| Abstract Scope |
Introducing a second transition metal to iron-nitrogen-carbon (Fe-N-C) catalysts has been demonstrated to offer a new opportunity to further enhance oxygen reduction reaction (ORR). However, due to the myriad possible structural configurations and the dynamic structure evolution of metal centers under reaction conditions, it has been challenging to elucidate the structure-property relationship at the atomic level for the rational design of these catalysts. Here, we develop a computational workflow integrating configuration generation, phase diagram construction, and reaction energy calculations to provide a fundamental understanding of ORR for designing dual-metal-site catalysts. We generated more than 30 configurations for each type of Fe-M catalyst (M = Mn, Cu, Co, etc.), and identified the configurations which possess higher catalytic activity than the state-of-the-art Pt. Furthermore, we revealed a relationship between the limiting potential and the magnetic moment on Fe. Combined with machine learning, promising candidates beyond currently available catalysts could be discovered. |