Nanoengineering the active site in heterogeneous catalysis

Adam F. Lee, Christine V. Ellis, Mark A. Newton, Chris M.A. Parlett, Karen Wilson

    Research output: Contribution to journalConference articlepeer-review

    Abstract

    Here we demonstrate the first application of time-resolved synchrotron X-ray absorption spectroscopy to simultaneously follow dynamic nanoparticle surface restructuring and the evolution of surface and gas-phase products during an organic reaction. Surface palladium oxide, and not metal, is identified as the catalytic species responsible for the selective oxidation (selox) of crotyl alcohol to crotonaldehyde. Elevated reaction temperatures facilitate reversible nanoparticle redox processes, and concomitant catalytic selectivity loss, in response to reaction conditions. These discoveries highlight the importance of stabilizing surface palladium oxide and minimizing catalyst reducibility in order to achieve high selox yields, and will aid the future design of Pd-derived selox catalysts. This discovery has important implications for the design of future liquid and vapor phase selox catalysts, and the thermochemical behavior of Pd nanostructures in general.

    Original languageEnglish
    JournalACS National Meeting Book of Abstracts
    Publication statusPublished - 1 Dec 2011
    Event242nd ACS National Meeting and Exposition - Denver, CO, United States
    Duration: 28 Aug 20111 Sept 2011

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