文献类型：期刊文献

英文题名：Strong Metal-Support Interactions between Copper and Iron Oxide during the High-Temperature Water-Gas Shift Reaction

作者：Zhu, Minghui[1];Tian, Pengfei[1];Kurtz, Ravi[2];Lunkenbein, Thomas[3];Xu, Jing[1];Schloegl, Robert[3];Wachs, Israel E.[2];Han, Yi-Fan[1,4]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Lehigh Univ, Dept Chem & Biomol Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA 18015 USA;[3]Fritz Haber Inst Max Planck Gesell, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany;[4]Zhengzhou Univ, Sch Chem Engn & Energy, Res Ctr Heterogeneous Catalysis & Engn Sci, Zhengzhou 450001, Henan, Peoples R China

年份：2019

卷号：58

期号：27

起止页码：9083

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20192907182261);WOS:【SCI-EXPANDED(收录号:WOS:000476691200019)】；

基金：This work was sponsored by the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Shanghai Sailing Program (19YF1410600) and the Fundamental Research Funds for the Central Universities (222201718002). P.T. acknowledges the support from National Natural Science Foundation of China (No. 21808057). I.E.W. and R.K. acknowledge the financial support from National Science Foundation Grant CBET-1511689. We thank Prof. Anatoly Frenkel for collaborating with us on the XAS measurements and analysis. Beamline X18A of the NSLS is supported in part by the U.S. DOE Grant No. DE-FG02-05ER15688. The NSLS is supported by U.S. DOE Contract No. DE-AC02-98CH10886. Dr. Henry Luftman is thanked for assisting with the collection of the HS-LEIS data. We appreciate the generous help in XAS experiments from the staff of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF).

语种：英文

外文关键词：copper; hydrogen; iron oxide; metal-support interactions; water-gas shift reaction

摘要：The commercial high-temperature water-gas shift (HT-WGS) catalyst consists of CuO-Cr2O3-Fe2O3, where Cu functions as a chemical promoter to increase the catalytic activity, but its promotion mechanism is poorly understood. In this work, a series of iron-based model catalysts were investigated with in situ or pseudo in situ characterization, steady-state WGS reaction, and density function theory (DFT) calculations. For the first time, a strong metal-support interaction (SMSI) between Cu and FeOx was directly observed. During the WGS reaction, a thin FeOx overlayer migrates onto the metallic Cu particles, creating a hybrid surface structure with Cu-FeOx interfaces. The synergistic interaction between Cu and FeOx not only stabilizes the Cu clusters, but also provides new catalytic active sites that facilitate CO adsorption, H2O dissociation, and WGS reaction. These new fundamental insights can potentially guide the rational design of improved iron-based HT-WGS catalysts.