[보고서]조사핵연료 내 악티나이드 화학거동 연구

하영경

보고서 정보

주관연구기관

한국원자력연구원
Korea Atomic Energy Research Institute

연구책임자

하영경

참여연구자

김종구 , 윤영상 , 이창헌 , 박순달 , 김정석 , 박양순 , 박재일 , 이정묵 , 한선호 , 송규석

보고서유형

1단계보고서

발행국가

대한민국

언어

한국어

발행년월

2015-01

과제시작연도

2014

주관부처

미래창조과학부
Ministry of Science, ICT and Future Planning

등록번호

TRKO201800009428

과제고유번호

1711010303

사업명

원자력기술개발사업

DB 구축일자

2018-05-26

키워드

금속핵연료.산화물핵연료.핵분열생성기체.조사거동.화학결합.침출.조사핵연료.동위원소 분포.Oxide fuel.metallic fuel.Irradiation behavior.PCCI(or FCCI).Retained fission gas.leaching.Irradiated fuel.Isotopic distribution.

DOI

https://doi.org/10.23000/TRKO201800009428

표 Multi-barriers against migration of radionuclides leached from spent nuclear fuels.
표 Disposal concepts of spent nuclear fuels in foreign countries
표 Flow sheet of 4-iodo-N,N-dimethylaniline formation from Iodide, iodate, iodine, and organo-iodine.
표 Isotopic compositions of annular fuel.
표 Burnup determined by 148Nd method.
표 Annular fuel specimen.
표 Structural changes of STS 316L cladding for an annular fuel
표 Changes in lattice parameter of irradiated annular fuel (ca. 10 GWd/tU)
표 Design parameters of a fuel rod, which was selected for retained fission gas measurement
표 Relationship between Xe release and short term leachability of 137Cs and 129I
표 Irradiation history of a selected fuel rod for measurement of fission gas distribution
표 Puncturing results of an irradiated fuel rod
표 Retention time of fission gas compositions
표 Concept of a puncturing/collection apparatus
표 A puncturing and collection device, which was installed in a hot cell.
표 Standard calibration curves using a gas chromatography.
표 Standard calibration curves for krypton and xenon using a quadrupole mass spectrometer.
표 Analysis results of a released fission gas
표 Isotopic composition of a released Kr gas
표 Isotopic composition of a released Xenon gas
표 Major input parameters for calculation of fission gas generation
표 Krypton generation by a code calculation
표 Xenon generation by a code calculation
표 Measurement results of fission gas release (FGR)
표 Sampling positions of an irradiated fuel rod for retained fission gas measurements
표 Eddy current test for oxide thickness measurement of the selected fuel rod.
표 Gamma scanning result of the selected fuel rod.
표 Rod diameter variation of the selected fuel rod.
표 Sampling positions of an spent fuel rod for retained fission gas measurement.
표 Optical microscopy images of a fuel fragment FG02 sample.
표 Kr and Xe concentrations in the sampling bottle for FG02 samples
표 Isotopic composition of Kr for FG02 samples
표 Isotopic composition of Xe for FG02 samples
표 Scanning spectrum of krypton for FG02 sample.
표 Scanning spectrum of xenon for FG02 sample.
표 Measured results of retained fission gas for FG02 samples
표 Kr and Xe concentrations in the sampling bottle for FG03 samples
표 Isotopic composition of Kr for FG03 samples
표 Isotopic composition of Xe for FG03 samples
표 Scanning spectrum of krypton for FG03 samples.
표 Scanning spectrum of krypton for FG03 samples.
표 Measured results of retained fission gas for FG03 samples
표 Optical microscopy images of a fuel fragment FG05 sample.
표 Krypton and xenon concentrations in the sampling bottle for FG05 samples.
표 Scanning spectrum of krypton for FG05 sample.
표 Scanning spectrum of xenon for FG05 sample.
표 Isotopic composition of Kr for FG05 samples
표 Isotopic composition of Xe for FG05 samples
표 Measured results of retained fission gas for FG05 samples
