Selectivity

Nanotechnology

Electrode

Organic chemistry

Nitrogen fixation

Limiting

Combinatorial chemistry

Atom (system on chip)

Transition metal

Engineering

Faraday efficiency

Catalysis

Physical chemistry

Embedded system

Inorganic chemistry

Ammonia production

Chemistry

Materials science

Computer science

Metal

Electrochemistry

Nitrogen

Redox

Mechanical engineering

Nano Letters

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by the discovery of metal–Nx 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.

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