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Issue 11, 2013
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Comparison of methane activation and catalytic ethylene formation on free gold and palladium dimer cations: product binding determines the catalytic turnover

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Abstract

The gas-phase dimers Au2+ and Pd2+ have been shown to readily activate methane and to facilitate its dehydrogenation eventually leading to the selective formation of ethylene at room temperature in the case of Au2+. Ion trap mass spectrometric investigations under multi-collision conditions reveal similar product ion distributions at room temperature for both dimer cations in reaction with methane. Yet, the corresponding kinetics disclose considerable differences in their catalytic properties. A detailed evaluation of the rate constants associated with the individual catalytic reaction steps in conjunction with temperature dependent reactivity studies allow for the determination of turnover frequencies, critical and rate-determining reaction steps, as well as activation barriers. These results emphasize that the propensity for the final liberation of the formed product from the metal center decisively determines the superior catalytic properties of the gold dimer compared to palladium.

Graphical abstract: Comparison of methane activation and catalytic ethylene formation on free gold and palladium dimer cations: product binding determines the catalytic turnover

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Publication details

The article was received on 25 Apr 2013, accepted on 08 Jul 2013 and first published on 30 Jul 2013


Article type: Paper
DOI: 10.1039/C3CY00286A
Catal. Sci. Technol., 2013,3, 2926-2933

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    Comparison of methane activation and catalytic ethylene formation on free gold and palladium dimer cations: product binding determines the catalytic turnover

    S. M. Lang, A. Frank and T. M. Bernhardt, Catal. Sci. Technol., 2013, 3, 2926
    DOI: 10.1039/C3CY00286A

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