First principles screening of transition metal single-atom catalysts for nitrogen reduction reaction

The discovery of metals as catalytic centers for nitrogen reduction reactions (NRR) has stimulated great enthusiasm for single-atom catalysts. However, the poor activity and low selectivity of available single-atom catalysts (SACs) are far away from the industrial requirement. Through the first principles screening, the doping engineering can effectively regulate the NRR performance of beta-Sb monolayer. Especially, the origin of activated N2 is discovered from the perspective of the electronic structure of the active center. Among the 24 transition metal dopants, Re@Sb showed the best NRR catalytic performance with a low limiting potential. The Re@Sb also could significantly inhibit hydrogen evolution reaction (HER) and achieve a high theoretical Faradaic efficiency of 100%. Our findings not only accelerate discovery of catalysts for ammonia synthesis but also contribute to further elucidate the structure-performance correlations.

Automated summary

The discovery of metals as catalytic centers for nitrogen reduction reactions (NRR) has led to interest in single-atom catalysts (SACs). However, existing SACs have poor activity and low selectivity, which falls short of industrial requirements. Through first principles screening, doping engineering can effectively regulate the NRR performance of beta-Sb monolayer. Among 24 transition metal dopants, Re@Sb shows the best NRR catalytic performance with low limiting potential and can inhibit hydrogen evolution reaction (HER) while achieving a high theoretical Faradaic efficiency of 100%. These findings accelerate catalyst discovery for ammonia synthesis and contribute to understanding structure-performance correlations.