표 Optical microscopy images of a fuel fragment FG06 sample.
표 Kr and Xe concentrations in the sampling bottle for FG06 samples
표 Composition of Kr isotopes for FG06 samples
표 Composition of Xenon isotopes for FG06 samples
표 Scanning spectrum of Kr for FG06 sample.
표 Scanning spectrum of Xe for FG06 sample
표 Measured results of retained fission gas for FG06 samples.
표 Optical microscopy images of a fuel fragment FG08 sample.
표 Kr and Xe concentrations in the sampling bottle for FG08 samples.
표 Scanning spectrum of krypton for FG08 samples.
표 Scanning spectrum of xenon for FG08 samples.
표 Krypton isotopes distribution for FG08 samples.
표 Xenon isotopes distribution for FG08 samples
표 Measured results of retained fission gas for FG08 sample
표 Kr and Xe concentrations in the sampling bottle for FG10 samples.
표 Isotopic composition of Kr for FG10 samples.
표 Scanning spectrum of krypton for FG10 samples.
표 Scanning spectrum of xenon for FG10 samples.
표 Isotopic composition of Xe for FG10 samples.
표 Measured results of retained fission gas for FG10 sample.
표 Retained Kr depending on local burn-up of an irradiated oxide fuel.
표 Retained Xe depending on local burn-up of an irradiated oxide fuel.
표 Retained fission gas depending on local burn-up of an irradiated oxide fuel.
표 Retained Kr concentrations depending on axial positions of an irradiated fuel rod.
표 Retained Xe concentrations depending on axial positions of an irradiated fuel rod.
표 Retained fission gas concentrations depending on axial positions of an irradiated fuel rod.
표 Xe/Kr ratio of fission gas depending on local burnup.
표 86Kr/134Xe of fission gas to fuel burnup.
표 Kr and Xe isotopes combination ratios of the measured fission gas.
표 Drawings of small cask for an irradiated fuel
표 Drawings of basket for a small cask.
표 Carrier for a small cask
표 Drawing of ante box for a small cask.
표 Ante box for a small Cask: (a), (b) after fabrication, (c) air compressor, (d) after installation, (e), (f) outer door closed/open.
표 Supporter for a small cask to bringing in and out of the ante box.
표 Cross section of SFR alloy fuel irradiated in Hanaro.
표 Chemical composition of T92 steel.
표 Isobars of Nd as a burnup monitor.
표 Preparation of a simulated SFR fuel solution.
표 Composition of standard solution of non-actinides mixture.
표 Dissolution rate of metallic fuel at mixed solution of 1 M HF and HNO3.
표 Dissolution rate of metallic fuel in 3 M HNO3 and HF mixed solution.
표 Dissolution rate of metallic fuel in 3 M HNO3 and HF mixed acid at different temperature.
표 Pretreatment for chemical analysis of U-Zr alloy.
표 Analytical scheme for Pu separation in a simulated SFR solution.
표 Isotopic Compositions of U, Pu and Nd separated from a simulated SFR fuel solution
표 Mass spectra of U, Pu and Nd separated from a simulated SFR fuel solution.
표 Metallic fuel specimen
표 Capsule for irradiation test
표 Photograph of the modified laser ablation system (green lines schematically represent a laser beam pathway to the sample chamber)
표 Drawing of modified ablation chamber
표 Modified ablation chamber
표 Measurement conditions for U-10Zr-5Ce samples by LA-ICP-MS system
표 Chiller for ICP-MS
표 (left) CCD image of U-10Zr-5Ce ablated craters (bright spots, scales bar is 200 μm). (middle) 90Zr/235U ratio, and (right) 140Ce/235U ratio measured by LA-ICP-MS (bold/dotted blue lines indicate the average/standard deviation value, respectively).
