4.8 Article

Oxidation-Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H2O2

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202218868

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Covalent Organic Framework; Full Reaction; H2O2; Oxidation-Reduction Molecular Junction; Photocatalysis

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A covalent organic framework (TTF-BT-COF) with oxidation-reduction molecular junction has been synthesized through the covalent-coupling of tetrathiafulvalene and benzothiazole. This framework has visible-light absorption region, effective electron-hole separation efficiency, and photo-redox sites, enabling full reaction generation of H2O2.
The full reaction photosynthesis of H2O2 that can combine water-oxidation and oxygen-reduction without sacrificial agents is highly demanded to maximize the light-utilization and overcome the complex reaction-process of anthraquinone-oxidation. Here, a kind of oxidation-reduction molecular junction covalent-organic-framework (TTF-BT-COF) has been synthesized through the covalent-coupling of tetrathiafulvalene (photo-oxidation site) and benzothiazole (photo-reduction site), which presents visible-light-adsorption region, effective electron-hole separation-efficiency and photo-redox sites that enables full reaction generation of H2O2. Specifically, a record-high yield (TTF-BT-COF, approximate to 276 000 mu M h(-1) g(-1)) for H2O2 photosynthesis without sacrificial agents has been achieved among porous crystalline photocatalysts. This is the first work that can design oxidation-reduction molecular junction COFs for full reaction photosynthesis of H2O2, which might extend the scope of COFs in H2O2 production.

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