Potential Difference-Modulated Synthesis of Self-Standing Covalent Organic Framework Membranes at Liquid/Liquid Interfaces,Journal of the American Chemical Society

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Potential Difference-Modulated Synthesis of Self-Standing Covalent Organic Framework Membranes at Liquid/Liquid Interfaces
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-06-22 , DOI: 10.1021/jacs.2c03864
Rongjie Yang ₁ , Shanshan Liu ₁ , Qi Sun ₂ , Qiaobo Liao ₃ , Kai Xi ₃ , Bin Su ₁

Affiliation

Covalent organic framework (COF) membranes with tailored functionalities hold great promise in diverse applications, but the key to realize their full advantages of highly ordered pore structures is the development of membrane fabrication approaches. In this work, we report a potential difference-modulated biphasic strategy to fabricate large-area, self-standing COF membranes under ambient conditions. The fabrication was conducted at the polarized water/1,2-dichloroethane (water/DCE) interface, where HCl was dissolved in water as a catalyst and monomers (both amine and aldehyde) were added to DCE. The external polarization of the water/DCE interface by cyclic voltammetry can continuously pump H⁺ from water to DCE to boost the Schiff base reaction of monomers and the growth of COF membranes. Moreover, the growth process can be real-time-monitored by interfacial double-layer capacitance measurement, and the permeability of COF membranes can be in situ-examined by heterogeneous ion transfer voltammetry. Given that the potential difference across the water/DCE interface can be also facilely modulated by dissolving proper electrolyte ions in two phases, the fabrication of large-area COF membranes is made possible in beakers. Using this strategy and different monomers, three types of centimeter-scale, free-standing COF membranes with tunable pore size and surface functionality were prepared, and their defect-free structure was proved by the molecular permeance and ultrafiltration test. We believe that this biphasic strategy offers a controllable and scalable way to fabricate COF membranes and sheds light on development of novel self-supporting membranes with unique functions.

中文翻译：

液/液界面处自立共价有机骨架膜的电位差调制合成

具有定制功能的共价有机框架 (COF) 膜在各种应用中具有广阔的前景，但实现其高度有序孔结构的全部优势的关键是膜制造方法的发展。在这项工作中，我们报告了一种电位差调制的双相策略，用于在环境条件下制造大面积、自立式 COF 膜。该制造是在极化水/1,2-二氯乙烷（水/DCE）界面进行的，其中将 HCl 作为催化剂溶解在水中，并将单体（胺和醛）添加到 DCE 中。循环伏安法对水/DCE界面的外部极化可以连续泵送H ⁺从水到 DCE 以促进单体的席夫碱反应和 COF 膜的生长。此外，通过界面双层电容测量可以实时监测生长过程，通过异相离子转移伏安法可以原位检测COF膜的渗透性。鉴于水/DCE界面上的电位差也可以通过将适当的电解质离子溶解在两相中来轻松调节，因此在烧杯中制造大面积COF膜成为可能。采用该策略和不同的单体，制备了三种具有可调孔径和表面功能的厘米级自支撑COF膜，并通过分子渗透和超滤测试证明了它们的无缺陷结构。

更新日期：2022-06-22

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