표 Phase diagram for the U-Zr system.[3-1-2]
표 Phase diagram for the U-Pu system by Chiotti[3-1-3].
표 Phase diagram for the Pu-Zr system[3-1-4].
표 Phase diagram for the U-Pu-Zr system.[3-1-6,7]
표 Phase transitions for actinides.[3-1-8∼10]
표 Phase transition of Pu.
표 Phase transition of Np.
표 Phase transition of Am.
표 Phase transition of Cm.
표 XRD spectrum of U-Zr and U-Zr-Ce
표 U-Zr-Ce specimen for micro-XRD experiments.
표 XRD spectra of U-Zr-Ce specimen at fuel, cladding, and resin.
표 A separation device for spent fuel from clad.
표 A malfunctioned turbo controller.
표 A new TURBO-INST controller (Part No. D39721000 BOC EDWARDS), installed on a quadrupole mass spectrometer.
표 A compressor and its cover.
표 A covered compressor.
표 A remote control brake for the compressor.
표 Traps for purification of compressed air.
표 Accessories for upgrade from RH-600 to TCH-600.
표 The operation manual and software license for TCH-600.
표 Upgrading to TCH-600 N, O, H determinator.
표 Reference materials for calibration of TCH-600 N/O/H determinator.
표 Performance test results of TCH-600 N, O, H determinator with standard materials
표 A broken Z-axis wire of the right manipulator.
표 Vinyl taping of the right installation hole.
표 Repairing of the broken wire.
표 (left) Apparatus for clamp insertion and remove, (middle) A new clamp and tung, (right) A remote exchange tool for tung, adaptor and etc
표 A boot and its accessories.
표 Installation tool for boot.
표 Insertion of a boot (left) and connecting of a new boot using an o-ring (right).
표 Expansion of an installed boot.
표 Installation of the manipulator.
표 The installed manipulator
표 A boot adaptor
표 Connection of a nipple on the end of manipulator master slave.
표 Connection of a new tung to the master slave nipple.
표 The connected tung to the master slave.
표 Installed moisture traps.
표 Retention time of gas compositions.
표 Gas chromatography (Agilent 6890N).
표 A new column for He measurement.
표 A 6-port valve for front detector.
표 Electronic boards and others
표 Separated spectrums of He, Kr and Xe.
표 Separated krypton area of mixed standard gas using a gas chromatography.
표 Separated xenon area of mixed standard gas using a gas chromatography.
표 Separated helium area of mixed standard gas using a gas chromatography.
표 Calibration curve of Kr and Xe by a gas chromatography.
표 Calibration curve of He by a gas chromatography.
표 Photo of U-10Zr fuel slug (A) at upper position.
표 SEM image (x40) of U-10Zr fuel slug (A) at upper position.
표 SEM image (x100) of U-10Zr fuel slug (A) at upper position.
표 Energy dispersive X-ray spectrum of U-10Zr fuel slug (A) at upper position.
표 Photo of U-10Zr fuel slug (A) at middle position.
표 SEM image of U-10Zr fuel slug (A) at middle position.
표 SEM image of U-10Zr fuel slug (A) at middle position.
표 Energy dispersive x-ray spectrum of U-10Zr fuel slug (A) at middle position.
표 Photo of U-10Zr fuel slug (A) at lower position.
표 SEM image of U-10Zr fuel slug (A) at lower position.
표 SEM image of U-10Zr fuel slug (A) at lower position.
표 Energy dispersive X-ray spectrum of U-10Zr fuel slug (A) at lower position.
표 Analysis results of A U-10Zr fuel slugs using an energy dispersive X-ray spectrometer
표 Photo of U-10Zr fuel slug (B) at upper position.
표 SEM image of U-10Zr fuel slug (B) at upper position.
표 SEM image of U-10Zr fuel slug (B) at upper position.
표 Energy dispersive X-ray spectrum of U-10Zr fuel slug (B) at upper position.
