Controlling Ethylene Hydrogenation Reactivity on Pt13 Clusters by Varying the Stoichiometry of the Amorphous Silica Support.

Autor: Crampton AS; Technische Universität München, Lehrstuhl für Physikalische Chemie, Zentralinstitut für Katalyseforschung und Fakultät für Chemie, Ernst-Otto-Fisher-Strasse 1 und Lichtenbergstrasse 4, 85747, Garching, Germany.; Harvard University, Department of Chemistry and Chemical Biology, 12 Oxford St., Cambridge, MA, 02138, USA., Rötzer MD; Technische Universität München, Lehrstuhl für Physikalische Chemie, Zentralinstitut für Katalyseforschung und Fakultät für Chemie, Ernst-Otto-Fisher-Strasse 1 und Lichtenbergstrasse 4, 85747, Garching, Germany., Schweinberger FF; Technische Universität München, Lehrstuhl für Physikalische Chemie, Zentralinstitut für Katalyseforschung und Fakultät für Chemie, Ernst-Otto-Fisher-Strasse 1 und Lichtenbergstrasse 4, 85747, Garching, Germany., Yoon B; School of Physics, Georgia Institute of Technology, Atlanta, GA, 30332-0430, USA., Landman U; School of Physics, Georgia Institute of Technology, Atlanta, GA, 30332-0430, USA., Heiz U; Technische Universität München, Lehrstuhl für Physikalische Chemie, Zentralinstitut für Katalyseforschung und Fakultät für Chemie, Ernst-Otto-Fisher-Strasse 1 und Lichtenbergstrasse 4, 85747, Garching, Germany.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2016 Jul 25; Vol. 55 (31), pp. 8953-7. Date of Electronic Publication: 2016 Jun 29.
DOI: 10.1002/anie.201603332
Abstrakt: Ethylene hydrogenation was investigated on size-selected Pt13 clusters supported on three amorphous silica (a-SiO2 ) thin films with different stoichiometries. Activity measurements of the reaction at 300 K revealed that on a silicon-rich and a stoichiometric film, Pt13 exhibits a similar activity to that of Pt(111), in line with the known structure insensitivity of the reaction. On an oxygen-rich film, a threefold increased rate was measured. Pulsing ethylene at 400 K, then measuring the activity at 300 K, resulted in complete loss of activity on the silicon-rich surface compared to only marginal losses on the other surfaces. The measured reactivity trends correlate with charging characteristics of a Pt13 cluster on the SiO2 films, predicted through first-principle calculations. The results reveal that the stoichiometry-dependent charging by the support can be used to tune the selectivity of reaction pathways during a catalytic hydrogenation reaction.
(© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)
Databáze: MEDLINE
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