First-principles based computational study on nucleation and growth mechanisms of U on Mo(110) surface solvated in an eutectic LiCl–KCl molten salt

Choah Kwon, Joonhee Kang, Byungchan Han

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11 Citations (Scopus)

Abstract

We utilize first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to identify underlying mechanisms elucidating the initial stage of electrocrystallization process of U on Mo(110) surface in a eutectic LiCl–KCl molten salt at T = 773 K. Our results clearly unveil surprisingly different principles on the nucleation of U in the media from that under vacuum conditions. U nanoclusters exposed to vacuum completely collapse into flat atomic layers on Mo(110) surface similar to an electrodeposition process. On the other hand, Cl ions in eutectic molten salt thermodynamically drive crystallite formation consisting of UCln(n = 3–6) through agglomeration of U atoms. Those crystallite gradually grows into bigger nuclei by adsorbing on Mo(110) surface. We propose that those behaviors are understandable only with revised conventional theories and that atomic level interactions among U, LiCl–KCl molten salt and Mo(110) surface play a key role to describe the atomic-scale dendrite formation of U in the electrorefining process. Our study can be one of the basic steps to design efficient electrorefining systems by identifying the fundamental cause of the experimentally observed uranium nucleation phenomena.

Original languageEnglish
Pages (from-to)1381-1388
Number of pages8
JournalInternational Journal of Energy Research
Volume40
Issue number10
DOIs
Publication statusPublished - 2016 Aug 1

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Eutectics
Molten materials
Nucleation
Salts
Vacuum
Nanoclusters
Electrodeposition
Uranium
Density functional theory
Molecular dynamics
Agglomeration
Atoms
Computer simulation
Ions

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Fuel Technology
  • Energy Engineering and Power Technology

Cite this

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abstract = "We utilize first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to identify underlying mechanisms elucidating the initial stage of electrocrystallization process of U on Mo(110) surface in a eutectic LiCl–KCl molten salt at T = 773 K. Our results clearly unveil surprisingly different principles on the nucleation of U in the media from that under vacuum conditions. U nanoclusters exposed to vacuum completely collapse into flat atomic layers on Mo(110) surface similar to an electrodeposition process. On the other hand, Cl ions in eutectic molten salt thermodynamically drive crystallite formation consisting of UCln(n = 3–6) through agglomeration of U atoms. Those crystallite gradually grows into bigger nuclei by adsorbing on Mo(110) surface. We propose that those behaviors are understandable only with revised conventional theories and that atomic level interactions among U, LiCl–KCl molten salt and Mo(110) surface play a key role to describe the atomic-scale dendrite formation of U in the electrorefining process. Our study can be one of the basic steps to design efficient electrorefining systems by identifying the fundamental cause of the experimentally observed uranium nucleation phenomena.",
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