A disubstituted quaterpyridine based cobalt complex non‐covalently tethered to multiwalled carbon nanotube(MWCNT)substrate,forming a hybrid catalyst,Co‐qpyCOOH/CNT,catalyzed the conversion of CO_(2) to CO under aque...A disubstituted quaterpyridine based cobalt complex non‐covalently tethered to multiwalled carbon nanotube(MWCNT)substrate,forming a hybrid catalyst,Co‐qpyCOOH/CNT,catalyzed the conversion of CO_(2) to CO under aqueous conditions.At an optimal and uniform loading,it exhibited remarkable catalytic activity,near‐exclusive selectivity,and high stability towards the formation of CO.At a mere cathodic potential of−0.65 V versus RHE(η=0.54 V),it achieved a high partial current density of−6.7 mA/cm^(2) and a F.E.CO=100%.In addition,with 20 h of stable operation,hydrogen evolution remained practically undetected.Its hybrid structure due to noncovalent immobilization on MWCNT imparted the intrinsic activity and much‐needed stability in performance whereas‒COOH groups may stabilize the intermediates by acting as H‐bond donors,promoting catalytic activity.Tethering to a conductive solid substrate and tuning of the second sphere of coordination played an important role in its performance to achieve desired reduction product with high selectivity and activity.展开更多
基金Zhejiang Provincial Natural Science Foundation of China,Grant/Award Number:LZ20B030001Agency for Science,Technology,and Research(A*STAR),Singapore,Grant/Award Number:AME Individual Research Grant(Grant A1983c0026)+1 种基金Campus for Research Excellence and Technological Enterprise(CREATE)program,National Research Foundation(NRF),Prime Minister's Office,SingaporeNational Natural Science Foundation of China,Grant/Award Numbers:21972106,51872209。
文摘A disubstituted quaterpyridine based cobalt complex non‐covalently tethered to multiwalled carbon nanotube(MWCNT)substrate,forming a hybrid catalyst,Co‐qpyCOOH/CNT,catalyzed the conversion of CO_(2) to CO under aqueous conditions.At an optimal and uniform loading,it exhibited remarkable catalytic activity,near‐exclusive selectivity,and high stability towards the formation of CO.At a mere cathodic potential of−0.65 V versus RHE(η=0.54 V),it achieved a high partial current density of−6.7 mA/cm^(2) and a F.E.CO=100%.In addition,with 20 h of stable operation,hydrogen evolution remained practically undetected.Its hybrid structure due to noncovalent immobilization on MWCNT imparted the intrinsic activity and much‐needed stability in performance whereas‒COOH groups may stabilize the intermediates by acting as H‐bond donors,promoting catalytic activity.Tethering to a conductive solid substrate and tuning of the second sphere of coordination played an important role in its performance to achieve desired reduction product with high selectivity and activity.
