期刊
NATURE CHEMISTRY
卷 10, 期 12, 页码 1180-1189出版社
NATURE PORTFOLIO
DOI: 10.1038/s41557-018-0141-5
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资金
- Engineering and Physical Sciences Research Council (EPSRC) [EP/N004884/1]
- European Union [321156, 692685]
- Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design
- China Scholarship Council
- NSFC [21421004]
- NSFC/China [21636002]
- Shanghai Oriental Scholarship
- ARCHER UK National Supercomputing Service [EP/N004884/1]
- EPSRC [EP/L000202/1, EP/K000225/1]
- N8 Research Partnership
- EPSRC [EP/N004884/1] Funding Source: UKRI
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 benzobis(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 fusedsulfone-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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