期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 27, 页码 9083-9087出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201903298
关键词
copper; hydrogen; iron oxide; metal-support interactions; water-gas shift reaction
资金
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Shanghai Sailing Program [19YF1410600]
- Fundamental Research Funds for the Central Universities [222201718002]
- National Natural Science Foundation of China [21808057]
- National Science Foundation [CBET-1511689]
- U.S. DOE [DE-FG02-05ER15688, DE-AC02-98CH10886]
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.
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