Citation: Xin Zhou, Yiting Huo, Songyu Yang, Bowen He, Xiaojing Wang, Zhen Wu, Jianjun Zhang. Understanding the effect of pH on protonated COF during photocatalytic H₂O₂ production by femtosecond transient absorption spectroscopy[J]. Acta Physico-Chimica Sinica, ;2025, 41(12): 100160. doi: 10.1016/j.actphy.2025.100160 shu

Understanding the effect of pH on protonated COF during photocatalytic H₂O₂ production by femtosecond transient absorption spectroscopy

Xin Zhou ^{1, 2, 3} ,
Yiting Huo ² ,
Songyu Yang ³ ,
Bowen He ³ ,
Xiaojing Wang ^1,, ,
Zhen Wu ^2,, ,
Jianjun Zhang ^3,,

1.
College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021, Inner Mongolia Autonomous Region, China
2.
Department of Chemical Engineering, Ordos Institute of Technology, Ordos, 017000, Inner Mongolia Autonomous Region, China
3.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Provicne, China

Corresponding author: Xiaojing Wang, wang_xiao_jing@hotmail.com Zhen Wu, wuzhen@oit.edu.cn Jianjun Zhang, zhangjianjun@cug.edu.cn
Received Date: 25 July 2025
Revised Date: 12 August 2025
Accepted Date: 14 August 2025

Fund Project: National Natural Science Foundation of China 52202375National Natural Science Foundation of China 22469001National Natural Science Foundation of China 22409181the Natural Science Foundation of Hubei Province of China 2022CFA001the Natural Science Foundation of Hubei Province of China 2025AFB631Ordos Institute of Technology Research Programs KYQN25Z012Ordos Institute of Technology Research Programs KYYB2023014the Scientific Research Funds at China University of Geosciences (Wuhan) 2025034Natural Science Foundation of Inner Mongolia Autonomous Region of China 2025QN05107Natural Science Foundation of Inner Mongolia Autonomous Region of China 2025ZDLH002

Covalent organic frameworks (COFs), recognized for their precisely tunable microstructures and high surface area, are promising photocatalysts for H₂O₂ production. However, the critical influence of pH on the stability of COF during the photocatalytic H₂O₂ production remains poorly understood. In this work, the photocatalytic H₂O₂ production performance of an imine-linked COF is significantly enhanced through a simple protonation strategy. Crucially, the protonated COF exhibits excellent stability under weakly acidic conditions (pH ≥ 3), but undergoes irreversible hydrolyzed under strongly acidic conditions (pH < 3). The protonation occurs specifically at the nitrogen atoms of imine units and serves a dual function: it suppresses ultrafast charge recombination (as revealed by femtosecond transient absorption spectroscopy) and directly provides a proton source for H₂O₂ generation. Moreover, fluoride ions (F⁻) are introduced into the photocatalytic system to further improve the photocatalytic H₂O₂ production rate. The strong electronegativity of F⁻ facilitates electron transfer from COF to F⁻, thus realizing the spatial separation of photogenerated carriers. Mechanistic studies confirm that H₂O₂ production follows a two-electron oxygen reduction reaction pathway. These findings elucidate the pH-dependent stability and activity of protonated COFs, provide fundamental insights into charge carrier dynamics, and establishe design principles to develop highly efficient and stable COF-based photocatalysts for solar-driven H₂O₂ generation.
- Covalent organic frameworks,
- Structural stability,
- Protonation,
- Fluoride ion surface modification,
- Femtosecond transient absorption spectroscopy
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Understanding the effect of pH on protonated COF during photocatalytic H2O2 production by femtosecond transient absorption spectroscopy

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通讯作者: 陈斌, bchen63@163.com

Understanding the effect of pH on protonated COF during photocatalytic H₂O₂ production by femtosecond transient absorption spectroscopy