Hybrid functional/embedded cluster study of uranium and actinide (actinide = Np, Pu, Am or Cm) mixed dioxides bulk and {110} surfaces
Hybrid functional/embedded cluster study of uranium and actinide (actinide = Np, Pu, Am or Cm) mixed dioxides bulk and {110} surfaces
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DOI：
10.1016/j.jnucmat.2021.153490
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发表时间：
2022-03-01
影响因子：
3.1
通讯作者：
Kaltsoyannis, Nikolas
中科院分区：
文献类型：
--
作者：
Chen, Jia-Li;Kaltsoyannis, Nikolas
了解锕系元素（An）混合氧化物（MOX）对开发含微量An的U-Pu MOX核燃料和长期贮存乏核燃料具有重要意义。在这项工作中，我们系统地模拟AnO（2）（An = U、Np、Pu、Am和Cm）和U-An MOX（An = Np，Pu，Am，and Cm）体表面和{110}表面的计算，重点研究了An从U到Cm系列的自旋密度以及AnO（2）体表面和表面的态密度;发现了O和An之间的自旋密度转移，并对其进行了详细讨论。对于U-An MOX体和表面，给出了几何结构、U和An自旋密度以及态密度。对于U-Np和U-Cm MOX体系中An的氧化态可以得出明确的结论，而U-Pu MOX和U-Am MOX不太清楚，但对模拟方法敏感，表明它们处于U-Np和U-Cm体系之间的过渡区。(c)2021爱思唯尔有限公司版权所有。
Understanding actinide (An) mixed oxides (MOX) is important for the development of minor An bearing U-Pu MOX nuclear fuel, and the long-term storage of spent nuclear fuel. In this work, we systematically simulate AnO(2) (An = U , Np, Pu, Am, and Cm) and U-An MOX (An = Np, Pu, Am, and Cm) bulk and {110} surfaces using hybrid density functional theory within an embedded cluster model, focusing on the spin density of An and the density of states of AnO(2) bulk and surface for the An series from U to Cm; spin density transfer is found between O and An and is discussed in detail. For U-An MOX bulk and surface, geometric structure, U and An spin densities and the densities of states are presented. Clear conclusions can be drawn regarding the oxidation state of An in the U-Np and U-Cm MOX systems, while U-Pu MOX and U-Am MOX are less clear but and sensitive to the simulation method, suggesting they are in a transition region between the U-Np and U-Cm systems. (c) 2021 Elsevier B.V. All rights reserved.