Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters
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 <1 nm size-scale the reaction exhibits characteristics consistent with structure sensitivity, in contrast to structure insensitivity found for larger particles. The onset of catalysed hydrogenation occurs for Ptn (n≥10) clusters at T>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. As a result, control of sub-nanometre particle size may be used for tuning catalysed hydrogenation activity and selectivity.
- Authors:
-
- Technische Univ. Munchen, Garching (Germany)
- Air Force Research Lab., Elgin, FL (United States); Technische Univ. Munchen, Garching (Germany)
- Georgia Institute of Technology, Atlanta, GA (United States)
- Publication Date:
- Research Org.:
- Georgia Institute of Technology, Atlanta, GA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1242980
- Grant/Contract Number:
- FG05-86ER45234
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical sciences; catalysis; materials science; physical chemistry
Citation Formats
Crampton, Andrew S., Rötzer, Marian D., Ridge, Claron J., Schweinberger, Florian F., Heiz, Ueli, Yoon, Bokwon, and Landman, Uzi. Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters. United States: N. p., 2016.
Web. doi:10.1038/ncomms10389.
Crampton, Andrew S., Rötzer, Marian D., Ridge, Claron J., Schweinberger, Florian F., Heiz, Ueli, Yoon, Bokwon, & Landman, Uzi. Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters. United States. https://doi.org/10.1038/ncomms10389
Crampton, Andrew S., Rötzer, Marian D., Ridge, Claron J., Schweinberger, Florian F., Heiz, Ueli, Yoon, Bokwon, and Landman, Uzi. Thu .
"Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters". United States. https://doi.org/10.1038/ncomms10389. https://www.osti.gov/servlets/purl/1242980.
@article{osti_1242980,
title = {Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters},
author = {Crampton, Andrew S. and Rötzer, Marian D. and Ridge, Claron J. and Schweinberger, Florian F. and Heiz, Ueli and Yoon, Bokwon and Landman, Uzi},
abstractNote = {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 <1 nm size-scale the reaction exhibits characteristics consistent with structure sensitivity, in contrast to structure insensitivity found for larger particles. The onset of catalysed hydrogenation occurs for Ptn (n≥10) clusters at T>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. As a result, control of sub-nanometre particle size may be used for tuning catalysed hydrogenation activity and selectivity.},
doi = {10.1038/ncomms10389},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Thu Jan 28 00:00:00 EST 2016},
month = {Thu Jan 28 00:00:00 EST 2016}
}
Web of Science
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