Designing Asymmetrical TMN4 Sites via Phosphorus or sulfur Dual Coordination as High-Performance Electrocatalysts for Oxygen Evolution Reaction

The development of highly efficient oxygen evolution reaction (OER) catalysts based on more cost-effective and earth-abundant elements is of great significance and still faces a huge challenge. In this work, a series of transition metal (TM)embedding a newly-defined monolayer carbon nitride phase is theoretically profiled and constructed as a catalytic platform for OER studies. Typically, a four-step screening strategy was proposed to rapidly identified high performance candidates and the coordination structure and catalytic performance relationship was thoroughly analyzed. Moreover, the eliminating criterion was established to condenses valid range based on the Gibbs free energy of OH*. Our results reveal that the as-constructed 2FeCN/P exhibits superior activity toward OER with an ultralow overpotential of 0.25 V, at the same time, the established 3FeCN/S configuration performed well as abifunctional OER/ORR electrocatalysis with extremely low overpotential ηOER/ηORR of 0.26/0.48 V. Overall, this work provides an effective framework for screening advanced OER catalysts, which can also be extended to other complex multistep catalytic reactions.