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Issue 12, 2012
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Catalytic reactions on neutral Rh oxide clusters more efficient than on neutral Rh clusters

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Abstract

Gas phase catalytic reactions involving the reduction of N2O and oxidation of CO were observed at the molecular level on isolated neutral rhodium clusters, Rhn (n = 10–28), using mass spectrometry. Sequential oxygen transfer reactions, RhnOm−1 + N2O → RhnOm + N2 (m = 1, 2, 3,…), were monitored and the rate constant for each reaction step was determined as a function of the cluster size. Oxygen extraction reactions by a CO molecule, RhnOm + CO → RhnOm−1 + CO2 (m = 1, 2, 3,…), were also observed when a small amount of CO was mixed with the reactant N2O gas. The rate constants of the oxygen extraction reactions by CO for m ≥ 4 were found to be two or three orders of magnitude higher than the rate constants for m ≤ 3, which indicates that the catalytic reaction proceeds more efficiently when the reaction cycles turn over around RhnOm (m ≥ 4) than around bare Rhn. Rhodium clusters operate as more efficient catalysts when they are oxidized than non- or less-oxidized rhodium clusters, which is consistent with theoretical and experimental studies on the catalyticCO oxidation reaction on a rhodium surface.

Graphical abstract: Catalytic reactions on neutral Rh oxide clusters more efficient than on neutral Rh clusters

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Publication details

The article was received on 19 Dec 2011, accepted on 02 Feb 2012 and first published on 02 Feb 2012


Article type: Paper
DOI: 10.1039/C2CP24036J
Citation: Phys. Chem. Chem. Phys., 2012,14, 4188-4195

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    Catalytic reactions on neutral Rh oxide clusters more efficient than on neutral Rh clusters

    A. Yamada, K. Miyajima and F. Mafuné, Phys. Chem. Chem. Phys., 2012, 14, 4188
    DOI: 10.1039/C2CP24036J

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