文献类型：期刊文献

英文题名：Pt-O4 moiety induced electron localization toward In2O-Triggered acetylene Semi-Hydrogenation

作者：Li, Yurou[1];Cao, Yueqiang[1];Ge, Xiaohu[1];Zhang, Hao[2];Yan, Kelin[1];Zhang, Jing[1];Qian, Gang[1];Jiang, Zheng[3,4];Gong, Xueqing[5,6];Li, Aoming[7];Zhou, Xinggui[1];Yuan, Weikang[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Soochow Univ, Inst Funct Nano & Soft Mat Lab FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China;[3]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China;[4]Chinese Acad Sci, Shanghai Adv Res Inst, Zhangiiang Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China;[5]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[7]TILON Grp Technol Ltd, Div China, Shanghai, Peoples R China

年份：2022

卷号：407

起止页码：290

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20220811697559);WOS:【SCI-EXPANDED(收录号:WOS:000779720900001)】；

基金：Acknowledgement This work was financially supported by the Natural Science Foundation of China (21922803 and 22008067) , the Innovation Program of Shanghai Municipal Education Commission, the Pro-gram of Shanghai Academic/Technology Research Leader (21XD1421000) , the China Postdoctoral Science Foundation (2020 M681202 and 2021 T140204) . We thank the BL14W1 XAFS beamline of Shanghai Synchrotron Radiation Facility (SSRF) for providing beamtime.

语种：英文

外文关键词：Acetylene semi-hydrogenation; Pt-O-4 moiety; Ensemble site; H-2 activation; Atomic layer deposition

摘要：Transition metal oxides are emerging as promising catalysts for selective hydrogenations, but elaborating oxides catalysts with excellent hydrogenation activity remains challenging, especially at atomic level. Here, we report a theoretical-guided atomic design strategy with experimental verification to fabricate an excellent In2O3-based catalyst with an Pt-O-4-In2O ensemble site for acetylene semi-hydrogenation. Theoretical calculations reveal that the presence of Pt-O-4 moiety in the ensemble site increases the electron localization surrounding with the moiety and thus strengthens the frustrated Lewis pair of In-O within the In2O site adjacent to the moiety. These structure features contribute to a promoted activation of hydrogen on the ensemble site via heterolytic dissociation and enhanced acetylene semi hydrogenation on the oxygen vacancy adjacent to the Pt-O-4 moiety. The Pt-1-In2O3 catalyst featured with the ensemble site was synthesized by atomic layer deposition technology and characterized by multiple technologies, including atomic-resolution electron microscopy, X-ray absorption spectroscopy, and H-2-D-2 exchange experiments, to validate the theoretical predictions. As expected, the experimental results elucidate an enhanced activation of hydrogen, and a full conversion of acetylene with 91% of ethylene selectivity on the Pt-1-In2O3 catalyst, which is remarkably higher than those of the pristine In2O3 catalyst. (C) 2022 Elsevier Inc. All rights reserved.