Regulating interfacial hydrophilicity in vinylene-linked covalent organic frameworks for efficient photocatalytic H2O2 production in water and air
Abstract
Photocatalytic hydrogen peroxide (H2O2) production offers a sustainable strategy for solar-to-chemical energy conversion and environmental remediation. However, the intrinsic role of interfacial hydrophilicity in aqueous photocatalysis remains rarely studied, largely due to the lack of a well-defined model system. Covalent organic frameworks (COFs), with their chemically tunable structure, provide an ideal platform to address this gap. Herein, we employ two vinylene-linked COFs with similar conjugated backbones but distinct interfacial hydrophilicity, namely TMT-TPA COF and TMT-BPA COF. The higher nitrogen atom density in TMT-TPA COF endows it with significantly enhanced surface hydrophilicity (contact angle: 49°), compared to TMT-BPA COF (contact angle: 101°). The enhanced hydrophilicity is associated with a more favorable interfacial microenvironment, which facilitates water adsorption and interfacial charge transfer. Consequently, even in a pure water-air system under visible-light irradiation, the more hydrophilic TMT-TPA COF achieves a H2O2 production rate of 3.69 mmol g−1 h−1 with good stability, approximately 2.49 times higher than that of TMT-BPA COF. Mechanistic studies reveal that TMT-TPA COF catalytic H2O2 generation predominantly involves a stepwise single-electron oxygen reduction pathway comprising a ·O2− intermediate, while photogenerated holes are consumed through water oxidation. This work highlights interfacial hydrophilicity as a critical enabler for designing high-performance photocatalysts.
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BibTeX
@article{li2026regulating,
title = {{Regulating interfacial hydrophilicity in vinylene-linked covalent organic frameworks for efficient photocatalytic H2O2 production in water and air}},
author = {Shun-Feng Li and Ya Lu and Mei-Mei Zhang and Xing Su and Fan Qiu and Peng-Ju Tian and Yubin Fu and Paolo Samorì and Shun-Qi Xu},
journal = {RSC Applied Interfaces},
year = {2026},
month = jul,
doi = {10.1039/d6lf00168h},
url = {https://univoak.hal.science/hal-05751558v1},
note = {CC BY-NC 4.0},
}
RIS
TY - JOUR
TI - Regulating interfacial hydrophilicity in vinylene-linked covalent organic frameworks for efficient photocatalytic H2O2 production in water and air
AU - Shun-Feng Li
AU - Ya Lu
AU - Mei-Mei Zhang
AU - Xing Su
AU - Fan Qiu
AU - Peng-Ju Tian
AU - Yubin Fu
AU - Paolo Samorì
AU - Shun-Qi Xu
PY - 2026
DA - 2026/07/10
JO - RSC Applied Interfaces
DO - 10.1039/d6lf00168h
UR - https://univoak.hal.science/hal-05751558v1
AB - Photocatalytic hydrogen peroxide (H2O2) production offers a sustainable strategy for solar-to-chemical energy conversion and environmental remediation. However, the intrinsic role of interfacial hydrophilicity in aqueous photocatalysis remains rarely studied, largely due to the lack of a well-defined model system. Covalent organic frameworks (COFs), with their chemically tunable structure, provide an ideal platform to address this gap. Herein, we employ two vinylene-linked COFs with similar conjugated backbones but distinct interfacial hydrophilicity, namely TMT-TPA COF and TMT-BPA COF. The higher nitrogen atom density in TMT-TPA COF endows it with significantly enhanced surface hydrophilicity (contact angle: 49°), compared to TMT-BPA COF (contact angle: 101°). The enhanced hydrophilicity is associated with a more favorable interfacial microenvironment, which facilitates water adsorption and interfacial charge transfer. Consequently, even in a pure water-air system under visible-light irradiation, the more hydrophilic TMT-TPA COF achieves a H2O2 production rate of 3.69 mmol g−1 h−1 with good stability, approximately 2.49 times higher than that of TMT-BPA COF. Mechanistic studies reveal that TMT-TPA COF catalytic H2O2 generation predominantly involves a stepwise single-electron oxygen reduction pathway comprising a ·O2− intermediate, while photogenerated holes are consumed through water oxidation. This work highlights interfacial hydrophilicity as a critical enabler for designing high-performance photocatalysts.
SN - 2755-3701
ER -