摘要
空气中活性气体在钚材料表面的吸附行为是引起钚材料表面腐蚀的重要原因。采用第一性原理方法对空气中N_(2)和O_(2)在δ-Pu(100)表面的吸附行为进行了研究。对所有稳定吸附构型进行Bader电荷分析以及吸附能与结合能分析的结果表明:N_(2)的最稳定吸附构型为H-S-N6,O_(2)的最稳定吸附构型为H-P-O4。对这2种吸附构型进行差分电荷密度分析、态密度(DOS)分析和晶体哈密顿轨道布居数(COHP)计算的结果表明:N_(2)和O_(2)在δ-Pu(100)表面的吸附均为强化学吸附,且O_(2)的吸附远远强于N_(2)。成键本质均为N原子或O原子的2s和2p轨道与表面Pu原子的6p、6d和5f轨道发生重叠杂化作用。研究结果对于N_(2)和O_(2)在δ-Pu(100)表面共吸附行为的研究奠定了良好基础,对揭示钚材料在空气中的表面腐蚀机制有重要意义。
The adsorption behavior of active gases in the air on the surface of Pu-based materials is an important cause of surface corrosion of Pu-based materials.The adsorption behavior of N_(2)and O_(2),two main gases in air,onδ-Pu(100)surface is studied using the first principle method.The Bader charge analysis and the adsorption energy and binding energy analysis of all stable adsorption configurations show that the most stable adsorption configuration of N_(2)molecule is H-S-N6 and the most stable adsorption configuration of O_(2)molecule is H-P-O4.The results of differential charge density analysis,density of states analysis and COHP calculation show that the adsorption of N_(2)and O_(2)onδ-Pu(100)surface is strong chemical adsorption,and the adsorption of O_(2)is much stronger than that of N_(2).Furthermore,the bonding essence is that the 2s and 2p orbitals of N atom or O atom overlap with the 6p,6d and 5f orbitals of Pu atom on the surface.These results can be a good foundation for the study of the co-adsorption behavior of N_(2)and O_(2)onδ-Pu(100)surface and are of great significance for revealing the surface corrosion mechanism of plutonium materials in air.
作者
赵朝阳
王国亮
翟鹏飞
戚春保
陈旭丹
ZHAO Zhaoyang;WANG Guoliang;ZHAI Pengfei;QI Chunbao;CHEN Xudan(School of Nuclear Engineering, Rocket Force University of Engineering, Xi’an 710025, China)
出处
《华南师范大学学报（自然科学版）》
CAS
北大核心
2022年第1期13-23,共11页
Journal of South China Normal University(Natural Science Edition)
基金
国家自然科学基金项目(22076219)
火箭军工程大学科研团队青年创新基金项目(2020-21)。
