Letter abstract
Nature Materials 8, 213 - 216 (2009)
Published online: 8 February 2009 | doi:10.1038/nmat2384
Subject Categories: Catalytic materials | Computation, modelling and theory
Subnanometre platinum clusters as highly active and selective catalysts for the oxidative dehydrogenation of propane
Stefan Vajda1,2,3, Michael J. Pellin4, Jeffrey P. Greeley2, Christopher L. Marshall1, Larry A. Curtiss1,2,4, Gregory A. Ballentine1,6, Jeffrey W. Elam5, Stephanie Catillon-Mucherie1, Paul C. Redfern1, Faisal Mehmood4 & Peter Zapol1,2,4
Small clusters are known to possess reactivity not observed in their bulk analogues, which can make them attractive for catalysis1, 2, 3, 4, 5, 6. Their distinct catalytic properties are often hypothesized to result from the large fraction of under-coordinated surface atoms7, 8, 9. Here, we show that size-preselected Pt8-10 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 alkanes10, 11.
- Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA
- Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA
- Department of Chemical Engineering, School of Engineering & Applied Science, Yale University, 9 Hillhouse Avenue, New Haven, Connecticut 06520, USA
- Materials Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA
- Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA
- Present Address: Max-Planck-Institut für Metallforschung, Stuttgart, Germany
Correspondence to: Stefan Vajda1,2,3 e-mail: vajda@anl.gov
Correspondence to: Larry A. Curtiss1,2,4 e-mail: curtiss@anl.gov
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