Keto-enol tautomerism as dynamic electron/hole traps promote charge carrier separation for hydrogen peroxide photosynthesis

Covalent organic frameworks (COFs) are promising photocatalysts for H<sub>2</sub>O<sub>2</sub> photosynthesis, but charge carrier separation remains a critical challenge. Donor-acceptor COFs enhance charge separation, but the slow kinetics of water oxidation and oxygen reduction reactions lead to carrier accumulation, thereby decreasing efficiency. Here, we report T-C type COFs (T = trap units, C = catalytic units), demonstrating that units with keto-enol tautomerism can serve as dynamic electron/hole traps (T) to mitigate Coulomb forces. This design effectively facilitates swift charge transfer and extends carrier lifetimes, thereby enhancing reactions at the C units. Imine COFs derived from 2,4,6-trihydroxybenzaldehyde (Tp) outperform those based on 1,3,5-benzenetricarboxaldehyde due to tautomerization. The optimal Tp COF (TpBpy) achieves an H<sub>2</sub>O<sub>2</sub> generation rate of 37.9 μmol h⁻¹ (or 8350 μmol h⁻¹ g⁻¹) under simulated light, and a solar-to-chemical conversion efficiency of 0.038% in a flow reactor under natural sunlight. This work provides molecular design strategies and standard criteria for efficient H<sub>2</sub>O<sub>2</sub> photocatalysts.

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Publication Details

Journal
Nature Communications
Published
2025-08-12
DOI
https://doi.org/10.1038/s41467-025-62286-9
Citations
13
Primary Topic
Covalent Organic Framework Applications
Type
article
Field-Weighted Citation Impact
6.73

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article

Keto-enol tautomerism as dynamic electron/hole traps promote charge carrier separation for hydrogen peroxide photosynthesis

Tao Gao, Yongye Wang, Anqiang Jiang, Xin Ying Kong et al.
13 citations
Nature Communications
Covalent Organic Framework Applications
6.73
article

Keto-enol tautomerism as dynamic electron/hole traps promote charge carrier separation for hydrogen peroxide photosynthesis

Tao Gao, Yongye Wang, Anqiang Jiang, Xin Ying Kong, Liqun Ye, Yingping Huang, Hongwei Huang, Chunqiu Han, Xiaodong Sun, Tianyi Ma, Ying Zhou, Guijie Liang, Niu Huang, Li Wang, Hui Li, Fang Ma, Huiqing Wang, Binbin Jia
article en
13 citations

Abstract

Covalent organic frameworks (COFs) are promising photocatalysts for H<sub>2</sub>O<sub>2</sub> photosynthesis, but charge carrier separation remains a critical challenge. Donor-acceptor COFs enhance charge separation, but the slow kinetics of water oxidation and oxygen reduction reactions lead to carrier accumulation, thereby decreasing efficiency. Here, we report T-C type COFs (T = trap units, C = catalytic units), demonstrating that units with keto-enol tautomerism can serve as dynamic electron/hole traps (T) to mitigate Coulomb forces. This design effectively facilitates swift charge transfer and extends carrier lifetimes, thereby enhancing reactions at the C units. Imine COFs derived from 2,4,6-trihydroxybenzaldehyde (Tp) outperform those based on 1,3,5-benzenetricarboxaldehyde due to tautomerization. The optimal Tp COF (TpBpy) achieves an H<sub>2</sub>O<sub>2</sub> generation rate of 37.9 μmol h⁻¹ (or 8350 μmol h⁻¹ g⁻¹) under simulated light, and a solar-to-chemical conversion efficiency of 0.038% in a flow reactor under natural sunlight. This work provides molecular design strategies and standard criteria for efficient H<sub>2</sub>O<sub>2</sub> photocatalysts.

Nature CommunicationsVol. 16(1)
Liaoning University (CN), China Three Gorges University (CN), Southwest Petroleum University (CN), Nanyang Technological University (SG), China University of Geosciences (Beijing) (CN), MIT University (MK), State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation (CN), ARC Centre of Excellence in Future Low-Energy Electronics Technologies (AU), Nanomaterials Research (United States) (US), Hubei University of Arts and Science (CN), RMIT University (AU)
Australian Government, European Commission, National Natural Science Foundation of China, Cooperative Research Centres, Australian Government Department of Industry, Natural Science Foundation of Hubei Province, Higher Education Discipline Innovation Project
Clean water and sanitation
Openalex Percentile: Top 2%
Covalent Organic Framework Applications
6.73
DOIOpen Access PDFOpenAlex
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