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Progress in Chemistry 2021, Vol. 33 Issue (12): 2173-2187 DOI: 10.7536/PC201053   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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
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
Fig.1 Typical process workflow based on 3D printing[36], Copyright 2020, ACS
Fig.2 Schematic diagrams of the phase inversion method for polymer sphere preparation[20], Copyright 2019, ACS
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
Fig.3 Combinations of MOFs with polymers form either mixed or covalent composites[49], Copyright 2020, ACS
Fig.4 Scheme of MOF-polymer bead preparation from the gelation of Ca2+, PAA and alginate[50], Copyright 2020, ACS
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
Fig.5 Polymer-MOF composites through surface-selective ligand exchange[51], Copyright 2020, ACS
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
Fig.7 Schematic diagram for a spiderweb-like ZIF-8 mono-lithic foam[53], Copyright 2020, Wiley
Fig.8 ZIF-8 films prepared by femtosecond pulsed-laser deposition[11], Copyright 2017, ACS
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
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
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
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
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
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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