Homologous heteropolyaromatic covalent organic frameworks for enhancing photocatalytic hydrogen peroxide production and aerobic oxidation

Jiani Yang, Zhenyang Zhao, Xu Liu, Heng Yang, Jin Yang, Mi Zhou, Shuang Li, Xikui Liu (), Xiaohui Xu () and Chong Cheng ()
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Jiani Yang: Sichuan University
Zhenyang Zhao: Sichuan University
Xu Liu: Sichuan University
Heng Yang: Sichuan University
Jin Yang: University of Oxford
Mi Zhou: Sichuan University
Shuang Li: Sichuan University
Xikui Liu: Sichuan University
Xiaohui Xu: Sichuan University
Chong Cheng: Sichuan University

Nature Communications, 2025, vol. 16, issue 1, 1-15

Abstract: Abstract The development of robust catalysts that can work under harsh conditions bring promise but a challenge for photocatalytic hydrogen peroxide production. Here, we report the design of thiazole-based homologous heteropolyaromatic COFs (TTT-COF) via post-cyclization reaction for photocatalytic H2O2 production and aerobic oxidation of C(sp3)-H bonds. Our studies demonstrate that the elemental S heteroatom enables modified COF materials with high chemical stability, continuous π-conjugation, efficient electron and energy transfer, and an enhanced donor-acceptor (D-A) structure and charge separation, thus boosting their intrinsic photocatalytic activities and stability. Consequently, TTT-COF achieves a photosynthetic H2O2 production rate of 29.9 mmol g−1 h−1 with more than 200 hours of long-term stability when employing 10 % benzyl alcohol (V/V) as a sacrificial agent. Notably, the TTT-COF photocatalyst exhibits high reactivity in the oxidation of ethylbenzene derivatives. We believe this strategy offers a promising pathway to synthesize homologous heteropolyaromatic COFs and holds the potential for large-scale production of COF materials with tailored properties for broad applications in photocatalysis and beyond.

Date: 2025
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DOI: 10.1038/s41467-025-62937-x

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