A study on the electrochemical deposition behavior of uranium ion in a LiCl–KCl molten salt on solid and liquid electrode

Kim, Gha-Young; Yoon, Dalsung; Paek, Seungwoo; Kim, Si-Hyung; Kim, Tack-Jin; Ahn, Do-Hee

doi:10.1016/j.jelechem.2012.07.025

Cited by 57 publications

(34 citation statements)

References 28 publications

(41 reference statements)

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“…In molten chloride salt, uranium ions electrochemical behavior was studied by Serrano et al between 973 K and 988 K in NaCl-KCl [27] , and in LiCl-KCl by various authors [28][29][30][31][32][33][34] . The U(III) ions are reduced in one step, exchanging 3 electrons, to U and oxidized to https://doi.org/10.1016/j.electacta.2020.136784 U(IV) in one step exchanging 1 electron.…”

Section: Introductionmentioning

confidence: 99%

Electrochemistry of uranium in molten LiCl-LiF

Geran

Chamelot

Serp

et al. 2020

Electrochimica Acta

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This work is focused on the electrochemical behaviour of uranium in molten eutectic LiCl-LiF (70-30 mol%) in the 550-650 °C temperature range. On tungsten electrode, U(III) ions were reduced in one step to U metal exchanging 3 electrons and oxidized also in one step to U(IV) exchanging one electron. Both systems were studied by cyclic and square wave voltammetries and chronopotentiometry. The reduction and oxidation mechanisms of U(III) ions were found to be diffusion controlled processes. The diffusion coefficient of U(III) was measured at different temperatures, and it followed an Arrhenius "type law". Apparent standard potentials were measured in chloride-fluoride (LiCl-LiF eutectic) and pure chloride media (LiC-KCl eutectic). The addition of fluoride ions into a chloride salt leads to the formation of more stable complexes reduced at more negative potentials. This shift of reduction potentials is more pronounced for the U(IV)/U(III) transition ( ~5 00 mV) than for the U(III)/U system ( ~1 00 mV).

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Section: Introductionmentioning

confidence: 99%

Electrochemistry of uranium in molten LiCl-LiF

Geran

Chamelot

Serp

et al. 2020

Electrochimica Acta

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“…14 The diffusion coefficients on the LCC were almost half of the values of the diffusion coefficients on the tungsten electrode. Gha-Young and co-workers 22 also had a similar trend with uranium chloride. That is, diffusion coefficient of uranium on LCC was about one tenth of the diffusion coefficient on solid cathode.…”

Section: Resultsmentioning

confidence: 59%

Electrochemical and Thermodynamic Properties of CeCl₃on Liquid Cadmium Cathode (LCC) in LiCl-KCl Eutectic Salt

