文献类型：期刊文献

英文题名：Higher alcohols synthesis from syngas over CoCu/SiO2 catalysts: Dynamic structure and the role of Cu

作者：Su, Junjie[1];Zhang, Zhengpai[1];Fu, Donglong[1];Liu, Da[1];Xu, Xin-Chao[1];Shi, Bianfang[1];Wang, Xu[2];Si, Rui[2];Jiang, Zheng[2];Xu, Jing[1];Han, Yi-Fan[1,3]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[3]Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Peoples R China

年份：2016

卷号：336

起止页码：94

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20160902007721);WOS:【SCI-EXPANDED(收录号:WOS:000371944100010)】；

基金：The authors are grateful to the support from the National Natural Science Foundation of China (21273070, 21576084, and 91534127), International Cooperation Project of Shanghai Ministry of Science and Technology (14230710700), International Cooperation Project of Ministry of Science and Technology (2015DFG42570) and Chinese Education Ministry 111 project (B08021). The authors sincerely thank the staff from the BL14W1 beam line, Shanghai Synchrotron Radiation Facility (SSRF), for their generous help in XAS experiments.

语种：英文

外文关键词：Higher alcohols synthesis; Intrinsic kinetics; Syngas; Bimetallic CoCu catalysts; Promotional effects

摘要：A comparative study of higher alcohols synthesis directly from syngas has been performed over monometallic Co and bimetallic CoCu/SiO2 catalysts. Particularly, the role of Cu on the origin. of active sites and reaction mechanism were investigated thoroughly using multiple techniques such as ex situ X-rays diffraction (XRD), X-ray absorption spectroscopy (XAS) and Raman spectroscopy. Reduction process of CoCu/SiO2 catalysts was also determined using in situ XRD and in situ Raman spectroscopy while the surface structure of reduced catalysts was detected by CO-DRIFTS. CoCu bimetallic particles covered by Cu atoms are responsible for alcohols synthesis. The intrinsic kinetics was performed over both catalysts under realistic reaction conditions. By comparing the kinetic parameters, including apparent activation energies and reaction orders, the promotional effects of Cu have been identified as: (1) weakening the CO/HCO dissociation and reducing the formation of CH species; (2) controlling surface Co ensemble size and inhibiting CHx insertion. (C) 2016 Elsevier Inc. All rights reserved.