Screening of single-atomic catalysts loaded on two-dimensional transition metal dichalcogenides for electrocatalytic oxygen reduction via high throughput ab initio calculations

The design and screening of low cost and high efficiency oxygen reduction reaction (ORR) electrocatalysts is vital in the realms of fuel cells and metal-air batteries. Existing studies largely rely on the calculation of absorption free energy, a method established 20 years ago by Jens K. Nørskov. However, the study of electrocatalysts grounded solely on free energy calculation often lacks in-depth analysis, particularly overlooking the influence of solvent and electrode potential. In this regard, we here present a novel approach using constant-potential and ab initio molecular dynamics (AIMD) simulation to screen single-atom catalysts loaded on transition metal dichalcogenides (SA@TMDs) for ORR. An extensive investigation of 1584 SA@TMDs results in 20 high performing ORR catalysts with overpotential less than 0.33 V and high working stability. In addition, our study shows that the electrode potential has different effects on the adsorption energy of *OOH, *O and *OH, which leads to a reversal of the rate-determining step (RDS) of the ORR. This work presents not only credible, high-performance catalyst candidates for experimental exploration, but also significantly improves our understanding on the reaction mechanism of ORR under realistic reaction conditions.