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化学进展 2021, Vol. 33 Issue (5): 726-739 DOI: 10.7536/PC200694 前一篇   后一篇

所属专题: 金属有机框架材料

• 研究论文 •

MOF基水凝胶材料的制备及其应用

杨宇州1, 李政1,3,*(), 黄艳凤2, 巩继贤1, 乔长晟3, 张健飞1,4   

  1. 1 天津工业大学纺织科学与工程学院 先进纺织复合材料教育部重点实验室 天津 300387
    2 天津工业大学化学与化工学院 天津 300387
    3 宁夏中宁枸杞产业创新研究院有限公司 中宁 755199
    4 国家先进印染技术创新中心 泰安 271001
  • 收稿日期:2020-06-20 修回日期:2020-07-30 出版日期:2021-05-20 发布日期:2020-12-22
  • 通讯作者: 李政
  • 作者简介:
    * Corresponding author e-mail:
  • 基金资助:
    天津市重点研发计划科技支撑重点项目(20YFZCSN00130); 国家重点研发计划(2017YFB0309800); 国家重点研发计划(2016YFC0400503-02); 新疆自治区重大专项(2016A03006-3); 天津自然科学基金项目(18JCYBJC89600); 中国纺织工业联合会科技指导性项目(2017011); 宁夏中宁枸杞产业创新研究院一般项目(ZNGQCX-B-2019006)

Preparation and Application of MOF-Based Hydrogel Materials

Yuzhou Yang1, Zheng Li1,3,*(), Yanfeng Huang2, Jixian Gong1, Changsheng Qiao3, Jianfei Zhang1,4   

  1. 1 Key Laboratory of Advanced Textile Composites of Ministry of Education, School of Textiles Science and Engineering, Tiangong University,Tianjin 300387, China
    2 School of Chemistry and Chemical Engineering, Tiangong University,Tianjin 300387, China
    3 Innovation Research Institute of Wolfberry Industry Co. LTD,Zhongning 755199, China
    4 National Innovation Center of Advanced Dyeing and Finishing Technology, Taian 271001, China
  • Received:2020-06-20 Revised:2020-07-30 Online:2021-05-20 Published:2020-12-22
  • Contact: Zheng Li
  • Supported by:
    Tianjin Key Research and Development Project(20YFZCSN00130); National Key Research and Development Project Foundation of China(2017YFB0309800); National Key Research and Development Project Foundation of China(2016YFC0400503-02); Xinjiang Autonomous Region Major Significant Project Foundation(2016A03006-3); Tianjin Natural Science Foundation(18JCYBJC89600); Science and Technology Guidance Project of China National Textile and Apparel Council(2017011); Innovation Research Institute of Wolfberry Industry Co. LTD(ZNGQCX-B-2019006)

近年来,金属-有机骨架材料(MOFs)因为具有优异的骨架结构、丰富的孔隙度和多功能性,吸引了众多研究者的注意,各种各样的MOFs材料和MOF基复合材料被研制。但是由于MOFs大多以晶体和粉末的形式存在,其本身的刚性和易碎性限制了它的实际应用,同时MOFs在溶液中的不稳定性会导致材料的分解,一些高结晶度的MOFs还十分脆弱易碎且不易加工,因此有研究者将MOFs与水凝胶相结合,开发出许多具有优异性能的MOF基水凝胶材料。本文综述了MOF基水凝胶材料近年的研究进展,重点介绍了MOF基水凝胶的种类及其与其他材料的协同作用,讨论了MOF基水凝胶在传感、催化、水处理、伤口敷料和药物载体等方面的优势。MOF基水凝胶具有的可加工性、稳定性、易处理性为MOFs在实际应用中的研究具有指导意义。我们概述了纯MOF水凝胶、MOF@生物有机大分子水凝胶、MOF@生物相容性水凝胶,其他MOF基复合水凝胶的最新进展以及这些复合材料的应用。

In recent years, metal-organic framework materials(MOFs) have attracted the attention of many researchers because of their excellent framework structure, rich porosity and versatility. A variety of MOFs materials and MOF-based composites have been developed. However, since most MOFs exist in the form of crystals and powders, their rigidity and fragility limit its practical application. Meanwhile, the instability of MOFs in solution can cause the decomposition of the material. Some high-crystallinity MOFs are also very fragile and difficult to process, so researchers combine MOFs with hydrogels and develop many MOF-based hydrogel materials with excellent properties. This review presents current developments of MOF-based hydrogels with emphasis on the specific categories and the synergistic effects of MOF-derived hydrogels between MOFs and additional materials. Particular emphasis is placed on discussing the advantages of MOF-based hydrogels in applications such as sensors, catalysts, water treatment, wound dressings, drug carriers, etc. MOF-based hydrogels can provide valuable guidance for the investigation of MOFs towards practical applications with processability, stability, and easy handling. Specifically, the recent progress of pure MOF hydrogels, MOF@bioorganic macromolecule hydrogels, MOF@biocompatible hydrogels, other MOF-based composite hydrogels, and the applications of these composite materials are summarized.

