2021/02/15 by Xingshuai Lv, Wei Wei, Baibiao Huang +2 · 1 citation
Chemical Engineering · Energy · Chemistry · #Ammonia Synthesis and Nitrogen Reduction #Advanced Photocatalysis Techniques #Nanomaterials for catalytic reactions
paper · doi:10.1021/acs.nanolett.0c05080
openalex publication_date 2021/02/15 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/31
Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by the discovery of metal–N x 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 (Fe 2 / g -CN) can manipulate the binding strength of the target reaction species (compromises the ability to adsorb N 2 H and NH 2 ), therefore achieving the best NRR performance among 23 transition metal (TM) centers. Our results show that Fe 2 / 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.