Static and dynamic evolution of CO adsorption onγ-U(100)surface with different levels of Mo doping using DFT and AIMD calculations

作     者：Jun-Wei Li Wei-Min Jia Chong Liu Sha-Sha Lv Jin-Tao Wang Zheng-Cao Li Jun-Wei Li;Wei-Min Jia;Chong Liu;Sha-Sha Lv;Jin-Tao Wang;Zheng-Cao Li

作者机构：Key Lab of Advanced Materials(MOE)School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Xi’an Research Institute of High-TechnologyXi’an 710025China Key Laboratory of Beam Technology(MOE)College of Nuclear Science and TechnologyBeijing Normal UniversityBeijing 100875China 

出 版 物：《Nuclear Science and Techniques》 (核技术（英文）)

年 卷 期：2023年第34卷第9期

页      面：142-154页

核心收录：

学科分类：08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0827[工学-核科学与技术] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China (Nos.11975135 and 12005017) the National Basic Research Program of China (No.2020YFB1901800) 

主　　题：Adsorption and dissociation Uranium CO molecule Density functional theory Ab initio molecular dynamics 

摘      要：Alloys of uranium and molybdenum are considered as the future of nuclear fuel and defense materials.However,surface corrosion is a fundamental problem in practical applications and storage.In this study,the static and dynamic evolution of carbon monoxide(CO)adsorption and dissociation onγ-U(100)surface with different Mo doping levels was investigated based on density functional theory and ab initio molecular dynamics.During the static calculation phase,parameters,such as adsorption energy,configuration,and Bader charge,were evaluated at all adsorption sites.Furthermore,the time-dependent behavior of CO molecule adsorption were investigated at the most favorable sites.The minimum energy paths for CO molecu-lar dissociation and atom migration were investigated using the transition state search method.The results demonstrated that the CO on the uranium surface mainly manifests as chemical adsorption before dissociation of the CO molecule.The CO molecule exhibited a tendency to rotate and tilt upright adsorption.However,it is difficult for CO adsorption on the surface in one of the configurations with CO molecule in vertical direction but oxygen(O)is closer to the surface.Bader charge illustrates that the charge transfers from slab atoms to the 2π*antibonding orbital of CO molecule and particularly occurs in carbon(C)atoms.The time is less than 100 fs for the adsorptions that forms embryos with tilt upright in dynamics evolution.The density of states elucidates that the overlapping hybridization of C and O 2p orbitals is mainly formed via the d orbitals of uranium and molybdenum(Mo)atoms in the dissociation and re-adsorption of CO molecule.In conclusion,Mo doping of the surface can decelerate the adsorption and dissociation of CO molecules.A Mo-doped surface,created through ion injection,enhanced the resistance to uranium-induced surface corrosion.