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化学进展 2021, Vol. 33 Issue (12): 2173-2187 DOI: 10.7536/PC201053   后一篇

• 综述 •

金属有机骨架材料的复合成型

董秀婷*, 张文*(), 赵颂*, 刘新磊, 王宇新   

  1. 天津大学化工学院 天津市膜科学与海水淡化重点实验室 化学工程联合国家重点实验室 天津 300350
  • 收稿日期:2020-10-29 修回日期:2021-01-31 出版日期:2021-03-04 发布日期:2021-03-04
  • 通讯作者: 董秀婷, 张文, 赵颂
  • 基金资助:
    国家自然科学基金项目(11705126); 国家自然科学基金项目(22076137)
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Shaping Methods for Metal-Organic Framework Composites

Xiuting Dong, Wen Zhang(), Song Zhao, Xinlei Liu, Yuxin Wang   

  1. Tianjin Key Laboratory of Membrane Science & Desalination Technology, State Key Laboratory of Chemical Engineering, School of Chemical Engineering, Tianjin University,Tianjin 300350, China
  • Received:2020-10-29 Revised:2021-01-31 Online:2021-03-04 Published:2021-03-04
  • Contact: Xiuting Dong, Wen Zhang, Song Zhao
  • Supported by:
    the National Natural Science Foundation of China(11705126); the National Natural Science Foundation of China(22076137)

金属有机骨架材料(MOFs)是由有机配体与金属离子(簇)配位而成的有序杂化多孔框架晶体材料,具有比表面积高、密度低、孔结构可调、配体可设计及易修饰等特性,已广泛应用于分离、催化、传感和药物递送等研究领域。MOFs本身以粉体形式存在,在实际应用中不易于加工处理和回收再利用,甚至会导致粉体污染。因此对MOFs粉末进行复合成型,制备成复合颗粒或者膜材料,有利于推进其工业应用。本文按照MOFs制备和成型的先后顺序,对MOFs复合微珠、薄膜和混合基质膜成型体的制备方法进行综述,对推进MOFs成型体的大规模制备以及开发新的MOFs成型方法提供技术参考。

关键词： 金属有机骨架材料, 成型方法, 复合微珠, 薄膜, 混合基质膜

Metal-organic frameworks (MOFs) are porous crystal materials formed by the self-assembling between organic ligands and metal ions (clusters). With the advantages of high specific surface areas, low densities, adjustable pore structures and easy modification, they have been used in the research fields of separation, catalysis, sensing and drug delivery. MOFs are often isolated as tiny powders, and this form is not suitable for industrial applications due to operating problems, such as dirtiness, mass loss, and difficulties in recycling. To address this issue, several composite materials containing MOFs have been developed with various shaping methods. In this review, we discuss the preparation methods to shape MOFs into beads, thin films and membranes, as well as their potential industrial applications. This paper could provide a reference for developing novel methods for shaping of MOFs and techniques to fabricate large-scale MOF composites.

