Alumina-supported sub-nanometer Pt_(10) clusters: amorphization and role of the support material in a highly active CO oxidation catalyst
Abstract
Catalytic CO oxidation is unveiled on size-selected Pt_(10) clusters deposited on two very different ultrathin (≈0.5–0.7 nm thick) alumina films: (i) a highly ordered alumina obtained under ultra-high vacuum (UHV) by oxidation of the NiAl(110) surface and (ii) amorphous alumina obtained by atomic layer deposition (ALD) on a silicon chip that is a close model of real-world supports. Notably, when exposed to realistic reaction conditions, the Pt_(10)/UHV-alumina system undergoes a morphological transition in both the clusters and the substrate, and becomes closely akin to Pt_(10)/ALD-alumina, thus reconciling UHV-type surface-science and real-world experiments. The Pt_(10) clusters, thoroughly characterized via combined experimental techniques and theoretical analysis, exhibit among the highest CO oxidation activity per Pt atom reported for CO oxidation catalysts, due to the interplay of ultra-small size and support effects. A coherent interdisciplinary picture then emerges for this catalytic system.
Additional Information
© 2017 Royal Society of Chemistry. Received 21st December 2016. Accepted 2nd February 2017. First published on the web 3rd February 2017. The work at the Argonne National Laboratory (C. Y., E. C. T., 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. The Argonne authors thank Drs Joseph Libera and Jeffrey Elam for performing the ALD alumina-coating of the silicon chips used for cluster deposition and Dr Sungsik Lee for his assistance at sample preparations. A. F. gratefully acknowledges 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. CM and SN 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. Fruitful discussions with Drs Ingo Barke, Akansha Singh and Profs Prasenjit Sen and Hisato Yasumatsu are highly appreciated. C. Y., F. R. N., G. B., and A. B. contributed equally to this work.Attached Files
Supplemental Material - c6ta10989f1.pdf
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Additional details
- Eprint ID
- 75554
- Resolver ID
- CaltechAUTHORS:20170330-152134180
- DE-AC-02-06CH11357
- Department of Energy (DOE)
- European Social Fund
- Mecklenburg-Vorpommer
- Bundesministerium für Bildung und Forschung (BMBF)
- SFB652
- Deutsche Forschungsgemeinschaft (DFG)
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2017-03-30Created from EPrint's datestamp field
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2021-11-15Created from EPrint's last_modified field