文献类型：期刊文献

英文题名：Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

作者：Cao, Yueqiang[1];Ge, Xiaohu[1];Li, Yurou[1];Si, Rui[2];Sui, Zhijun[1];Zhou, Jinghong[1];Duan, Xuezhi[1];Zhou, Xinggui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China

年份：2021

卷号：7

期号：1

起止页码：103

外文期刊名：ENGINEERING

收录：;EI(收录号：20210409825919);WOS:【SCI-EXPANDED(收录号:WOS:000632826600006)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803, 21776077, and 22008067), the Innovation Program of Shanghai Municipal Education Commission, the Shanghai Natural Science Foundation (17ZR1407300 and 17ZR1407500), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the Shanghai Rising-Star Program (17QA1401200), the China Postdoctoral Science Foundation (2020M681202), the Open Project of State Key Laboratory of Chemical Engineering (SKLChe-15C03), the State Key Laboratory of Organic-Inorganic Composites (oic-201801007), and the Fundamental Research Funds for the Central Universities (222201718003). We also thank the BL14W1 beam line of Shanghai Synchrotron Radiation Facility for the XAFS measurement.

语种：英文

外文关键词：Acetylene semi-hydrogenation; Reaction kinetics; Support effects; Electronic effects; Pd local environment

摘要：In this study, the support effects on the Pd-catalyzed semi-hydrogenation of acetylene have been investigated from the structural and kinetic perspectives. According to the results of kinetic analysis and X-ray photoelectron spectroscopy, hydrogen temperature-programmed reduction, temperature-programmed hydride decomposition, and in situ X-ray diffraction measurements, using carbon nanotubes as support for Pd nanocatalysts with various sizes instead of alpha-Al2O3 decreases the Pd-0 3d binding energy and suppresses the formation of undesirable palladium hydride species, thus increasing the ethylene yield. Furthermore, X-ray absorption spectroscopy, high-resolution transmission electron microscopy, and C2H4 temperature-programmed desorption studies combined with density-functional theory calculations reveal the existence of a unique Pd local environment, containing subsurface carbon atoms, that produces positive geometric effects on the acetylene conversion reaction. Therefore, tailoring the Pd local environment and electronic properties represents an effective strategy for the fabrication and design of highly active and selective Pd semi-hydrogenation catalysts. (C) 2020 THE AUTHORS. Published by Elsevier LTD on behalf of Chinese Academy of Engineering and Higher Education Press Limited Company.