Long-term stable acidic electroreduction of CO2 to C2 products at industrial current density using passivated copper
Qin Chen, Yao Tan, Xiqing Wang, Qiyou Wang, Hongmei Li, Kang Liu, Junwei Fu, Liyuan Chai, Min Liu, Zhang Lin
Abstract
Acidic CO2 electroreduction to multi-carbon (C2+) products using Cu-based catalyst has attracted considerable attention for CO2 recycling due to high single-pass CO2 utilization. However, its development is drastically limited by the poor stability, especially at high current density, caused by Cu dissolution/reconstruction during the reaction. Herein, we find the trace dissolved oxygen in the electrolyte accounts for the Cu dissolution/reconstruction and report an in-situ passivation strategy to prevent oxygen adsorption for inhibiting Cu dissolution/reconstruction for high stability CO2-to-C2+ conversion. Theoretical and in situ spectroscopy demonstrate that aluminum citrate (AC) passivation layer decreases the adsorption of oxygen on Cu surface to effectively prevent the Cu oxidation, which is beneficial for the formation and adsorption of linearly bonded *CO toward C-C coupling. As the result, the Cu catalysts with AC layer achieve over 60% Faradaic efficiency C2H4 and 38.7% energy efficiency to C2+ for over 150 h stability at 500 mA cm−2 in strong acidic electrolyte. The use of Cu catalysts for the CO2 reduction reaction is hindered by their poor stability. The authors find that traces dissolved oxygen in the electrolyte results in Cu dissolution/reconstruction and report an in-situ passivation strategy to prevent oxygen adsorption in high stability.