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

Choah Kwon, Joonhee Kang, Woojong Kang, Dohyun Kwak, Byungchan Han

Research output: Contribution to journalArticle

11 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)216-222
Number of pages7
JournalElectrochimica Acta
Volume195
DOIs
Publication statusPublished - 2016 Mar 20

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Molybdenum
Eutectics
Molten materials
Cathodes
Salts
Spent fuels
Nuclear fuels
Thermodynamics
Radioactive wastes
Kinetics
Radioactive Waste
Activity coefficients
Density functional theory
Molecular dynamics
Thermodynamic stability
Viscosity
Electrodes
Computer simulation

All Science Journal Classification (ASJC) codes

  • Chemical Engineering(all)
  • Electrochemistry

Cite this

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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.",
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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. / Kwon, Choah; Kang, Joonhee; Kang, Woojong; Kwak, Dohyun; Han, Byungchan.

In: Electrochimica Acta, Vol. 195, 20.03.2016, p. 216-222.

Research output: Contribution to journalArticle

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AU - Kwak, Dohyun

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