Urea electrosynthesis from the coelectrolysis of NO and CO (UENC) presents a fascinating approach for simultaneously migrating NO pollutants and producing valuable urea. In this study, isolated Rh-alloyed copper (RhCu) is explored as a highly active and selective catalyst toward the UENC. Combined in situ spectroscopic analysis and theoretical calculations reveal the relay catalysis of the Rh site and Cu site to promote the UENC energetics, in which the Rh site activates NO to form *NH while the Cu site activates CO to form *CO. The formed *CO is then migrated from the Cu substrate to the nearby Rh site, which promotes the C-N coupling of *NH and *CO toward the urea formation. Prominently, RhCu achieves an exceptional UENC performance in the flow cell, exhibiting the highest urea-Faradaic efficiency of 67.10% and urea yield rate of 50.36 mmol h g at -0.6 V versus RHE.
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