金属有机框架基复合材料的制备及其光热性能研究

doi:10.6023/A21040173

化学学报 ›› 2021, Vol. 79 ›› Issue (8): 967-985.DOI: 10.6023/A21040173 上一篇下一篇

所属专题：多孔材料：金属有机框架(MOF)

综述

金属有机框架基复合材料的制备及其光热性能研究

郭彩霞, 马小杰^*(), 王博^*()

北京理工大学化学与化工学院北京 100081

投稿日期:2021-04-22 发布日期:2021-05-26
通讯作者: 马小杰, 王博

作者简介:

郭彩霞, 北京理工大学硕士研究生. 2018年本科毕业于山东师范大学, 现于北京理工大学攻读硕士学位. 主要研究领域为MOF复合材料的制备及光催化性能.

马小杰, 北京理工大学化学与化工学院预聘助理教授, 于兰州大学化学与化工学院取得本科与硕士学位, 中科院化学研究所获得博士学位. 主要从事多孔材料的环境催化研究工作.

王博, 北京理工大学化学与化工学院教授, 2004年于北京大学化学与分子工程学院获理学学士学位, 2006年于美国密歇根大学获化学材料学硕士学位, 2008年于美国加州大学洛杉矶分校获化学材料学博士学位. 王博教授主要从事新型纳米多孔材料、开放框架聚合物理论与设计及其在关键分离过程、环境防护等领域的应用研究.

基金资助:
国家自然科学基金(21625102); 国家自然科学基金(21801017); 国家自然科学基金(21490570); 国家自然科学基金(21674012); 北京市科委科技计划项目(Z181100004418001); 北京理工大学科研基金项目资助

Metal-organic Frameworks-based Composites and Their Photothermal Applications

Caixia Guo, Xiaojie Ma(), Bo Wang()

School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China

Received:2021-04-22 Published:2021-05-26
Contact: Xiaojie Ma, Bo Wang
Supported by:
National Natural Science Foundation of China(21625102); National Natural Science Foundation of China(21801017); National Natural Science Foundation of China(21490570); National Natural Science Foundation of China(21674012); Beijing Municipal Science and Technology Project(Z181100004418001); Beijing Institute of Technology Research Fund Program

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摘要/Abstract

金属有机框架材料(metal-organic frameworks, MOFs)是一类新型的有机-无机杂化材料, 具有可功能化的骨架结构、高比表面积、可调控的孔径尺寸等优势. 将MOFs与性质多样的有机/无机功能纳米材料复合, 不仅有可能充分发挥组分各自的优势, 而且有可能产生“1+1>2”的协同效应, 因而引起了人们的广泛关注. 具有光热效应的MOF复合物作为一类重要的MOF复合材料, 在生物诊疗、催化等领域展现出了良好的应用前景. 作者首先综述了近年来MOF复合材料的主要可控制备方法, 随后讨论了光热MOF复合材料的应用研究, 最后对该类材料的未来研究方向和挑战进行了展望.

关键词: 金属有机骨架材料, 复合材料, 光热效应, 肿瘤治疗, 协同催化

Metal-organic frameworks (MOFs) are a growing class of organic-inorganic hybrid crystalline porous materials, showing high levels of structural and chemical diversity. They have a wide range of applications in gas adsorption and separation, catalysis, sensing, biomedicine and other fields. Due to their intriguing properties such as high porosity, adjustable pore size and tunable surface functionality, MOFs have been gaining popularity as a promising platform for integration of various organic/inorganic functional nanomaterials in a predictable and controllable way. The combination of MOFs and functional components offers a possibility to generate synergetic effect between functional units, thus leading to the creation of multifunctional materials with performance superior to each individual components. In this review, we summarized recent research progress on controllable synthesis of MOF composites. There are basically two strategies, including “bottle in ship” and “ship in bottle”. Following that, preparation methods including solution infiltration, deposition, solid grinding and template synthesis, were discussed in detail. Light-to-heat conversion materials have always been a research focus due to their important applications in solar powered water evaporation and near-infrared (NIR) excited bioimaging and noninvasive cancer treatment. MOFs can not only show intrinsic structure-dependent photoresponse activity, but also serve as porous supports to facilitate the stabilization and spatial distribution of photothermal nanoparticles. Recently, MOF composites with photothermal effects have aroused increasing attention in the fields like tumor diagnosis and treatment, bacterial disinfection and synergistic catalysis. This review mainly focused on the recent research progress on photothermal MOF composites. We discussed the integration of functional MOFs with various inorganic/organic photothermal nanoparticles (e.g. Au, Pt, porphyrin, polydopamine etc.), along with the structure and photothermal application of the composites. Research about MOFs based light-to-heat conversion is at the stage of rapid development. Finally, we also give a prospect to the future development of multifunctional and photothermal MOF composites.

