文献类型：期刊文献

英文题名：Increasing the Distance of Adjacent Palladium Atoms for Configuration Matching in Selective Hydrogenation

作者：Ge, Xiaohu[1];Cao, Yueqiang[1];Yan, Kelin[1];Li, Yurou[1];Zhou, Lihui[2,3];Dai, Sheng[2,3];Zhang, Jing[1];Gong, Xueqing[4,5];Qian, Gang[1];Zhou, Xinggui[1];Yuan, Weikang[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China

年份：2022

卷号：61

期号：51

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20224913212725);WOS:【SCI-EXPANDED(收录号:WOS:000888889900001)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803, 22008067, 22008074 and 22178100), the Innovation Program of Shanghai Municipal Education Commission, the Shanghai Science and Technology Innovation Action Plan (22JC1403800), the Program of Shanghai Academic/Technology Research Leader (21XD1421000), the Natural Science Foundation of Shanghai (20ZR1415700), the China Postdoctoral Science Foundation (2020M681202 and 2021T140204). We highly appreciate Dr. Xi Liu and Mr. Zhouhong Ren at Shanghai Jiao Tong University for their help with the HAADF-STEM measurements. We thank the BL14W1 XAFS beamline of Shanghai Synchrotron Radiation Facility (SSRF) for providing beamtime.

语种：英文

外文关键词：Configuration Matching; Intermetallic Compounds; Local Environment; Selective Hydrogenation; Site Distance

摘要：Precisely tailoring the distance between adjacent metal sites to match adsorption configurations of key species for the targeted reaction pathway is a great challenge in heterogeneous catalysis. Here, we report a proof-of-concept study on the atomically sites-tailored pathway in Pd-catalyzed acetylene hydrogenation, i.e., increasing the distance of adjacent Pd atoms (d(Pd-a-Pd)) for configuration matching in acetylene semi-hydrogenation against coupling. d(Pd-a-Pd) is identified as a structural descriptor for describing the competitiveness for reaction pathways, and the increased d(Pd-a-Pd) prefers the semi-hydrogenation pathway due to simultaneously promoted C2H4 desorption and the destabilized transition state of the C2H3* coupling. Spectroscopic, kinetics and electronic structure studies reveal that increasing d(Pd-a-Pd) to 3.31 angstrom delivers superior selectivity and stability due to energy matching and appropriate hybridization of Pd 4d with In 2s and, especially, 2p orbitals.