文献类型：期刊文献

中文题名：Influence of Cl substitution on the electronic structure and catalytic activity of ceria

英文题名：Influence of Cl substitution on the electronic structure and catalytic activity of ceria

作者：Li-Li Yin[1,2];Xue-Qing Gong[1,2]

机构：[1]Key Laboratory for Advanced Materials;[2]Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology

年份：2015

卷号：58

期号：4

起止页码：601

中文期刊名：Science China Chemistry

外文期刊名：中国科学（化学英文版）

收录：Scopus;CSCD:【CSCD2015_2016】；PubMed;

基金：supported by the National Basic Research Program of China(2011CB808505);the National Natural Science Foundation of China(21322307,21421004);the"Shu Guang"project of Shanghai Municipal Education Commission;Shanghai Education Development Foundation(13SG30)for financial support

语种：英文

中文关键词：cerium dioxide; Cl substitution; DFT＋U; O2 adsorption; CO oxidation

外文关键词：二氧化铈;催化活性;电子结构;氯;密度泛函理论;物理化学性质;计算结果;交互系统

摘要：Cl-containing cerium dioxide(Ce O2) catalysts have been found to exhibit unique catalytic activities. In the present work, using density functional theory calculations with the inclusion of on-site Coulomb correction, we systematically studied the effect of Cl on the physicochemical properties of Ce O2 surfaces by substituting one subsurface O with Cl. The calculated results show that substituting an O atom with a Cl atom results in structural distortion and the reduction of one surface Ce4+ cation to Ce3+. The protruding Ce3+ cation greatly improves the adsorption energy of O2 to produce an active O2- species, and maintains the catalytic oxidation cycle of CO on Ce O2(110). These results may help us obtain a better understanding of Cl-ceria interacting systems and provide some guidance for the design of effective Ce O2-based catalysts.
Cl-containing cerium dioxide （CeO2） catalysts have been found to exhibit unique catalytic activities. In the present work, using density functional theory calculations with the inclusion of on-site Coulomb correction, we systematically studied the effect of Cl on the physicochemical properties of CeO2 surfaces by substituting one subsurface O with Cl. The calculated results show that substituting an O atom with a Cl atom results in structural distortion and the reduction of one surface Ce4＋ cation to Ce3＋. The protruding Ce3＋ cation greatly improves the adsorption energy of O2 to produce an active O2- species, and maintains the catalytic oxidation cycle of CO on CeO2（110）. These results may help us obtain a better understanding of Cl-ceria interacting systems and provide some guidance for the design of effective CeO2-based catalysts.