[보고서]용융염내 악티나이드 화학연구

연제원

보고서 정보

주관연구기관

한국원자력연구원
Korea Atomic Energy Research Institute

연구책임자

연제원

참여연구자

조영환 , 김종윤 , 배상은 , 박태홍 , 정의창 , 차완식 , 이창헌 , 김정석 , 박용준 , 최광순 , 하영경 , 이명호 , 이치규 , 임상호 , 오승용 , 지광용 , 송규석

보고서유형

1단계보고서

발행국가

대한민국

언어

한국어

발행년월

2015-01

과제시작연도

2014

주관부처

미래창조과학부
Ministry of Science, ICT and Future Planning

과제관리전문기관

한국연구재단
National Research Foundation of Korea

등록번호

TRKO201800009430

과제고유번호

1711009901

사업명

원자력기술개발사업

DB 구축일자

2018-05-26

키워드

핵연료주기.사용후핵연료.용융염.악티나이드.란타나이드.전기화학.분광학.물성.nuclear fuel cycle.spent nuclear fuel.molten salt.actinide.lanthanide.electrochemistry.spectroscopy.physical property.

DOI

https://doi.org/10.23000/TRKO201800009430

표 Electronic absorption spectra of LaCl3 (a), CeCl3 (b), NdCl3 (c), and a representative molar absorptivity calculation of NdCl3 at 588 nm in LiCl-KCl at 450℃
표 Molar absorptivity of CeCl3 (a) and NdCl3 (b) in LiCl-KCl at 450℃
표 Absorption spectra of multi-component systems obtained from the addition of subsequent addition of UCl3, LaCl3, CeCl3 and NdCl3 in LiCl-KCl at 450℃.
표 Absorption spectrum of NpCl4 in LiCl-KCl at 450 ℃
표 Absorption spectrum of NpCl4 in LiCl-KCl at 450 ℃ with subsequent addition of LaCl3, CeCl3, and NdCl3 before (a) and after (b) purification of lanthanide chlorides.
표 Schematic description of an electrochemical spectroscopic cell
표 Cyclic voltamogram of a multi-component LiCl-KCl eutectic system including UCl3, LaCl3, CeCl3, and NdCl3 at 450 ℃.
표 Chronological electronic absorption spectra of a multi-component LiCl-KCl eutectic system at 450 ℃ including UCl3, LaCl3, CeCl3, and NdCl3 under a constant potential of 0 V (a) and subsequently under a constant potential of -0.7 V (b).
표 Chronological electronic absorption spectra of a multi-component LiCl-KCl eutectic system at 450 ℃ including UCl3, LaCl3, CeCl3, and NdCl3 under constant potentials of -1.5∼-1.7 V (a) and then -2.1 V (b).
표 Chronological electronic spectra of the electrochemical reaction of Np3+ to Np4+ in LiCl-KCl melt at 450 ℃. Constant potentials were subsequently applied at 0.6 V (a) and 1.1 V (b).
표 Overview of electronic spectral change of Np ion in LiCl-KCl melt at 450 ℃ with a variation of applied potential.
표 Chronological electronic spectrum of a multi-component LiCl-KCl eutectic system at 450 ℃ including NpCl4, LaCl3, CeCl3, and NdCl3 under constant potentials of 0.3 and then 0.1 V.
표 Chronological electronic spectrum of a multi-component LiCl-KCl eutectic system at 450 ℃ including NpCl3, LaCl3, CeCl3, and NdCl3. Constant potentials were subsequently applied at -1.0 V (a), -1.5 V (b), -1.7 V (c), -2.1 V (d), and -2.2 V (e).
표 Schematic diagram of experimental setup.
표 Electronic absorption spectra of SmCl3 (a), YbCl3 (b), EuCl2 (c) in LiCl-KCl at 450℃
표 Absorption spectra of multi-component systems obtained from the subsequent addition of UCl3, SmCl3, YbCl3 and EuCl3 in LiCl-KCl at 450℃. UCl3 concentration was approximately 0.01 wt% (a) and 0.04 wt% (b).
표 Absorption spectra of multi-component systems obtained from the subsequent addition of NpCl4, SmCl3, YbCl3 and EuCl3 in LiCl-KCl at 450℃.
표 Absorption spectra change with the addition of Li2O to LiCl-KCl eutectic including NpCl4 at 450℃.
표 Absorption spectra change with the addition of Li2O to LiCl-KCl eutectic including NpCl4 at 450℃.
표 Absorption spectra of multi-component systems obtained from the subsequent addition of UCl3, SmCl3, YbCl3 and EuCl3 in LiCl-KCl at 450℃.
표 Electronic absorption spectra after applying potentials to a multi-component LiCl-KCl eutectic system at 450 ℃ including UCl3, SmCl3, YbCl3, and EuCl3. Working electrode: tungsten plate, counter electrode: Al foil, reference electrode Ag wire in 1 wt% AgCl.
표 Electronic absorption spectra after applying potentials to a multi-component LiCl-KCl eutectic system at 450 ℃ including NpCl4, SmCl3, YbCl3, and EuCl3. Working electrode: glassy carbon, counter electrode: Al foil, reference electrode Ag wire in 1 wt% AgCl.
