KCl-UCl3 molten salts investigated by Ab Initio Molecular Dynamics (AIMD) simulations

Andersson, Anders David Ragnar; Wang, Gaoxue; Yang, Ping; Beeler, Benjamin

doi:10.1016/j.jnucmat.2024.155226

Title: KCl-UCl₃ molten salts investigated by Ab Initio Molecular Dynamics (AIMD) simulations

Journal Article · 10 June 2024 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2024.155226 · OSTI ID:2426798

^[1];

^[1]; Beeler, Benjamin ^[2]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
North Carolina State University, Raleigh, NC (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Ab Initio Molecular Dynamics (AIMD) simulations are performed on molten KCl-UCl3 salt mixtures to determine energies, heat capacities, and densities. The density-dependent energy correction (DFT-dDsC), Grimme et al.'s DFT-D3, and Langreth & Lundqvist (vdW-cx) models are used for dispersion forces and combined with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation potential with a Hubbard U parameter for the 5f electrons of uranium. After validating predictions for the end-member systems to literature data, KCl-UCl₃ mixtures are studied at select temperatures. Densities and energies both deviate from ideal solution behavior, with the maximum deviation occurring around 36% UCl₃ for mixing energies and slightly lower (29% UCl3) for densities. Compared to the NaCl-UCl₃ system, which was previously investigated using the same simulation methodologies, the KCl-UCl₃ density and mixing energy deviations from ideal solution behavior are larger by almost a factor of two. No deviation from ideal solution behavior for heat capacity was observed. The AIMD predictions for mixing energies and densities agree qualitatively with experimental data, though the spread in data obtained from the various dispersion force models utilized, measurements, and empirical estimates makes strong conclusions difficult. The dependence of thermodynamic and thermophysical properties on composition is correlated with the local chemistry of the solution phase, in particular, the tendency of UCl₃ to form network structures.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: 89233218CNA000001; AC07-05ID14517

OSTI ID:: 2426798

Report Number(s):: LA-UR--23-34202

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 599; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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