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Molecular modulating of cobalt phthalocyanines on aminofunctionalized carbon nanotubes for enhanced electrocatalytic CO_(2)conversion

作     者:Huajian Xu Huizhu Cai Linxia Cui Limei Yu Rui Gao Chuan Shi Huajian Xu;Huizhu Cai;Linxia Cui;Limei Yu;Rui Gao;Chuan Shi

作者机构:State Key Laboratory of Fine ChemicalsCollege of Chemical EngineeringDalian University of TechnologyDalian 116024China College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot 010021China 

出 版 物:《Nano Research》 (纳米研究(英文版))

年 卷 期:2023年第16卷第3期

页      面:3649-3657页

核心收录:

学科分类:081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基  金:supported by the National Natural Science Foundation of China(Nos.21872014,21932002,21902018,21962013,and 22172083) the National Key Research and Development(R&D)Program of China(No.2017YFA0700103) the Fundamental Research Funds for the Central Universities(No.DUT20ZD205) the Natural Science Foundation of Liaoning Province(No.2019-MS-053) the Liaoning Revitalization Talent Program(No.XLYC2008032) 

主  题:electrocatalytic CO_(2)reduction cobalt tetracarboxylphthalocyanine amino functionalized carbon nanotubes amidation 

摘      要:Metal porphyrins and metal phthalocyanines(Pc)constitute a promising class of metal molecular catalysts(MMCs)for efficient CO_(2)-to-CO electrocatalytic conversion due to their well-defined molecular *** to adjust the local coordination and electronic environment of the metal center and enhance the molecular-level dispersion of the active components remains as great challenges for further improving the ***,a cobalt(II)Pc(CoPc)-COOH/carbon nanotube(CNT)-NH_(2)hybrid catalyst was rationally designed by clicking the CoPc-COOH molecules onto the surface of CNT-NH_(2)through amidation *** novel hybrid catalyst exhibited the enhanced current density of 22.4 mA/cm2 and CO selectivity of 91%at−0.88 V *** hydrogen electrode(RHE)in the CO_(2)electroreduction,as compared with CoPc-COOH/CNT and CoPc/CNT *** superior activity was ascribed to the charge transfer induced by introduction of-COOH and-NH_(2)functional groups to CoPc and CNT,respectively,facilitating the active centers of CoI being generated at lower potentials,and leading to the highest turnover frequency(TOF)being obtained over the CoPc-COOH/CNT-NH_(2)hybrid *** inherent directivity and saturability of covalent bonds formed via the amidation reaction ensure not only a higher density of Co active centers,but also an improved stability for CO_(2)reduction reaction(CO_(2)RR).The present study represents an effective strategy for improving MMCs performance by molecular modulating of metal phthalocyanines on functionalized carbon substrates directed by click confinement chemistry.

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