Contents

1 Introduction

2 Methods to prepare MOF-based hydrogels

2.1 Direct mixing method

2.2 In situ growth

3 Classification of MOF-based hydrogels

3.1 Pure MOF hydrogels

3.2 MOF@bioorganic macromolecule hydrogels

3.3 MOF@biocompatible hydrogels

3.4 Other MOF-based composite hydrogels

4 Application of MOF-based hydrogels

4.1 Sensing

4.2 Catalytic

4.3 Water treatment

4.4 Wound healing

4.5 Drug carrier

5 Conclusion and outlook

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表1 不同材料的BET比表面积和孔体积[3]
Table 1 BET specific surface area and pore volume of different materials[3]
图1 采用直接合成法制备MOF基水凝胶[38]
Fig. 1 The preparation processes of MOF-based hydrogels by using the direct mixing method[38]
图2 采用原位生长法制备MOF基水凝胶[38]
Fig. 2 The preparation processes of MOF-based hydrogels in situ on hydrogels[38]
图3 (a)Tb-Dy MOF水凝胶,(b)Eu-Tb MOF水凝胶,(c)Eu-Dy MOF水凝胶,(d)Eu-Tb-Dy MOF水凝胶在阳光(左侧)和275 nm(右侧)光激发下的形态(混合金属比为1∶1或1∶1∶1),(e,f) 不同放大比例的Tb-MOF 水凝胶透射图[41]
Fig. 3 Photographs of(a) Tb-Dy MOF hydrogel,(b) Eu-Tb MOF hydrogel,(c) Eu-Dy MOF hydrogel, and(d) Eu-Tb-Dy MOF hydrogel with mixed-metal ratios of 1∶1 or 1∶1∶1 under sunlight(left) and under excitation at 275 nm(right).(e, f) Transmission electron microscopy(TEM) images with different amplification of Tb-MOF[41]
表2 MOF基水凝胶分类
Table 2 Classification of MOF-based hydrogels
图4 UIO-66的合成、Tr分子在UIO-66孔中的负载以及用卡拉胶包覆Tr@UIO-66的过程[44]
Fig. 4 The schematic representation of the synthesis of UIO-66, loading of Tr molecules into the UIO-66 pores and the general procedure for coating of Tr@UIO-66 with k-Cr[44]
图5 含MOF-Pt的ABEI/Co2+/CS的Cl-成像传感器检测OPs和D-AAs示意图[48]
Fig. 5 Schematic diagram of detection of OPs and D-AAs based on MOF-Pt enhanced long-lasting CL of ABEI/Co2+/CS hydrogels[48]
图6 (i) HKUST-1-藻酸盐复合物(ii) ZIF-8-藻酸盐复合物(iii) MIL-100(Fe)-藻酸盐复合物(iv) ZIF-67- 藻酸盐复合物(A) MOF 结构.(B)交联金属离子的纤维状水凝胶照片(C) MOF@藻酸盐水凝胶照片[52]
Fig. 6 (i) HKUST-1-alginate composite.(ii) ZIF-8-alginate composite.(iii) MIL-100(Fe)-alginate composite.(iv) ZIF-67- alginate composite.(A) MOF structure.(B) Photographs of the ?berlike metal ion cross-linked hydrogels.(C) Photographs of the corresponding MOF-alginate composites [52]
图7 (a)合成带有染料或药物的DNA/聚丙烯酰胺水凝胶涂层的MOFs示意图,(b) MOFs的SEM图像,(c)涂有水凝胶的MOFs的SEM图像[58]
Fig. 7 (a) Synthesis of DNA/polyacrylamide-hydrogel-coated MOFs loaded with dye or drug. Typical SEM image of the MOFs(b), and the MOFs coated with hydrogel(c)[58]
图8 制备ZIF-8/rGO复合水凝胶的自组装机制图[62]
Fig. 8 Schematic of the self-assembly mechanism of the rGO and ZIF-8 nanoparticles for the formation of ZIF-8/rGO composite hydrogels[62]
图9 用羧甲基纤维素包封Cu-MOF@IBU和从CMC/Cu-MOF@IBU释放IBU的程序示意图[67]
Fig. 9 Schematic of the general procedure employed for encapsulating Cu-MOF@IBU with carboxymethylcellulose and IBU release from CMC/Cu-MOF@IBU[67]
图10 (a)HM对不同浓度β-内酰胺酶的发光响应,(b)HM发光强度与β-内酰胺酶浓度之间的关系,(c)不同浓度的β-内酰胺酶血清溶液中HM的照片[75]
Fig. 10 (a) Luminescence responses of HM for the varying β-lactamase.(b) The relationship between intensities of HM and the concentrations of β-lactamase.(c) Photographs of the HM toward the various β-lactamase serum solutions with various concentrations [75]
图11 (A)合成Ag NPs@MIL100(Fe)/GG杂化水凝胶的示意图;(B)光催化降解的应用;(C)油/水分离;(D)Ag NPs@MIL-100(Fe)/GG杂化水凝胶的抗菌活性[57]
Fig. 11 (A) Schematic for synthesis of Ag NPs@MIL100(Fe)/GG hybrid hydrogel.(B) Applications for photocatalytic degradation.(C) Oil/Water separation.(D) Antibacterial activity of the Ag NPs@MIL-100(Fe)/GG hybrid hydrogel[57]
图12 疏水性MOFs@PVA多孔水凝胶膜的制备及应用(a)通过微流体方法制备载有ZIF-8的全疏水性水凝胶膜以及将所得膜用于伤口愈合的应用。(b)具有均匀孔的膜的显微光学图像。(插图显示了10 μL水滴在膜上的状态图)(c)ZIF-8@PVA水凝胶多孔膜上有滴一滴血的光学图像 [84]
Fig. 12 The fabrication and application of the omniphobic MOFs@PVA porous hydrogel membrane.(a) Schematic showing the fabrication of the ZIF8-loaded omniphobic hydrogel membranes by a microfluidic approach and the application of resultant membranes for wound healing.(b) Microscopic optical image of the membrane with uniform pores. The inset shows the CA of a water droplet of 10 μL.(c) Optical image showing a drop of blood on the ZIF-8@PVA hydrogel porous membrane [84]
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