Journal
SMALL
Volume 16, Issue 52, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202005254
Keywords
CO; CO2; conductive covalent organic frameworks; electrocatalysis
Categories
Funding
- National Key Research and Development Program of China [2018YFA0208600, 2018YFA0704502]
- NSFC [21871263, 21671188, 22071245, 21520102001]
- Key Research Program of Frontier Science, CAS [QYZDJ-SSW-SLH045]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- Youth Innovation Promotion Association, CAS [Y201850]
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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.
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