Key words: metal-organic framework, composite material, photothermal effect, tumor treatment, synergistic catalysis

引用此文

郭彩霞, 马小杰, 王博. 金属有机框架基复合材料的制备及其光热性能研究[J]. 化学学报, 2021, 79(8): 967-985.

Caixia Guo, Xiaojie Ma, Bo Wang. Metal-organic Frameworks-based Composites and Their Photothermal Applications[J]. Acta Chimica Sinica, 2021, 79(8): 967-985.

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图/表 31

图1. (a~c) 光热机制示意图; (d) 光热MOF复合物示意图

Figure 1. (a~c) Schematic illustration of photothermal mechanisms; (d) schematic illustration of the photothermal MOF composites

图2. MOF复合材料制备策略及光热应用(光热肿瘤治疗、光热杀菌及光热协同催化领域)示意图

Figure 2. Schematic illustration of synthetic strategies and photothermal applications (photothermal tumor treatment, photothermal-disinfection, photothermal synergistic catalysis) for MOF composites

图3. MOF复合材料的合成方法示意图

Figure 3. Schematic illustration of synthetic methods for MOF composites

图4. 制备方法示意图. 改编自文献[45]

Figure 4. Schematic illustration for the preparation methods. Adapted from the literature [45]

图5. 在无水乙醇中制备MIL-101@MS复合材料的路线. 通过去除MIL-101中的配位水, 可以暴露MIL-101的配位不饱和金属位(CUSs). 颜色键: 铬(青绿色)、氮(紫色)、硫(深黄色)、碳(灰色)、氧(红色), 为了清楚起见, 省略了氢原子. 改编自文献[50]

Figure 5. Synthesis route to MIL-101@MS composites prepared in anhydrous ethanol. The coordinatively unsaturated metal sites (CUSs) of MIL-101 are exposed by removing coordinated water in MIL-101. Color key: chromium (teal), nitrogen (purple), sulfur (dark yellow), carbon (gray), oxygen (red), hydrogen atoms are omitted for clarity. Adapted from the literature [50]

图6. 使用DSM结合液相CCR策略在MIL-101孔道中生长AuNi纳米颗粒的示意图. 改编自文献[54]

Figure 6. Schematic representation of immobilization of the AuNi nanoparticles by the MIL-101 matrix using the DSM combined with a liquid-phase CCR strategy. Adapted from the literature [54]

图7. ALD反应周期的四个脉冲. 改编自文献[74]

Figure 7. The four pulses of an ALD reaction cycle. Adapted from the literature [74]

图8. 机械力化学法合成Pd@ZIF-8的过程. 改编自文献[90]

Figure 8. Synthesis procedure of Pd@ZIF-8 via the mechanochemistry-assisted approach. Adapted from the literature [90]

图9. Cu2O@HKUST-1取向生长和Cu2O/HKUST-1复合材料随机生长示意图. 改编自文献[101]

Figure 9. Schematic illustration for the oriented growth of Cu2O@HKUST-1 and random growth of Cu2O/HKUST-1 composites. Adapted from the literature [101]

图10. AuNS@MOF-ZD2纳米探针的合成示意图, 及其在T1-加权MR成像和光热疗法中特别针对MDA-MB-231肿瘤(TNBC)的应用. 改编自文献[98]

