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Electrochemical reduction of nitrate to ammonia (NO3RR) holds a great promise for attaining both NH3 electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi1Pd) is reported as a highly effective NO3RR catalyst, showing a near 100% NH3‐Faradaic efficiency with the corresponding NH3 yield of 33.8 mg h−1 cm−2 at −0.6 V versus RHE, surpassing those of almost all ever reported NO3RR catalysts. In‐depth theoretical and operando spectroscopic investigations unveil that single‐atom Bi electronically couples with its neighboring Pd atoms to synergistically activate NO3− and destabilize *NO on Bi1Pd, leading to the reduced energy barrier of the potential‐determining step (*NO→*NOH) and enhanced protonation energetics of NO3−‐to‐NH3 pathway.
Single‐atom Bi alloyed Pd metallene (Bi1Pd) is reported as a highly efficient and durable catalyst for electrocatalytic reduction of nitrate to ammonia (NO3RR). Combined operando spectroscopic characterizations and theoretical calculations reveal that single‐atom Bi electronically couples with the neighboring Pd atoms to synergistically boost the protonation energetics of Bi1Pd for the enhanced NO3RR.