Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction.

Appropriate adsorption strength and modes of intermediates on catalysts and the reaction kinetic energy barrier directly determine the selectivity and productivity of final products during CO 2 electroreduction. This work systematically reveals the mechanisms for enhanced CO 2 electroreduction on nitrogen-doped Cu 2 O (N-Cu 2 O) catalyst by in-situ surface enhanced Raman spectroscopy (SERS) and theoretical calculation. The introduction of N into Cu 2 O can significantly enhance the CO 2 adsorption capacity, binding strength of key intermediates and increase the local pH value, resulting in two-fold enhancement of CO and C 2 H 4 production as compared to bare Cu 2 O. Meanwhile, the protonation step is promoted, making the formation of COOH· quickly and earlier. Therefore, the adsorbed CO 2 ·- intermediate formation is produced more rapidly, and the rate-determining step is transferred, continually facilitating the electroreduction of CO 2. This study is inspiring in designing high-performance electrocatalysts for CO 2 reduction. [Display omitted] • A facile and fruitful strategy is proposed to prepare superior CO 2 RR catalysts. • N-Cu 2 O catalyst delivers an improvement for C 2 product production. • The reaction mechanism on Cu 2 O and N-Cu 2 O catalysts are revealed. • The function of N doping is profoundly analyzed. [ABSTRACT FROM AUTHOR]