文献类型：期刊文献

英文题名：Catalytic activities of CeO2(110)-2 x 1 reconstructed surface

作者：Zhang, Jie[1,2,3];Gong, Xue-Qing[1,2,3];Lu, Guanzhong[1]

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

年份：2015

卷号：632

起止页码：164

外文期刊名：SURFACE SCIENCE

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000347605600024)】；

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), Shanghai Rising-Star Program (12QH1400700) and "Shu Guang" project of Shanghai Municipal Education Commission and Shanghai Education Development Foundation (13SG30). The authors also thank the computing time in the National Super Computing Center in Jinan.

语种：英文

外文关键词：DFT plus U; Cerium dioxide; Surface reconstruction; Oxygen vacancy; CO oxidation; Electron localization

摘要：Density functional theory calculations with on-site Coulomb interaction correction (DFT + U) have been performed to study the structures and catalytic activities of 2 x 1 reconstructed surface of CeO2(110). The reconstructed surface gives better thermal stability compared with the bulk truncated one and exhibits unique surface activity. We comprehensively calculated the O vacancy formation and diffusion on the reconstructed surface and found that the vacancy formation energy corresponding to the removal of one subsurface four-fold coordinated O is 1.71 eV only, which is smaller than that of the top-surface O vacancy or the sub-surface O vacancy at the bulk truncated surface. Accordingly, the O vacancy diffusion at 2 x 1 reconstructed surface is also much more feasible than that at the unreconstructed CeO2(110) with the highest diffusion barrier of only 0.84 eV. By calculating the detailed pathways of CO reaction with lattice O, we found that CO2 can directly occur without forming a bent negatively charged CO2- intermediate on the reconstructed surface, which may reduce the chance for the carbonate formation. It has also been clearly shown that strong localization characteristics of Ce 4f orbital indeed favor electron transfer from reaction intermediates to the CeO2 support. (C) 2014 Elsevier B.V. All rights reserved.