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
An original interfacial hybrid cross-linker molecule combined electrochemical and photochemical properties by substitution of two functional groups,pyrene,and diazirine.The first group enables anchoring by strong p-st...An original interfacial hybrid cross-linker molecule combined electrochemical and photochemical properties by substitution of two functional groups,pyrene,and diazirine.The first group enables anchoring by strong p-stacking interaction or by electropolymerization onto multi-walled carbon nanotubes(MWCNT).The other photoreactive group allows the covalent link with biomolecules under long-wavelength UV illumination.Diazirine was chosen due to its ability to photogenerate high reactive radicals under UV irradiation.The photoreactivity of these immobilized nanostructured conductive surfaces was tested towards the covalent attachment of tyrosinase which is well known to oxidize a large range of phenolic compounds and its yield and availability was evaluated by amperometric measurements of catechol by using molecular dioxygen.The architecture exhibiting the best analytical characteristics obtained for catechol was then chosen to detect dopamine.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.
基金the Labex ARCANE(ANR-11-LABX-0003-01)Grenoble Institute Carnot POLYNAT(ANR-16-CARN-0025-01)platform Chimie NanoBio ICMG FR 2607(PCN-ICMG).Besides,the authors are grateful for financial support from PHC Braˆncus¸i program 2015–2016 number 32602 QD,the Romanian National Authority for Scientific Research,CNCS—UEFISCDI,Project Number PNII-RU-TE-2014-4-0460 and UMF regarding the internal Grant Number 7690/56/15.04.2016.
文摘An original interfacial hybrid cross-linker molecule combined electrochemical and photochemical properties by substitution of two functional groups,pyrene,and diazirine.The first group enables anchoring by strong p-stacking interaction or by electropolymerization onto multi-walled carbon nanotubes(MWCNT).The other photoreactive group allows the covalent link with biomolecules under long-wavelength UV illumination.Diazirine was chosen due to its ability to photogenerate high reactive radicals under UV irradiation.The photoreactivity of these immobilized nanostructured conductive surfaces was tested towards the covalent attachment of tyrosinase which is well known to oxidize a large range of phenolic compounds and its yield and availability was evaluated by amperometric measurements of catechol by using molecular dioxygen.The architecture exhibiting the best analytical characteristics obtained for catechol was then chosen to detect dopamine.
