Assessing the concept of structure sensitivity or insensitivity for sub-nanometer catalyst materials

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

doi:10.1016/j.susc.2016.02.006

Title: Assessing the concept of structure sensitivity or insensitivity for sub-nanometer catalyst materials

Journal Article · Sat Feb 13 00:00:00 EST 2016 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2016.02.006· OSTI ID:1534354

Crampton, Andrew S. ^[1]; Rötzer, Marian D. ^[1]; Ridge, Claron J. ^[2]; Yoon, Bokwon ^[3]; Schweinberger, Florian F. ^[1]; Landman, Uzi ^[3]; Heiz, Ueli ^[1]

Technische University, Munich (Germany)
Technische University, Munich (Germany); Air Force Research Laboratory (AFRL), Eglin Air Force Base, FL (United States)
Georgia Institute of Technology, Atlanta, GA (United States)

In this report the nature of the nano-catalyzed hydrogenation of ethylene, yielding benchmark information pertaining to the concept of structure sensitivity/insensitivity and its applicability at the bottom of the catalyst particle size-range, is explored with experiments on size-selected Ptn (n = 7–40) clusters soft-landed on MgO, in conjunction with first-principles simulations. As in the case of larger particles both the direct ethylene hydrogenation channel and the parallel hydrogenation–dehydrogenation ethylidyne-producing route must be considered, with the fundamental uncovering that at the < 1 nm size-scale the reaction exhibits characteristics consistent with structure sensitivity, in contrast to the structure insensitivity found for larger particles. In this size-regime, the chemical properties can be modulated and tuned by a single atom, reflected by the onset of low temperature hydrogenation at T > 150 K catalyzed by Pt_n (n ≥ 10) clusters, with maximum room temperature reactivity observed for Pt₁₃ using a pulsed molecular beam technique. Structure insensitive behavior, inherent for specific cluster sizes at ambient temperatures, can be induced in the more active sizes, e.g. Pt₁₃, by a temperature increase, up to 400 K, which opens dehydrogenation channels leading to ethylidyne formation. This reaction channel was, however found to be attenuated on Pt₂₀, as catalyst activity remained elevated after the 400 K step. Pt₃₀ displayed behavior which can be understood from extrapolating bulk properties to this size range; in particular the calculated d-band center. In the non-scalable sub-nanometer size regime, however, precise control of particle size may be used for atom-by-atom tuning and manipulation of catalyzed hydrogenation activity and selectivity.

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Research Organization:: Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); European Research Council (ERC); German Research Foundation (DFG); Air Force Office for Scientific Research (AFOSR)

Grant/Contract Number:: FG05-86ER45234; 246645-ASC3; He3454/23-1; FA9550-15-1-0519

OSTI ID:: 1534354

Alternate ID(s):: OSTI ID: 1397343

Journal Information:: Surface Science, Vol. 652, Issue C; ISSN 0039-6028

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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Title: Assessing the concept of structure sensitivity or insensitivity for sub-nanometer catalyst materials

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