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Highly selective and efficient electroreduction of CO_(2) in water by quaterpyridine derivative‐based molecular catalyst noncovalently tethered to carbon nanotubes

查看全文 作  者:Vikas [1]Reddu;Libo [1,2]Sun;Xiaogang [1]Li;Huile [3]Jin;Shun [3]Wang;Xin [1,2]Wang 高影响力作者 机构地区:[1]School of Chemical and Biomedical Engineering,Nanyang Technological University,Singapore,Singapore;[2]Cambridge Centre for Advanced Research and Education in Singapore Ltd(Cambridge CARES),CREATE Tower,Singapore,Singapore;[3]College of Chemistry&Materials Engineering,Wenzhou University,Wenzhou,China高影响力机构 出  处:《SmartMat》索引2022年第3卷第1期,共12页高影响力期刊 基  金:Zhejiang Provincial Natural Science Foundation of China,Grant/Award Number:LZ20B030001;Agency for Science,Technology,and Research(A*STAR),Singapore,Grant/Award Number:AME Individual Research Grant(Grant A1983c0026);Campus for Research Excellence and Technological Enterprise(CREATE)program,National Research Foundation(NRF),Prime Minister's Office,Singapore;National Natural Science Foundation of China,Grant/Award Numbers:21972106,51872209。 摘  要: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. 关 键 词:carbon dioxide reduction cobalt complex disubstituted quaterpyridine heterogeneous molecular catalysis second coordination sphere
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