Selective liquid-phase molecular sieving via thin metal–organic framework membranes with topological defects

Xiansong Shi, He Li, Ting Chen, Yidan Duan, Dongchen Shi, Chengjun Kang, Zhaoqiang Zhang, Dan Zhao
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Abstract

Separating fine and similarly sized targets in liquids is a crucial but challenging task. Although current membranes have the potential to be sustainable and energy-efficient options, their molecular selectivity and durability remain limited. Here we report robust and accurate molecular-sieving membranes created through the topological design of a Zr-based metal–organic framework, namely UiO-66, for use in durable liquid-phase separations. Our findings reveal that crystallizing UiO-66 using a bimetallic method yields distinctive reo-topology frameworks with periodic missing-cluster defects. We crystallize reo-UiO-66 into thin polycrystalline membranes that exhibit improved and robust performance, lasting for over 1,500 h. The modified Ferry transport model provides a quantitative description of solute rejection from the polycrystalline membrane. Multiple molecular-sieving experiments recognize excellent membrane selectivity to accurately discriminate fine complex mixtures with molecular weights below 350 g mol−1. In addition, our membrane demonstrates promise in purifying and recovering high-value pharmaceuticals and catalysts. This work paves the way for developing polycrystalline membrane technology for the sustainable separation of chemical mixtures in liquids. Efficiently separating high-value targets with small structural differences in liquids is important to the chemical industry. Here the authors develop a metal–organic framework-based membrane with engineered topologic defects for accurate and prolonged sieving of species with molecular weights below 350 g mol−1.

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通过具有拓扑缺陷的金属有机框架薄膜实现选择性液相分子筛分
分离液体中的细小和类似大小的目标是一项至关重要但又极具挑战性的任务。尽管目前的膜有可能成为可持续的节能选择,但其分子选择性和耐久性仍然有限。在此,我们报告了通过对一种基于 Zr 的金属有机框架(即 UiO-66)进行拓扑设计而制造出的用于持久液相分离的坚固而精确的分子筛分膜。我们的研究结果表明,使用双金属方法使 UiO-66 结晶,可产生具有周期性缺失簇缺陷的独特 reo 拓扑框架。我们将 reo-UiO-66 结晶成薄薄的多晶膜,这种多晶膜的性能得到了改善,而且非常坚固耐用,可持续使用超过 1,500 小时。多项分子筛分实验表明,膜具有出色的选择性,能准确分辨分子量低于 350 g mol-1 的精细复杂混合物。此外,我们的膜在提纯和回收高价值药物和催化剂方面也大有可为。这项工作为开发可持续分离液体中化学混合物的多晶膜技术铺平了道路。有效分离液体中结构差异较小的高价值目标对化学工业非常重要。在此,作者开发了一种基于金属有机框架的膜,该膜具有工程拓扑缺陷,可准确、长时间地筛分分子量低于 350 g mol-1 的物质。
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