Electrochemical tandem C–N coupling toward efficient urea synthesis enabled on highly exposed metal hydroxide interface

<h2>Summary</h2> In the context of the dual-carbon target, green-electricity-driven urea electrosynthesis from carbon dioxide and nitrates is recognized as a promising alternative to the industrial Bosch-Meiser process. However, achieving efficient activation of the reactants, especially the inert carbon dioxide, as well as enabling directional C–N coupling toward urea formation, is a significant challenge. Here, we report a highly exposed metal/hydroxide interface for efficient tandem C–N coupling. The highly exposed Ag active sites on the ridges of Ag nanowires (Ag NWs) facilitate the CO₂ reduction reaction. The hydroxide layer catalyzes the nitrate reduction process and regulates the interfacial water network structure, promoting rapid water splitting to boost active hydrogen atoms. ∗CO and ∗NH₂ spontaneously occur during C–N coupling to urea on the Ag/CuNi(OH)₂ interface. The synthesized Ag NWs@CuNi(OH)₂ composite delivers a urea yield rate of 36.1 mmol g_cat.⁻¹ h⁻¹ and a Faradaic efficiency of 36.2%, as well as excellent cycling stability.