文献类型：期刊文献

英文题名：Origin of Efficient Catalytic Combustion of Methane over Co3O4(110): Active Low-Coordination Lattice Oxygen and Cooperation of Multiple Active Sites

作者：Hu, Wende[1,2];Lan, Jinggang[1,2];Guo, Yun[1,2];Cao, Xiao-Ming[1,2];Hu, P.[1,2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2016

卷号：6

期号：8

起止页码：5508

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20163302717732);WOS:【SCI-EXPANDED(收录号:WOS:000381236700078)】；

基金：This project was supported financially by the NSFC (21333003, 21303051), the Shanghai Natural Science Foundation (13ZR1453000), and the Fundamental Research Funds for the Central Universities. The authors also acknowledge the support from the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) for computing time.

语种：英文

外文关键词：spinel cobalt oxides; DFT; methane combustion; C-H bond activation; multiple active sites

摘要：A complete catalytic cycle for methane combustion on the Co3O4(110) surface was investigated and compared with that on the Co3O4(100) surface on the basis of first-principles calculations. It is found that the 2-fold coordinated lattice oxygen (O-2c) would be of vital importance for methane combustion over Co3O4 surfaces, especially for the first two C-H bond activations and the C-O bond coupling. It could explain the reason the Co3O4(110) surface significantly outperforms the Co3O4(100) surface without exposed O-2c for methane combustion. More importantly, it is found that the cooperation of homogeneous multiple sites for multiple elementary steps would be indispensable. It not only facilitates the hydrogen transfer between different sites for the swift formation of H2O to effectively avoid the passivation of the active low-coordinated O-2c site but also stabilizes surface intermediates during the methane oxidation, optimizing the reaction channel. An understanding of this cooperation of multiple active sites not only might be beneficial in developing improved catalysts for methane combustion but also might shed light on one advantage of heterogeneous catalysts with multiple sites in comparison to single-site catalysts for catalytic activity.