Structural and Morphological Engineering of Benzothiadiazole-Based Covalent Organic Frameworks for Visible Light-Driven Oxidative Coupling of Amines,ACS Applied Materials & Interfaces

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Structural and Morphological Engineering of Benzothiadiazole-Based Covalent Organic Frameworks for Visible Light-Driven Oxidative Coupling of Amines
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-08-14 , DOI: 10.1021/acsami.1c08951
Qing Li ₁ , Juan Wang ₁ , Yize Zhang ₁ , Luis Ricardez-Sandoval ₂ , Guoyi Bai ₁ , Xingwang Lan ₁

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Covalent organic frameworks (COFs) are appealing platforms for photocatalysts because of their structural diversity and adjustable optical band gaps. The construction of efficient COFs for heterogeneous photocatalysis of organic transformations is highly desirable. Herein, we constructed a photoactive COF containing benzothiadiazole and triazine (BTDA–TAPT), for which the morphology and crystallinity might be easily tuned by slight synthetic variation. To unveil the relationship of photocatalytic properties between the structure and morphology, analogous COFs were synthesized by precisely tailoring building blocks. Systematic investigations indicated that tuning the structure and morphology might greatly impact photoelectric properties. The BTDA–TAPT featuring ordered alignment and perfect crystalline nature was more beneficial for promoting charge transfer and separation, which exhibited superior photocatalytic activity for visible light-driven oxidative coupling of amines. Outcomes from this study reveal the intrinsic synergy effects between the structure and morphology of COFs for photocatalysis.

中文翻译：

苯并噻二唑基共价有机骨架的结构和形态工程，用于可见光驱动的胺氧化偶联

共价有机骨架（COF）因其结构多样性和可调节的光学带隙而成为光催化剂的有吸引力的平台。非常需要构建用于有机转化的多相光催化的高效 COF。在此，我们构建了一种含有苯并噻二唑和三嗪（BTDA-TAPT）的光活性 COF，其形态和结晶度可以通过轻微的合成变化轻松调整。为了揭示结构和形态之间光催化性能的关系，通过精确定制构建块合成了类似的 COF。系统研究表明，调整结构和形态可能会极大地影响光电性能。具有有序排列和完美结晶性质的 BTDA-TAPT 更有利于促进电荷转移和分离，对可见光驱动的胺氧化偶联表现出优异的光催化活性。该研究的结果揭示了用于光催化的 COF 的结构和形态之间的内在协同效应。

更新日期：2021-08-25

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