Developing high-efficiency catalyst is crucial for electrochemical conversion of carbon dioxide(CO_(2))to high-value products.In the present work,a three-chamber electrolysis cell has been developed for CO_(2)reductio...Developing high-efficiency catalyst is crucial for electrochemical conversion of carbon dioxide(CO_(2))to high-value products.In the present work,a three-chamber electrolysis cell has been developed for CO_(2)reduction to carbon monoxide(CO)in an organic electrolyte,with sodium hydroxide(NaOH)and chlorine(Cl_(2))produced as byproducts.In order to improve the performance of the three-chamber electrolyzer,a gallium-based(Ga-based)ternary-porous catalyst(Ga-In_(4)Ag_(9))has been fabricated.During the long-term electrolysis process,Ga-In_(4)Ag_(9)catalyst exhibits good performance toward CO_(2)reduction reaction(CO_(2)RR),the CO partial current density achieves to 139.21 mA·cm^(-2)at-2.4 V(vs.SHE),with the Faraday efficiency(FE)of CO formation stabled at 92.3%.Density functional theory(DFT)analysis reveals that the position of the d-band center of Ga-In_(4)Ag_(9)is regulated by silver(Ag)atoms,which is beneficial for enhancing the binding ability between the catalyst and the intermediate.Owing to the adsorption of Cl^(-)on the surface of Ga-In_(4)Ag_(9),the reconfiguration of electron density has been altered,which is beneficial for the stabilization of*CO_(2)-intermediate.This work provides valuable insights for designing Ga-based metal catalysts toward CO_(2)electrolysis to produce high-value chemicals.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52164048 and 52067012)the Natural Science Foundation of Kunming University of Science and Technology(No.KKZ3202437105)the Analysis and Testing Foundation of Kunming University of Science and Technology(No.2023P20221102026).
文摘Developing high-efficiency catalyst is crucial for electrochemical conversion of carbon dioxide(CO_(2))to high-value products.In the present work,a three-chamber electrolysis cell has been developed for CO_(2)reduction to carbon monoxide(CO)in an organic electrolyte,with sodium hydroxide(NaOH)and chlorine(Cl_(2))produced as byproducts.In order to improve the performance of the three-chamber electrolyzer,a gallium-based(Ga-based)ternary-porous catalyst(Ga-In_(4)Ag_(9))has been fabricated.During the long-term electrolysis process,Ga-In_(4)Ag_(9)catalyst exhibits good performance toward CO_(2)reduction reaction(CO_(2)RR),the CO partial current density achieves to 139.21 mA·cm^(-2)at-2.4 V(vs.SHE),with the Faraday efficiency(FE)of CO formation stabled at 92.3%.Density functional theory(DFT)analysis reveals that the position of the d-band center of Ga-In_(4)Ag_(9)is regulated by silver(Ag)atoms,which is beneficial for enhancing the binding ability between the catalyst and the intermediate.Owing to the adsorption of Cl^(-)on the surface of Ga-In_(4)Ag_(9),the reconfiguration of electron density has been altered,which is beneficial for the stabilization of*CO_(2)-intermediate.This work provides valuable insights for designing Ga-based metal catalysts toward CO_(2)electrolysis to produce high-value chemicals.
