First-principles investigation of the thermophysical properties of NaCl, PuCl3, and NaCl-PuCl3 Molten salts

Duemmler, Kai; Andersson, Anders David Ragnar; Beeler, Benjamin

doi:10.1016/j.jnucmat.2024.154902

Title: First-principles investigation of the thermophysical properties of NaCl, PuCl₃, and NaCl-PuCl₃ Molten salts

Journal Article · Thu Jan 11 00:00:00 EST 2024 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2024.154902· OSTI ID:2283370

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North Carolina State University, Raleigh, NC (United States)
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)

Molten salts have a variety of applications that span the nuclear and solar industries, and which involve thermal storage and heat transfer. There is a present knowledge gap in the thermophysical properties of molten salts, which limits the readiness level of molten salt applications. This is especially pertinent for molten salt reactors where the fissile material is dissolved within the molten salt. Ab initio molecular dynamics is a common method employed to investigate the structural and thermophysical properties at elevated temperatures. NaCl-PuCl₃ is a candidate fuel salt in molten salt reactors. The scope of this study is to investigate the seven unique compositions and a range of temperatures of NaCl-PuCl₃ and calculate the density, heat capacity, compressibility, enthalpy of mixing, and coefficient of thermal expansion. Within this work, the van der Waals (vdW) interactions are primarily handled with the vdW-DF2 functional but spot-checked with both the dDsC and DFT-D3 methods. The calculated densities are in good agreement with the NaCl and the eutectic compositions, and no experimental values exist for PuCl₃ at these temperatures. The densities are fit to a first-order Redlich-Kister expansion as a function of both composition and temperature. The heat capacity in the literature is scattered but the calculated values agree well with one of the experimental results. Here, the heat capacity increases as a linear function with respect to concentration at a rate of about 7.5 J/mol-K per 10 mol% PuCl₃.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

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

OSTI ID:: 2283370

Alternate ID(s):: OSTI ID: 2281739

Report Number(s):: LA-UR-23-30110

Journal Information:: Journal of Nuclear Materials, Vol. 591; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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