Theoretical Investigations of the Activation of CO2 on the Transition Metal-doped Cu(100) and Cu(111) Surfaces  

作　　者：邱美 刘禹 吴娟 李奕 黄昕 陈文凯 章永凡 

机构地区：[1]College of Chemistry, Fuzhou University [2]Key Laboratory of Optoelectronic Materials Chemistry and Physics, Chinese Academy of Sciences

出　　处：《Chinese Journal of Structural Chemistry》2016年第5期669-678,共10页结构化学（英文）

基　　金：supported by the National Natural Science Foundation of China(21373048,21203027,and 21371034)

摘　　要：Periodic density functional theory calculations have been performed to investigate the chemisorption behavior of COz molecule on a series of surface alloys that are built by dispersing individual middle-late transition metal （TM） atoms （TM = Fe, Co, Ni, Ru, Rh, Pd, Ag, Os, lr, Pt, Au） on the Cu（100） and Cu（lll） surfaces. The most stable configurations of CO2 chemisorbed on different TM/Cu surfaces are determined, and the results show that among the late transition metals, Co, Ru, and Os are potentially good dopants to enhance the chemisorption and activation of CO2 on copper surfaces. To obtain a deep understanding of the adsorption property, the bonding characteristics of the adsorption bonds are carefully examined by the crystal orbital Hamilton population technique, which reveals that the TM atom primarily provides d orbitals with z-component, namely dz2, dxz, and dvz orbitals to interact with the adsorbate.Periodic density functional theory calculations have been performed to investigate the chemisorption behavior of COz molecule on a series of surface alloys that are built by dispersing individual middle-late transition metal （TM） atoms （TM = Fe, Co, Ni, Ru, Rh, Pd, Ag, Os, lr, Pt, Au） on the Cu（100） and Cu（lll） surfaces. The most stable configurations of CO2 chemisorbed on different TM/Cu surfaces are determined, and the results show that among the late transition metals, Co, Ru, and Os are potentially good dopants to enhance the chemisorption and activation of CO2 on copper surfaces. To obtain a deep understanding of the adsorption property, the bonding characteristics of the adsorption bonds are carefully examined by the crystal orbital Hamilton population technique, which reveals that the TM atom primarily provides d orbitals with z-component, namely dz2, dxz, and dvz orbitals to interact with the adsorbate.

关 键 词：carbon dioxide  chemisorption  transition metal surfaces  DFT 

分 类 号：O647.3[理学—物理化学]