Gold and Methane: A Noble Combination for Delicate Oxidation

Abstract

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 CH 4, CH 3, nor H adsorb on a neutral gold nanoparticle. However, by positively charging gold nanoparticles, e.g., through charge transfer to the TiO 2 substrate, CH 4 binding increases while O 2 binding remains relatively unchanged. We demonstrate that CH 4 adsorption is via bonding with the metal s levels. This holds from small gold clusters (Au 2 ) to large gold nanoparticles (Au 201 ), and for all face-centered cubic (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.