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−1cat. 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. [ABSTRACT FROM AUTHOR]