Chemically stable polyarylether-based covalent organic frameworks
Chemically stable polyarylether-based covalent organic frameworks
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化学稳定的聚芳醚基共价有机骨架
DOI：
10.1038/s41557-019-0238-5
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发表时间：
2019-06-01
期刊：
影响因子：
21.8
通讯作者：
Qiu, Shilun
中科院分区：
文献类型：
--
作者：
Guan, Xinyu;Li, Hui;Qiu, Shilun
开发具有高化学稳定性的结晶多孔材料对其实际应用至关重要。在这里，我们报告了基于聚芳醚的共价有机框架（PAE-COFs）的合成，具有高结晶度，孔隙率和化学稳定性，包括对水的化学稳定性，由于其基于聚芳醚的结构单元的惰性。PAE-COFs是通过邻二氟苯和邻苯二酚结构单元之间的亲核芳族取代反应合成的，所述邻二氟苯和邻苯二酚结构单元形成醚键。所得到的材料显示出对苛刻的化学环境（包括沸水、强酸和强碱以及氧化和还原条件）是稳定的。它们的稳定性超过了其他已知的结晶多孔材料如沸石、金属有机骨架和共价有机骨架的性能。我们还证明了这些材料与羧基或氨基官能团的合成后官能化。官能化的PAE-COF结合了联合收割机多孔性、高稳定性和可回收性。这些材料的初步应用证明了在很宽的pH范围内从水中去除抗生素。
The development of crystalline porous materials with high chemical stability is of paramount importance for their practical application. Here, we report the synthesis of polyarylether-based covalent organic frameworks (PAE-COFs) with high crystallinity, porosity and chemical stability, including towards water, owing to the inert nature of their polyarylether-based building blocks. The PAE-COFs are synthesized through nucleophilic aromatic substitution reactions between ortho-difluoro benzene and catechol building units, which form ether linkages. The resulting materials are shown to be stable against harsh chemical environments including boiling water, strong acids and bases, and oxidation and reduction conditions. Their stability surpasses the performance of other known crystalline porous materials such as zeolites, metal-organic frameworks and covalent organic frameworks. We also demonstrate the post-synthetic functionalization of these materials with carboxyl or amino functional groups. The functionalized PAE-COFs combine porosity, high stability and recyclability. A preliminary application of these materials is demonstrated with the removal of antibiotics from water over a wide pH range.