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

Andrew S. Crampton, Marian D. Rötzer, Claron J. Ridge, Florian F. Schweinberger, Ueli Heiz, Bokwon Yoon and Uzi Landman ()
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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
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

Nature Communications, 2016, vol. 7, issue 1, 1-12

Abstract: 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.

Date: 2016
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DOI: 10.1038/ncomms10389

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