A first-principles simulation study on solubility of La, Nd, Zr and Mo in UO2 and U3O8

IF 2.8 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2024-09-19 DOI:10.1016/j.jnucmat.2024.155414

Zhiyuan Huang , Lidong Ma , Jianbao Zhang , Qing Zhou , Lei Yang , Haifeng Wang

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Abstract

Solubility of fission products (FPs) in spent nuclear fuels is a key issue in understanding their performance. In this study, a detailed density functional theory study on solubility of La, Nd, Zr and Mo in uranium dioxide (UO₂) and triuranium octoxide (U₃O₈) was carried out. The most favorable sites of La, Nd, Zr and Mo were calculated by analyzing the solution energies of these four FP elements in UO₂ and U₃O₈. Thermodynamic properties of FPs doping in UO₂ as well as in U₃O₈ were determined from 0 K to 2000 K. The results reveal that the effect of FPs on thermodynamic properties of U₃O₈ is slightly larger than that of UO₂ due to the presence of an oxygen vacancy in FP-doped U₃O₈. On this basis, the solubility of La, Nd, Zr and Mo in UO₂ and U₃O₈ was predicted, showing a good agreement with available experiments. Subsequently, the difference in solubility behaviors was studied through electronic properties. The simulation results indicate that the solubility of La, Nd, Zr and Mo in U₃O₈ is much lower than that in UO₂. Therefore, an idea to separate FPs from spent nuclear fuel is using mutual transformations between FP-doped UO₂ and FP-doped U₃O₈ under different temperatures, which is a promising way to promote the development of nuclear fuel cycles.

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关于镭、钕、锆和钼在二氧化铀和八氧化三铀中溶解度的第一原理模拟研究

裂变产物（FPs）在乏核燃料中的溶解度是了解其性能的一个关键问题。本研究对 La、Nd、Zr 和 Mo 在二氧化铀（UO2）和八氧化三铀（U3O8）中的溶解度进行了详细的密度泛函理论研究。通过分析这四种元素在二氧化铀和八氧化三铀中的溶解能，计算出了 La、Nd、Zr 和 Mo 的最有利位点。结果表明，由于掺杂了 FP 的 U3O8 中存在氧空位，FP 对 U3O8 热力学性质的影响略大于 UO2。在此基础上，预测了 La、Nd、Zr 和 Mo 在二氧化铀和八氧化三铀中的溶解度，结果与现有实验吻合。随后，通过电子特性研究了溶解度行为的差异。模拟结果表明，La、Nd、Zr 和 Mo 在 U3O8 中的溶解度远远低于在二氧化钛中的溶解度。因此，利用掺杂FP的UO2和掺杂FP的U3O8在不同温度下的相互转化来分离乏核燃料中的FP是一种可行的思路，也是促进核燃料循环发展的一种可行方法。

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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.