Urea Electrosynthesis via an Integrated Pd1-Cu Interface Strategy
Electrocatalytic co-reduction of CO2 and nitrate offers a sustainable route for urea synthesis, valorizing nitrogenous waste and CO2. However, achieving high-performance urea electrosynthesis under ambient conditions remains challenging due to the need for simultaneous activation of CO2 and efficient H2O dissociation to supply active *H for *NOx hydrogenation, ultimately forming key C- and N-containing intermediates for C–N coupling. Here, we report a bifunctional Pd-single-atom-modified Cu (Pd1Cu) nanorod catalyst that synergistically promotes adsorption and stepwise activation of CO2 and H2O, steering the reaction pathway toward selective urea synthesis. Integrating experimental evidence, in situ spectroscopy, and computational analyses, we disclose that atomically dispersed Pd sites kinetically favor co-generation of *CO and *NH2 via H2O dissociation-driven proton transfer, forming an optimal intermediate balance. The dual metal active sites enhance C–N coupling via combined electronic and geometric effects, substantially lowering the reaction energy barrier and improving selectivity. This work provides a rational design strategy for advanced multifunctional catalysts for urea electrosynthesis, contributing to carbon neutrality and waste nitrogen valorization.