Regulating kinetics and thermodynamics of electrochemical nitrogen reduction with metal single-atom catalysts in a pressurized electrolyser

Significance The present-day industrial ammonia synthesis is overreliance on the Haber–Bosch process, yet consumes more than 1% of the global energy supply along with gigatonne greenhouse-gas emission per year. Electrochemical nitrogen reduction reaction (ENRR) offers a sustainable path to produce ammonia under mild conditions, while its efficiency achieved by far is fairly low, which requires the development of both catalysts and electrolyzers. Here, by the cooperation of densely populated metal single atoms on graphdiyne substrate with the pressurized electrocatalytic system, the kinetics and the thermodynamic driving force of ENRR are effectively regulated, leading to a record-high ammonia yield rate. This work motivates the technological and material coevolution for the ENRR toward its envisioned application.