Yoon

Phongikaroon

Zhang

2016

J. Electrochem. Soc.

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Electrochemical and thermodynamic properties of Ce 3+ /Ce on liquid cadmium cathode (LCC) were investigated in LiCl-KCl salt at various temperatures. Cyclic voltammograms only attributing to Ce 3+ /Ce reaction were obtained by background subtraction method and diffusion coefficients of Ce on the LCC were determined at temperatures ranging from 723 K to 798 K. Furthermore, thermodynamic properties of the Ce-Cd intermetallic compound formations were measured via an open circuit chronopotentiometry technique at temperature from 698 K to 823 K. The linear dependence of the Gibbs free energy of the formation was observed as a function of temperature, from which the enthalpy and entropy of the formation were calculated. Here, activity and partial molar Gibbs free energies of Ce in two phase coexisting states were calculated through the measurement of electromotive force. Tafel and linear polarization were conducted with varying Ce concentration in Cd. The exchange current densities (i 0 ) of Ce on the LCC were calculated from both techniques in LiCl-KCl-1 wt% CeCl 3 at 773 K. The resulting data sets of i 0 from both methods show a near linear trend of i 0 within the solubility limit of Ce in Cd. However, i 0 of Ce remains unchanged with increasing Ce concentration beyond the solubility limit. Treatment of the long term radioactive wastes from nuclear fuel cycle have become an essential matter in nuclear industries and public concern.1 One of the most promising option is known as Pyrochemical or Pyroprocessing technology, whose main method is electrorefining in chloride form of salt. This technology has a potential to treat used oxide/metal fuels and produce plutonium (Pu) in company with uranium (U), and minor actinides (MAs), resulting strong resistance for nuclear proliferation.1-3 The main step within this system is an electrorefining process, in which most of U is selectively recovered using a solid cathode in molten lithium-potassium chloride (LiCl-KCl) salt at high temperature (typically at 773 K). Then, the residual U, Pu and MAs are simultaneously collected with small amount of lanthanides into a liquid cadmium cathode (LCC) due to their small activity in liquid metals. 4 Since the operation of the LCC plays an important role in the feasibility of electrochemical processes toward material detections and accountability, 5 extensive studies have been done to understand electrochemical and thermodynamic features of U, Pu, and MAs on the LCC. Shirai et al. 6,7 investigated the reaction of U 3+ /U and Pu 3+ /Pu couples on the LCC. The redox reaction for both couples were almost reversible, and the reduction potential on the LCC showed more positive values than that at the molybdenum electrode. Murakami and co-workers 8 measured diffusion coefficients of actinides and rare earth elements with LCC by performing chronopotentiometry (CP) in LiCl-KCl at temperature ranging from 723 K to 823 K. Castrillejo et al. 5,9,10 investigated the activities and Gibbs energy of rare earth materials in both Cd and Bi liquid electro...

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“…This is an important detail that was not previously accounted for in theoretical investigations of uranium adsorption. Including the surface diffusion in the model is important in light of recent experimental evidence from impedance spectra [29]. When attempting a diffusion move for particle i, a random displacement vector dr (uniformly distributed within a circle of radius R ion /4 ) is added to the position vector of particle i r i .…”

Section: The Monte Carlo Simulationmentioning

confidence: 99%

A study of uranium adsorption to single-crystal tungsten

Samin

Hastings

Zhang

2015

Journal of Nuclear Materials

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In this study we explore the adsorption of uranium to the (110) plane of tungsten. Potential functions were constructed to describe the interaction of adsorbed uranium atoms with the tungsten surface and the lateral interaction between adsorbed uranium atoms. Next, the behavior of the uranium adlayer under different conditions was studied through a Monte Carlo simulation of the grand canonical Hamiltonian in an off-lattice model. Our results are consistent with available studies in the literature. The simulation results indicate that the temperature and dipole-dipole interactions play an important role in governing the adsorption process. Introduction:Nuclear power is a key energy alternative for efficient generation of electricity. However, an essential factor in nuclear power is the safe management of spent fuel. Electrochemical reprocessing (or Pyroprocessing) of used nuclear fuel is a promising technology that has been extensively studied (e.g [1][2][3][4]). This process allows for the selective recovery of actinides from used fuels. The process has many advantages such as compactness of process equipment and the potential of the development of the integrated irradiation-reprocessing facility which can significantly reduce the costly and complicated transport of nuclear materials [5].

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A study on the electrochemical deposition behavior of uranium ion in a LiCl–KCl molten salt on solid and liquid electrode

Cited by 57 publications

References 28 publications

Electrochemistry of uranium in molten LiCl-LiF

Electrochemistry of uranium in molten LiCl-LiF

Electrochemical and Thermodynamic Properties of CeCl₃on Liquid Cadmium Cathode (LCC) in LiCl-KCl Eutectic Salt

A study of uranium adsorption to single-crystal tungsten

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A study on the electrochemical deposition behavior of uranium ion in a LiCl–KCl molten salt on solid and liquid electrode

Cited by 57 publications

References 28 publications

Electrochemistry of uranium in molten LiCl-LiF

Electrochemistry of uranium in molten LiCl-LiF

Electrochemical and Thermodynamic Properties of CeCl3on Liquid Cadmium Cathode (LCC) in LiCl-KCl Eutectic Salt

A study of uranium adsorption to single-crystal tungsten

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Electrochemical and Thermodynamic Properties of CeCl₃on Liquid Cadmium Cathode (LCC) in LiCl-KCl Eutectic Salt