Understanding the CH activation of methane over single‐atom alloy catalysts by density functional theory calculations

Abstract

AbstractAs an important rate‐determining step in the oxidation of methane, the catalytic behaviors of single‐atom alloys (SAAs) on the CH activation reactions have not been fully understood. In this work, density functional theory calculations are performed to investigate the CH activation of methane on a series of SAAs with Cu(111/100) and Ag(111/100) as hosts. The reaction energies and the barriers for the CH dissociation reaction follow the traditional Brønsted–Evans–Polanyi (BEP) relationship, but the deviation from this linearity fitting is relatively large. To better describe the catalytic activity, a new nonlinear binary function is proposed to correlate the reaction barrier with the adsorption energies of *H and *CH3 products, which has higher correlation than the BEP relationship, and showed more accurate predictions of the CH activation reaction for unknown SAAs catalysis. Such mode might be able to extend to other catalyst systems to achieve large‐scale catalyst screening.