Promoting CO<sub>2</sub> Electroreduction to Acetate by an Amine-Terminal, Dendrimer-Functionalized Cu Catalyst
Li Yang, Ximeng Lv, Peng Chen, Shuyi Kong, Fuqiang Huang, Yi Tang, Lijuan Zhang, Gengfeng Zheng
Abstract
High Resolution Image Download MS PowerPoint Slide Acetate derived from electrocatalytic CO 2 reduction represents a potential low-carbon synthesis approach. However, the CO 2 -to-acetate activity and selectivity are largely inhibited by the low surface coverage of in situ generated *CO, as well as the inefficient ethenone intermediate formation due to the side reaction between CO 2 and alkaline electrolytes. Tuning catalyst microenvironments by chemical modification of the catalyst surface is a potential strategy to enhance CO 2 capture and increase local *CO concentrations, while it also increases the selectivity of side reduction products, such as methane or ethylene. To solve this challenge, herein, we developed a hydrophilic amine-tailed, dendrimer network with enhanced *CO intermediate coverage on Cu catalytic sites while at the same time retaining the in situ generated OH – as a high local pH environment that favors the ethenone intermediate toward acetate. The optimized amine-network coordinated Cu catalyst (G 3 -NH 2 /Cu) exhibits one of the highest CO 2 -to-acetate Faradaic efficiencies of 47.0% with a partial current density of 202 mA cm –2 at −0.97 V versus the reversible hydrogen electrode.