표 Electronic absorption spectra after applying potentials to a multi-component LiCl-KCl eutectic system at 450 ℃ including NpCl4, SmCl3, YbCl3, and EuCl3. Working electrode: glassy carbon (a) or tungsten plate (b), counter electrode: Al foil, reference electrode Ag wire in 1 wt%
표 Photo of the tungsten electrode in molten LiCl-KCl after electrodeposition of Np
표 Electronic absorption spectra of (a) a mixture of U and Np and (b-c) a mixture of U, La, Ce, Nd and Np in LiCl-KCl melt at 450 ℃.
표 Cyclic voltammograms obtained from W wire in LiCl-KCl melt containing various concentration of UCl3
표 Peak currents of the electrodeposition and its dissolution as a function of concentration in Fig. 2-1-1.
표 Repeating chronoamperometry results obtained from W wire in LiCl-KCl melt containing various concentration of UCl3
표 Schematic of repeating chronoamperometry for Pyrochemical process
표 Steady state currents of repeating chronoamperometry as a function of concentration in Fig. 2-1-3.
표 Charge passed during the repeating chronoamperometry as a function of concentration in Fig. 2-1-3.
표 Repeating chronoamperometry results obtained from W wire in LiCl-KCl melt containing various concentration of UCl3.
표 Steady state currents of repeating chronoamperometry as a function of concentration in Fig. 2-1-7.
표 Charge passed during the repeating chronoamperometry as a function of concentration in Fig. 2-1-7.
표 Schematic of repeating multi-step voltammetry for Pyrochemical process.
표 Repeating multi-step voltammetry results obtained from W wire in LiCl-KCl melt containing CeCl3 and various concentrations of UCl3 and LaCl3
표 Steady state currents (a) and passed charge (b) of repeating multi-step voltammetry as a function of concentration in Fig. 2-1-11.
표 Linear sweep voltammograms and (a) and passed charge (b) obtained from W wire in LiCl-KCl melt containing CeCl3 and various concentrations of UCl3 and LaCl3
표 Cyclic voltammograms obtained from W wire in LiCl-KCl melt containing UCl3, CeCl3, LaCl3, and NdCl3
표 Cyclic voltammograms obtained from W wire in LiCl-KCl melt containing CdCl2, UCl3, CeCl3, LaCl3, and NdCl3.
표 Cyclic voltammogram obtained from W wire in LiCl-KCl melt containing BiCl3, and UCl3.
표 Cyclic voltammograms obtained from W wire in LiCl-KCl melt containing BiCl3, UCl3, CeCl3, LaCl3, and NdCl3
표 Cyclic voltammograms obtained from W wire (a) and W plate (b) in LiCl-KCl melt containing various concentration of CeCl3
표 Repeating multi-step voltammograms obtained from W plate in LiCl-KCl melt containing UCl3 and various concentration of CeCl3.
표 CV results obtained from W (a) and GC (b) in LiCl-KCl melt containing 2 wt.% NdCl3 at various temperature. (c) temperature dependence of apparent reduction potential and (d) Gibbs free energy change of NdCl3 formation
표 CV results obtained from W (a) and GC (b) in LiCl-KCl melt containing 2 wt.% LaCl3 at various temperature. (c) temperature dependence of apparent reduction potential and (d) Gibbs free energy change of LaCl3 formation
표 CV results obtained from W (a) and GC (b) in LiCl-KCl melt containing 2 wt.% CeCl3 at various temperature. (c) temperature dependence of apparent reduction potential and (d) Gibbs free energy change of CeCl3 formation.
표 CV results obtained from W (a) and GC (b) in LiCl-KCl melt containing 1 wt.% UCl3 at various temperature. (c) temperature dependence of apparent reduction potential and (c) Gibbs free energy change of UCl3 formation
표 Enthalpy and entropy changes of formation in LiCl-KCl
표 Electronic absorption spectra of UCl3 in LiCl-KCl at 450℃.
표 Electronic absorption spectra of concentrated UCl3 in LiCl-KCl at 450℃.
표 Electronic absorption spectra of concentrated UCl3 in LiCl-KCl at 450℃ with a 2 mm path length cell (a) and absorbance change with UCl3 concentration at 750 nm and 900 nm
표 Cyclic voltammogram obtained from W wire in LiCl-KCl melt containing 2 wt.% UCl3 and CeCl3
표 Potentials applied during RCA measurement in LiCl-KCl melt containing 2 wt.% UCl3 and CeCl3
표 RCA results obtained from W wire in LiCl-KCl melt containing 3 wt.% CeCl3 and various concentration of UCl3
표 RCA results obtained from W wire in LiCl-KCl melt containing 3 wt.% UCl3 and various concentration of CeCl3.
