Gold and Methane: A Noble Combination for Delicate Oxidation

TL;DR

This study uses DFT calculations to explore how positively charged gold nanoparticles can facilitate the partial oxidation of methane at low temperatures, providing insights into tuning catalytic activity.

Contribution

It reveals that charging gold nanoparticles enhances methane binding, offering a new approach to catalyze methane oxidation under mild conditions.

Findings

Positive charging increases methane adsorption on gold nanoparticles.

Methane binds via metal s orbitals across various gold cluster sizes.

Gold nanoparticles can be tuned for catalytic activity through charge manipulation.

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 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.