摘要
Electrochemical CO_(2)reduction is a sustainable approach in green chemistry that enables the production of valuable chemicals and fuels while mitigating the environmental impact associated with CO_(2)emissions.Despite its several advantages,this technology suffers from an intrinsically low CO_(2)solubility in aqueous solutions,resulting in a lower local CO_(2)concentration near the electrode,which yields lower current densities and restricts product selectivity.Gas diffusion electrodes(GDEs),particularly those with tubular architectures,can solve these issues by increasing the local CO_(2)concentration and triple-phase interface,providing abundant electroactive sites to achieve superior reaction rates.In this study,robust and self-supported Cu flow-through gas diffusion electrodes(FTGDEs)were synthesized for efficient formate production via electrochemical CO_(2)reduction.They were further compared with traditional Cu electrodes,and it was found that higher local CO_(2)concentration due to improved mass transfer,the abundant surface area available for the generation of the triple-phase interface,and the porous structure of Cu FTGDEs enabled high formate Faradaic efficiency(76%)and current density(265 mA¸cm^(−2))at–0.9 V vs.reversible hydrogen electrode(RHE)in 0.5 mol·L^(−1)KHCO3.The combined phase inversion and calcination process of the Cu FTGDEs helped maintain a stable operation for several hours.The catalytic performance of the Cu FTGDEs was further investigated in a non-gas diffusion configuration to demonstrate the impact of local gas concentration on the activity and performance of electrochemical CO_(2)reduction.This study demonstrates the potential of flow-through gas-diffusion electrodes to enhance reaction kinetics for the highly efficient and selective reduction of CO_(2),offering promising applications in sustainable electrochemical processes.
基金
supported by the National Key Research and Development Plan Project of China(Grant No.2018YFA0702300)
the National Natural Science Foundation of China(Grant No.52227813).
作者简介
Bachirou Guene Lougou,E-mail:lougou@hit.edu.cn;Yong Shuai,E-mail:shuaiyong@hit.edu.cn。
