Cu–Mo Dual Sites in Cu-Doped MoSe2 for Enhanced Electrosynthesis of Urea

The quest for sustainable urea production has directed attention toward electrocatalytic methods that bypass the energy-intensive traditional Haber–Bosch process. This study introduces an approach to urea synthesis through the coreduction of CO2 and NO3– using copper-doped molybdenum diselenide (Cu–MoSe2) with Cu–Mo dual sites as electrocatalysts. The electrocatalytic activity of the Cu–MoSe2 electrode is characterized by a urea yield rate of 1235 μg h–1 mgcat.–1 at −0.7 V versus the reversible hydrogen electrode and a maximum Faradaic efficiency of 23.43% at −0.6 V versus RHE. Besides, a continuous urea production with an enhanced average yield rate of 9145 μg h–1 mgcat.–1 can be achieved in a flow cell. These figures represent a substantial advancement over that of the baseline MoSe2 electrode. Density functional theory (DFT) calculations elucidate that Cu doping accelerates *NO2 deoxygenation and significantly decreases the energy barriers for C–N bond formation. Consequently, Cu–MoSe2 demonstrates a more favorable pathway for urea production, enhancing both the efficiency and feasibility of the process. This study offers valuable insights into electrode design and understanding of the facilitated electrochemical pathways.