Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202309820
Keywords
CO2 Photoreduction; Charge Transfer; Covalent Organic Framework; Edge Microstructure; One-Dimensional
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This study presents a valuable approach to address the limitations of in-plane charge transfer in imine-based covalent organic frameworks (COFs) by constructing a one-dimensional PyTTA-COF framework. The dimensionality-induced local electronic modulation strategy enables significantly enhanced CO2 photoreduction activity, providing a potential solution to improve the efficiency of CO2 reduction.
Two-dimensional (2D) imine-based covalent organic frameworks (COFs) hold potential for photocatalytic CO2 reduction. However, high energy barrier of imine linkage impede the in-plane photoelectron transfer process, resulting in inadequate efficiency of CO2 photoreduction. Herein, we present a dimensionality induced local electronic modulation strategy through the construction of one-dimensional (1D) pyrene-based covalent organic frameworks (PyTTA-COF). The dual-chain-like edge architectures of 1D PyTTA-COF enable the stabilization of aromatic backbones, thus reducing energy loss during exciton dissociation and thermal relaxation, which provides energetic photoelectron to traverse the energy barrier of imine linkages. As a result, the 1D PyTTA-COF exhibits significantly enhanced CO2 photoreduction activity under visible-light irradiation when coordinated with metal cobalt ion, yielding a remarkable CO evolution of 1003 mu mol g(-1) over an 8-hour period, which surpasses that of the corresponding 2D counterpart by a factor of 59. These findings present a valuable approach to address in-plane charge transfer limitations in imine-based COFs.
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