Dual atomic catalysts from COF‐derived carbon for CO<sub>2</sub>RR by suppressing HER through synergistic effects
Minghao Liu, Sijia Liu, Qing Xu, Qiyang Miao, Shuai Yang, Svenja Hanson, George Z. Chen, Jun He, Zheng Jiang, Gaofeng Zeng
Abstract
Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) for high‐value‐added products is a promising strategy to tackle excessive CO 2 emissions. However, the activity of and selectivity for catalysts for CO 2 RR still need to be improved because of the competing reaction (hydrogen evolution reaction). In this study, for the first time, we have demonstrated dual atomic catalytic sites for CO 2 RR from a core–shell hybrid of the covalent–organic framework and the metal–organic framework. Due to abundant dual atomic sites (with CoN 4 O and ZnN 4 of 2.47 and 11.05 wt.%, respectively) on hollow carbon, the catalyst promoted catalysis of CO 2 RR, with the highest Faradic efficiency for CO of 92.6% at –0.8 V and a turnover frequency value of 1370.24 h –1 at –1.0 V. More importantly, the activity and selectivity of the catalyst were well retained for 30 h. The theoretical calculation further revealed that CoN 4 O was the main site for CO 2 RR, and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.