표 Tafel plots for anodic and cathodic branches of the current-overpotential curve
표 Schematics of rotating disk electrode.
표 Schematics of rotating disk electrode system for high temperature molten salts
표 Picture of rotating disk electrode system manufactured by Pine Instrument
표 Stand for height control of RDE.
표 Glove box design for RDE system in molten salts.
표 Furnace design for RDE system in molten salts.
표 MgO insulated RDE. (a) Hole in MgO rod, (b) MgO rod and W rod, and (c) Mgo insulated RDE
표 Cycle voltammograms obtained from MgO insulated RDE in LiCl-KCl containing 1.5 wt.% CeCl3.
표 Rotating disk electrodes. (a) W electrode extended with stainelss steel and (b) W electrode and polished electrode surface
표 Cycle voltammograms obtained from W RDE in LiCl-KCl containing 1.5 wt.% LaCl3
표 (a) Cycle voltammograms and (b) scan rate dependence of peak currents obtained from W RDE in LiCl-KCl containing 1.5 wt.% SmCl3., YbCl3, and EuCl3.
표 (a) Linear sweep voltammograms at various rotation rates and (b) Levich plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% YbCl3. Scan rate: 4 mV/s.
표 Tafel plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% YbCl3
표 Chronoamperometry result obtained from W RDE in LiCl-KCl containing 1.5 wt.% YbCl3.
표 (a) Linear sweep voltammograms at various rotation rates and (b) Levich plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% SmCl3. Scan rate: 4 mV/s.
표 Tafel plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% SmCl3.
표 (a) Linear sweep voltammograms at various rotation rates and (b) Levich plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% EuCl3. Scan rate: 4 mV/s
표 Tafel plot obtained from W RDE in LiCl-KCl containing 1.5 wt.% EuCl3.
표 Diffusion coefficients of lanthanide ions in LiCl-KCl melt obtained with RDE measurements
표 Electron transfer resistances and exchange current densities of lanthanide ions in LiCl-KCl melt obtained with RDE measurements.
표 (a) Linear sweep voltammograms at various rotation rates and (b) Levich plot obtained from W RDE in LiCl-KCl containing 1.83 wt.% UCl3. Scan rate: 4 mV/s.
표 Tafel plot obtained from W RDE in LiCl-KCl containing 1.83 wt.% UCl3. (a)U(III/IV) and (b) U(0/III) redox reactions.
표 Diffusion coefficients of uranium ions in LiCl-KCl melt obtained with RDE measurements.
표 Electron transfer coefficients and exchange current densities of uraium ions in LiCl-KCl melt obtained with RDE measurements
표 Dissolution of uraium in LiCl-KCl containing 1.83 wt.% UCl3. (a)current and (b) mole number.
표 Dissolution of uraium in LiCl-KCl containing 1.83 wt.% UCl3. (a)weight and (b) temperature dependence of dissolution rate.
표 Dissolution rate of uraium metal in LiCl-KCl melt at various temperatures.
표 Design of electrode system for electrochemical on-line monitoring in LiCl-KCl
표 Pictures of electrode system for electrochemical on-line monitoring in LiCl-KCl. (a) side view and (b) bottom view.
표 Schematics of testing system for electrochemical on-line monitoring in LiCl-KCl.
표 Chronoamperometry result obtained during height controlling of the guide electrode
표 Chronopotentiometry result obtained from Bi Pool.
표 RCA results obtained from W wire before and after U electrodeposition into Bi pool
표 RCA results obtained from W wire before and after U dissolution from Bi pool.
표 RCA results obtained from W wire after U electrodeposition into Bi pool.
표 Molar absorptivity of lanthanides and actinides in LiCl-KCl at 450 ℃
표 (a) Absorption spectra of UCl3 in LiCl-KCl eutectic at 450 ℃ using a cell with 1 cm light path length. Concentration: 0.2-0.7 wt%. (b) Photo of the cell containing 0.7 wt% of UCl3.
표 NIR molar absorptivity of UCl3 in LiCl-KCl at 450 ℃
표 (a) Absorption spectra of UCl3 in LiCl-KCl eutectic at 450 ℃ using a cell with 1 mm light path length. Concentration: 2.0-13.3 wt%. (b) Photo of the cell containing 13.3 wt% of UCl3.
표 Concentration dependent absorbance changes of the NIR f-d transitions of UCl3 in LiCl-KCl eutectic at 450 ℃ using a 1 mm light path cell.
