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Progress in Chemistry 2023, Vol. 35 Issue (5): 683-698 DOI: 10.7536/PC221112 Previous Articles   Next Articles

• Review •

Synthetic Strategies of Chemically Stable Metal-Organic Frameworks

Mengrui Yang, Yuxin Xie, Dunru Zhu()   

  1. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
  • Received: Revised: Online: Published:
  • Contact: * e-mail: zhudr@njtech.edu.cn
  • Supported by:
    National Natural Science Foundation of China(21476115); Postgraduate Research & Practice Innovation Program of Jiangsu Province(KYCX23_1472)
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Metal-organic frameworks (MOFs) are a new generation of crystalline porous materials with void space structures constructed from metal ions or clusters and organic ligands through coordination bonds, and have been a hot research topic in the field of coordination chemistry over the past two decades. As the novel multifunctional materials, MOFs have been widely used in various fields due to their high porosities, low densities, large surface areas, tunable pore sizes, diverse topological structures and tailorabilities. Although MOFs have many advantages, most of MOFs materials have relatively lower water and chemical stability and cannot maintain their structures under harsh conditions, which greatly restrict their practical applications under moisture-rich conditions. Therefore, chemically stable MOFs materials will have greater application prospects. In recent years, researchers have carried out a lot of exploration in improving the chemical stability of MOFs, and developed some excellent methods to synthesize chemically stable MOFs. This review will mainly focus on the latest research progress in the syntheses of chemically stable MOFs during the past five years.

Contents

1 Introduction

2 Synthetic strategies of chemically stable MOFs

2.1 Increase the strength of coordination bonds

2.2 Attaching hydrophobic groups onto the linker

2.3 Using pore-partioning ligands for the pore space partition

2.4 Post-synthetic exchange method

2.5 Hydrophobic surface treatment

2.6 Other methods

3 Conclusion and Outlook

Key words: metal-organic frameworks(MOFs), chemical stability, synthetic strategy
Table 1 Comparison of some stable MOFs in the early stages
MOF Linker SBU Dimension Chemical stability Characterization ref
MIL-100(Cr) H3BTC Cr3O 3D water (RT): 12 months PXRD 17
MIL-101(Cr) H2BDC Cr3O 3D boiling water: 7 d; pH = 0~12 (RT): 2 months PXRD
N2 adsorption		 18
ZIF-8 MeIMa) [ZnN4] 3D boiling water: 7 d; 8 M NaOH (100 ℃):
1 d		 PXRD 19
UiO-66 H2BDC [Zr6O4(OH)4(CO2)12] 3D pH = 1~14: 2 h PXRD
N2 adsorption		 20
MIL-53(Cr) H2BDC [CrO4(OH)2] 3D 0.07 M HCl or NaOH (RT): 2 d PXRD 31
Fig. 1 Strategies to construct stable MOFs guided by HSAB theory[12]. Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig. 2 (a) The crystal engineering approach used to design BUT-53~58; (b) PXRD patterns of BUT-53[28]. Copyright 2022, Springer Nature
Fig. 3 (a) Crystal structure of ZnF(daTZ); (b) PXRD patterns of ZnF(daTZ) after treatment with acids and bases at various pH values[29]. Copyright 2020, ACS
Fig. 4 (a) The well-defined channels and cages in Cr-soc-MOF-1; (b) the calculated and the experimental PXRD pattern of the Cr-soc-MOF-1 after multiple water adsorption cycles[36]. Copyright 2020, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences
Fig. 5 (a) The structure of Al-MOF-1; (b) PXRD patterns of Al-MOF-1 after treatment with aqueous solutions ranging from pH = 2~12[38]. Copyright 2022, ACS
Fig. 6 (a) The structure of PCN-226; (b) The ztt topological net; (c) PXRD patterns of PCN-226(Cu) after being treated in pH = 1~13 solutions for 7 days[41]. Copyright 2020, ACS
Fig. 7 (a) Construction of PCN-625 using an 8-connected Zr6 cluster and 4-connected BBCPPP ligand; (b) PXRD patterns of soaked PCN-625 in different solutions[43]. Copyright 2021, ACS
Fig. 8 (a) A flu-a network constructed by 4-connected ligands and 8-connected Zr nodes; (b) PXRD patterns of CE-1 under different conditions[47]. Copyright 2021, ACS
Fig. 9 (a) The soc topological net of MIP-201; (b) PXRD patterns of MIP-201 samples treated under various chemical conditions[48]. Copyright 2022, Springer Nature
Fig. 10 (a) 3D structure of IEF-11; (b) PXRD patterns of IEF-11 after treatment with acids and bases at various pH values[49]. Copyright 2021, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig.11 (a) 1D rhombus channels in 1 along the c axis; (b) 1D inorganic rod-shaped chain [Eu(-CO2)2]n; (c) the 3D bnn network; (d) PXRD patterns for water-treated LnMOF 1[52]. Copyright 2017, ACS
Fig. 12 3D Ln-MOFs constructed from H3L5 and Ln3+[53]. Copyright 2022, RSC
Fig. 13 (a) Ball-and-stick representation of Fe-HAF-1; (b) PXRD patterns of Fe-HAF-1 after exposure to aqueous solutions at different pH for one week[58]. Copyright 2020, ACS
Fig. 14 (a) 3D structure of FJU-112; (b) PXRD patterns of FJU-112 after treatment with acids and bases at various pH values[60]. Copyright 2023, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig. 15 Construction of superhydrophobic UiO-67-Rs from Zr6O8 clusters and 3,3'-dialkyloxy-4,4'-biphenyldicarboxylic acids (H2Ln, n = 7~10)[63]. Copyright 2019, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig. 16 (a) The structural components of CPM-243, together with the framework along the c axis; (b) stability comparison of select MOFs. The arrow indicates stability under pH < 0 or pH > 14[68]. Copyright 2021, ACS
Fig. 17 (a) Synthetic approach of Pd-MOF: BUT-33(Pd); (b) PXRD patterns of BUT-33(Pd) after different conditions treatments[69]. Copyright 2021, ACS
Fig. 18 (a) The as-synthesized achiral UiO-68-Me was converted to chiral UiO-68-M via PSE of H2LM; (b) PXRD patterns of UiO-68-Cu after treatment in different solutions for 24 h[71]. Copyright 2018, ACS
Fig. 19 (a) Scheme showing the one-step surface polymerization of HKUST-1 to afford hydrophobic HKUST-1-P composite; (b) PXRD profiles of HKUST-1 and HKUST-1-P before and after treatment in water for 3 days[74]. Copyright 2020, Chinese Chemical Society
Fig. 20 (a, b) The 12-connected Zr6 node and the spirobifluorene-linker H4L in Zr-IAM-4; (c, d) 3D framework of Zr-IAM-4 without and with a two-fold interpenetrating structure; (e) PXRD patterns of Zr-IAM-4 and Eu-IAM-4 upon treatment in boiling water and acidic and basic solutions for 24 h[76]. Copyright 2020, ACS
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