Contents

1 Introduction

2 MOF beads

2.1 Beads prepared by MOF powders

2.2 MOFs growth in beads

3 MOF films

3.1 Films prepared by MOF powders

3.2 MOFs growth on films

4 MOF mixed-matrix membranes

4.1 Membranes prepared by MOF powders

4.2 MOFs growth in membranes

5 Conclusion and outlook

Key words: MOFs, shaping methods, composite beads, thin films, mixed matrix membranes
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表1 挤压造粒法制备MOFs成型体的比表面积变化
Table 1 The specific surface area of different MOF composites by granulation method
MOFs/binders MOFs
content wt%		 Specific surface area (m2/g) MOFs/binders MOFs
content wt%		 specific surface area (m2/g)
MOFs compounds MOFs compounds
MOF-5@Graphite[10] 90 2763 2665 UiO-66@PMMA[30] 90 1375 1162
MIL-100(Cr)@ρ-Al2O3[8] 95 4066 3685 ZIF-8@PEG[30] 90 1842 1045
MIL-100(Fe)@ρ-Al2O3[8] 95 2088 1831 ZIF-8@PMMA[30] 90 1842 1584
UiO-66@ρ-Al2O3[8] 95 1050 911 MOF-801@PVB[17] 95 899 605
UiO-66-NH2@ρ-Al2O3[8] 95 875 823 MIL-101(Cr)@PIM-1[34] 80 2720 2347
MIL-100(Fe)@Silica col[7] 90 1772 1619 Cu-BTC@PVA[15] 85 1737 963
UiO-66@Graphite[9] 99 1140 885 UTSA-16@PVA[32] 97 746 708
UiO-66@Sucrose[31] 90 1367 674 MIL-127(Fe)@ρ-Al2O3[8] 95 1413 1266
UiO-66@PEG[30] 90 1375 764 UiO-66@Polysiloxane[29] 73 710 418
图1 典型的3D打印工作流程[36]
Fig.1 Typical process workflow based on 3D printing[36], Copyright 2020, ACS
图2 微珠制备的相转化法及溶剂交换原理图[20]
Fig.2 Schematic diagrams of the phase inversion method for polymer sphere preparation[20], Copyright 2019, ACS
表2 相转移法制备MOFs成型体性质比较
Table 2 The specific surface area of molded MOF composites by phase inversion methods
MOFs/binders MOFs
content wt%		 Specific surface area (m2/g)
MOFs Compounds
Cu-BTC@PES[45] 70 1370 1250
Cu-BTC@PEI[45] 70 1370 990
Cu-BTC@PVDF[45] 60 1370 1100
ZIF-8@PS[47] 80 1023 761
Cu-BTC@PES[20] 75 1053 237
ZIF-8@PES[21] 80 1849 1382
MOF-808@PVDF[48] 70 2205 668
图3 共混或交联法进行MOFs聚合物复合[49]
Fig.3 Combinations of MOFs with polymers form either mixed or covalent composites[49], Copyright 2020, ACS
图4 钙诱导丙烯酸和海藻酸交联制备多孔MOFs微球[50]
Fig.4 Scheme of MOF-polymer bead preparation from the gelation of Ca2+, PAA and alginate[50], Copyright 2020, ACS
表3 聚合物交联法制备MOFs成型体性质比较
Table 3 The specific surface area of molded MOF composites by polymer crosslinking method
MOFs Matrix MOFs
content wt%		 Specific surface area (m2/g)
MOFs Compounds
CPO-27-Ni[22] SA 95 1319 1014
MIL-127-Fe[50] PAA/SA 91.1 1205 1117
MIL-101(Cr)[50] PAA/SA 92.7 2246 2007
UiO-66[50] PAA/SA 88.5 1476 1303
ZIF-67[50] PAA/SA 84.9 1573 1256
ZIF-8[50] PAA/SA 90.7 1688 1357
Fe-BTC[50] PAA/SA 87 1618 1240
Fe-BTC[50] PDA 92.9 997 915
MIL-101[52] SA/CS 70 4000 800
ZIF-8[24] CS 60 1080 628
ZIF-8[23] CS 80 1080 221.4
UiO-66[25] SA 85 1241 1029
图5 配体交换法制备MOFs杂化聚合物[51]
Fig.5 Polymer-MOF composites through surface-selective ligand exchange[51], Copyright 2020, ACS
图6 (a)含咪唑酯MOFs原位生长氧化铝示意图[14]; (b)HKUST-1 @γ-Al2O3复合材料制备示意图[13]
