Catalyst regulated interfacial synthesis of self-standing covalent organic framework membranes at room temperature for molecular separation.
Catalyst regulated interfacial synthesis of self-standing covalent organic framework membranes at room temperature for molecular separation.
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DOI：
10.1016/j.jcis.2022.09.036
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发表时间：
2022-09
影响因子：
9.9
通讯作者：
Jia He;Lingzhu Yu;Zhiyu Li;Shengdong Ba;Fang Lan;Yao Wu
中科院分区：
文献类型：
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作者：
Jia He;Lingzhu Yu;Zhiyu Li;Shengdong Ba;Fang Lan;Yao Wu
共价有机骨架（COF）膜由于其大的表面积和可预先设计的结构而显示出巨大的分子分离潜力。然而，具有高结晶度的COF膜的温和和方便的制备仍然是一个重大的挑战。在这项工作中，我们报道了一种简单的液-液界面聚合方法，以制备自支撑的亚胺基COF膜具有优异的结晶度和可调的厚度在室温下。当二氯甲烷中的单体与催化剂水溶液相遇时，聚合被限制在不互溶的有机溶剂-水界面。这种独特的设计理念利用了COF在液-液界面处的快速形成来控制催化剂扩散和结构重排，从而实现了COF膜的高结晶度。此外，通过对生长过程的灵活调控，自支撑COF膜的厚度可以在50 nm ~ 1 μm范围内任意调节。得益于COF膜的大比表面积（378 m2/g）以及COF与有机染料之间强烈的π-π共轭效应，所得COF膜对Chrome Black T和Rose Bengal表现出较高的吸附能力。这一工作可能开辟一条可行的途径，以方便和温和地制备COF膜用于水处理。
Covalent organic framework (COF) membranes have shown enormous potential for molecular separation due to their large surface areas and pre-designable structures. However, the mild and convenient preparation of COF membranes with high crystallinity has remained a significant challenge. In this work, we reported on a facile liquid–liquid interfacial polymerization method to fabricate self-standing imine-based COF membranes with excellent crystallinity and a tunable thickness at room temperature. Polymerization was confined at the immiscible organic solvent–water interface when the monomers in the dichloromethane met the catalyst aqueous solution. This unique design concept exploited the rapid formation of COF monolayers at the liquid–liquid interface to control catalyst diffusion and structural rearrangement, achieving high crystallinity of the COF membrane. Moreover, the thickness of the self-standing COF membranes could be regulated from 50 nm to 1 μm through the flexible regulation of the growth process. Benefiting from the large surface area of the COF membranes (378 m2/g) and the intensive π–π conjugate effect between the COFs and organic dyes, the obtained COF membranes exhibited high adsorption capacities toward Chrome Black T and Rose Bengal. This work may open a viable avenue to easily and mildly prepare COF membranes for water treatment.