The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high select...The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high selectivity and high rate.However,the gas diffusion layer(GDL)of the gas diffusion electrode(GDE)still suffers from low tolerance and limited active sites.Here,the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE,which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.The resultant GDE exhibits multi-carbon(C_(2+))product selectivity over faradaic efficiency(FE)of 70.0%in the range of 100 to 800 mA·cm^(-2),with the peak FE^(c2+)of 85.2%at 800 mA·cm^(-2).Notably,the strengthened GDE could continuously drive high-current electrolysis for more than 100 h without flooding.This work opens a new way to improve CO_(2) gas diffusion electrolysis via surface molecular engineering.展开更多
基金supported by the International(Regional)Cooperation and Exchange Projects of the National Natural Science Foundation of China(No.51920105003)the National Natural Science Funds for Distinguished Young Scholars(No.51725201)+5 种基金the Innovation Program of Shanghai Municipal Education Commission(No.E00014)the National Natural Science Foundation of China(Nos.51902105 and 22072045)the Shanghai Engineering Research Center of Hierarchical Nanomaterials(No.18DZ2252400)the Shanghai Sailing Program(No.19YF1411600)support by Shanghai Rising-star and Shuguang Programs(Nos.20QA1402400 and 17SG30)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning.
文摘The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high selectivity and high rate.However,the gas diffusion layer(GDL)of the gas diffusion electrode(GDE)still suffers from low tolerance and limited active sites.Here,the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE,which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.The resultant GDE exhibits multi-carbon(C_(2+))product selectivity over faradaic efficiency(FE)of 70.0%in the range of 100 to 800 mA·cm^(-2),with the peak FE^(c2+)of 85.2%at 800 mA·cm^(-2).Notably,the strengthened GDE could continuously drive high-current electrolysis for more than 100 h without flooding.This work opens a new way to improve CO_(2) gas diffusion electrolysis via surface molecular engineering.