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

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Nano Research 2023年第3期16卷 3649-3657页

作者： Huajian Xu Huizhu Cai Linxia Cui Limei Yu Rui Gao Chuan Shi State Key Laboratory of Fine Chemicals College of Chemical EngineeringDalian University of TechnologyDalian 116024China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

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.

关键词： electrocatalytic CO_(2)reduction cobalt tetracarboxylphthalocyanine amino functionalized carbon nanotubes amidation

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