High-throughput identification of high activity and selectivity transition metal single-atom catalysts for nitrogen reduction

Developing efficient catalysts to achieve electrochemical nitrogen reduction reaction (NRR) under mild conditions remains a great challenge. Herein, 24 different transition metal (TM) single atom centers anchored on the C9N4 substrate were employed to form [email protected]9N4 candidates catalyzing N2 reduction. By means of high-throughput density functional theory (DFT) calculations, we conduct a comprehensive screening of catalytic activity, selectivity, and electronic origins of [email protected]9N4 candidates. Particularly, we reported a new descriptor φ based on the intrinsic characteristics of TM active centers, realizing a fast-scan/estimation among various candidates. Most importantly, we found that the established [email protected]9N4 catalyst simultaneously realizes both excellent selectivity and activity toward NRR with an extremely low limiting potential of −0.24 V. These results offer useful insights into designing high-performance [email protected]9N4 NRR catalysts for advancing sustainable NH3 production.