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Electrochemical NO reduction reaction (NORR) to generate NH3 emerges as a fascinating approach to achieve both NO pollution mitigation and sustainable NH3 synthesis. Herein, we demonstrate that single-atomic Cu anchored on MoS2 (Cu1/MoS2) comprising Cu1-S3 motifs can serve as a highly efficient NORR catalyst. Cu1/MoS2 exhibits an NH3 yield rate of 337.5 μmol·h−1·cm−2 with a Faradaic efficiency of 90.6% at −0.6 V vs. reversible hydrogen electrode (RHE). Combined experiments and theoretical calculations reveal that Cu1-S3 motifs enable the effective activation and hydrogenation of NO through a mixed pathway and simultaneously retard proton coverage, contributing to the high activity and selectivity of Cu1/MoS2 for the NORR.
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