Selective urea electrosynthesis nitrate and CO reduction on uncoordinated Zn nanosheets

Electroreduction of NO 3 − and CO 2 to urea (ENCU) represents a fascinating strategy to enable waste NO 3 − /CO 2 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 −1 g −1 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 2 /CO 2 coupling and *CO 2 NH 2 protonation to *COOHNH 2 , while retarding the competitive side reactions. Uncoordinated Zn nanosheets are developed as a selective catalyst for electroreduction of NO 3 − and CO 2 to urea, attributed to the critical role of uncoordinated Zn sites in promoting C-N coupling while suppressing the competitive side reactions.