Gold and Methane: A Noble Combination for Delicate Oxidation

Journal Of Physical Chemistry Letters 4, 3006 - 3012 (2013)

Gold and Methane: A Noble Combination for Delicate Oxidation

Duncan J. Mowbray, Annapaola Migani, Guido Walther, David M. Cardamone, Angel Rubio

The ability to partially oxidize methane at low temperatures and pressures would have important environmental and economic applications. Although methane oxidation on gold nanoparticles has been observed experimentally, our density functional theory (DFT) calculations indicate neither CH4, CH3, nor H adsorb on a neutral gold nanoparticle. However, by positively charging gold nanoparticles, e.g. through charge transfer to the TiO2 substrate, CH4 binding increases while O2 binding remains relatively unchanged. We demonstrate that CH4 adsorption is via bonding with the metal s levels. This holds from small gold clusters (Au2) to large gold nanoparticles (Au201), and for all fcc transition metal dimers. These results provide the chemical understanding necessary to tune the catalytic activity of metal nanoparticles for the partial oxidation of methane under delicate conditions.

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We acknowledge funding by the European Research Council Advanced Grant DYNamo (ERC-2010-AdG - 267374), Spanish Grants (FIS2010-21282-C02-01 and PIB2010US-00652), Grupos Consolidados UPV/EHU del Gobierno Vasco (IT-578-13), and the European Commission project CRONOS (280879-2 CRONOS CPFP7). DJM acknowledges funding through the Spanish “Juan de la Cierva” program (JCI-2010-08156). AM acknowledges funding through JAE DOC and the European Social Fund. GW acknowledges funding through the HPC-Europa2 Programme (Project No. 228398).

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