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Linkage microenvironment of azoles‐related covalent organic frameworks precisely regulates photocatalytic generation of hydrogen peroxide
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Type
Article
Citation
Mou, Y., Wu, X., Qin, C., Chen, J., Zhao, Y., Jiang, L., Zhang, C., Yuan, X., Ang, E. H., & Wang, H. (2023). Linkage microenvironment of azoles‐related covalent organic frameworks precisely regulates photocatalytic generation of hydrogen peroxide. Angewandte Chemie, 135(36), Article e202309480. https://doi.org/10.1002/ange.202309480
Author
Mou, Yi
•
Wu, Xiaodong
•
Qin, Chencheng
•
Chen, Junying
•
Zhao, Yanlan
•
Jiang, Longbo
•
Zhang, Chen
•
Yuan, Xingzhong
•
•
Wang, Hou
Abstract
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.
Date Issued
2023
Publisher
Wiley
Journal
Angewandte Chemie
DOI
10.1002/ange.202309480