文献类型：期刊文献

英文题名：Unexpected C-C Bond Cleavage Mechanism in Ethylene Combustion at Low Temperature: Origin and Implications

作者：Wang, Hai-Feng[1,2];Wang, Dong[1,2];Liu, Xiaohui[1,2];Guo, Yang-Long[1,2];Lu, Guan-Zhong[1,2];Hu, Peijun[1,2,3]

机构：[1]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, 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：5393

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20163302717572);WOS:【SCI-EXPANDED(收录号:WOS:000381236700065)】；

基金：This work was supported by 973 Program (No. 2013CB933201), NSFC (Nos. 21421004, 21303052, 21333003), Shanghai Rising-Star Program (No. 14QA1401100) and Chen-Guang project (No. 13CG24), Fundamental Research Funds for the Central Universities. H.F.W. also thanks the Special Program for Applied Research on Super Computation of the NSFC-Guandong Joint Fund (the second phase) for computing time.

语种：英文

外文关键词：C-C bond activation; DFT; valency-saturation-driven mechanism; heterogeneous catalysis; Co3O4

摘要：Achieving low-temperature C=C bond activation has been of interest in heterogeneous catalysis, and understanding the subject (i.e., establishing the mechanism and identifying the origin) is desirable. Herein, taking the CH2CH2 combustion on spinel Co3O4(110) as an example, we report a systematic investigation on the C-C bond breaking processes using first principles calculations. An unexpected pathway for C-C cracking, called the valency-saturation-driven mechanism, is determined, and the high activity of Co3O4 in catalyzing CH2CH2 combustion at low temperature is rationalized. More importantly, some basic C-C bond activation rules on metal oxides with isolated single-atom sites, which differ from the traditional metal catalysis with multiatom active sites, are revealed. The understandings derived from this work may underpin the structure activity relationship in oxide catalysis.