Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N₂ to NH₃

At present, the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia (NH₃). Herein, we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets (Zn/NC NSs) as an efficient nitrogen reduction reaction catalyst, which achieves a high ammonia yield of 46.62 μg h⁻¹ mg_cat.⁻¹ at −0.85 V (vs RHE) and Faradaic efficiency of 95.8% at −0.70 V (vs RHE). In addition, Zn/NC NSs present great stability and selectivity, and there is no significant change in NH₃ rate and Faradaic efficiencies after multiple cycles. The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn–N₄ sites in the catalyst. DFT calculation confirms that Zn/NC with Zn–N₄ configuration has a lower energy barrier for the formation of *NNH intermediate compared with pure N-doped carbon nanosheets (N-C NSs), thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.