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<p>Calorimetric determination of enthalpies of mixing (Δ<i>H</i><sub>mix</sub>) in multicomponent molten salts is often interpreted using empirical models that lack physically meaningful parameters. However, for improving pyrochemical separation of spent nuclear fuel, where lanthanides are major fission products and critical elements, a deeper thermodynamic understanding of the link between excess thermodynamic properties and solvation structure is critically needed. In this work, we implement a hybrid and physics-informed framework, MIVM+Calorimetry+AIMD, which integrates experimentally measured Δ<i>H</i><sub>mix</sub> (via high temperature drop calorimetry) with solvation structures from ab initio molecular dynamics (AIMD). This approach is demonstrated using LaCl<sub>3</sub> mixed with eutectic LiCl-KCl (58 mol% – 42 mol%) at 873 K and 1133 K. MIVM-derived parameters enable extrapolation of excess Gibbs energy and La<sup>3+</sup> activity across compositions. In contrast, direct Δ<i>H</i><sub>mix</sub> predictions from AIMD and polarizable ion model simulations deviate significantly. By incorporating experimentally benchmarked solvation structures into an interpretable thermodynamic model, the MIVM+Calorimetry+AIMD formalism achieves higher accuracy and generalizable method for studying molten salts, offering a robust path for understanding and optimizing molten salt chemistry relevant to nuclear fuel cycles and separation science.</p>

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A hybrid calorimetry-simulation model of mixing enthalpy for molten salt

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月7日

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  • Vitaliy G. Goncharov,
  • William Smith,
  • Jiahong Li,
  • Jeffrey A. Eakin,
  • Erik D. Reinhart,
  • James Boncella,
  • Luke D. Gibson,
  • Vyacheslav S. Bryantsev,
  • Rushi Gong,
  • Shun-Li Shang,
  • Zi-Kui Liu,
  • Hongwu Xu,
  • Aurora Clark,
  • Xiaofeng Guo

摘要

Calorimetric determination of enthalpies of mixing (ΔHmix) in multicomponent molten salts is often interpreted using empirical models that lack physically meaningful parameters. However, for improving pyrochemical separation of spent nuclear fuel, where lanthanides are major fission products and critical elements, a deeper thermodynamic understanding of the link between excess thermodynamic properties and solvation structure is critically needed. In this work, we implement a hybrid and physics-informed framework, MIVM+Calorimetry+AIMD, which integrates experimentally measured ΔHmix (via high temperature drop calorimetry) with solvation structures from ab initio molecular dynamics (AIMD). This approach is demonstrated using LaCl3 mixed with eutectic LiCl-KCl (58 mol% – 42 mol%) at 873 K and 1133 K. MIVM-derived parameters enable extrapolation of excess Gibbs energy and La3+ activity across compositions. In contrast, direct ΔHmix predictions from AIMD and polarizable ion model simulations deviate significantly. By incorporating experimentally benchmarked solvation structures into an interpretable thermodynamic model, the MIVM+Calorimetry+AIMD formalism achieves higher accuracy and generalizable method for studying molten salts, offering a robust path for understanding and optimizing molten salt chemistry relevant to nuclear fuel cycles and separation science.