Unexpected C–C Bond Cleavage Mechanism in Ethylene Combustion at Low Temperature: Origin and Implications

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• 作者：Hai-Feng Wang ; Dong Wang ; Xiaohui Liu ; Yang-Long Guo ; Guan-Zhong Lu ; Peijun Hu
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：August 5, 2016
• 年：2016
• 卷：6
• 期：8
• 页码：5393-5398
• 全文大小：362K
• 年卷期：0
• ISSN：2155-5435

文摘

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.