Abstract

Urea electrosynthesis from coelectrolysis of NO3- and CO2 (UENC) holds a significant prospect to achieve efficient and sustainable urea production. Herein, atomically dispersed Cu on In2O3 (Cu1/In2O3) is designed as an effective and robust catalyst for the UENC. Combined theoretical calculations and in situ spectroscopic analysis reveal the synergistic effect of the Cu1-O2-In site and the In site to boost the UENC energetics via a relay catalysis pathway, where the Cu1-O2-In site drives *NO3 → *NH2 and the In site catalyzes *CO2 → *CO. The generated *CO is then migrated from the In site to the Cu1-O2-In site, followed by C-N coupling with *NH2 on the Cu1-O2-In site to generate urea. Consequently, Cu1/In2O3 assembled within a flow cell exhibits an impressive urea yield rate of 28.97 mmol h-1 g-1 with a urea-Faradaic efficiency (FEurea) of 50.88%.

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