Covalent Organic Frameworks Containing Dual O2 Reduction Centers for Overall Photosynthetic Hydrogen Peroxide Production

被引:217
作者
Chen, Dan [1 ]
Chen, Weiben [1 ]
Wu, Yuting [2 ]
Wang, Lei [2 ]
Wu, Xiaojun [2 ]
Xu, Hangxun [2 ]
Chen, Long [1 ,3 ]
机构
[1] Tianjin Univ, Dept Chem, Tianjin Key Lab Mol Optoelect Sci, Tianjin 300072, Peoples R China
[2] Univ Sci & Technol China, Dept Polymer Sci & Engn, Dept Mat Sci & Engn, Hefei 230026, Peoples R China
[3] Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
Catalytic Sites; Charge Transfer; Covalent Organic Frameworks; Hydrogen Peroxide; Photocatalysis; H2O2; PHOTOCATALYSTS; PERSPECTIVE; POLYMERS;
D O I
10.1002/anie.202217479
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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 O-2 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 O-2 reduction active centers of s-heptazine and triazine moieties. Accordingly, HEP-TAPT-COF bearing dual O-2 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.
引用
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页数:9
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