ABSTRACT The electrocatalytic urea oxidation reaction (UOR) demonstrates significant potential in energy conversion and wastewater treatment. In nickel‐based electrocatalytic systems, the UOR process characterized by NiOOH (Ni 3+ ) formation in the conventional pathway tends to generate harmful by‐products at high potentials while facing oxygen evolution reactuion (OER) competition. Herein, we synthesized a MoS 2 /NiMoO 4 heterostructure and regulate the built‐in electric field in the heterojunction, while the conversion process from Ni 3+ to Ni 2+ is accelerated, thus resulting in a reduction in the static accumulation of Ni 3+ . This delays the cleavage of the carbon‐nitrogen (C─N) bond, thereby steering the reaction pathway toward the complete oxidation products, CO 2 and N 2 . The MoS 2 /NiMoO 4 catalyst exhibits exceptional electrocatalytic activity toward UOR, requiring a low driving potential of just 1.365 V to achieve a current density of 100 mA cm −2 . The urea electrolyzer assembled with MoS 2 /NiMoO 4 and Pt electrodes achieves the same current density at 1.61 V and operates stably for 180 h. This work provides fundamental insights into the UOR mechanism and offers a new direction for designing efficient nickel‐based heterostructure catalysts.
Xu et al. (2026) studied this question.