文献类型：期刊文献

英文题名：Evidence To Challenge the Universality of the Horiuti-Polanyi Mechanism for Hydrogenation in Heterogeneous Catalysis: Origin and Trend of the Preference of a Non-Horiuti-Polanyi Mechanism

作者：Yang, Bo[1,2];Gong, Xue-Qing[1,2];Wang, Hai-Feng[1,2];Cao, Xiao-Ming[1,2];Rooney, John J.[3];Hu, P.[1,2,3]

机构：[1]E China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]E 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：2013

卷号：135

期号：40

起止页码：15244

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20134316876386);WOS:【SCI-EXPANDED(收录号:WOS:000326356400050)】；

基金：This work is financially supported by National Key Basic Research Program of China (2013CB933201, 2010CB732300, and 2011CB808505), National Natural Science Foundation of China (21073060, 21333003 and 21303051), and "111" program (B08021). Computing time in the National Super Computing Center in Jinan is acknowledged.

语种：英文

外文关键词：Catalysis - Calculations - Aldehydes

摘要：The Horiuti-Polanyi mechanism has been considered to be universal for explaining the mechanisms of hydrogenation reactions in heterogeneous catalysis for several decades. In this work, we examine this mechanism for the hydrogenation of acrolein, the simplest alpha,beta-unsaturated aldehyde, in gold-based systems as well as some other metals using extensive first-principles calculations. It is found that a non-Horiuti-Polanyi mechanism is favored in some cases. Furthermore, the physical origin and trend of this mechanism are revealed and discussed regarding the geometrical and electronic effects, which will have a significant influence on current understandings on heterogeneous catalytic hydrogenation reactions and the future catalyst design for these reactions.