Regulating energy band structures of triazine covalent organic frameworks with electron-donating/withdrawing substituents for visible-light-responsive photocatalytic tetracycline degradation and Cr(VI) reduction

Zhang, H; Zhang, L; Dong, S; Duan, X; Zhu, D; Ni, BJ; Lyu, C

Regulating energy band structures of triazine covalent organic frameworks with electron-donating/withdrawing substituents for visible-light-responsive photocatalytic tetracycline degradation and Cr(VI) reduction

Zhang, H Zhang, L Dong, S Duan, X Zhu, D Ni, BJ Lyu, C

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Publisher:: Elsevier
Publication Type:: Journal Article
Citation:: Journal of Hazardous Materials, 2023, 446, pp. 130756
Issue Date:: 2023-03-15

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Field	Value	Language
dc.contributor.author	Zhang, H
dc.contributor.author	Zhang, L
dc.contributor.author	Dong, S
dc.contributor.author	Duan, X
dc.contributor.author	Zhu, D
dc.contributor.author	Ni, BJ
dc.contributor.author	Lyu, C
dc.date.accessioned	2023-03-22T02:32:26Z
dc.date.available	2023-03-22T02:32:26Z
dc.date.issued	2023-03-15
dc.identifier.citation	Journal of Hazardous Materials, 2023, 446, pp. 130756
dc.identifier.issn	0304-3894
dc.identifier.issn	1873-3336
dc.identifier.uri	http://hdl.handle.net/10453/168042
dc.description.abstract	Environmental contaminations have raised soaring concerns about human health worldwide. Developing metal-free photocatalysts as green agents to solve these problems is urgent. Covalent organic frameworks (COFs) are considered a promising platform for the molecule-level design of visible-light-responsive photocatalysts due to their tailored coordination/electronic structures and excellent charge carrier mobility. However, COFs without substituents (e.g., COFs-H) still suffer from broad bandgaps and low electron-hole separation efficiency. In this work, we introduced electron-donating/withdrawing substituents on COFs-H to fine-tune the bandgap and photocatalytic performance of COFs. Theoretical and experimental studies revealed that all substituents narrowed the bandgap of COFs and enhanced the electron-hole separation efficiency. Electron-withdrawing/donating substituents significantly alter the energy level of COFs-R, improving the redox capacities of photo-generated holes and electrons for tetracycline (TC) degradation and Cr(VI) reduction. The large difference in electrostatic potential between the two monomers in COFs-R enhances the charge carrier generation and intramolecular electron transfer intrinsically. This work unravels how substituents with different electronic effects regulate the energy band structures and photo-redox capacities of COFs. It further provides new insight into the precise regulation of COFs toward highly efficient visible-light-driven photocatalytic remediation of organic contaminants and heavy metal ions.
dc.language	en
dc.publisher	Elsevier
dc.relation.ispartof	Journal of Hazardous Materials
dc.relation.isbasedon	10.1016/j.jhazmat.2023.130756
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	03 Chemical Sciences, 05 Environmental Sciences, 09 Engineering
dc.subject.classification	Strategic, Defence & Security Studies
dc.title	Regulating energy band structures of triazine covalent organic frameworks with electron-donating/withdrawing substituents for visible-light-responsive photocatalytic tetracycline degradation and Cr(VI) reduction
dc.type	Journal Article
utslib.citation.volume	446
utslib.for	03 Chemical Sciences
utslib.for	05 Environmental Sciences
utslib.for	09 Engineering
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology/School of Civil and Environmental Engineering
pubs.organisational-group	/University of Technology Sydney/Strength - CTWW - Centre for Technology in Water and Wastewater Treatment
utslib.copyright.status	closed_access	*
dc.date.updated	2023-03-22T02:32:07Z
pubs.publication-status	Published
pubs.volume	446

Abstract:

Environmental contaminations have raised soaring concerns about human health worldwide. Developing metal-free photocatalysts as green agents to solve these problems is urgent. Covalent organic frameworks (COFs) are considered a promising platform for the molecule-level design of visible-light-responsive photocatalysts due to their tailored coordination/electronic structures and excellent charge carrier mobility. However, COFs without substituents (e.g., COFs-H) still suffer from broad bandgaps and low electron-hole separation efficiency. In this work, we introduced electron-donating/withdrawing substituents on COFs-H to fine-tune the bandgap and photocatalytic performance of COFs. Theoretical and experimental studies revealed that all substituents narrowed the bandgap of COFs and enhanced the electron-hole separation efficiency. Electron-withdrawing/donating substituents significantly alter the energy level of COFs-R, improving the redox capacities of photo-generated holes and electrons for tetracycline (TC) degradation and Cr(VI) reduction. The large difference in electrostatic potential between the two monomers in COFs-R enhances the charge carrier generation and intramolecular electron transfer intrinsically. This work unravels how substituents with different electronic effects regulate the energy band structures and photo-redox capacities of COFs. It further provides new insight into the precise regulation of COFs toward highly efficient visible-light-driven photocatalytic remediation of organic contaminants and heavy metal ions.

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http://hdl.handle.net/10453/168042