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Electrochemical converting NO2− into NH3 (NO2RR) holds an enormous prospect to attain efficient NH3 electrosynthesis and polluted NO2− mitigation. Herein, we report single-atom Co alloyed Ru (Co1Ru) as an efficient and durable NO2RR catalyst. Extensive experimental and theoretical investigations reveal that single-atom Co alloying of Ru enables the construction of Co1-Ru heteronuclear active sites to synergistically promote NO2− activation/hydrogenation while suppressing the competitive H2 evolution, rendering the greatly enhanced activity and selectivity of Co1Ru towards the NO2RR. Consequently, Co1Ru assembled within a flow cell exhibits an impressive NH3 yield rate of 2379.2 μmol·h−1·cm−2 with an NH3-Faradaic efficiency of 92% at a high current density of 415.9 mA·cm−2, which is among the highest NO2RR performances reported to date.
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