표 Electrical conductivity measurement system using a AC impedance analysis method.
표 Various types of the glass capillary electrodes combined with platinum wires.
표 Various equivalent circuits of the electrochemical cells, and the Nyquist plots for the equivalent circuits
표 Nyquist plot of the conductivity standards (0.001M KCl).
표 Nyquist plot of the conductivity standards. (a) 0.01M KCl, (b) 0.1M KCl, (c) 1M KCl, and (d) 3M KCl.
표 Cell constants of the glass capillary cells with the KCl concentrations.
표 Current vs. time curve in chronoamperometry.
표 The effect of electrical conductivity on the peak currents in chronoamperometry.
표 Current vs. time curve in chronoamperometry with the multiple-potential steps.
표 Effect of the time interval in the multiple-potential step chronoamperometry on the polarizaiton of the electrochemicla cell
표 Effect of the open circuit potential on the current-voltage curve
표 Effect of applied voltages on the cell constants.
표 Electrical conductivity measurement system where x = the cell distance from the bottom of the vessel, and y = the immersion depth of the cell.
표 The effect of the cell distance from the bottom of the vessel, and the immersion depth of the cell on the cell constants of the glass capillary cells
표 Viscosity measurement system using a double-walled falling cylinder method.
표 Determination of the time of fall in a double-walled falling cylinder method
표 Effect of the height of fall on the time of fall.
표 Calibration curve obtained by using the viscosity standards.
표 Viscosity measurement system equipped with the Brookfield viscometer and the control program for the high-temperature application
표 Various tools and accessaries in the viscosity measurement system
표 Specially-designed viscometer and the electric furnace.
표 Driving unit for the precise alignment of viscometer and the sample vessel.
표 Temperature correction using KNO3 as the reference molten salts.
표 SINTERFACE BPA-1SX tensiometer and the high-temperature maximum bubble pressure measurement system.
표 Determination of the density by using maximum bubble pressure method
표 Determination of the liquid level based on the pressure method.
표 Circuit diagram of the liquid level measurement system based on the pressure method
표 Special equipment for the measurement of the differential scanning calorimetry
표 Special equipment for the measurement of the differential scanning calorimetry
표 Electrical conductivity of pure LiCl(44wt%)-KCl(56wt%) molten salts measured by using the AC impedance method
표 Conductivity of pure LiCl-KCl eutectic using a short time interval multiple-potential step chronoamperometry
표 Viscosities of pure LiCl-KCl molten salts.
표 Effect of temperature on the viscosities of pure KNO3 molten salts
표 Kinematic viscosities of pure LiCl-KCl molten salts at various temperature.
표 Viscosity of the LiCl-KCl eutectic molten salts with temperatures measured by using rotational viscometer.
표 Variation in the bubble pressures with time depending on the immersion depth.
표 Densities of pure KNO3 molten salts at various temperatures.
표 Dynamic surface tension of pure KNO3 molten salts at various temperatures.
표 Static surface tension of pure KNO3 molten salts at various temperatures.
표 Result of the distance measurements using the tube pressure method
표 Result of the LiCl-KCl eutectic using the differential scanning calorimetry.
표 Determination of the melting point of the LiCl-KCl eutectic using the electrical conductivity method.
표 Effect of the temperature on the viscosity of eutectic LiCl-KCl molten salt comprising 30 wt% of LaCl3 : CeCl3 : NdCl3 = 1 : 1 : 1.
표 3-component phase diagram obtained using FactSage 6.3.
표 Phase diagram of the 3-component LiCl-KCl-LaCl3 system at 873 K.
표 Calculated results of the phase behavior of CeCl3 in LiCl-KCl molten salts using FactSage 6.3.
표 Conductivities of NdCl3-LiCl-KCl molten salts measured by using Short-time Interval Multiple-potential Step Chronoamperometry in order to determine the liquidus and solidus temperatures.
표 DataChoa ver. 0.9. (a) initial front web page, and (b) administrator's page.
