Negreiros, Fabio R. and Halder, Avik and Yin, Chunrong and Singh, Akansha and Barcaro, Giovanni and Sementa, Luca and Tyo, Eric C. and Pellin, Michael J. and Bartling, Stephan and Meiwes-Broer, Karl-Heinz and Seifert, Sönke and Sen, Prasenjit and Nigam, Sandeep and Majumder, Chiranjib and Fukui, Nobuyuki and Yasumatsu, Hisato and Vajda, Stefan and Fortunelli, Alessandro (2018) Bimetallic Ag-Pt Sub-nanometer Supported Clusters as Highly Efficient and Robust Oxidation Catalysts. Angewandte Chemie International Edition, 57 (5). pp. 1209-1213. ISSN 1433-7851. doi:10.1002/anie.201709784. https://resolver.caltech.edu/CaltechAUTHORS:20180102-160055526
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Abstract
A combined experimental and theoretical investigation of Ag-Pt sub-nanometer clusters as heterogeneous catalysts in the CO→CO_2 reaction (COox) is presented. Ag_9Pt_2 and Ag_9Pt_3 clusters are size-selected in the gas phase, deposited on an ultrathin amorphous alumina support, and tested as catalysts experimentally under realistic conditions and by first-principles simulations at realistic coverage. In situ GISAXS/TPRx demonstrates that the clusters do not sinter or deactivate even after prolonged exposure to reactants at high temperature, and present comparable, extremely high COox catalytic efficiency. Such high activity and stability are ascribed to a synergic role of Ag and Pt in ultranano-aggregates, in which Pt anchors the clusters to the support and binds and activates two CO molecules, while Ag binds and activates O_2, and Ag/Pt surface proximity disfavors poisoning by CO or oxidized species.
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| Additional Information: | © 2017 Wiley-VCH Verlag. Issue online: 22 January 2018; Version of record online: 29 December 2017; Accepted manuscript online: 14 December 2017; Manuscript Revised: 15 November 2017; Manuscript Received: 21 September 2017. The work at the Argonne National Laboratory (A.H., C.Y., E.C.T., M.J.P., S.V.) was supported by the U.S. Department of Energy, BES-Materials Science and Engineering, under Contract DE-AC-02–06CH11357, with UChicago Argonne, LLC, the operator of Argonne National Laboratory. The work at the Advanced Photon Source (S.S.) was supported by the US Department of Energy, Scientific User Facilities under Contract DE-AC-02–06CH11357 with UChicago Argonne LLC, the operator of Argonne National Laboratory. N.F. and H.Y. are grateful for the Special Cluster Research Project of Genesis Research Institute, Inc. H.Y. acknowledges JSPS Grant-in-Aid for Scientific Research (KAKENHI) (C) Grant Number 15K04594. A.F. gratefully acknowledge support from the ERC-AG SEPON project and the use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Computations on the Ag_9Pt_2 clusters were performed at the HPC cluster facility at HRI (http://www.hri.res.in/cluster/). C.M. and S.N. are thankful to the members of the Computer Division, BARC, for their kind cooperation during this work. S.B. acknowledges funding by the European Social Fund (ESF), the federal state Mecklenburg-Vorpommern within the project Nano4Hydrogen, the Federal Ministry of Education and Research (BMBF) within the project Light2Hydrogen, and the Deutsche Forschungsgemeinschaft (DFG) through the SFB652. The authors declare no conflict of interest. | ||||||||||||||||
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| Subject Keywords: | ab initio calculations; alloys; reaction mechanisms; supported catalysts; ultrathin oxide films | ||||||||||||||||
| Issue or Number: | 5 | ||||||||||||||||
| DOI: | 10.1002/anie.201709784 | ||||||||||||||||
| Record Number: | CaltechAUTHORS:20180102-160055526 | ||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20180102-160055526 | ||||||||||||||||
| Official Citation: | F. R. Negreiros, A. Halder, C. Yin, A. Singh, G. Barcaro, L. Sementa, E. C. Tyo, M. J. Pellin, S. Bartling, K.-H. Meiwes-Broer, S. Seifert, P. Sen, S. Nigam, C. Majumder, N. Fukui, H. Yasumatsu, S. Vajda, A. Fortunelli, Angew. Chem. Int. Ed. 2018, 57, 1209 | ||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||
| ID Code: | 84041 | ||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||
| Deposited By: | George Porter | ||||||||||||||||
| Deposited On: | 03 Jan 2018 15:32 | ||||||||||||||||
| Last Modified: | 15 Nov 2021 20:16 |
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