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First principles study of the thermodynamic and kinetic properties of U in an electrorefining system using molybdenum cathode and LiCl-KCl eutectic molten salt

Title
First principles study of the thermodynamic and kinetic properties of U in an electrorefining system using molybdenum cathode and LiCl-KCl eutectic molten salt
Authors
Kwon, C[Kwon, Choah]Kang, J[Kang, Joonhee]Kang, W[Kang, Woojong]Kwak, D[Kwak, Dohyun]Han, B[Han, Byungchan]
DGIST Authors
Kang, J[Kang, Joonhee]; Kwak, D[Kwak, Dohyun]
Issue Date
2016-03-20
Citation
Electrochimica Acta, 195, 216-222
Type
Article
Article Type
Article
Keywords
Ab Initio Molecular DynamicsActivity CoefficientActivity CoefficientsCalculationsCathodesComputation TheoryCorrosionDensity Functional TheoryDesign for TestabilityElectrochemical ConditionsElectrodepositionElectrodesElectrorefining of Spent Nuclear FuelElectrorefining ProcessEutecticsExperimental DatabaseFirst-Principles CalculationFirst-Principles StudyFirst Principles Density Functional Theory (DFT) CalculationsFuelsFused SaltsKineticsMolecular DynamicsNuclear FuelsRadioactive WastesSpent FuelsSpent Nuclear FuelsThermodynamic StabilityThermodynamicsViscosity
ISSN
0013-4686
Abstract
Using first principles density functional theory (DFT) calculations we obtain thermodynamic and kinetic properties of U in an electrorefining process for spent nuclear fuels using a LiCl-KCl eutectic molten salt and Mo as a cathode. The thermodynamic stability of electrodeposited U from the molten salt onto the Mo(110) surface electrode is evaluated by activity coefficients as function of surface coverages of U and Cl. Additionally, ab-initio molecular dynamic simulations combined with the Stokes-Einstein-Sutherland relation enables us to calculate the viscosity of the LiCl-KCl eutectic molten salt. Our results well agree with previously reported experimental data endorsing the credibility. Based on our atomic-level mechanical understanding we propose that an accurate computational model system incorporating the electrochemical conditions of the electrorefining process essential for the purpose of establishing thermodynamic and kinetic database of U, otherwise critical deviations are inevitable. More interestingly, the effect of coadsorption of Cl with U on the Mo(110) surface plays a key role in stabilizing electrodeposited U on the cathode. Our approach can be useful for validating published experimental database and for identifying key factors guiding a rational design of highly efficient electrorefining system for spent nuclear fuels, and thus reducing high-level radioactive nuclear wastes. © 2016 Elsevier Ltd. All rights reserved.
URI
http://hdl.handle.net/20.500.11750/2708
DOI
10.1016/j.electacta.2016.02.123
Publisher
Elsevier Ltd
Files:
There are no files associated with this item.
Collection:
Energy Science and EngineeringETC1. Journal Articles
Energy Science and EngineeringMNEDL(Multifunctional Nanomaterials & Energy Devices Lab)1. Journal Articles


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