Fig.6 (a) Postulated anchoring of imidazolate-based MOFs on alumina[14], Copyright 2016, ACS; (b) The Structure of HKUST-1@γ-Al2O3 composite[13], Copyright 2010, RSC
图7 蜘蛛网状ZIF-8整体泡沫制备示意图[53]
Fig.7 Schematic diagram for a spiderweb-like ZIF-8 mono-lithic foam[53], Copyright 2020, Wiley
图8 飞秒脉冲激光沉积制备的ZIF-8膜示意图[11]
Fig.8 ZIF-8 films prepared by femtosecond pulsed-laser deposition[11], Copyright 2017, ACS
图9 (a)原位合成UiO-66@Al2O3示意图;(b)UiO-66@Al2O3膜截面图和(c)纵向剖面图[68]
Fig.9 (a) Diagram of in-situ fabrication for UiO-66@Al2O3; SEM images of (b) cross section and (c) top view of the UiO-66@Al2O3[68], Copyright 2015, ACS
图10 (a)反应播种法制备MIL-53/α-Al2O3膜[75];(b)逐层浸渍组装法制备HKUST-1/α-Al2O3膜[76];(c)共价辅助接种法制备ZIF-8/PI复合膜[77];(d)取向播种法联用可控二次生长法制备择优取向的NH2-MIL-125膜[78]
Fig.10 (a) Reactive seeding method for the preparation of continuous MOF films[75], Copyright 2011, RSC; (b) Step-by-step seeding procedure for preparing HKUST-1 films[76], Copyright 2011, ACS; (c) Fabrication procedure of ZIF-8/PI by covalent-assisted seeding methods[77], Copyright 2019, Wiley; (d) Preparation of oriented NH2-MIL-125(Ti) films by combining oriented seeding and controlled in-plane secondary growth[78], Copyright 2018, Wiley
图11 (a)在ZnAl-LDH层修饰的γ-Al2O3基底上原位生长ZIF-8膜[60];(b)GO-ZnO层限域取向生长Zn2(bIm)4膜[64];(c)原子层沉积和配体气相处理制备ZIF膜示意图[79];(d)利用氢氧化铜纳米链制备自支撑HKUST-1膜[85]
Fig.11 (a) Scheme of in situ growth of ZIF-8 on a ZnAl-LDH buffer layer-modified γ-Al2O3[60], Copyright 2014, Wiley; (b) Scheme of the preparation of oriented Zn2(bIm)4 membranes by ZnO self-conversion growth in a GO confined space[64], Copyright 2018, RSC; (c) Schematic of ZIF membranes made by ligand-induced permselectivation[79]; (d) Synthesis of free-standing HKUST-1 membranes from copper hydroxide nanostrands[85], Copyright 2013, RSC
图12 (a)干燥粉体和直接液相法制备ZIF-8@PVA膜[99];(b)聚合物刷修饰MOFs前后的界面相互作用示意图[100];(c)利用MOFs中间层构筑双界面制膜示意图[101]
Fig.12 (a) Preparation of ZIF-8@PVA from ZIF-8 suspensions with and without drying[99], Copyright 2016, Wiley; (b) Interfacial interaction in a traditional and a polymer brush modified MMM[100], Copyright 2018, ACS; (c) MOF-801@Ni-MOF-74 MMMs with a dual-interfacial engineering approach[101], Copyright 2020, ACS
图13 (a)UiO-66-NH2膜后合成修饰示意图[112];(b)可聚合的Ln-MOFs与甲基丙烯酸丁酯单体聚合为杂化膜[113];(c)喷雾自组装技术辅助合成ZIF-8-PDMS复合膜示意图[114]
Fig.13 (a) Postsynthetic modification of UiO-66-NH2 and subsequent polymerization[112], Copyright 2015, Wiley; (b) Copolymerization of polymerizable Ln-MOFs with butyl methacrylate monomers into polyMOF membrane[113], Copyright 2014, Wiley; (c) Formation of the ZIF-8-PDMS composite membrane by the simultaneous spray self-assembly technique[114], Copyright 2014, Wiley
图14 (a)原位生长UiO-66-MMM膜示意图[116];(b)ZIF-8 @MMMs膜合成示意图[117]
Fig.14 (a) Fabrication method for MMM with in situ MOF growth[116], Copyright 2018, ACS; (b) Preparation procedure of ZIF-8 @MMMs[117], Copyright 2018, Elsevier
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