First-principles thermodynamical modeling of molecular reactions on α-U(001) and α-UH3(001) surfaces and their influence on hydrogen activation

IF 2.8 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2024-10-10 DOI:10.1016/j.jnucmat.2024.155455

Jinfan Chen, Tao Tang

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Abstract

Density functional theory calculations coupled with thermodynamic analysis have been performed to investigate the reactions of hydrogen and impurity gases including O₂, CO₂, CO, N₂ on α-U(001) and α-UH₃(001) surfaces. Binding strength of adsorbates on α-UH₃ is calculated to be weaker than α-U, suggesting enhanced poisoning-resistant properties of U-hydride compared to its metallic state. Surface phase diagrams of U under binary H₂-O₂, H₂-N₂ and H₂-CO gaseous environments show that while N and C elements prefer to stay in their hydrogenated states on the hydride surface, isolated O atoms favorably interact with both α-U(001) and α-UH₃(001), indicating the heavily poisoning effect of impurities containing oxygen. Global optimization of partially oxidized α-U(001) slabs induces surface geometry reconstruction and the activity of oxidized surfaces toward hydrogen adsorption can be linearly correlated with local electronic and atomic properties of the adsorption site.

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α-U(001)和α-UH3(001)表面分子反应的第一原理热力学模型及其对氢活化的影响

通过密度泛函理论计算和热力学分析，研究了氢气和杂质气体（包括 O2、CO2、CO 和 N2）在 α-U(001) 和 α-UH3(001) 表面上的反应。根据计算，α-UH3 上吸附剂的结合强度比 α-U 弱，这表明 U-hydride 的抗中毒特性比金属态更强。在二元 H2-O2、H2-N2 和 H2-CO 气体环境下的 U 表面相图显示，N 和 C 元素更喜欢保持氢化物表面的氢化状态，而孤立的 O 原子则与α-U(001) 和 α-UH3(001) 发生有利的相互作用，这表明含氧杂质具有严重的中毒效应。部分氧化的 α-U(001)板的全局优化引起了表面几何重构，氧化表面的氢吸附活性与吸附位点的局部电子和原子特性成线性关系。

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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.