As the“emission peak and carbon neutrality peak”are proceeding all over the world,CO_(2) electroreduction is studied extensively as it is a powerful way to transform CO_(2)into value-added products.The earthabundant...As the“emission peak and carbon neutrality peak”are proceeding all over the world,CO_(2) electroreduction is studied extensively as it is a powerful way to transform CO_(2)into value-added products.The earthabundant Sn-based materials and copper sulfides as electrochemical catalysts have shown activity for generating formate from CO_(2) electroreduction.Herein,the composite of CuS and S-doped SnO_(2)(CuS/SnO_(2)-S)was synthesized by a redox reaction under room temperature.The unique structural reconstruction of CuS/SnO_(2)-S nanoparticles to Cu/Sn/Cu_(6.26)Sn_(5) nanowires decreases the energy barrier of the adsorption of CO_(2),and increases the adsorption of^(*)H,primarily suppressing the competing reaction of hydrogen evolution reaction(HER).As a result,at-0.8 V vs.RHE,it reaches an electrochemical CO_(2)-to-formate conversion with a Faradaic efficiency(FE)of 84.9%at a yield of 8860μmol h-1cm^(-2) under a partial current density of~18.8 mA cm^(-2) in an H-type reactor.This study provides significant insight into the structural evolution of the CuSn sulfides and the mechanism of formate formation.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22278020,2177060378)the Program for Changjiang Scholars,Innovative Research Teams in Universities of China(Grant No.IRT1205)the Fundamental Research Funds for the Central Universities of China(Grant Nos.12060093063,XK1803-05)。
文摘As the“emission peak and carbon neutrality peak”are proceeding all over the world,CO_(2) electroreduction is studied extensively as it is a powerful way to transform CO_(2)into value-added products.The earthabundant Sn-based materials and copper sulfides as electrochemical catalysts have shown activity for generating formate from CO_(2) electroreduction.Herein,the composite of CuS and S-doped SnO_(2)(CuS/SnO_(2)-S)was synthesized by a redox reaction under room temperature.The unique structural reconstruction of CuS/SnO_(2)-S nanoparticles to Cu/Sn/Cu_(6.26)Sn_(5) nanowires decreases the energy barrier of the adsorption of CO_(2),and increases the adsorption of^(*)H,primarily suppressing the competing reaction of hydrogen evolution reaction(HER).As a result,at-0.8 V vs.RHE,it reaches an electrochemical CO_(2)-to-formate conversion with a Faradaic efficiency(FE)of 84.9%at a yield of 8860μmol h-1cm^(-2) under a partial current density of~18.8 mA cm^(-2) in an H-type reactor.This study provides significant insight into the structural evolution of the CuSn sulfides and the mechanism of formate formation.