Oxygen vacancies in metal oxides can serve as electron trap centers to capture CO_(2) and lower energy barriers for the electrochemical CO_(2) reduction reaction(CO_(2)RR).Under aqueous electrolytes,however,such charg...Oxygen vacancies in metal oxides can serve as electron trap centers to capture CO_(2) and lower energy barriers for the electrochemical CO_(2) reduction reaction(CO_(2)RR).Under aqueous electrolytes,however,such charge-enriched active sites can be occupied by adsorbed hydrogen(H∗)and lose their effectiveness for the CO_(2)RR.Here,we develop an efficient catalyst consisting of Cu-doped,defect-rich ZnO(Cu–ZnO)for the CO_(2)RR,which exhibits enhanced CO Faradaic efficiency and current density compared to pristine ZnO.The introduced Cu dopants simultaneously stabilize neighboring oxygen vacancies and modulate their local electronic structure,achieving inhibition of hydrogen evolution and acceleration of the CO_(2)RR.In a flow cell test,a current density of more than 45mAcm^(−2) and a CO Faradaic efficiency of>80%is obtained for a Cu–ZnO electrocatalyst in the wide potential range of−0.76V to−1.06V vs.Reversible Hydrogen Electrode(RHE).This work opens up great opportunities for dopant-modulated metal oxide catalysts for the CO_(2)RR.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51773165,51973171)Natural Science Foundation of Shaanxi Province(2020JC-09)Key Laboratory Construction Program of Xi'an Municipal Bureau of Science and Technology(201805056ZD7CG40).
文摘Oxygen vacancies in metal oxides can serve as electron trap centers to capture CO_(2) and lower energy barriers for the electrochemical CO_(2) reduction reaction(CO_(2)RR).Under aqueous electrolytes,however,such charge-enriched active sites can be occupied by adsorbed hydrogen(H∗)and lose their effectiveness for the CO_(2)RR.Here,we develop an efficient catalyst consisting of Cu-doped,defect-rich ZnO(Cu–ZnO)for the CO_(2)RR,which exhibits enhanced CO Faradaic efficiency and current density compared to pristine ZnO.The introduced Cu dopants simultaneously stabilize neighboring oxygen vacancies and modulate their local electronic structure,achieving inhibition of hydrogen evolution and acceleration of the CO_(2)RR.In a flow cell test,a current density of more than 45mAcm^(−2) and a CO Faradaic efficiency of>80%is obtained for a Cu–ZnO electrocatalyst in the wide potential range of−0.76V to−1.06V vs.Reversible Hydrogen Electrode(RHE).This work opens up great opportunities for dopant-modulated metal oxide catalysts for the CO_(2)RR.
