Regulating Active Hydrogen Supply Over Cu Clusters‐Interspersed MoS ₂ /MoO ₂ Nanosheets for Efficient Urea Electrosynthesis

Abstract Electrochemical urea synthesis is critically restricted by insufficient supply of active hydrogen ( * H) for the hydrogeneration of CO 2 and nitrate (NO 3 − ). Here, a tandem sites catalyst is designed by anchoring Cu clusters on MoS 2 /MoO 2 nanosheets (Cu‐MoS 2 /MoO 2 ), with the Cu sites activating CO 2 and NO 3 − and the Mo sites dissociating water to produce * H. In situ spectroscopic analysis and theoretical calculations reveal that the sufficient * H supply greatly promotes intermediate hydrogenation, thus enhancing C─N coupling for urea synthesis. Consequently, the Cu‐MoS 2 /MoO 2 catalyst displays significantly enhance performance of urea synthesis from CO 2 and NO 3 − , achieving a high yield of 117.5 mmol h −1 g cat. −1 at −0.6 V versus the reversible hydrogen electrode (RHE). Besides, stable electrocatalytic urea production is maintained for 68 h without a decline in yield or Faradaic efficiency. This work provides a meaningful perspective on modulating active hydrogen to promote urea production.