Synergistic Cu Single Atoms and MoS₂‐Edges for Tandem Electrocatalytic Reduction of NO₃⁻ and CO₂ to Urea

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) under ambient conditions is recognized as an appealing approach for effective and sustainable urea production, while it requires high‐efficiency UENC electrocatalysts to promote the C─N coupling and hydrogenation processes. Herein, single‐atom Cu anchored on MoS 2 (Cu 1 ‐MoS 2 ) is explored as a highly active and selective UENC catalyst. Theoretical calculations and operando spectroscopic characterizations unveil the synergistic tandem catalysis of Cu 1 ‐MoS 2 for the UENC, where Cu single atoms trigger the early C─N coupling, while MoS 2 ‐edges promote the key hydrogenation step of * CO 2 NH 2 to * COOHNH 2 for urea generation. Strikingly, Cu 1 ‐MoS 2 equipped in a flow cell achieves the excellent UENC performance with a maximum urea‐Faradaic efficiency of 57.02% at −0.6 V and the corresponding urea yield rate of 23.3 mmol h −1 g −1 , surpassing nearly all previously reported UENC catalysts.