Figure 10. Schematic illustration of the synthesis of AuNS@MOF-ZD2 nanoprobes, and application for T1-weighted MR imaging and photothermal therapy specifically toward MDA-MB-231 tumor (TNBC). Adapted from the literature [98]

图11. (a) 卵黄壳结构Au@MOF TEM图像; (b) 体内DOX、Au@MOF、Au@MOF-DOX分别静脉注射于荷瘤小鼠体内, 经1064 nm激光照射或不照射处理, 各组荷瘤小鼠在治疗期间的平均体重; (c) 各组荷瘤小鼠的相对肿瘤体积(归一化); (d) 不同处理后荷瘤小鼠的代表性照片. 改编自文献[97]

Figure 11. (a) TEM images of yolk-shell structured Au@MOF; (b) in vivo DOX, Au@MOF, and Au@MOF-DOX were injected intravenously to the tumor-bearing mice and treated with or without 1064 nm laser irradiation. The average body weight of tumor-bearing mice in each group during the treatment periods; (c) the relative tumor volumes (normalized) of tumor-bearing mice in each group; (d) the representative photographs of tumor-bearing mice after different treatments. Adapted from the literature [97]

图12. LA-AuNR/ZIF-8 JNP的制备示意图. 改编自文献[96]

Figure 12. Schematic illustration of fabricating LA-AuNR/ZIF-8 JNPs. Adapted from the literature [96]

图13. (a) 制备PUA-Ce6的流程以及通过将肿瘤内的H2O2转化为O2应用于PTT潜在增强的PDT结合以进行肿瘤治疗的情况; (b) 添加PBS或PUA-Ce6置于黑暗中或用670和808 nm激光照射孵育的MCF-7细胞的荧光图像, 处理5 min(用Calcein-AM/PI染色, 绿色表示活体, 红色表示死亡); (c) 不同反应时间下, PUA水溶液对应的紫外可见吸收光谱; (d)不同处理后小鼠的肿瘤体积曲线变化(每组5只小鼠). 改编自文献[95]

Figure 13. (a) Schematic illustration for the preparation of PUA-Ce6 and its application on combination of PTT and potential enhanced PDT by converting intratumor H2O2 into O2 for tumor therapy; (b) fluorescent images of MCF-7 cells incubated with PBS or PUA-Ce6 nanoparticles with or without 670 and 808 nm laser irradiation, each for 5 min separately (stained by Calcein-AM/PI, green for live and red for dead); (c) the corresponding UV-vis-NIR absorbance spectra of PUA aqueous solution at different reaction times; (d) tumor volume curves change of mice after different treatments (5 mice per group). Adapted from the literature [95]

图14. BQ和过氧化氢酶在MOF层中的逐步组装及其作为串联催化剂增强对缺氧肿瘤细胞的治疗. 改编自文献[114]

Figure 14. Stepwise assembly of BQ and catalase in MOF layers and its application as tandem catalyst for enhanced therapy against hypoxic tumor cells. Adapted from the literature [114]

图15. (a) Fe3O4/ZIF-8-Au25样品的场相关磁化回路; (b) 使用3T MR扫描仪记录的Fe3O4/ZIF-8-Au25纳米复合材料的T2加权MRI图像; (c) 使用Fe3O4/ZIF-8-Au25样品在体内进行MRI成像. 在注射IZA之前(左)和之后(右)拍摄MRI图像. 改编自文献[32]

Figure 15. (a) Field-dependent magnetization loop of the Fe3O4/ZIF-8-Au25 sample; (b) T2-weighted MR images of Fe3O4/ZIF-8-Au25 nanocomposite recorded using a 3T MR scanner; (c) MR imaging for in vivo mapping using Fe3O4/ZIF-8-Au25 sample. MR images were taken before (left) and after (right) injection of IZA. Adapted from the literature [32]

图16. (a) CSD-MOFs的合成程序示意图; (b) 示意图: CSD-MOFs@DOX作为一种有效的多模式协同肿瘤治疗药物. 改编自文献[132]

Figure 16. (a) Schematic illustration of synthetic procedure of CSD-MOFs and (b) schematic representation: CSD-MOFs@DOX as an effective multi-model therapeutic agents for synergistic tumor therapy. Adapted from the literature [132]

