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首页> 外文期刊>ACS applied materials & interfaces >Structural Engineering of Two-Dimensional Covalent Organic Frameworks for Visible-Light-Driven Organic Transformations
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Structural Engineering of Two-Dimensional Covalent Organic Frameworks for Visible-Light-Driven Organic Transformations

机译：可见光有机转化二维共价有机框架的结构工程

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摘要

Covalent organic frameworks (COFs) emerging as a novel kind of visible light-responsive organic semiconductor have attracted extensive research attention in the field of photocatalytic organic transformations. However, the key parameters affecting their photocatalytic properties are still not clear. In this work, a series of [3 + 3] COFs with similar two-dimensional hexagonal structure but different compositions are synthesized and employed as model materials for investigating the key factors affecting the photocatalytic properties in the visible-light-driven reductive dehalogenation reaction and the aerobic cross-dehydrogenative coupling reaction. In comparison with -H and -CF3, the -OH substituent in the aromatic ring could narrow the band gap of the COFs. The COFs with a triazine skeleton in the framework usually boost the photocatalytic activity, possibly because of the enhanced charge separation efficiency by the formation of a donor-acceptor domain. As a combined result of the narrow band gap, efficient charge separation, and high conductivity, the COF possessing both a -OH group and triazine skeleton shows the highest activity in the photocatalytic reductive dehalogenation reaction. Notably, COFs could be easily recovered and reused several times without the loss of crystallinity. Our primary results may shed light on the design of efficient COF-based semiconductors for photocatalytic organic transformations.
机译：作为一种新颖的可见光响应有机半导体的共价有机框架（COF）在光催化有机转化领域吸引了广泛的研究。然而，影响其光催化性能的关键参数仍然尚不清楚。在这项工作中，合成了一系列具有相似二维六方结构但不同组成的[3 + 3] COFs，并采用作为模型材料，用于研究影响可见光的还原脱氢反应中的光催化性能的关键因素有氧交叉脱氢偶联反应。与-H和-CF 3相比，芳环中的-OH取代基可以缩小COF的带隙。在框架中具有三嗪骨架的COF通常可以提高光催化活性，可能是因为通过形成供体 - 受体结构域提高电荷分离效率。作为窄带隙，有效电荷分离和高导电性的组合结果，具有-OH基团和三嗪骨架的COF显示了光催化还原脱离反应中的最高活性。值得注意的是，在没有结晶度的情况下，COF可以很容易地恢复并重复使用几次。我们的主要结果可能会阐明光催化有机转化的高效COF基半导体的设计。

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