高亲水性共价有机骨架作为有效且可重复使用的光催化剂用于水溶液中胺的氧化偶联,Catalysis Science & Technology

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高亲水性共价有机骨架作为有效且可重复使用的光催化剂用于水溶液中胺的氧化偶联
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2022-03-12 , DOI: 10.1039/d2cy00167e
Shufang Liu ₁ , Qing Su ₁ , Wei Qi ₁ , Kexin Luo ₁ , Xiaoman Sun ₁ , Hao Ren ₂ , Qiaolin Wu ₁

Affiliation

作为一类新兴的结晶多孔材料，光活性共价有机框架（COFs）在光催化无金属有机转化方面表现出巨大潜力。在这项研究中，我们报告了三种亲水性二维 (2D) COF，它们是通过 2,5-二甲氧基对苯二甲酰肼 ( DMTH )、1,3,5-三甲酰苯 ( TFB ) 和 2-羟基-1,3,5的缩聚反应实现的-苯三甲醛 ( SOH ) 在溶剂热条件下。所得到的 COF 材料TFB-XX-DMTH（XX = 33、50 和 66，对应于TFB/SOH = 1:2、1:1 和 2:1 的摩尔比）由三原位组件组装策略，因此表现出高结晶度、大表面积（高达 1808 m ² g ^-1）以及良好的热稳定性和化学稳定性。此外，得益于增强的电荷分离效率和高亲水性，TFB-XX-DMTH材料可用作可见光驱动的苄胺在水溶液中的氧化偶联反应的光催化剂。具有高转化率、选择性和可回收性的光催化性能可归因于该平台中光生载流子的高效生成、迁移和分离的综合结果。我们的结果提供了对 COF 光催化剂的结构-功能相关性的见解，并强调了它们在开发用于可持续有机转化的光功能 COF 方面的潜力。

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Highly hydrophilic covalent organic frameworks as efficient and reusable photocatalysts for oxidative coupling of amines in aqueous solution

As a class of new emerging crystalline porous materials, photoactive covalent organic frameworks (COFs) have exhibited great potential for photocatalytic applications for metal-free organic transformations. In this study, we report three hydrophilic two-dimensional (2D) COFs achieved by a polycondensation reaction of 2,5-dimethoxyterephthalohydrazide (DMTH), 1,3,5-triformylbenzene (TFB) and 2-hydroxy-1,3,5-benzenetricarbaldehyde (SOH) under solvothermal conditions. The resulted COF materials, TFB-XX-DMTH (XX = 33, 50 and 66, corresponding to a molar ratio of TFB/SOH = 1 : 2, 1 : 1, and 2 : 1), are successfully constructed by a three-component in situ assembly strategy and thus exhibit high crystallinity, large surface areas (up to 1808 m² g⁻¹) and good thermal and chemical stability. Moreover, benefiting from the enhanced charge separation efficiency and high hydrophilicity, the TFB-XX-DMTH materials could be employed as photocatalysts for visible-light-driven oxidative coupling reactions of benzylamines in aqueous solution. The photocatalytic performance with high conversion, selectivity and recyclability could be attributed to a combined result of efficient generation, migration and separation of photogenerated carriers in such a platform. Our results provide insights into the structure–function correlation of COF photocatalysts and also highlight their potential in developing photofunctional COFs for sustainable organic transformations.

更新日期：2022-03-12

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