面向一/二价离子分离的金属有机骨架膜研究进展

doi:10.11949/0438-1157.20231219

摘要/Abstract

摘要：

膜分离技术因操作简单、效率高、环境友好等特点，被誉为最具发展潜力的分离技术之一。金属有机骨架是一种新兴的分离膜材料，其可调变的孔道微结构、高孔隙率、拓扑结构多样性，使其在一/二价离子分离方面具有良好潜力。回顾了近二十年金属有机骨架膜在一/二价离子分离的研究进展并深入探讨了其传递机理，此外，也系统总结了金属有机骨架膜的制备方法，探讨了金属有机骨架膜在一/二价离子分离领域面临的挑战及未来研究方向。

关键词: 膜, 分离, 传递, 金属有机骨架, 一/二价离子

Abstract:

Membrane separation technology with the merits of operational simplicity, high efficiency, and environmental friendliness is considered as one of the most promising separation technologies. Metal-organic framework (MOF) is an emerging separation membrane material. Its tunable channel microstructure, high porosity, and topological diversity make it have good potential in the separation of mono/divalent ions. This article aims to review the research progress of MOF membranes for mono/divalent ions separation over the past two decades and discuss the transport mechanism in depth. It summarizes the membranes fabrication methods systematically and explores the challenges and future research directions of MOF membranes in the field of mono/divalent ions separation.

Key words: membrane, separation, transport, metal-organic framework, mono/divalent ions

中图分类号:

TQ 028

莫滨宇, 张雅馨, 刘国振, 刘公平, 金万勤. 面向一/二价离子分离的金属有机骨架膜研究进展[J]. 化工学报, 2024, 75(4): 1183-1197.

Binyu MO, Yaxin ZHANG, Guozhen LIU, Gongping LIU, Wanqin JIN. Recent progress of metal-organic framework membranes for mono/divalent ions separation[J]. CIESC Journal, 2024, 75(4): 1183-1197.

图/表 11

图1 通过RS方法在氧化铝载体上制备MIL-53膜的示意图[52]

Fig.1 Schematic diagram of preparation of MIL-53 membrane via the RS method[52]

图2 （a）Zn2+和Hmim通过尼龙支撑体反向扩散在尼龙支撑物两侧形成ZIF-8薄膜的示意图[54]；（b）反向扩散法制备ZIF-71示意图[55]

Fig.2 (a) Schematic diagram of the formation of ZIF-8 film by contra diffusion of Zn2+ and Hmim through porous nylon support[54]; (b) Schematic diagram of the preparation of ZIF-71 membrane via the contra diffusion method[55]

图3 反向扩散界面微流法制备ZIF-8中空纤维膜[56]

Fig.3 Preparation of ZIF-8 hollow fiber membrane via the interfacial microfluidic membrane processing (IMMP) approach[56]

图4 （a）FCDS制备ZIF-8膜示意图；（b）空白支撑体的SEM图像；（c）ZIF-8膜表面SEM图像；（d）ZIF-8 膜横截面的SEM图像[61]

Fig.4 (a) Schematic diagram of the preparation of ZIF-8 membrane via FCDS method; (b) SEM image of blank support; SEM images of surface (c) and cross-section (d) of ZIF-8 membrane [61]

图5 无缺陷MOF膜制备示意图（a）及MOF膜的超低剂量球差矫正透射电镜图：缺陷晶格（b）；完美晶格（c）[53]

Fig.5 Schematic diagram of formation of MOF membranes without lattice defects (a); Ultra-low dose spherical aberration correction transmission images of MOF membrane: defective lattice (b) and perfect lattice (c)[53]

图6 （a）层层组装法制备CuBTC膜[65]；（b）快速热沉积法制备ZIF-8膜[70]

Fig.6 Schematic diagrams of preparation of CuBTC film by layer-by-layer (LBL) assembly method (a)[65] and preparation of ZIF-8 film by rapid thermal deposition (RTD) method (b)[70]

图7 （a）通过界面生长法在PET纳米通道中构筑UiO-66-COOH SNC的示意图；（b）采用二次生长法制备异质结构UiO-66-(COOH)2 SCN膜的示意图[73]

Fig.7 (a) Schematic diagram of the formation process for UiO-66-COOH SCN membrane via interfacial growth method; (b) Schematic diagram of the formation process for UiO-66-(COOH)2 SCN membrane via secondary growth method[73]

图8 （a）MOF-303膜用于离子截留示意图[49]；（b）压力驱动离子筛分装置示意图

Fig.8 Schematic diagrams of MOF-303 membrane for ion retention (a)[49] and performance evaluation device of pressure-driven ion sieving (b)

图9 （a）PSS@HKUST-1膜制备过程示意图[81]；电场强化离子渗透过程（b）及装置示意图（c）[82]；（d）UiO-67膜一/二价离子分离性能[82]；（e）UiO-67膜离子分离性能对比[82]；（f）UiO-67膜离子分离机理示意图[82]（1 Å =0.1 nm）；（g）TA-Fe Ⅲ/ZIF-8膜离子分离性能[84]

Fig.9 (a) Schematic diagram of PSS@HKUST-1 membrane preparation[81]; (b) Schematic diagram of electric field enhanced ions permeation process and (c) measurement device[82]; (d) Mono/divalent ions separation performance of UiO-67 membrane; (e) Li+/Mg2+ separation performance comparison of UiO-67 membrane; (f) Schematic diagram of ions separation mechanism in UiO-67 membrane[82]; (g) Ions separation performance of TA- Fe Ⅲ/ZIF-8 membrane[84]

图10 （a）UiO-66-(COOH)2亚纳米通道膜制备示意图[74]；（b）荷负电荷UiO-66-COOH纳米通道膜用于离子的传输示意图[72]；（c）UiO-66-(COOH)2-SCN通道膜在0.1 mol·L-1电解质溶液(pH=5.7)时测量的I-V曲线；（d）UiO-66-(COOH)2-SCN通道膜的一/二价分离性能（内插图是离子渗透实验的示意图）；（e）UiO-66(COOH)2膜内空腔在不同条件的分子结构变化；（f）溶液pH对膜分离性能的影响[74]；（g）UiO-66(COOH)2膜测试不同离子的I-V曲线;（h）UiO-66(COOH)2膜的K+/Mg2+性能对比[72]

Fig.10 (a) Schematic of UiO-66-(COOH)2 SNC membrane fabrication[74]; (b) Illustration of negatively charged porous UiO-66-COOH-SCN membrane for ions transport[72]; (c) I - V curves of UiO-66-(COOH)2-SCN channel membranes measured in 0.1 mol·L-1 electrolyte solution (pH 5.7); (d) Ions separation performance of UiO-66-(COOH)2-SCN membrane（The inset is schematic diagram of ions permeation experiments); (e) Molecular structure change of the large cavity of UiO-66-(COOH)2 under different conditions; (f) Effect of pH on the conductivity of ions in UiO-66-(COOH)2 membrane[74]; (g) I-V curves of UiO-66-COOH-SNC measured in 0.1 mol·L-1 chloride salt solution; (h) K+/Mg2+ separation performance comparison of UiO-66-COOH-SNC membrane[72]

图11 UiO-66-NH2膜的SEM图：表面（a）和断面（b）；电渗析测试MOF膜离子筛分性能示意图（c）[87]；UiO-66-NH2膜的离子筛分性能（d）[88]

Fig.11 SEM surface (a) and cross-sectional (b) images of UiO-66-NH2 membrane; Schematic diagram of ionic sieving performance evaluation device by electrodialysis (c)[87]; Ions separation performance of UiO-66-NH2 membrane (d)[88]

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