Activity And Stability of Single‐ And Di‐Atom Catalysts for the O2 Reduction Reaction

Abstract Efficient and inexpensive catalysts for the O 2 reduction reaction (ORR) are needed for the advancement of renewable energy technologies. In this study, we designed a computational catalyst‐screening method to identify single and di‐atom metal dopants from first‐row transition elements supported on defect‐containing nitrogenated graphene surfaces for the ORR. Based on formation‐energy calculations and micro‐kinetic modelling of reaction pathways using intermediate binding free energies, we have identified four potentially interesting single‐atom catalysts (SACs) and fifteen di‐atom catalysts (DACs) with relatively high estimated catalytic activity at 0.8 V vs RHE. Among the best SACs, MnNC shows high stability in both acidic and alkaline media according to our model. For the DACs, we found four possible candidates, MnMn, FeFe, CoCo, and MnNi doped on quad‐atom vacancy sites having considerable stability over a wide pH range. The remaining SACs and DACs with high activity are either less stable or show a stability region at an alkaline pH.