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Title: Subnanometer platinum clusters highly active and selective catalysts for the oxidative dehydrogenation of propane.

Abstract

Small clusters are known to possess reactivity not observed in their bulk analogues, which can make them attractive for catalysis. Their distinct catalytic properties are often hypothesized to result from the large fraction of under-coordinated surface atoms. Here, we show that size-preselected Pt{sub 8-10} clusters stabilized on high-surface-area supports are 40-100 times more active for the oxidative dehydrogenation of propane than previously studied platinum and vanadia catalysts, while at the same time maintaining high selectivity towards formation of propylene over by-products. Quantum chemical calculations indicate that under-coordination of the Pt atoms in the clusters is responsible for the surprisingly high reactivity compared with extended surfaces. We anticipate that these results will form the basis for development of a new class of catalysts by providing a route to bond-specific chemistry, ranging from energy-efficient and environmentally friendly synthesis strategies to the replacement of petrochemical feedstocks by abundant small alkanes.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
957391
Report Number(s):
ANL/CSE/JA-63277
TRN: US201002%%959
DOE Contract Number:  
DE-AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Nature Mater.
Additional Journal Information:
Journal Volume: 8; Journal Issue: Mar. 2009
Country of Publication:
United States
Language:
ENGLISH
Subject:
02 PETROLEUM; ALKANES; ATOMS; CATALYSIS; CATALYSTS; CHEMICAL FEEDSTOCKS; CHEMISTRY; DEHYDROGENATION; PETROCHEMICALS; PLATINUM; PROPANE; PROPYLENE; SYNTHESIS

Citation Formats

Vajda, S, Pellin, M. J., Greeley, J. P., Marshall, C. L., Curtiss, L. A., Ballentine, G. A., Elam, J. W., Catillon-Mucherie, S., Redfern, P. C., Mehmood, F., Zapol, P., and Yale Univ. Subnanometer platinum clusters highly active and selective catalysts for the oxidative dehydrogenation of propane.. United States: N. p., 2009. Web. doi:10.1038/NMAT2384.
Vajda, S, Pellin, M. J., Greeley, J. P., Marshall, C. L., Curtiss, L. A., Ballentine, G. A., Elam, J. W., Catillon-Mucherie, S., Redfern, P. C., Mehmood, F., Zapol, P., & Yale Univ. Subnanometer platinum clusters highly active and selective catalysts for the oxidative dehydrogenation of propane.. United States. doi:10.1038/NMAT2384.
Vajda, S, Pellin, M. J., Greeley, J. P., Marshall, C. L., Curtiss, L. A., Ballentine, G. A., Elam, J. W., Catillon-Mucherie, S., Redfern, P. C., Mehmood, F., Zapol, P., and Yale Univ. Sun . "Subnanometer platinum clusters highly active and selective catalysts for the oxidative dehydrogenation of propane.". United States. doi:10.1038/NMAT2384.
@article{osti_957391,
title = {Subnanometer platinum clusters highly active and selective catalysts for the oxidative dehydrogenation of propane.},
author = {Vajda, S and Pellin, M. J. and Greeley, J. P. and Marshall, C. L. and Curtiss, L. A. and Ballentine, G. A. and Elam, J. W. and Catillon-Mucherie, S. and Redfern, P. C. and Mehmood, F. and Zapol, P. and Yale Univ.},
abstractNote = {Small clusters are known to possess reactivity not observed in their bulk analogues, which can make them attractive for catalysis. Their distinct catalytic properties are often hypothesized to result from the large fraction of under-coordinated surface atoms. Here, we show that size-preselected Pt{sub 8-10} clusters stabilized on high-surface-area supports are 40-100 times more active for the oxidative dehydrogenation of propane than previously studied platinum and vanadia catalysts, while at the same time maintaining high selectivity towards formation of propylene over by-products. Quantum chemical calculations indicate that under-coordination of the Pt atoms in the clusters is responsible for the surprisingly high reactivity compared with extended surfaces. We anticipate that these results will form the basis for development of a new class of catalysts by providing a route to bond-specific chemistry, ranging from energy-efficient and environmentally friendly synthesis strategies to the replacement of petrochemical feedstocks by abundant small alkanes.},
doi = {10.1038/NMAT2384},
journal = {Nature Mater.},
number = Mar. 2009,
volume = 8,
place = {United States},
year = {2009},
month = {3}
}