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 Cu-1-Ru site and the Ru-Ru site on Cu1Ru to promote the UENC via a tandem catalysis pathway, in which the Cu-1-Ru site drives *NO2/CO2 coupling and followed the *CO2NO2-to-*CO2NH step. The formed *CO2NH then migrates from the Cu-1-Ru site to the adjacent Ru-Ru site which promotes the *CO2NH*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) g(cat)(-1) and Faradaic efficiency of 51.27% at -0.6 V, outperforming most reported UENC catalysts.