Modulating electronic structure of triazine-based covalent organic frameworks for photocatalytic organic transformations,Journal of Materials Chemistry A

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Modulating electronic structure of triazine-based covalent organic frameworks for photocatalytic organic transformations
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-08-01 , DOI: 10.1039/d2ta04541a
Zhangjie Gu ₁ , Jinjian Wang ₁ , Zhen Shan ₁ , Miaomiao Wu ₁ , Tongtong Liu ₁ , Liang Song ₁ , Guixiang Wang ₁ , Xuehai Ju ₁ , Jian Su ₁ , Gen Zhang ₁

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By virtue of visible light absorption ability, the energy band structure and electronic affinity of covalent organic frameworks (COFs) can be easily tuned at the molecular level, making them attractive photocatalysts for metal-free organic transformation. However, the relationship between the electronic structure and photocatalytic properties of COFs is still vague. In this study, we developed a bottom-up strategy to construct three triazine-based COFs with different electronic structures through introducing various building blocks. The photocatalytic oxidation of sulfides to sulfoxides showed that electron-deficient COF afforded higher conversion and selectivity than that of electron-rich or neutral structures, which due to the electron-deficient triazine-based COF can not only facilitate the generation and separation of charge, but also enrich the photocatalytic active sites. This result was further confirmed by photoelectrochemical measurements and theoretical calculations. This work lights up the design and application of high-efficient metal-free photocatalysts by modulation of electronic structures.

中文翻译：

调节基于三嗪的共价有机框架的电子结构用于光催化有机转化

凭借可见光吸收能力，共价有机框架（COFs）的能带结构和电子亲和力可以在分子水平上轻松调节，使其成为有吸引力的无金属有机转化光催化剂。然而，COFs的电子结构与光催化性能之间的关系仍然模糊不清。在这项研究中，我们开发了一种自下而上的策略，通过引入各种构建块来构建三种具有不同电子结构的三嗪基 COF。硫化物光催化氧化为亚砜表明，缺电子COF比富电子或中性结构具有更高的转化率和选择性，由于缺电子三嗪基COF不仅可以促进电荷的产生和分离，同时也丰富了光催化活性位点。光电化学测量和理论计算进一步证实了这一结果。这项工作通过调制电子结构照亮了高效无金属光催化剂的设计和应用。

更新日期：2022-08-01

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