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Boron Switch for Selectivity of Catalytic Dehydrogenation on Size-Selected Pt Clusters on Al2O3.


Size-selected supported clusters of transition metals can be remarkable and highly tunable catalysts. A particular example is Pt clusters deposited on alumina, which have been shown to dehydrogenate hydrocarbons in a size-specific manner. Pt7, of the three sizes studied, is the most active and, therefore, like many other catalysts, deactivates by coking during reactions in hydrocarbon-rich environments. Using a combination of experiment and theory, we show that nanoalloying Pt7 with boron modifies the alkene-binding affinity to reduce coking. From a fundamental perspective, the comparison of experimental and theoretical results shows the importance of considering not simply the most stable cluster isomer, but rather the ensemble of accessible structures as it changes in response to temperature and reagent coverage.

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