표 Selection of appropriate solution for selective dissolution of metallic uranium
표 Block flow diagram for selective dissolution analysis of lanthanide metals from their oxide mixtures.
표 Enthalpy of formation for LnBr3, LnCl3 and Ln2O3
표 Thermodynamical basis of bromine method.
표 Schematic presentation of bromine method.
표 Chemical stripping of lanthanides from organic phase (upper) into aquesous (lower) phase
표 metallic (dissolved by Br2-ethylacetate) protion (a) and oxide (insoluble) portion (b).
표 Evaporation of solvent and drying for Nd sample.
표 Examples of pretreatment failure (side reaction, particle formation by aging).
표 Pretreatment by adding oxidat (H2O2) in case of fine particle formation.
표 Schematic presentation of bromine-dissolution and sample pretreatment for analysis
표 Measurement of metallic contents in the carefully selected lanthanide metal samples by bromine method.
표 Corrosion property of lanthanide metals.
표 Corrosion properties of Nd metal.
표 Measurement of metallic contents (blue) in the samples and recovery (red) by bromine method.
표 Dissolution of Ln2O3 by bromine method.
표 Chemical Composition of SIMFUEL sample.
표 Schematic presentation of electrolytic reduction process and samples for analysis (1) opearation salt (2) reduced SIMFUEL, and (3) reduced sample after CP process
표 Bromine dissolved (metallic) lower portion and undissolved (oxides) upper portion after bromination process
표 Dependence of U metal conversion yield of reduced SIMFUEL on bromination time
표 Application of bromine method to determine the conversion yield of a reduced SIMFUEL
표 Reduction yield of U and lanthanide elements of electrolytically reduced SIMFUEL sample
표 Comparison of U metal conversion yield before and after CP process.
표 Variation of dissolved Ba, Sr and Rh in various operation salt samples
표 Eight different voloxidized samples produced by varying operation conditions.
표 Raw data sheet of chemical analysis of voloxidized samples produced by varying operation conditions.
표 Information of samples for chemical analysis.
표 Photos taken during the dissolution of sample #4 resulting from the LCC electrodeposition and Cd distillation.
표 ICP-AES result of sample #4
표 SEM image of the insoluble solid recovered from the dissolution of sample #4.
표 EDX result of spot 1 in Fig. 4-2-7.
표 EDX result of spot 2 in Fig. 4-2-7.
표 EDX result of spot 3 in Fig. 4-2-7.
표 EDX result of spot 4 in Fig. 4-2-7.
표 Results of chemical analysis of solids obtained from the LCC electrodeposition-Cd distillation (top) and trace elements found (bottom)
표 Flow sheet of separation of U, Am/Cm, and Pu using UTEVA and TRU column chromatography
표 Extraction chromatography where a flow rate is controlled by gravity (left) and reduced pressure (right).
표 ICP-AES result of 4 M NH4SCN-0.1 M formic acid solution eluted from TEVA resin
표 Flow sheet of separation of Am and rare earth elements using TEVA column chromatography
표 Flow sheet of recovery of Np from LiCl-KCl eutectic waste.
표 Photos of anion exchange chromatography of Np (left) and recovered Np (right).
표 Photos of coupled-column chromatography system for the separation of U, Pu and lanthanides
표 (a) Structure of sodium eicosyl sulfate and (b) hydrophobic interaction between C18 functionalized silica surface and sodium eicosyl sulfate
표 Schematic of coupled-column chromatography system for the separation of U, Pu and lanthanides
표 Structures of Arsenanzo III (a) and α-hydroxyisobutyric acid.
표 Separation of lanthanides from uranium matrix using C18 reversed phase column (15× 0.46 cm, 5 μm particle size) and sodium eicosyl sulfate coated column.
표 Scheme of SI system. D: detector.
표 SI-networks assembled using extraction or anion exchange chromatography.
표 Photos of the SI-system assembly.

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[국가R&D연구보고서] 용융염내 악티나이드 화학연구
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[국가R&D연구보고서] 용융염내 악티나이드 화학연구 Research on Actinide Chemistry in Molten Salt 원문보기

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