Sulfone-containing covalent organic frameworks for photocatalytic hydrogen evolution from water
Open accessAbstract
Nature uses organic molecules for light harvesting and photosynthesis, but most man-made water splitting catalysts are inorganic semiconductors. Organic photocatalysts, while attractive because of their synthetic tunability, tend to have low quantum efficiencies for water splitting. Here we present a crystalline covalent organic framework (COF) based on a benzo-bis(benzothiophene sulfone) moiety that shows a much higher activity for photochemical hydrogen evolution than its amorphous or semicrystalline counterparts. The COF is stable under long-term visible irradiation and shows steady photochemical hydrogen evolution with a sacrificial electron donor for at least 50 hours. We attribute the high quantum efficiency of fused-sulfone-COF to its crystallinity, its strong visible light absorption, and its wettable, hydrophilic 3.2 nm mesopores. These pores allow the framework to be dye-sensitized, leading to a further 61% enhancement in the hydrogen evolution rate up to 16.3 mmol g-1 h-1. The COF also retained its photocatalytic activity when cast as a thin film onto a support.
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The photocatalytic aerogel achieved a hydrogen generation rate of 60.7 mmol m−2 h−1, significantly outperforming conventional thin-film photocatalytic platforms.
“As a result, the photocatalytic aerogels achieved a high hydrogen generation rate of 60.7 mmol m 2 h 1 , significantly outperforming the conventional thin-film photocatalytic platforms.”
From Gradient-structured directional porous floatable aerogels for effective solar-driven hydrogen production and steam generation (2025) · cites this paper as [60]
The section “Photocatalysis experiments with thin COF films” (page unavailable) reports thin-film hydrogen evolution rates of 24.9 and 15.8 mmol m−2 h−1, providing a comparison point below 60.7. It does not report a photocatalytic aerogel, its claimed 60.7 rate, or a direct comparison establishing that it significantly outperformed thin films. (LLM, conf=0.87)
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References 80 · Cited by 1,320
Research works printed but not linked: 12
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- Authors
- Wang, X., Chen, L., Chong, S. Y., Little, M. A., Wu, Y., Zhu, W.-H., Clowes, R., Yan, Y., Zwijnenburg, M. A., Sprick, R. S., & Cooper, A. I.
- Affiliations
- University of Liverpool (GB)
- East China University of Science and Technology (CN)
- University College London (GB)
- Corresponding author
- Cooper, Andrew I.
- ORCID
- Venue
- Nature Chemistry
- Published
- 2018-10-01
- Volume
- 10
- Issue
- 12
- Pages
- 1180-1189
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- OpenAlex
- W2893441209
- Cited by
- 1,320
- References
- 80
- Citations by year
- 2026: 77 · 2025: 178 · 2024: 222 · 2023: 185 · 2022: 193 · 2021: 189 · 2020: 169 · 2019: 104 · 2018: 3
- FWCI
- 43.43
- Type
- journal article
- Language
- en
- Open access
- Licence
- www.springer.com/tdm (tdm)
- Locations
- Nature Chemistry (publishedVersion)
- PubMed (publishedVersion)
- Strathprints: The University of Strathclyde institutional repository (University of Strathclyde) (acceptedVersion)
- UCL Discovery (University College London) (submittedVersion)
- Funders
- Leverhulme Trust
- European Commission
- China Scholarship Council
- Engineering and Physical Sciences Research Council (EP/L000202/1, EP/N004884/1, EP/K000225/1)
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Covalent Organic Framework Applications
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › TiO2 Photocatalysis and Solar Cells
- Keywords
- covalent organic frameworks, photocatalytic hydrogen evolution, water splitting, crystallinity, visible light absorption, mesopores, dye-sensitized photocatalysis, thin film photocatalyst, sacrificial electron donor, quantum efficiency
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