文献类型：期刊文献

英文题名：Role of oxygen vacancies in the surface evolution of H at CeO2(111): a charge modification effect

作者：Wu, Xin-Ping[1,2];Gong, Xue-Qing[1,2];Lu, Guanzhong[1,3]

机构：[1]E China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Ctr Computat Chem, Shanghai 200237, Peoples R China;[3]E China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China

年份：2015

卷号：17

期号：5

起止页码：3544

外文期刊名：PHYSICAL CHEMISTRY CHEMICAL PHYSICS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000348203200066)】；

基金：This work was supported by the National Basic Research Program (2011CB808505), National Natural Science Foundation of China (21322307, 21421004), Open Project of State Key Laboratory of Chemical Engineering (SKL-ChE-12C02) and the "Shu Guang'' project of Shanghai Municipal Education Commission and Shanghai Education Development Foundation (13SG30). The authors also thank the computing time at the National Super Computing Center in Jinan.

语种：英文

摘要：Diffusion processes and reactions of H at stoichiometric and reduced CeO2(111) surfaces have been studied by using density functional theory calculations corrected by on-site Coulomb interactions (DFT + U). Oxygen vacancies on the surface are determined to be able to significantly affect the behavior of H by modifying the charge of surface lattice O through the occurrence of Ce3+. It has been found that, at the reduced CeO2(111) surface, the adsorption strength of H as well as the H coupling barrier can be dramatically reduced compared to those at the stoichiometric surface, while H2O formation barrier is not significantly affected. Moreover, the diffusion of H at the reduced surface or into the bulk can occur more readily than that at stoichiometric CeO2(111).