표 Photo of U-10Zr fuel slug (B) at middle position.
표 SEM image of U-10Zr fuel slug (B) at middle position.
표 SEM image of U-10Zr fuel slug (B) at middle position.
표 Energy dispersive X-ray spectrum of U-10Zr (B) fuel slug at middle position.
표 Photo of U-10Zr (B) fuel slug at lower position.
표 SEM image of U-10Zr (B) fuel slug at lower position.
표 SEM image of U-10Zr (B) fuel slug at lower position.
표 Energy dispersive x-ray spectrum of U-10Zr (B) fuel slug at lower position.
표 Analysis results of B U-10Zr fuel slugs using an energy dispersive X-ray spectrometer.
표 Photo of U-10Zr-5Ce fule slug.
표 Secondary electron image of U-10Zr-5Ce fuel slug.
표 Secondary electron image of U-10Zr-5Ce fuel slug.
표 EDS spectrum of U-10Zr-5Ce fule slug.
표 EDS analysis result of a U-10Zr-5Ce fuel sulg
표 Non metal impurity analysis results of U-10Zr (A) fuel slugs using elemental analyzers.
표 Non metal impurity analysis results of U-10Zr (B) fuel slugs using elemental analyzers.
표 Impurities of U-10Zr-5Ce fuel sulg
표 Compositions of metal fuel.
표 Hydrogen determinator (LECO RH-404).
표 Nickel basket (LECO 502-344).
표 High temperature graphite crucible (LECO 782-820).
표 U-10Zr sample.
표 A melt of U-Zr fuel with a nickel basket.
표 A melt of U-Zr fuel with a nickel basket.
표 Analytical results of U-Zr by Energy dispersive x-ray spectrometer.
표 Analytical results of U-Zr-RE by energy dispersive x-ray spectrometer.
표 Energy dispersive x-ray spectrum of a melt of U-Zr fuel with a nickel basket.
표 Back-scattering electron image (BEI) and area mapping of U, Zr, Ni for a melt of U-Zr fuel with nickel basket.
표 Energy dispersive x-ray spectrum of a U-10Zr-3RE fuel melt with a nickel basket.
표 Back-scattering electron image (BEI) and area mapping of U, Zr, Nd, Ni for a melt of U-Zr-RE fuel with nickel basket.
표 A calculation of fission gas release from a SFR fuel rod.
표 Puncturing of an irradiated metal fuel rod.
표 A sampling bottle for collection of punctured gas of a metal fuel rod.
표 After puncturing of a metal fuel rod
표 Separation of SFR fission gas compositions.
표 Connection of a sampling bottle to the inlet of a gas chromatography.
표 Separated peaks of released fission gas from a SFR fuel.
표 Calibration of a gas chromatography using mixed standard gases.
표 Fission gas analysis results using a GC.
표 Isotopic composition of Krypton for released fission gas.
표 Isotopic composition of Xe for released fission gas.
표 Connection of a sampling bottle to the inlet of a QMS system.
표 Scanning spectrum of krypton
표 Scanning spectrum of xenon
표 Calibration of a quadrupole mass spectrometer using mixed gases.
표 Fission gas analysis results using a quadrupole mass spectrometer.
표 Specifications for metal fuel capsule.
표 Irradiated metal fuel rods at HANARO
표 Preparation of an irradiated metal fuel.
표 Sampling bottle of irradiated fuel fragments.
표 A fragment of irradiated fuel, U-10Zr.
표 A fragment of irradiated fuel, U-10Zr-5Ce.
표 Retained krypton and xenon measurement results of irradiated U-10Zr and U-10-5Ce samples
표 Retained krypton isotopes distributions for irradiated U-10Zr and U-10Zr-5Ce samples
표 Retained xenon isotopes distributions for irradiated U-10Zr and U-10Zr-5Ce samples
표 Scanning spectrum of retained krypton isotopes for U-10Zr sample.
표 Scanning spectrum of retained krypton isotopes for U-10Zr-5Ce sample.
표 Scanning spectrum of retained xenon isotopes for U-10Zr sample.
