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

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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.