Boosting CO2 Photoreduction via Regulating Charge Transfer Ability in a One‐Dimensional Covalent Organic Framework

Author:

Zou Lei12,Chen Zi‐Ao13,Si Duan‐Hui12,Yang Shuai‐Long12,Gao Wen‐Qiang4,Wang Kai4,Huang Yuan‐Biao123ORCID,Cao Rong123ORCID

Affiliation:

1. State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 350002 Fujian Fuzhou P. R. China

2. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian P. R. China

3. University of Chinese Academy of Sciences 100049 Beijing P. R. China

4. Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences 100190 Beijing P. R. China

Abstract

AbstractTwo‐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 μmol 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.

Funder

Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China

Natural Science Foundation of Fujian Province

National Key Research and Development Program of China

Publisher

Wiley

Subject

General Chemistry,Catalysis

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