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First-principles study of hydrogen behavior in α-Pu2O3
Computational Materials Science ( IF 3.3 ) Pub Date : 2020-06-01 , DOI: 10.1016/j.commatsci.2020.109688
Le Zhang , Bo Sun , Qili Zhang , Haifeng Liu , Kezhao Liu , Haifeng Song

Abstract The in-depth understanding of hydrogen permeation through plutonium-oxide overlayers is the prerequisite to evaluate the complex hydriding induction period of Pu. In this work, the incorporation, diffusion and dissolution of hydrogen in α-Pu2O3 are investigated by the first-principles calculations and ab initio thermodynamic method based on DFT+U and DFT-D3 schemes. Our study reveals that the hydrogen incorporation is endothermic and the separated H atoms prefer to recombine as H2 molecules rather than reacting with α-Pu2O3. The H and H2 diffusion are both feasible, generally, H will recombine first as H2 and then migrate. Both pressure PH2 and temperature T can promote the hydrogen dissolution in α-Pu2O3. The single H2 molecule incorporation and (H + H2) mixed dissolution will successively appear when increasing PH2. Compared to PuO2, this work indicates that Pu sesquioxide is hardly reduced by hydrogen, but the porous α-Pu2O3 facilitates hydrogen transport in Pu-oxide layers. We present the microscopic picture of hydrogen behavior in the defect-free α-Pu2O3, which could shed some light on the study of the hydriding induction period of Pu.

中文翻译:

α-Pu2O3 中氢行为的第一性原理研究

摘要 深入了解氢通过氧化钚覆盖层的渗透是评估Pu复杂氢化诱导期的前提。在这项工作中,基于 DFT+U 和 DFT-D3 方案,通过第一性原理计算和从头算热力学方法研究了氢在 α-Pu2O3 中的掺入、扩散和溶解。我们的研究表明,氢结合是吸热的,分离的 H 原子更喜欢重新结合为 H2 分子,而不是与 α-Pu2O3 反应。H 和 H2 的扩散都是可行的,一般情况下,H 会先重组为 H2,然后再迁移。压力 PH2 和温度 T 都可以促进氢在 α-Pu2O3 中的溶解。随着PH2的增加,H2分子的掺入和(H+H2)混合溶解会相继出现。与 PuO2 相比,这项工作表明,Pu 倍半氧化物几乎不会被氢还原,但多孔的 α-Pu2O3 促进了 Pu 氧化物层中的氢传输。我们展示了无缺陷 α-Pu2O3 中氢行为的微观图片,这可以为研究 Pu 的氢化诱导期提供一些启示。
更新日期:2020-06-01
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