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  • Conductive Phthalocyanine‐B...
    Zhang, Meng‐Di; Si, Duan‐Hui; Yi, Jun‐Dong; Zhao, Shao‐Shuai; Huang, Yuan‐Biao; Cao, Rong

    Small (Weinheim an der Bergstrasse, Germany), 12/2020, Letnik: 16, Številka: 52
    Journal Article

    The electroreduction of CO2 to value‐added chemicals such as CO is a promising approach to realize carbon‐neutral energy cycle, but still remains big challenge including low current density. Covalent organic frameworks (COFs) with abundant accessible active single‐sites can offer a bridge between homogeneous and heterogeneous electrocatalysis, but the low electrical conductivity limits their application for CO2 electroreduction reaction (CO2RR). Here, a 2D conductive Ni‐phthalocyanine‐based COF, named NiPc‐COF, is synthesized by condensation of 2,3,9,10,16,17,23,24‐octa‐aminophthalocyaninato Ni(II) and tert‐butylpyrene‐tetraone for highly efficient CO2RR. Due to its highly intrinsic conductivity and accessible active sites, the robust conductive 2D NiPc‐COF nanosheets exhibit very high CO selectivity (>93%) in a wide range of the applied potentials of −0.6 to −1.1 V versus the reversible hydrogen electrode (RHE) and large partial current density of 35 mA cm−2 at −1.1 V versus RHE in aqueous solution that surpasses all the conventional COF electrocatalysts. The robust NiPc‐COF that is bridged by covalent pyrazine linkage can maintain its CO2RR activity for 10 h. This work presents the implementation of the conductive COF nanosheets for CO2RR and provides a strategy to enhance energy conversion efficiency in electrocatalysis. A conductive nickelophthalocyanine‐based 2D covalent organic framework is synthesized and employed as a robust and efficient electrocatalyst for CO2 electroreduction reaction, providing a new route to design highly efficient porous framework materials for the enhanced electrocatalysis via improving electrical conductivity.