Bimetallic Ag‐Pt Sub‐nanometer Supported Clusters as Highly Efficient and Robust Oxidation Catalysts

A combined experimental and theoretical investigation of Ag‐Pt sub‐nanometer clusters as heterogeneous catalysts in the CO→CO2 reaction (COox) is presented. Ag9Pt2 and Ag9Pt3 clusters are size‐selected in the gas phase, deposited on an ultrathin amorphous alumina support, and tested as catalysts exp...

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Published in:Angewandte Chemie (International ed.) 2018-01, Vol.57 (5), p.1209-1213
Main Authors: Negreiros, Fabio R., Halder, Avik, Yin, Chunrong, Singh, Akansha, Barcaro, Giovanni, Sementa, Luca, Tyo, Eric C., Pellin, Michael J., Bartling, Stephan, Meiwes‐Broer, Karl‐Heinz, Seifert, Sönke, Sen, Prasenjit, Nigam, Sandeep, Majumder, Chiranjib, Fukui, Nobuyuki, Yasumatsu, Hisato, Vajda, Stefan, Fortunelli, Alessandro
Format: Article
Language:English
Subjects:
Ab initio calculations
Alloys
Aluminum oxide
Bimetals
Carbon dioxide
Catalysis
Catalysts
Clusters
Cobalt
Deactivation
First principles
High temperature
Oxidation
Platinum
Reaction mechanisms
Silver
Supported Catalysts
Ultrathin Oxide Films
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Summary:A combined experimental and theoretical investigation of Ag‐Pt sub‐nanometer clusters as heterogeneous catalysts in the CO→CO2 reaction (COox) is presented. Ag9Pt2 and Ag9Pt3 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 O2, and Ag/Pt surface proximity disfavors poisoning by CO or oxidized species. Ag9Pt2 and Ag9Pt3 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 show comparable, high COox catalytic efficiency.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201709784