文献类型：期刊文献

英文题名：Adsorption Site Regulation to Guide Atomic Design of Ni-Ga Catalysts for Acetylene Semi-Hydrogenation

作者：Cao, Yueqiang[1];Zhang, Hao[2,6];Ji, Shufang[3];Sui, Zhijun[1];Jiang, Zheng[2,7];Wang, Dingsheng[3];Zaera, Francisco[4,5];Zhou, Xinggui[1];Duan, Xuezhi[1];Li, Yadong[3]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China;[3]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;[4]Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA;[5]Univ Calif Riverside, UCR Ctr Catalysis, Riverside, CA 92521 USA;[6]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[7]Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China

年份：2020

卷号：59

期号：28

起止页码：11647

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20202108692586);WOS:【SCI-EXPANDED(收录号:WOS:000530678100001)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803 and 21776077), the Natural Science Foundation of Shanghai (17ZR1407300), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the Shanghai Rising-Star Program (17QA1401200), the Fundamental Research Funds for the Central Universities (222201718003) and the Open Project of State Key Laboratory of Chemical Engineering (SKL-Che-15C03). F.Z. acknowledges funding from the US National Science Foundation (CHE-1953843). 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; heterogeneous catalysis; Ni-Ga intermetallic catalyst; semi-hydrogenation; site regulation

摘要：Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory-guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi-hydrogenation processes. Such Ni sites show not only preferential acetylene pi-adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration-corrected high-resolution scanning transmission electron microscopy and X-ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi-atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.