표 Scanning spectrum of retained xenon isotopes for U-10Zr-5Ce sample.
표 Retained fission gas results for irradiated U-10Zr and U-10Zr-5Ce samples
표 Developed program (ChemPro-SNF)
표 Contour map of (left) axial surface and (right) radial cross-section properties of fuel rod.
표 Graph from a database of a fuel.
표 User-friendly toolbar.
표 Effective data management system.
표 Contour map of distribution of 239Pu/235U isotopes.
표 Heat flow curves of DSC measurements for the reaction between Cs2O and UO2.
표 Thermogravimetric measurements for the reaction between Cs2O and UO2.
표 Formation extent of Cs-U-O depending on the Cs/U ratio of the blended samples.
표 XRD patterns for the reaction products of Cs2O and UO2.
표 Reaction between fuel and clad at various temperatures.
표 Preparation of UO2-Zr couple. (top) horizontal layer, (bottom) vertical layer.
표 Electrode furnace equipped with a pyrometer, which measures the temperature in the range of 1000 to 3000 ℃.
표 SEM images (×1,000 and ×8,500) for interface between UO2 and Zr in UO2-Zr pellet.
$X-ray diffraction spectrum of raw UO2-Zr, pure UO2, and pure Zr pellets.$ 표 X-ray diffraction spectrum of raw UO2-Zr, pure UO2, and pure Zr pellets.
표 Pictures of UO2-Zr samples before and after annealing at 400, 500, 550, and 600 A. UO2-Zr sample after annealing at 600 A was incompletely melted with a piece of raw UO2-Zr in graphite crucible.
표 SEM images (×500∼×17,000) obtained from UO2-Zr after annealing at 400, 500, 550, and 600 A.
표 XRD spectrum obtained from UO2-Zr samples after annealing at 400, 500, 550, and 600 A.
표 SEM images (×3,000) of UO2 and Zr pellets.
표 XPS spectra of U 4f and Zr 3d measured from (a) UO2 and (b) Zr pellets at room temperature.
표 SEM images (×4,000) of UO2 pellets after heating with Zr at (a) 875, (b) 1890, (c) 2040, and (d) 2230 ℃.
표 SEM images (×1,000) of Zr pellets after heating withZr at (a) 875, (b) 1270, (c) 1890, and (d) 2230 ℃.
표 U 4f core-level spectra of UO2 pellets heated at (a) 875, (b) 1890, and (c) 2230 ℃.
표 Zr 3d core-level spectra of Zr pellets annealed at (a) 1195, (b) 1270, and (c) 1890 ℃.
표 (a) U 4f and (b) Zr 3d core-level spectra of the molten product produced after the complete melting of a UO2-Zr sample.
표 (a) SEM image and EDS results of (b) uranium and (c) zirconium elements acquired from the identical region of the molten product. The brighter the part is, the richer the element is in (b) and (c).
표 Sample holder for UO2 leaching test. ① Sample holder, ② Sample supporter, ③ Sample suspender.
표 Leaching cell. for evaluation of UO2 leaching behaviour. ① leaching bottle, ② Sample suspender, ③ Sampling needle, ④ Stirring bar, ⑤ Cooling condenser (less than 10 ℃) ⑥ Syringe for sampling, ⑦ Temperature sensor.
표 Measurement system for an evaluation of UO2 leaching behaviour; (left) under oxic atmosphere ① Cooler, ② Heating mantle, ③ Temperature controller, (right) under anoxic atmosphere (in a glove box charging with argon).
표 Dynamic leaching cell (A type) for evaluation of dissolution behaviour of UO2 at 70 ℃ under anoixic atmosphere. ① Upper stopper, ② Lower stopper ③ Leaching cell
표 Supporter of a leaching cell with lead shield for evaluation of dissolution behaviour of UO2. ① Stand of leaching cell.
표 Dynamic leaching system for evaluation of dissolution behaviour of UO2 at the elevated temperature (70℃) under anoxic atmosphere. ① Heating sensor, ② Heating mantle, ③ Heating controller.
표 A pump of leachant for dynamic leaching system
