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Issue 29, 2012
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DFT studies of oxidation routes for Pd9 clusters supported on γ-alumina

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Abstract

This research is focused on the analysis of adsorbed bare and oxidized Pd9 nanoparticles supported on γ-alumina. From first-principle density functional theory calculations, several configurations, charge transfer and electronic density of states have been analyzed in order to determine feasible paths for the oxidation process. Studies of Pd/PdO nanoparticles prove that they are stable at γ-alumina supports. It is shown that the Pd9 nanoparticle favors dissociative adsorption of oxygen molecules. The most energetically preferable sites for adsorption are close to the contact between the cluster and the support, where one oxygen atom interacts with a 5-coordinated aluminium atom, and the remaining oxygen is in contact with the closest palladium atom. After first dissociation, one oxygen atom creates a bridge between the palladium atom and the 5-coordinated aluminium atom and the second oxygen atom moves to the top of the Pd9 cluster, making a bridge between two palladium atoms. Subsequent dissociations arise analogously, with the difference that oxygen atoms in the second layer of the palladium cluster occupy hollow sides of the cluster. Investigation of the charge distribution in each oxidation step reveals that charge transfer increases towards the Pd/PdO nanoclusters. The electronic density of states indicates that gradual oxygen molecule adsorption and dissociation shift the highest states of the Pd/PdO nanoparticles in different ways. The overall investigation is found to be beneficial for studying methane oxidation.

Graphical abstract: DFT studies of oxidation routes for Pd9 clusters supported on γ-alumina

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Publication details

The article was received on 06 Mar 2012, accepted on 15 May 2012 and first published on 16 May 2012


Article type: Paper
DOI: 10.1039/C2CP40715A
Citation: Phys. Chem. Chem. Phys., 2012,14, 10243-10247
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    DFT studies of oxidation routes for Pd9 clusters supported on γ-alumina

    K. A. Kacprzak, I. Czekaj and J. Mantzaras, Phys. Chem. Chem. Phys., 2012, 14, 10243
    DOI: 10.1039/C2CP40715A

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