Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)represents an advanced technology for converting CO_(2)into highly valuable chemicals.Although significant progress has been achieved in producing multi-carbon chemic...Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)represents an advanced technology for converting CO_(2)into highly valuable chemicals.Although significant progress has been achieved in producing multi-carbon chemicals such as ethylene(C2H4),addressing(bi)carbonate salt formation and precipitation in alkaline electrolytes remains a critical challenge for achieving longterm stability during industrialization.We developed a Cu_(2)(OH)_(2)CO_(3)/Mg^(2+)/C pre-catalyst,which transforms into a catalytically active Cu0/Cu^(2+)/Mg^(2+)composite by electroreduction.Crucially,the application of different ionomers(specifically Sustainion XA-9)on this composite catalyst effectively alleviates salt precipitation issues,thereby enabling high-selectivity,durable CO_(2)-to-C^(2+)conversion.In a membrane electrode assembly,the maximum Faradaic efficiency for C^(2+)products reaches 80%,with stable operation at 200 mA cm^(−2)for 50 h.In situ Raman spectroscopy reveals that only top-type*CO intermediate exists on the Cu0/Cu^(2+)/Nafion cathode,whereas both bridge-type and top-type of*CO sites coexist on the Cu^(0)/Cu^(2+)/Mg^(2+)/Sustainion XA-9 cathode.This dual adsorption configuration facilitates the C─C coupling kinetics on the catalyst,inducing a favorable microenvironment for selective C^(2+)formation.Therefore,strategic optimization of catalyst architectures and ionomer engineering enables CO_(2)RR with improved efficiency and durability,advancing green chemistry and carbon-neutral technologies.展开更多
基金supported by the National Natural Science Foundation of China(No.22303087)the Joint Fund of the Technical R&D Program of Henan Province(No.232301420049)the Natural Science Foundation of Henan Province(No.212300410281).
文摘Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)represents an advanced technology for converting CO_(2)into highly valuable chemicals.Although significant progress has been achieved in producing multi-carbon chemicals such as ethylene(C2H4),addressing(bi)carbonate salt formation and precipitation in alkaline electrolytes remains a critical challenge for achieving longterm stability during industrialization.We developed a Cu_(2)(OH)_(2)CO_(3)/Mg^(2+)/C pre-catalyst,which transforms into a catalytically active Cu0/Cu^(2+)/Mg^(2+)composite by electroreduction.Crucially,the application of different ionomers(specifically Sustainion XA-9)on this composite catalyst effectively alleviates salt precipitation issues,thereby enabling high-selectivity,durable CO_(2)-to-C^(2+)conversion.In a membrane electrode assembly,the maximum Faradaic efficiency for C^(2+)products reaches 80%,with stable operation at 200 mA cm^(−2)for 50 h.In situ Raman spectroscopy reveals that only top-type*CO intermediate exists on the Cu0/Cu^(2+)/Nafion cathode,whereas both bridge-type and top-type of*CO sites coexist on the Cu^(0)/Cu^(2+)/Mg^(2+)/Sustainion XA-9 cathode.This dual adsorption configuration facilitates the C─C coupling kinetics on the catalyst,inducing a favorable microenvironment for selective C^(2+)formation.Therefore,strategic optimization of catalyst architectures and ionomer engineering enables CO_(2)RR with improved efficiency and durability,advancing green chemistry and carbon-neutral technologies.
