Catalytic methane oxidation is kinetically challenging, as it requires activating the strongest C-H bond among all hydrocarbons, which occurs most effectively on Pd containing catalysts. Here, we describe the active site modifications, the structural dynamics, and the catalytic effects when incorporating Pt into Pd catalysts. In reducing atmosphere, Pt-Pd clusters form alloy, with their surface and bulk chemical compositions depend markedly on the cluster size. Contacting these clusters to oxidizing atmosphere converts the Pt-Pd alloy clusters into a core-shell structure, where a thin PdO shell layer covering the underneath Pt core. This structural transition creates Pd2+-O2- site pairs residing on the Pt-rich core that are highly effective for the initial activation of the C-H bond in methane. These site pairs cleave the C-H bond of methane at an intrinsic barrier of 37 kJ mol-1, much smaller than those on monometallic PdO and on O* covered Pt clusters.

Structural transition of Pd and Pt bimetallic clusters and their reactivity for methane oxidation catalysis

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.