期刊
ACS CATALYSIS
卷 12, 期 1, 页码 616-623出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05233
关键词
covalent organic frameworks; heptazine; metal-free photocatalysts; oxygenation; carbon nitride
资金
- National Natural Science Foundation of China [51973153]
- National Key Research and Development Program of China [2017YFA0207500]
This study successfully synthesized two highly ordered N-rich COFs by designing a novel heptazine monomer and condensing it with aromatic amines, one of which showed significantly enhanced photocatalytic performance under mild conditions compared to the pristine photocatalyst.
Heptazine serves as the solely repetitive unit of graphitic carbon nitride (g-C3N4), which represents a progressive metal-free photocatalyst. However, synthesizing high-quality 2D heptazine-based covalent organic frameworks (COFs) remains a formidable challenge, probably due to the scarcity of suitable and ample reactive heptazine-based building blocks. Herein, we designed and synthesized a 4-(methylene diacetate)phenyl-substituted heptazine monomer (HEP-OAc) by oxidation of tris(4-tolyl)heptazine. Accordingly, two highly ordered N-rich COFs (HEP-TAPT-COF and HEP-TAPB-COF) were readily prepared by the direct condensation of HEP-OAc with two C-3-symmetric aromatic amines under solvothermal conditions. In comparison to the pristine g-C3N4, HEP-TAPT-COF exhibited greatly enhanced photocatalytic performance for benzylic C-H oxidation and selective sulfoxidation under mild conditions. This work provides meaningful insights into developing highly crystalline N-rich COFs with better photocatalytic capacities.
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