Electroreduction of NO and CO to urea (ENCU) represents a fascinating strategy to enable waste NO/CO removal and sustainable urea production. Herein, uncoordinated Zn nanosheets (U-Zn) are developed as a highly selective ENCU catalyst, exhibiting the highest urea-faradaic efficiency of 31.8% with the corresponding urea yield rate of 39.3 mmol h g in a flow cell. Theoretical calculations and electrochemical spectroscopic measurements reveal that the high ENCU performance of U-Zn arises from the critical role of uncoordinated Zn sites that can promote both key steps of *NO/CO coupling and *CONH protonation to *COOHNH, while retarding the competitive side reactions.
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