@article{822acbcc713649efbae65c0a3c5f22fd,
title = "Dual Metal Active Sites in an Ir1/FeOx Single-Atom Catalyst: A Redox Mechanism for the Water-Gas Shift Reaction",
abstract = "Herein, we report a theoretical and experimental study of the water-gas shift (WGS) reaction on Ir1/FeOx single-atom catalysts. Water dissociates to OH* on the Ir1 single atom and H* on the first-neighbour O atom bonded with a Fe site. The adsorbed CO on Ir1 reacts with another adjacent O atom to produce CO2, yielding an oxygen vacancy (Ovac). Then, the formation of H2 becomes feasible due to migration of H from adsorbed OH* toward Ir1 and its subsequent reaction with another H*. The interaction of Ir1 and the second-neighbouring Fe species demonstrates a new WGS pathway featured by electron transfer at the active site from Fe3+−O⋅⋅⋅Ir2+−Ovac to Fe2+−Ovac⋅⋅⋅Ir3+−O with the involvement of Ovac. The redox mechanism for WGS reaction through a dual metal active site (DMAS) is different from the conventional associative mechanism with the formation of formate or carboxyl intermediates. The proposed new reaction mechanism is corroborated by the experimental results with Ir1/FeOx for sequential production of CO2 and H2.",
keywords = "active sites, density functional theory, redox mechanism, single-atom catalysts, water-gas shift reaction",
author = "Liang, {Jin Xia} and Jian Lin and Jingyue Liu and Xiaodong Wang and Tao Zhang and Jun Li",
note = "Funding Information: This work was supported by the National Science Foundation of China (Nos. 21763006, 21878283, 21576251, 91645203 and 21590792), the Natural Science Foundation of the Department of Education of Guizhou Province (No. QJTD[2015]55), and the Youth Innovation Promotion Association CAS (2017223). The support of Guangdong Provincial Key Laboratory of Catalysis (No. 2020B121201002) is also acknowledged. J.L. acknowledges the start‐up fund of the College of Liberal Arts and Sciences of Arizona State University and the use of facilities in the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University. This project is partially supported by the Open Fund of Shaanxi Key Laboratory of Catalysis to J.X.L. (No. SXKLC‐2017‐01). The beam line 14W at Shanghai Synchrotron Radiation Facility for EXAFS and XANES experiments are gratefully acknowledged. The calculations were performed by using supercomputers at SUSTech and Shanghai Supercomputing Center. Funding Information: This work was supported by the National Science Foundation of China (Nos. 21763006, 21878283, 21576251, 91645203 and 21590792), the Natural Science Foundation of the Department of Education of Guizhou Province (No. QJTD[2015]55), and the Youth Innovation Promotion Association CAS (2017223). The support of Guangdong Provincial Key Laboratory of Catalysis (No. 2020B121201002) is also acknowledged. J.L. acknowledges the start-up fund of the College of Liberal Arts and Sciences of Arizona State University and the use of facilities in the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University. This project is partially supported by the Open Fund of Shaanxi Key Laboratory of Catalysis to J.X.L. (No. SXKLC-2017-01). The beam line 14W at Shanghai Synchrotron Radiation Facility for EXAFS and XANES experiments are gratefully acknowledged. The calculations were performed by using supercomputers at SUSTech and Shanghai Supercomputing Center. Publisher Copyright: {\textcopyright} 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Copyright: Copyright 2020 Elsevier B.V., All rights reserved.",
year = "2020",
month = jul,
day = "27",
doi = "10.1002/anie.201914867",
language = "English (US)",
volume = "59",
pages = "12868--12875",
journal = "Angewandte Chemie - International Edition",
issn = "1433-7851",
publisher = "John Wiley and Sons Ltd",
number = "31",
}