High-Throughput Screening of Transition Metal Single-Atom Catalysts for Nitrogen Reduction Reaction

TL;DR

This study employs high-throughput first-principles calculations to identify transition metal-doped b-Sb monolayers as efficient and selective catalysts for nitrogen reduction, revealing key electronic factors and promising candidates Re@Sb and Tc@Sb.

Contribution

It introduces a high-throughput computational screening method to discover and analyze transition metal single-atom catalysts for nitrogen reduction, highlighting the role of doping and electronic structure.

Findings

Re@Sb and Tc@Sb show the best NRR performance with low limiting potential.

Re@Sb and Tc@Sb can inhibit HER and achieve 100% Faradaic efficiency.

Doping engineering effectively regulates NRR activity of b-Sb monolayer.

Abstract

The discovery of metals as catalytic centers for nitrogen reduction reactions has stimulated great enthusiasm for single-atom catalysts. However, the poor activity and low selectivity of available SACs are far away from the industrial requirement. Through the high throughout first principles calculations, the doping engineering can effectively regulate the NRR performance of b-Sb monolayer. Especially, the origin of activated N2 is revealed from the perspective of the electronic structure of the active center. Among the 24 transition metal dopants, Re@Sb and Tc@Sb showed the best NRR catalytic performance with a low limiting potential. The Re@Sb and Tc@Sb also could significantly inhibit 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.