved to Nagoya Univ.), K. KinoJapan Atomic Energy Agency: H. Harada, S. Nakamura, A. Kimura, N. IwamotoTokyo Institute of Technology: T. KatabuchiKyoto University: J. Hori, H. Yashima
This Work was supported by JSPS KAKENHI Grant Number 22226016.
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