Alkaline Ionic Liquid Microphase Promotes Deep Reduction of CO2 on Copper

作者：Zhonghao Tan, Jianling Zhang, Yisen Yang, Jiajun Zhong, Yingzhe Zhao, Jingyang Hu, Buxing Han, Zhongjun Chen · 发表于：Journal of the American Chemical Society · 年份：2023 · DOI：10.1021/jacs.3c06860 · 被引用次数：82 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Carbon dioxide utilization in catalysis

Abstract Electrochemical reduction of CO2 to multicarbon (C2+) products using renewable energy sources is an important route to storing sustainable energy and achieving carbon neutrality. It remains a challenge to achieve high C2+ product faraday efficiency (FE) at ampere-level current densities. Herein, we propose the immobilization of an alkaline ionic liquid on copper for promoting the deep reduction of CO2. By this strategy, a C2+ FE of 81.4% can be achieved under a current density of 0.9 A·cm–2 with a half-cell energy conversion efficiency of 47.4% at −0.76 V vs reversible hydrogen electrode (RHE). Particularly, when the current density is as high as 1.8 A·cm–2, the C2+ FE reaches 71.6% at an applied potential of −1.31 V vs RHE. Mechanistic studies demonstrate that the alkaline ionic liquid plays multiple roles of improving the accumulation of CO2 molecules on the copper surface, promoting the activation of the adsorbed CO2, reducing the energy barrier of CO dimerization, stabilizing intermediates, and facilitating the C2+ product formation.