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

Abstract

AbstractUrea electrosynthesis from co‐electrolysis of NO3− and CO2 (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 MoS2 (Cu1‐MoS2) is explored as a highly active and selective UENC catalyst. Theoretical calculations and operando spectroscopic characterizations unveil the synergistic tandem catalysis of Cu1‐MoS2 for the UENC, where Cu single atoms trigger the early C─N coupling, while MoS2‐edges promote the key hydrogenation step of *CO2NH2 to *COOHNH2 for urea generation. Strikingly, Cu1‐MoS2 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.