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Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters

Author

Listed:
  • Andrew S. Crampton

    (Chair of Physical Chemistry, Catalysis Research Center, Technische Universität München)

  • Marian D. Rötzer

    (Chair of Physical Chemistry, Catalysis Research Center, Technische Universität München)

  • Claron J. Ridge

    (Chair of Physical Chemistry, Catalysis Research Center, Technische Universität München
    Air Force Research Laboratory, Energetic Materials Branch)

  • Florian F. Schweinberger

    (Chair of Physical Chemistry, Catalysis Research Center, Technische Universität München)

  • Ueli Heiz

    (Chair of Physical Chemistry, Catalysis Research Center, Technische Universität München)

  • Bokwon Yoon

    (School of Physics, Georgia Institute of Technology)

  • Uzi Landman

    (School of Physics, Georgia Institute of Technology)

Abstract

The sensitivity, or insensitivity, of catalysed reactions to catalyst structure is a commonly employed fundamental concept. Here we report on the nature of nano-catalysed ethylene hydrogenation, investigated through experiments on size-selected Ptn (n=8–15) clusters soft-landed on magnesia and first-principles simulations, yielding benchmark information about the validity of structure sensitivity/insensitivity at the bottom of the catalyst size range. Both ethylene-hydrogenation-to-ethane and the parallel hydrogenation–dehydrogenation ethylidyne-producing route are considered, uncovering that at the 150 K, with maximum room temperature reactivity observed for Pt13. Structure insensitivity, inherent for specific cluster sizes, is induced in the more active Pt13 by a temperature increase up to 400 K leading to ethylidyne formation. Control of sub-nanometre particle size may be used for tuning catalysed hydrogenation activity and selectivity.

Suggested Citation

  • Andrew S. Crampton & Marian D. Rötzer & Claron J. Ridge & Florian F. Schweinberger & Ueli Heiz & Bokwon Yoon & Uzi Landman, 2016. "Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters," Nature Communications, Nature, vol. 7(1), pages 1-12, April.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms10389
    DOI: 10.1038/ncomms10389
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