Linkage Microenvironment of Azoles‐Related Covalent Organic Frameworks Precisely Regulates Photocatalytic Generation of Hydrogen Peroxide

Artificial H2O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry of COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds of...

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Published in:Angewandte Chemie International Edition 2023-09, Vol.62 (36), p.e202309480-n/a
Main Authors: Mou, Yi, Wu, Xiaodong, Qin, Chencheng, Chen, Junying, Zhao, Yanlan, Jiang, Longbo, Zhang, Chen, Yuan, Xingzhong, Huixiang Ang, Edison, Wang, Hou
Format: Article
Language:English
Subjects:
Azoles
Azoles Linkage
Benzene
Charge transfer
COFs
Density functional theory
H2O2
Heterocyclic compounds
Hydrogen peroxide
Imidazole
Microenvironments
Oxazole
Photocatalysis
Photosynthesis
Pyrene
Recombination
Wastewater treatment
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cited_by cdi_FETCH-LOGICAL-c4130-f56c97e45ef3b71f53007f4df110f0f2c0cd93a4fce0ed2ac5ccdc681848f7ea3
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container_title Angewandte Chemie International Edition
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creator Mou, Yi
Wu, Xiaodong
Qin, Chencheng
Chen, Junying
Zhao, Yanlan
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Zhang, Chen
Yuan, Xingzhong
Huixiang Ang, Edison
Wang, Hou
description Artificial H2O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry of COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds of azoles‐linked COFs including thiazole‐linked TZ‐COF, oxazole‐linked OZ‐COF and imidazole‐linked IZ‐COF were successfully synthesized. More accessible channels of charge transfer were constructed in TZ‐COF via the donor‐π‐acceptor structure between thiazole linkage and pyrene linker, leading to efficient suppression of photoexcited charge recombination. Density functional theory calculations support the experimental studies, demonstrating that the thiazole linkage is more favorable for the formation of *O2 intermediate in H2O2 production than that of the oxazole and imidazole linkages. The real active sites in COFs located at the benzene ring fragment between pyrene unit and azole linkage. A tunable covalent organic framework (COF) platform with three azole‐related linkages was prepared through linker exchange reactions. The linkage microenvironment changes the photoelectric properties and photocatalytic performance. The thiazole linkage was more favorable than the oxazole and imidazole linkages for the formation of *O2 intermediate in H2O2 production.
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The effect of linkage chemistry of COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds of azoles‐linked COFs including thiazole‐linked TZ‐COF, oxazole‐linked OZ‐COF and imidazole‐linked IZ‐COF were successfully synthesized. More accessible channels of charge transfer were constructed in TZ‐COF via the donor‐π‐acceptor structure between thiazole linkage and pyrene linker, leading to efficient suppression of photoexcited charge recombination. Density functional theory calculations support the experimental studies, demonstrating that the thiazole linkage is more favorable for the formation of *O2 intermediate in H2O2 production than that of the oxazole and imidazole linkages. The real active sites in COFs located at the benzene ring fragment between pyrene unit and azole linkage. A tunable covalent organic framework (COF) platform with three azole‐related linkages was prepared through linker exchange reactions. The linkage microenvironment changes the photoelectric properties and photocatalytic performance. 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subjects Azoles
Azoles Linkage
Benzene
Charge transfer
COFs
Density functional theory
H2O2
Heterocyclic compounds
Hydrogen peroxide
Imidazole
Microenvironments
Oxazole
Photocatalysis
Photosynthesis
Pyrene
Recombination
Wastewater treatment
title Linkage Microenvironment of Azoles‐Related Covalent Organic Frameworks Precisely Regulates Photocatalytic Generation of Hydrogen Peroxide
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