文献类型：期刊文献

英文题名：A DFT + U study of CO oxidation at CeO2(110) and (111) surfaces with oxygen vacancies

作者：Song, Ya-Ling[1]; Yin, Li-Li[1]; Zhang, Jie[1]; Hu, P.[1]; Gong, Xue-Qing[1]; Lu, Guanzhong[1]

机构：[1] Key Laboratory for Advanced Materials, Centre for Computational Chemistry, East China University of Science and Technology, Shanghai 200237, China

年份：2013

卷号：618

起止页码：140

外文期刊名：Surface Science

收录：EI(收录号：20134316878138)

语种：英文

外文关键词：Oxidation - Cerium oxide - Density functional theory - Surface reactions

摘要：Density functional theory calculations corrected by on-site Coulomb interaction have been conducted to illuminate the effect of O vacancies on the surface reactivities toward direct CO oxidation at CeO2(110) and (111). CO adsorption at and further reaction with various surface O at the vacancy were systematically calculated, and extensive geometric and electronic analyses were also performed to understand the calculation results. It has been shown that though the existence of O vacancy can reduce the activities of neighboring O as the barriers of elementary steps are generally higher than those at stoichiometric surfaces, the relative preference for CO2 desorption is also increased due to the missing of nearby O for carbonate formation. Moreover, our calculation results also showed that the characteristic localized 4f orbitals/electrons of Ce still play the key role in determining the surface reactivities as the vacancy induced localized electrons can hinder their further occurrence and the corresponding reactions. ? 2013 Elsevier B.V.