High-Throughput Screening of Synergistic Transition Metal Dual-Atom Catalysts for Efficient Nitrogen Fixation

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by the discovery of metal-N as a promising catalytic center. However, the poor activity and low selectivity of available SACs are far away from the industrial requirement. Through the first-principles high-throughput screening, we find that Fe-Fe distributed on graphite carbon nitride (Fe₂/g-CN) can manipulate the binding strength of the target reaction species (compromises the ability to adsorb N₂H and NH₂), therefore achieving the best NRR performance among 23 transition metal (TM) centers. Our results show that Fe₂/g-CN achieves a high theoretical Faradaic efficiency of 100% and, impressively, the lowest limiting potential of -0.13 V. Particularly, multiple-level descriptors shed light on the origin of NRR activity, achieving a fast prescreening among various candidates. Our predictions not only accelerate discovery of catalysts for ammonia synthesis but also contribute to further elucidate the structure-performance correlations.