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• W4210362764 endingPage "1981" @default.
• W4210362764 startingPage "1972" @default.
• W4210362764 abstract "Supported subnano-cluster catalysts are highly dynamic, developing true active sites only under the pressures and temperatures of reaction conditions. Operando X-ray absorption near-edge structure (XANES) spectroscopy can track changes in the oxidation state and the local environment of cluster atoms, providing insight into the development of these active sites. While bulk metal, oxide, and hydroxide standards are often used for fitting experimental XANES spectra to obtain average oxidation states, we recently showed that computed cluster standards of relevant compositions are a more suitable basis, producing more accurate fits. Here, we theoretically interpret the operando XANES of supported Cu3Pd and Cu4 clusters during temperature-programmed reaction (TPRx) of oxidative dehydrogenation of propane. We use an expanded basis set including both globally optimized computed clusters and bulk standards. Not only can we track reversible composition/oxidation state change with temperature, but also the irreversible growth of the bulk fraction upon heating, which we attribute to cluster sintering. This has important implications for the mechanism of the catalyzed reaction and the nature of the available active sites. We propose that operando XANES provides most significant insight into the nature of supported cluster catalysts in reaction conditions when interpreted using mixed computed cluster and bulk standards." @default.
• W4210362764 created "2022-02-08" @default.
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• W4210362764 creator A5063093801 @default.
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• W4210362764 date "2022-01-20" @default.
• W4210362764 modified "2023-09-25" @default.
• W4210362764 title "Interpreting the<i>Operando</i>X-ray Absorption Near-Edge Structure of Supported Cu and CuPd Clusters in Conditions of Oxidative Dehydrogenation of Propane: Dynamic Changes in Composition and Size" @default.
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• W4210362764 doi "https://doi.org/10.1021/acs.jpcc.1c10356" @default.
• W4210362764 hasPublicationYear "2022" @default.
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