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Covalent Organic Frameworks Containing Dual O2 Reduction Centers for Overall Photosynthetic Hydrogen Peroxide Production |
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| Authors: | Dan Chen Weiben Chen Yuting Wu Dr Lei Wang Prof Xiaojun Wu Prof Hangxun Xu Prof Long Chen |
| Institution: | 1. Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Tianjin, 300072 China
These authors contributed equally to this work.;2. Department of Polymer Science and Engineering, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026 China These authors contributed equally to this work.;3. Department of Polymer Science and Engineering, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026 China;4. Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Tianjin, 300072 China |
| Abstract: | Covalent organic frameworks (COFs) are highly desirable for achieving high-efficiency overall photosynthesis of hydrogen peroxide (H2O2) via molecular design. However, precise construction of COFs toward overall photosynthetic H2O2 remains a great challenge. Herein, we report the crystalline s-heptazine-based COFs (HEP-TAPT-COF and HEP-TAPB-COF) with separated redox centers for efficient H2O2 production from O2 and pure water. The spatially and orderly separated active sites in HEP-COFs can efficiently promote charge separation and enhance photocatalytic H2O2 production. Compared with HEP-TAPB-COF, HEP-TAPT-COF exhibits higher H2O2 production efficiency for integrating dual O2 reduction active centers of s-heptazine and triazine moieties. Accordingly, HEP-TAPT-COF bearing dual O2 reduction centers exhibits a remarkable solar-to-chemical energy efficiency of 0.65 % with a high apparent quantum efficiency of 15.35 % at 420 nm, surpassing previously reported COF-based photocatalysts. |
| Keywords: | Catalytic Sites Charge Transfer Covalent Organic Frameworks Hydrogen Peroxide Photocatalysis |