Pyrene-Based Covalent Organic Frameworks for Photocatalytic Hydrogen Peroxide Production

被引:192
作者
Sun, Jiamin [1 ]
Jena, Himanshu Sekhar [1 ]
Krishnaraj, Chidharth [1 ]
Rawat, Kuber Singh [2 ]
Abednatanzi, Sara [1 ]
Chakraborty, Jeet [1 ]
Laemont, Andreas [1 ]
Liu, Wanlu [1 ]
Chen, Hui [1 ]
Liu, Ying-Ya [3 ]
Leus, Karen [1 ]
Vrielinck, Henk [4 ]
Van Speybroeck, Veronique [2 ]
Van Der Voort, Pascal [1 ]
机构
[1] Univ Ghent, Ctr Ordered Mat, Dept Chem, COMOC, Krijgslaan 281, Bldg S3, B-9000 Ghent, Belgium
[2] Univ Ghent, Ctr Mol Modeling CMM, Technologiepark 46, B-9052 Zwijnaarde, Belgium
[3] Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116023, Peoples R China
[4] Univ Ghent, Dept Solid State Sci, Krijgslaan 281, Bldg S1, B-9000 Ghent, Belgium
关键词
Covalent Organic Frameworks; Hydrogen Peroxide Generation; Oxygen Reduction; Photocatalysis; Pyrene; H2O2; PRODUCTION; CARBON;
D O I
10.1002/anie.202216719
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Four highly porous covalent organic frameworks (COFs) containing pyrene units were prepared and explored for photocatalytic H2O2 production. The experimental studies are complemented by density functional theory calculations, proving that the pyrene unit is more active for H2O2 production than the bipyridine and (diarylamino)benzene units reported previously. H2O2 decomposition experiments verified that the distribution of pyrene units over a large surface area of COFs plays an important role in catalytic performance. The Py-Py-COF though contains more pyrene units than other COFs which induces a high H2O2 decomposition due to a dense concentration of pyrene in close proximity over a limited surface area. Therefore, a two-phase reaction system (water-benzyl alcohol) was employed to inhibit H2O2 decomposition. This is the first report on applying pyrene-based COFs in a two-phase system for photocatalytic H2O2 generation.
引用
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页数:9
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