图17. 用于癌症治疗的光激活TCPC-UiO的合成及其机理. (a) TCPC-UiO NMOF的合成及激光辐照下产热和单线态氧的原理描述; (b) 在CT/热/光声成像引导下在体内利用单一光源进行联合癌症治疗的光物理机制(Phos, 磷光; NRR, 无辐射复合; ISC, 系间窜越). 改编自文献[143]

Figure 17. Synthesis and mechanism for cancer therapy of TCPC-UiO by light activation. (a) Synthesis of TCPC-UiO NMOF and schematic description of heat and singlet oxygen generation under laser irradiation; (b) photophysical mechanism for cancer therapy under light activation (Phos., phosphorescence; NRR, nonradiative recombination; ISC, intersystem crossing) of a combination therapy utilizing a single light source in vivo guided by CT/thermal/photoacoustic imaging. Adapted from the literature [143]

图18. Mn-IR825@PDA-PEG的合成过程. 改编自文献[144]

Figure 18. Schematic illustration to show the fabrication process of Mn-IR825@PDA-PEG. Adapted from the literature [144]

图19. MIL-100(Fe) NPs的合成过程、HA偶联、ICG加载和多模态成像引导PTT的示意图. 改编自文献[147]

Figure 19. Schematic representation of the synthesis procedure, HA conjugation, ICG loading, and multimodal imaging-guided PTT of MIL-100(Fe) NPs. Adapted from the literature [147]

图20. PPy@MIL-100(Fe) NCs作为药物载体用于双模成像和具有pH/NIR响应的化疗和光热治疗的合成策略示意图. 改编自文献[150]

Figure 20. Schematic illustration of the synthetic strategy for PPy@MIL-100(Fe) NCs as pH/NIR-responsive drug carriers for dualmode imaging and synergistic chemo-photothermal therapy in vitro. Adapted from the literature [150]

图21. PPy@MIL-53/DOX的合成及用于光热化学疗法和肿瘤MRI的流程. 改编自文献[151]

Figure 21. Illustration of PPy@MIL-53/DOX synthesis for photothermal-chemotherapy and MRI of tumors. Adapted from the literature [151]

图22. (a) MCH NPs的制备流程; (b) MCH NPs用于PAI引导的化学/光热联合肿瘤治疗的示意图. 改编自文献[154]

Figure 22. (a) Preparation procedure of MCH NPs and (b) schematic illustration of MCH NPs for PAI-guided chemo-/photothermal combinational tumor therapy. Adapted from the literature [154]

图23. (a) 制备MCP, MCP-PEG和MCP-PEG-RGD NPs的示意图; (b) 在不同的锰浓度下, MCP-PEG NPs的T1加权MR图像和MRI图像的R1图; (c) 不同处理后小鼠的肿瘤生长曲线(n=6). 改编自文献[155]

Figure 23. (a) The schematic representation of the preparation of MCP, MCP-PEG, and MCP PEG-RGD NPs; (b) T1-weighted MR images and R1 map of MRI phantom images of MCP-PEG NPs at different Mn concentration; (c) tumor growth curves of mice after different treatments (n=6). Adapted from the literature [155]

图24. (a) 制备2D TRB-ZnO@G纳米片的示意图; (b) 示意图说明了NIR触发的TRB-ZnO@G的相到尺寸转化, 以及与包裹和杀死的细菌相应的微米聚集体的形成. 改编自文献[179]

Figure 24. (a) Schematic illustrations for the preparation of 2D TRB-ZnO@G nanosheets; (b) schematic illustration of the NIR-triggered phase-to-size transformation of TRB-ZnO@G, and the corresponding formation of micrometer-aggregations with wrapped and killed bacteria. Adapted from the literature [179]

图25. (a) PB@MOF的核壳结构示意图; (b) PB@MOF在双光照射下杀死细菌的过程示意图; (c) PB@MOF异质结光催化剂合理的光催化机理示意图. 改编自文献[180]

