N-Rich 2D Heptazine Covalent Organic Frameworks as Efficient Metal-Free Photocatalysts,ACS Catalysis

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N-Rich 2D Heptazine Covalent Organic Frameworks as Efficient Metal-Free Photocatalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-12-22 , DOI: 10.1021/acscatal.1c05233
Dan Chen ₁ , Weiben Chen ₁ , Guang Zhang ₁ , Shen Li ₁ , Weihua Chen ₂ , Guolong Xing ₁ , Long Chen _{1,

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Affiliation

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 C₃-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.

中文翻译：

富氮二维庚嗪共价有机骨架作为高效的无金属光催化剂

庚嗪作为石墨氮化碳 ( g -C ₃ N ₄ )的唯一重复单元，它代表了一种渐进的无金属光催化剂。然而，合成高质量的二维庚嗪基共价有机框架（COFs）仍然是一项艰巨的挑战，这可能是由于缺乏合适且充足的活性庚嗪基构件。在此，我们通过氧化三（4-甲苯基）庚嗪设计并合成了一种 4-（二乙酸亚甲酯）苯基取代的庚嗪单体（HEP-OAc）。因此，通过 HEP-OAc 与两个C ₃直接缩合很容易制备两种高度有序的富氮 COF（HEP-TAPT-COF 和 HEP-TAPB-COF）溶剂热条件下的-对称芳香胺。与原始的g -C ₃ N _{4 相比}，HEP-TAPT-COF 在温和条件下对苄基 C-H 氧化和选择性磺化氧化表现出显着增强的光催化性能。这项工作为开发具有更好光催化能力的高结晶富氮 COF 提供了有意义的见解。

更新日期：2022-01-07

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