Polarizable force fields for the structural and thermophysical properties of molten actinide chlorides

IF 3.2 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2025-04-11 DOI:10.1016/j.jnucmat.2025.155822

Giovanni Pireddu , Agustin Salcedo , Hugo Sauzet , Sylvie Delpech , David Lambertin , Timothée Kooyman

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Abstract

New nuclear technologies could involve the extensive use of molten salts, including actinide halides. Despite their importance, several practical challenges limit experimental measurements, resulting in knowledge gaps for structural and thermophysical properties. In this work, new polarizable force fields based on ab initio calculations for the simulation of molten actinide chlorides are introduced. The new force fields are used to compute structural properties, density, heat capacity, and isothermal compressibility of pure actinide molten salts (ThCl₄, PaCl₃, NpCl₃, AmCl₃, CmCl₃) at various temperatures. UCl₃ and PuCl₃, which were parameterized in previous works, are also included. The results are discussed in the context of already existing theoretical and experimental datasets, showing good agreement with the literature. Predictions are extended to systems not considered in previous works. Notably, the results highlight the peculiarity of ThCl₄ compared to actinide trichlorides in terms of structural and thermophysical properties. The new force fields can be used in future works for the simulation of molten salts mixtures containing actinides.

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熔态锕系氯化物的结构和热物理性质的极化力场

新的核技术可能涉及广泛使用熔盐，包括锕系卤化物。尽管它们很重要，但一些实际挑战限制了实验测量，导致结构和热物理性质的知识空白。本文介绍了一种新的基于从头计算的可极化力场，用于模拟锕系元素氯化物熔融过程。利用新力场计算了不同温度下纯锕系熔盐（ThCl4、PaCl3、NpCl3、AmCl3、cmccl3）的结构性质、密度、热容量和等温压缩率。UCl3和PuCl3在之前的作品中也被参数化。结果在已经存在的理论和实验数据集的背景下进行了讨论，显示出与文献的良好一致性。预测被扩展到以前工作中没有考虑到的系统。值得注意的是，这些结果突出了ThCl4在结构和热物理性质方面与三氯化锕系元素相比的特殊性。新的力场可用于今后含锕系元素熔盐混合物的模拟工作。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Nuclear Materials 工程技术-材料科学：综合

CiteScore

5.70

自引率

25.80%

发文量

601

审稿时长

63 days

期刊介绍： The Journal of Nuclear Materials publishes high quality papers in materials research for nuclear applications, primarily fission reactors, fusion reactors, and similar environments including radiation areas of charged particle accelerators. Both original research and critical review papers covering experimental, theoretical, and computational aspects of either fundamental or applied nature are welcome. The breadth of the field is such that a wide range of processes and properties in the field of materials science and engineering is of interest to the readership, spanning atom-scale processes, microstructures, thermodynamics, mechanical properties, physical properties, and corrosion, for example. Topics covered by JNM Fission reactor materials, including fuels, cladding, core structures, pressure vessels, coolant interactions with materials, moderator and control components, fission product behavior. Materials aspects of the entire fuel cycle. Materials aspects of the actinides and their compounds. Performance of nuclear waste materials; materials aspects of the immobilization of wastes. Fusion reactor materials, including first walls, blankets, insulators and magnets. Neutron and charged particle radiation effects in materials, including defects, transmutations, microstructures, phase changes and macroscopic properties. Interaction of plasmas, ion beams, electron beams and electromagnetic radiation with materials relevant to nuclear systems.