Atomically Dispersed Cu on In2O3 for Relay Electrocatalytic Conversion of Nitrate and CO2 to Urea

ACS Nano. 2024 Sep 10;18(36):25316-25324. doi: 10.1021/acsnano.4c09141. Epub 2024 Aug 26.

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%.

Keywords: electrochemical urea production; in situ spectroscopic analysis; relay catalysis; single-atom catalysts; theoretical calculations.