표 Stability of the pump for dynamic leaching system.
표 Shielding concept of Leaching cell (A type)
표 Concept of Leaching cell (B type)
표 Dismantling the old glove-boxes
표 Break-up the old glove-boxes to small pieces.
표 Installing an alpha-shielded glove-box.
표 Electrochemical measurement system. PAR 263A Potentiostat
표 Electrochemical cell (Type A).
표 Fabricated electrochemical cell (Type B)
표 Electochemical analyzer (CH Instrument Model 600D) and cell (Type C).
표 Fabricated working electrode (Type A): (left, S-01) UO2, U0.977Gd0.023O2, U0.933Gd0.067O2, (center, S-02) UO2, U0.975Gd0.025O2, U0.95Gd0.05O2, U0.9Gd0.1O2, (right S-03) UO2, U0.975Ce0.025O2, U0.95Ce0.05O2, U0.9Ce0.1O2
표 Prepared Pt mesh counter electrode for Type C electrochemical cell.
표 Properties of prepared working electrode (Type A).
표 Preparation of working electrode (Type C) (top) WE with fixed cover, (middle) electrodeposition of Cu on a WE for electrical connection, (bottom) WE with detachable cover and electrode holder.
표 Drawing of the UO2 specimen holder.
표 Installed Raman system for the measurement of electrode surface
표 Raman spectrum of UO2 electrode surface.
표 Mother solutions of Na2CO3 and NaHCO3.
표 Variation of dissolved oxygen in mg/L as a function of purging time. Sample: distilled water, 5 L, purging gas; Ar (99.999%), 15 SCFH (~7 L/min).
표 Chemical composition of carbonate solutions adjusted to pH 9.
표 Chemical composition of 1×10-3 mol/L carbonate solution adjusted to pH 8~10.
표 Specification of UO2 pellets.
표 UO2 pellets prepared for the evaluation of UO2 dissolution behaviour
표 Spectrums measured by X-Ray photon spectrometry before dissolution experiment (Left) 4f5/2 and 4f7/2 peaks, (Right) 4f7/2 peak.
표 Reliability of the uranium separation procedure in the range of 1∼10 μg.
표 Reliability of uranium separation procedure in the range of nanogram.
표 Inductively coupled plasma mass spectrometer (Spectro/ICP-MS, Germany).
표 Elution behaviour of Na and U in carbonate solution (pH 9, 5×10-2 mol/L) on the U-TEVA column. Column : 100 mg of U-TEVA, Elution : Sample (10 ug/5 mL/2 M HNO3), washing (4 mL/2 M HNO3), recovery of U (5 mL/0.01 M HCl).
표 Separation procedure of U from carbonate solutions.
표 Dissolved oxygen measurement system. ① Port for DO electrode, ② Port for injecting water and benting excess water, ③ DO measurement cell, ④ Dissolved oxygen meter, ⑤ Stirrer, ⑥ DO electrode.
표 Effect of temperature on dissolution of oxygen in distilled water.
표 Amount of oxygen dissolved in distilled water in the range of 60∼90 ℃.
표 Effect of temperature on leaching of UO2 in the range of 60∼90 ℃ under oxic atmosphere.
표 Relation of leaching rate to amount of oxygen dissolved in distilled water in the range of 60∼90 ℃ under oxic atmosphere.
표 Dissolution rate of UO2 in distilled water in the range of 60∼90 ℃ under oxic atmosphere.
표 Uranium dissolved in distilled water at 60~90 ℃ under anoxic atmosphere after 40 days.

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조사핵연료 내 악티나이드 화학거동 연구
Reaearch on the Actinides Chemistry in an Irradiated Nuclear Fuel 원문보기

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조사핵연료 내 악티나이드 화학거동 연구 Reaearch on the Actinides Chemistry in an Irradiated Nuclear Fuel 원문보기

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조사핵연료 내 악티나이드 화학거동 연구
Reaearch on the Actinides Chemistry in an Irradiated Nuclear Fuel 원문보기

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