Citation: Jun Gao, Lichao Wang, Shunwei Huang, Hao Du, Huayue Zhu, Derek Hao, Yanling Wu, Qi Wang, Limin Jin. Optimizing exciton interactions in covalent organic frameworks for boosting photocatalytic hydrogen peroxide production toward water decontamination[J]. Chinese Chemical Letters, ;2026, 37(8): 112283. doi: 10.1016/j.cclet.2025.112283 shu

Optimizing exciton interactions in covalent organic frameworks for boosting photocatalytic hydrogen peroxide production toward water decontamination

Jun Gao ^a ,
Lichao Wang ^a ,
Shunwei Huang ^a ,
Hao Du ^a ,
Huayue Zhu ^b ,
Derek Hao ^c ,
Yanling Wu ^{a, *,} ,
Qi Wang ^{a, *,} ,
Limin Jin ^{a, *,}

a.
Zhejiang Key Laboratory of Solid Waste Pollution Control and Resource Utilization, School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310012, China
b.
Institute of Environmental Engineering Technology, Taizhou University, Taizhou 318000, China
c.
School of Science, RMIT University, Melbourne 3000, Australia

wuyanling@zjgsu.edu.cn

wangqi8327@zjgsu.edu.cn

jinlimin@zjgsu.edu.cn

Received Date: 21 July 2025
Revised Date: 10 October 2025
Accepted Date: 14 December 2025
Available Online: 15 December 2025

Figures(5)

Solar-driven hydrogen peroxide (H₂O₂) production presents a sustainable alternative to energy-intensive industrial methods, yet its efficiency using covalent organic frameworks (COFs) suffer from energy loss caused by strong exciton interactions. Herein, we designed COFs with donor-π-acceptor (D-π-A) architectures, using 2,5-dimethoxy-1,4-benzenedicarboxaldehyde as the D unit and optimizing the N-containing π-bridge units. The resulting TAPT–OCH₃ COF, incorporating 4,4′,4′'-(1,3,5-triazine-2,4,6-triyl)trianiline as the A unit, demonstrated the extended electron pathways and the reduced exciton recombination, markedly boosting photocatalytic performance. Experimental results revealed that TAPT–OCH₃ achieved a solar-to-chemical efficiency of 0.23% and a quantum yield of 2.21% at 420 nm, outperforming most reported COFs and metal-free catalysts. In situ characterization and theoretical calculations revealed that the TAPT–OCH₃ enhances charge separation to drive H₂O₂ production via a 2e^- oxygen reduction pathway, while its tailored electronic structure simultaneously improves the 1e^- water oxidation process. Crucially, TAPT–OCH₃ maintained high efficacy across diverse water sources and continuous-flow reactors under natural sunlight, enabling scalable H₂O₂ synthesis for water purification. Life cycle assessment confirmed the application stability of this material, underscoring its potential for sustainable environmental remediation. This work establishes a design paradigm for optimizing exciton dynamics in COF, highlighting the critical role of structural design for artificial H₂O₂ photosynthesis.
- Covalent organic frameworks,
- Donor-π-acceptor,
- Exciton binding energy,
- Photocatalytic H₂O₂ production,
- Water decontamination
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