Boosting the CO2 electroreduction performance of La2-Ag CuO4- perovskites via A-site substitution mechanism

The electrochemical CO2 reduction reaction (CO2RR) has been widely recognized as a promising approach to achieve the carbon cycle balance in human society. However, potent electrocatalysts are required to achieve the selective conversion of CO2 to high value-added chemical products. Here, we reported a Ruddlesden-Popper layered perovskite catalyst, namely La2-xAgxCuO4-δ, which exhibits enhanced activity and selectivity towards CO2RR by tuning the A-site cations with Ag doping. Combinatorial characterizations and theoretical calculation reveal the partial replacement of Ag+ on the A-site of La2CuO4 can tune the electronic structure of Cu2+ ions of the B site, improving the adsorption/activation of crucial reaction intermediates. Importantly, Ag doping constructs oxygen vacancies, which shifts the reaction pathways from the two-electron transfer reduction to the multi-electron/proton transfer reduction, thereby promoting the formation of multi-carbon products. Taken together, these findings offer fresh insights for the strategic development of efficient perovskite electrocatalysts for CO2RR.