The corrosion and oxidation of actinide metals, leading to the formation of metal-oxide surface layers with the catalytic evolution of hydrogen, impacts the management of nuclear materials. Here, the interaction of hydrogen with actinide dioxide (AnO₂, An = U, Np, or Pu) (011) surfaces by Hubbard corrected density functional theory (PBEsol+U) has been studied, including spin–orbit interactions and non-collinear 3k anti-ferromagnetic behavior. The actinide dioxides crystalize in the fluorite-type structure, and although the (111) surface dominates the crystal morphology, the (011) surface energetics may lead to more significant interaction with hydrogen. The dissociative adsorption of hydrogen on the UO₂ (0.44 eV), NpO₂ (−0.47 eV), and PuO₂ (−1.71 eV) (011) surfaces has been calculated. It is found that hydrogen dissociates on the PuO₂ (011) surface; however, UO₂ (011) and NpO₂ (011) surfaces are relatively inert. Recombination of hydrogen ions is likely to occur on the UO₂ (011) and NpO₂ (011) surfaces, whereas hydroxide formation is shown to occur on the PuO₂ (011) surface, which distorts the surface structure.

中文翻译：

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氢与二氧化act（011）表面的相互作用。

act系元素金属的腐蚀和氧化，随着氢的催化放出而导致形成金属氧化物表面层，从而影响了核材料的管理。在这里，通过哈伯校正密度泛函理论（PBEsol + U）研究了氢与act系元素二氧化dioxide（AnO ₂，An = U，Np或Pu）（011）表面的相互作用，包括自旋轨道相互作用和非共线性3k反铁磁行为。act系元素二氧化物以萤石型结构结晶，尽管（111）表面主导了晶体形态，但（011）表面高能可能导致与氢的更显着相互作用。氢在UO ₂（0.44 eV），NpO ₂（-0.47 eV）和PuO ₂上的解离吸附已计算出（−1.71 eV）（011）曲面。发现氢在PuO ₂（011）表面上解离；但是，UO ₂（011）和NpO ₂（011）表面相对惰性。在UO ₂（011）和NpO ₂（011）表面上很可能发生氢离子的重组，而显示在PuO ₂（011）表面上发生了氢氧化物的形成，这扭曲了表面结构。