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The Ionic Liquid–H2O Interface: A New Platform for the Synthesis of Highly Crystalline and Molecular Sieving Covalent Organic Framework Membranes
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-07-26 , DOI: 10.1021/acsami.1c08789 Shuaiqi Gao 1 , Zhiyong Li 1 , Yingying Yang 1 , Zhenzhen Wang 1 , Yanlei Wang 2 , Shuangjiang Luo 2 , Kaisheng Yao 3 , Jikuan Qiu 1 , Huiyong Wang 1 , Li Cao 4 , Zhiping Lai 4 , Jianji Wang 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-07-26 , DOI: 10.1021/acsami.1c08789 Shuaiqi Gao 1 , Zhiyong Li 1 , Yingying Yang 1 , Zhenzhen Wang 1 , Yanlei Wang 2 , Shuangjiang Luo 2 , Kaisheng Yao 3 , Jikuan Qiu 1 , Huiyong Wang 1 , Li Cao 4 , Zhiping Lai 4 , Jianji Wang 1
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Covalent organic frameworks (COFs) are highly porous crystalline polymers with uniform pores and large surface areas. Combined with their modular design principle and excellent properties, COFs are an ideal candidate for separation membranes. Liquid–liquid interfacial polymerization is a well-known approach to synthesize membranes by reacting two monomers at the interface. However, volatile organic solvents are usually used, which may disturb the liquid–liquid interface and affect the COF membrane crystallinity due to solvent evaporation. Simultaneously, the domain size of the organic solvent–water interface, named the reaction zone, can hardly be regulated, and the diffusion control of monomers for favorable crystallinity is only achieved in the water phase. These drawbacks may limit the widespread applications of liquid–liquid interfacial polymerization to synthesize diverse COF membranes with different functionalities. Here, we report a facile strategy to synthesize a series of imine-linked freestanding COF membranes with different thicknesses and morphologies at tunable ionic liquid (IL)–H2O interfaces. Due to the H-bonding of the catalysts with amine monomers and the high viscosity of the ILs, the diffusion of the monomers was simultaneously controlled in water and in ILs. This resulted in the exceptionally high crystallinity of freestanding COF membranes with a Brunauer–Emmett–Teller (BET) surface area up to 4.3 times of that synthesized at a dichloromethane–H2O interface. By varying the alkyl chain length of cations in the ILs, the interfacial region size and interfacial tension could be regulated to further improve the crystallinity of the COF membranes. As a result, the as-fabricated COF membranes exhibited ultrahigh permeance toward water and organic solvents and excellent selective rejection of dyes.
中文翻译：
离子液体-H2O 界面：合成高结晶和分子筛共价有机骨架膜的新平台
共价有机骨架 (COF) 是高度多孔的结晶聚合物，具有均匀的孔和大的表面积。结合其模块化设计原理和优异性能，COF 是分离膜的理想选择。液-液界面聚合是一种众所周知的通过使两种单体在界面上反应来合成膜的方法。然而，通常使用挥发性有机溶剂，这可能会由于溶剂蒸发而扰乱液-液界面并影响 COF 膜的结晶度。同时，有机溶剂-水界面的域尺寸（称为反应区）难以调节，单体的扩散控制仅在水相中实现。这些缺点可能会限制液-液界面聚合在合成具有不同功能的多种 COF 膜方面的广泛应用。在这里，我们报告了一种在可调离子液体 (IL)-H 下合成一系列具有不同厚度和形态的亚胺连接的独立 COF 膜的简便策略2 O 接口。由于催化剂与胺单体的 H 键合和离子液体的高粘度，单体在水中和离子液体中的扩散同时受到控制。这导致独立式 COF 膜具有极高的结晶度，其布鲁瑙尔-埃米特-特勒 (BET) 表面积高达在二氯甲烷-H 2 O 界面合成的 4.3 倍。通过改变离子液体中阳离子的烷基链长度，可以调节界面区域的大小和界面张力，以进一步提高 COF 膜的结晶度。因此，制造的 COF 膜对水和有机溶剂表现出超高的渗透性和优异的染料选择性排斥。
更新日期：2021-08-04
中文翻译：
离子液体-H2O 界面：合成高结晶和分子筛共价有机骨架膜的新平台
共价有机骨架 (COF) 是高度多孔的结晶聚合物，具有均匀的孔和大的表面积。结合其模块化设计原理和优异性能，COF 是分离膜的理想选择。液-液界面聚合是一种众所周知的通过使两种单体在界面上反应来合成膜的方法。然而，通常使用挥发性有机溶剂，这可能会由于溶剂蒸发而扰乱液-液界面并影响 COF 膜的结晶度。同时，有机溶剂-水界面的域尺寸（称为反应区）难以调节，单体的扩散控制仅在水相中实现。这些缺点可能会限制液-液界面聚合在合成具有不同功能的多种 COF 膜方面的广泛应用。在这里，我们报告了一种在可调离子液体 (IL)-H 下合成一系列具有不同厚度和形态的亚胺连接的独立 COF 膜的简便策略2 O 接口。由于催化剂与胺单体的 H 键合和离子液体的高粘度，单体在水中和离子液体中的扩散同时受到控制。这导致独立式 COF 膜具有极高的结晶度，其布鲁瑙尔-埃米特-特勒 (BET) 表面积高达在二氯甲烷-H 2 O 界面合成的 4.3 倍。通过改变离子液体中阳离子的烷基链长度，可以调节界面区域的大小和界面张力，以进一步提高 COF 膜的结晶度。因此，制造的 COF 膜对水和有机溶剂表现出超高的渗透性和优异的染料选择性排斥。
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