Figure 25. (a) Schematic illustration of the core-shell structure of PB@MOF; (b) schematic illustration of the bacteria killing processes with the PB@MOF under dual light irradiation; (c) schematic illustration of rational photocatalytic mechanism for PB@MOF heterojunction photocatalysts. Adapted from the literature [180]

图26. (a) GF@UiO-66-NH2水解DMNP的反应机理; (b) 在模拟太阳光(0.6 W•cm-2)下, GF@UiO-66-NH2在干燥状态及水悬浮液中红外照片; (c) GF@UiO-66-NH2存在下不同光照射下DMNP的水解动力学线性拟合曲线. 改编自文献[25]

Figure 26. (a) Proposed reaction mechanism for the hydrolysis of DMNP by GF@UiO-66-NH2; (b) infrared photograph of GF@UiO-66-NH2 in dry state and in its aqueous suspension under the simulated solar light (0.6 W•cm-2); (c) hydrolysis kinetic linear fitting curves of DMNP in the presence of GF@UiO-66-NH2 under different light irradiations. Adapted from the literature [25]

图27. Dpa@UiO-66-NH2 CSNs及其织物用于CWA模拟物光热增强解毒的制作过程示意图. 改编自文献[24]

Figure 27. Schematic illustration of the fabrication procedures for Dpa@UiO-66-NH2 CSNs and their fabrics for photothermally enhanced detoxification of CWA simulants. Adapted from the literature [24]

图28. (a) 照片显示了具有较大面积的独立柔性UiO-66-NH2/PAN纤维毡及其相应的SEM图像; (b) 在不同的光照条件下, 在过滤器测试中使用UiO-66-NH2/PAN, 混合物/PAN和Dpa@UiO-66-NH2/PAN纤维毡, 将DMNP转化为对硝基苯氧化物的百分比. 误差条是三倍读数的标准偏差. 改编自文献[24]

Figure 28. (a) Photographs showing a stand-alone flexible UiO-66-NH2/PAN fibrous mat with a large area and its corresponding SEM image; (b) percentage conversion of DMNP to p-nitrophenoxide using UiO-66-NH2/PAN, mixture/PAN, and Dpa@UiO-66-NH/PAN fibrous mats in the filter test under different light irradiation conditions. Error bars are the standard deviation in triplicate readings. Adapted from the literature [24]

图29. PDA介导的MOF织物的制备步骤: 将PDA涂覆在静电纺丝的PA-6纳米纤维上, 然后进行多巴胺聚合和Zr-MOF UiO-66-NH2在PA-6@PDA纳米纤维上的溶剂热生长. 改编自文献[26]

Figure 29. Steps for the preparation of PDA-mediated MOF fabrics: PDA coating on electrospun PA-6 nanofibers by dopamine polymerization and solvothermal growth of Zr-MOF UiO-66-NH2 on PA-6@PDA nanofibers. Adapted from the literature [26]

图30. (a) Pd NCs@ZIF-8的自组装和等离子体激元驱动的烯烃加氢选择性催化; (b) Pd NCs@ZIF-8和Pd NCs对1-己烯氢化的可回收性; (c) 在Pd NCs@ZIF-8和Pd NCs上各种烯烃的氢化转化. (b)和(c)中的反应条件: 室温下100 mW•cm-2全光谱辐射. 改编自文献[100]

Figure 30. (a) Self-assembly of Pd NCs@ZIF-8 and plasmon-driven selective catalysis of the hydrogenation of olefins; (b) recyclability of Pd NCs@ZIF-8 and Pd NCs for the hydrogenation of 1-hexene; (c) conversions of the hydrogenation of various alkenes over Pd NCs@ZIF-8 and Pd NCs. Reaction conditions in (b) and (c): 100 mW•cm-2 full-spectrum irradiation, room temperature. Adapted from the literature [100]

图31. 在可见光照射下, Pt/PCN-224(M)醇的选择性氧化示意图. 改编自文献[195]

Figure 31. Schematic illustration showing the selective oxidation of alcohols over Pt/PCN-224(M) under visible-light irradiation. Adapted from the literature [195]

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金属有机框架基复合材料的制备及其光热性能研究

Metal-organic Frameworks-based Composites and Their Photothermal Applications

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