First-principles study of helium incorporation in Pu-La2Zr2O7 pyrochlore

IF 3.5 3区材料科学 Q1 MATERIALS SCIENCE, CERAMICS

Journal of the American Ceramic Society Pub Date : 2024-09-20 DOI:10.1111/jace.20119

Chenguang Liu, Rongrong Gao, Xiaoyi Xia, Kunjie Yang, Yuelin Liu, Pan Yang, Qing Peng, Fei Gao

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引用次数: 0

Abstract

Helium (He) exerts significant influence on the physicochemical, structural, and electronic properties of pyrochlores. This paper reviews recent advancements in computer simulations aimed at stabilizing nuclear waste, focusing on disordered structures of pyrochlores, zirconate pyrochlores, and high-entropy pyrochlores. Using Pu-La₂Zr₂O₇ as a case study, we demonstrate how a first-principles approach facilitates the understanding of how He modifies the structural and electronic properties of this system. The incorporation of He interstitials in Pu-La₂Zr₂O₇ typically leads to an expansion in lattice constant and volume swelling. Analysis of the formation energies in this system reveals that octahedral interstitial sites or zirconium (Zr) vacancy sites are favored for He occupation, resulting in the formation of substitutional He atoms. The low concentration of He atoms in Pu-La₂Zr₂O₇ reduces the formation energy of cation antisite defects. Bader charge analysis indicates that the < Zr-O > bond exerts a greater influence on the irradiation resistance of the He-Pu-La₂Zr₂O₇ system compared to the < La-O > bond. Moreover, the capacity for He interstitials increases with higher Pu concentration in the octahedrons.

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氦掺入钚-La2Zr2O7 热绿宝石的第一性原理研究

氦气（He）对热胶体的物理化学、结构和电子特性具有重大影响。本文回顾了旨在稳定核废料的计算机模拟的最新进展，重点是热胶体、锆酸盐热胶体和高熵热胶体的无序结构。以 Pu-La2Zr2O7 为例，我们展示了第一原理方法如何帮助理解 He 如何改变该体系的结构和电子特性。在 Pu-La2Zr2O7 中加入 He 间隙通常会导致晶格常数和体积膨胀。对该体系形成能量的分析表明，八面体间隙位点或锆（Zr）空位有利于 He 占据，从而形成置换的 He 原子。He 原子在 Pu-La2Zr2O7 中的低浓度降低了阳离子反位缺陷的形成能。Bader 电荷分析表明，与 La-O 键相比，Zr-O 键对 He-Pu-La2Zr2O7 体系的抗辐照能力影响更大。此外，八面体中的钚浓度越高，He间隙的容量就越大。

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 the American Ceramic Society 工程技术-材料科学：硅酸盐

CiteScore

7.50

自引率

7.70%

发文量

590

审稿时长

2.1 months

期刊介绍： The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials. Papers on fundamental ceramic and glass science are welcome including those in the following areas: Enabling materials for grand challenges[...] Materials design, selection, synthesis and processing methods[...] Characterization of compositions, structures, defects, and properties along with new methods [...] Mechanisms, Theory, Modeling, and Simulation[...] JACerS accepts submissions of full-length Articles reporting original research, in-depth Feature Articles, Reviews of the state-of-the-art with compelling analysis, and Rapid Communications which are short papers with sufficient novelty or impact to justify swift publication.