Selective Urea Electrosynthesis from Nitrate and CO2 on Isolated Copper Alloyed Ruthenium

Urea electrosynthesis by coelectrolysis of NO3– and CO2 (UENC) represents a promising method to enable efficient and sustainable urea production. In this work, isolated Cu alloyed Ru (Cu1Ru) is developed as a highly active and selective UENC catalyst. Combined theoretical computations and in situ spectroscopic measurements reveal the synergistic effect of the Cu1–Ru site and the Ru–Ru site on Cu1Ru to promote the UENC via a tandem catalysis pathway, in which the Cu1–Ru site drives *NO2/CO2 coupling and followed the *CO2NO2-to-*CO2NH step. The formed *CO2NH then migrates from the Cu1–Ru site to the adjacent Ru–Ru site which promotes the *CO2NH⃗*CO2NH2 → *COOHNH2 steps toward urea generation. Impressively, Cu1Ru achieves a high UENC performance in flow cell, exhibiting the urea yield rate of 21.04 mmol h–1 gcat–1 and Faradaic efficiency of 51.27% at −0.6 V, outperforming most reported UENC catalysts.