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Research Article | Online first | Published: 22 March 2024

Primitive functional groups directed distinct photocatalytic performance of imine-linked donor–acceptor covalent organic frameworks

Show Author's Information Xitong Ren1,  Jiajie Sun2,  Yusen Li1( ),  Feng Bai1( )
Key Laboratory for Special Functional Materials of Ministry of Education, National and Local Joint Engineering Research Center for High-Efficiency Display and Lighting Technology, School of Materials Science and Engineering, and Collaborative Innovation Center of Nano Functional Materials and Applications, Henan University, Kaifeng 475004, China
School of Physics and Electronics, Henan University, Kaifeng 475004, China
Keywords:
photocatalysis, functional group, covalent organic frameworks, donor-acceptor
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Photocatalytic activity
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Ren X, Sun J, Li Y, et al. Primitive functional groups directed distinct photocatalytic performance of imine-linked donor–acceptor covalent organic frameworks. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6509-5
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Abstract Full text Electronic supplementary material About this article

The combination of donor–acceptor (D–A) structures presents a viable strategy for fabricating covalent organic frameworks (COFs) with exceptional photocatalytic performances. Nevertheless, the selection of functional groups on donor or acceptor building blocks and their effect on the macroscopic properties of COFs are ambiguous. In this study, we tactfully synthesized a pair of Py-DBT-COFs from the same pyrene (Py) donor and 4,7-diphenylbenzo[c][1,2,5]thiadiazole (DBT) acceptor cores with distinct primitive functional groups. The primitive functional groups of building units determine the photocatalytic properties of corresponding Py-DBT-COFs. Specifically, Py-C-DBT-COF synthesized from Py-4CHO and DBT-2NH2 showcases a splendid H2 evolution rate as high as 21,377.7 μmol/(g·h) (with 5 wt.% Pt) originating from better charge transfer capacity, which is significantly superior to that of Py-N-DBT-COF constructed from Py-4NH2 and DBT-2CHO. The distinct photocatalytic performances of the two COFs are demonstrated to originate from the different charge separation and transfer capabilities. This work supplies a new avenue for optimizing the photocatalytic performance of D–A COFs from the perspective of primitive functional group selections.


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Electronic supplementary material
About this article

Primitive functional groups directed distinct photocatalytic performance of imine-linked donor–acceptor covalent organic frameworks

Show Author's information Xitong Ren1, Jiajie Sun2, Yusen Li1( ), Feng Bai1( )
Key Laboratory for Special Functional Materials of Ministry of Education, National and Local Joint Engineering Research Center for High-Efficiency Display and Lighting Technology, School of Materials Science and Engineering, and Collaborative Innovation Center of Nano Functional Materials and Applications, Henan University, Kaifeng 475004, China
School of Physics and Electronics, Henan University, Kaifeng 475004, China

Abstract

The combination of donor–acceptor (D–A) structures presents a viable strategy for fabricating covalent organic frameworks (COFs) with exceptional photocatalytic performances. Nevertheless, the selection of functional groups on donor or acceptor building blocks and their effect on the macroscopic properties of COFs are ambiguous. In this study, we tactfully synthesized a pair of Py-DBT-COFs from the same pyrene (Py) donor and 4,7-diphenylbenzo[c][1,2,5]thiadiazole (DBT) acceptor cores with distinct primitive functional groups. The primitive functional groups of building units determine the photocatalytic properties of corresponding Py-DBT-COFs. Specifically, Py-C-DBT-COF synthesized from Py-4CHO and DBT-2NH2 showcases a splendid H2 evolution rate as high as 21,377.7 μmol/(g·h) (with 5 wt.% Pt) originating from better charge transfer capacity, which is significantly superior to that of Py-N-DBT-COF constructed from Py-4NH2 and DBT-2CHO. The distinct photocatalytic performances of the two COFs are demonstrated to originate from the different charge separation and transfer capabilities. This work supplies a new avenue for optimizing the photocatalytic performance of D–A COFs from the perspective of primitive functional group selections.

Keywords: photocatalysis, functional group, covalent organic frameworks, donor-acceptor

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Publication history
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Acknowledgements

Publication history

Received: 21 December 2023
Revised: 21 January 2024
Accepted: 21 January 2024
Published: 22 March 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22201063 and U21A2085), Science and Technology Research and Development Plan Joint Fund of Henan Province (No. 225200810083), Science and Technology Research and Development Program of Henan Province (No. 232102230083), High-level talents international training project of Henan Province (K2306Y), Project of Scientific and Technological Innovation Team in University of Henan Province, China (No. 20IRTSTHN001), and the Zhongyuan High-Level Talents Special Support Plan of China (No. 204200510009). Y. S. L. gratefully acknowledges financial support from the Zhongyuan Youthful Postdoctoral Innovative Talent Program of Henan Province, China.

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