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化学进展 2022, Vol. 34 Issue (3): 696-716 DOI: 10.7536/PC210345 前一篇   后一篇

• 综述 •

介孔二氧化硅基智能递送体系的构建及其在各类疾病治疗中的应用

钟琴1, 周帅1,*(), 王翔美1, 仲维1, 丁晨迪2, 傅佳骏1,*()   

  1. 1 南京理工大学化工学院 南京 210094
    2 茂名市人民医院临床科研中心 茂名 525000
  • 收稿日期:2021-03-29 修回日期:2021-05-26 出版日期:2021-07-29 发布日期:2021-07-29
  • 通讯作者: 周帅, 傅佳骏
  • 基金资助:
    国家自然科学基金面上项目(52072177); 中央高校基本科研业务费(30918012201); 中央高校基本科研业务费(30919011405)
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Construction of Mesoporous Silica Based Smart Delivery System and its Therapeutic Application in Various Diseases

Qin Zhong1, Shuai Zhou1(), Xiangmei Wang1, Wei Zhong1, Chendi Ding2, Jiajun Fu1()   

  1. 1 School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
    2 Clinical Research Center of Maoming People's Hospital, Maoming 525000, China
  • Received:2021-03-29 Revised:2021-05-26 Online:2021-07-29 Published:2021-07-29
  • Contact: Shuai Zhou, Jiajun Fu
  • Supported by:
    National Natural Science Foundation of China(52072177); Fundamental Research Funds for the Central Universities(30918012201); Fundamental Research Funds for the Central Universities(30919011405)

利用先进纳米技术开发的药物递送体系能够改善药物的理化性质和治疗效果,同时削弱其毒副作用,因而纳米药物递送体系成为现代药剂学研究的热点和主流方向。其中,介孔二氧化硅作为纳米载体的基质材料具有比表面积大、形貌结构可调、表面易于修饰及生物相容性良好等优点,引发生物医学研究人员的广泛关注,为构筑新型智能药物递送体系提供了新的设计思路。本文就介孔二氧化硅基智能递送体系在设计构筑和疾病治疗应用等方面的最新研究进展进行了综述。首先,本文对介孔硅的发展历程、制备方法及结构特性进行了简要概述;其次,从药物装载和门控释放两大角度系统阐述了近些年介孔硅基智能递送体系的构建策略,重点介绍了各种刺激响应性介孔硅基递送体系的门控开关(如聚合物、无机纳米颗粒、超分子组装体及生物大分子等)及其可控释放机制;随后,详细描述了介孔硅基控释体系在各种类型疾病(包括癌症、细菌感染、糖尿病和阿尔茨海默病等)治疗中的应用进展;最后,总结和分析了介孔硅基智能纳米载体研究中存在的问题并对其未来发展作了展望。

关键词： 介孔二氧化硅纳米颗粒, 刺激响应, 靶向递送, 药物装载, 可控释放, 疾病治疗

The drug delivery systems (DDSs) developed with advanced nanotechnologies can improve the physicochemical properties and therapeutic effects of drugs, while weakening their side effects. Therefore, nanoscale DDSs have become a hot spot and mainstream direction of current pharmacy research. Among them, mesoporous silica nanoparticles (MSNs) have the advantages of large specific surface area, adjustable morphology/structure, easy surface modification and good biocompatibility, thereby have attracted extensive attention of biomedical researchers and provided new design ideas for constructing new smart DDSs. In this paper, the latest research progress of MSNs-based smart delivery systems in construction and disease treatment applications is reviewed. Firstly, the development process, preparation methods and structural characteristics of MSNs are briefly summarized. Secondly, the construction strategies of MSNs-based smart delivery systems in recent years were systematically expounded from the perspectives of drug loading and gate-controlled release. The gatekeepers (such as polymers, inorganic nanoparticles, supramolecular assemblies and biomacromolecules, etc.) and controlled release mechanisms of various stimuli-responsive MSNs-based delivery systems were emphatically introduced. Afterwards, the applications of MSNs-based controlled release system in the treatment of various diseases (including cancer, bacterial infection, diabetes and Alzheimer's disease, etc.) was described in detail. Finally, the challenges in the investigations of MSNs-based smart nanocarriers are summarized, and the prospects of their future development are presented.

Contents

1 Introduction

2 Overview of mesoporous silica nanoparticles

3 Construction strategy of MSNs-based smart delivery systems

3.1 Drug loading strategies

3.2 Gated release strategies

4 Applications of MSNs-based smart delivery systems in disease treatment

4.1 Anticancer application of MSNs-based smart delivery systems

4.2 Antibacterial application of MSNs-based smart delivery systems

4.3 Application of MSNs-based smart delivery systems in diabetes treatment

4.4 Application of MSNs-based smart delivery systems in the treatment of other diseases

5 Conclusion and outlook

Key words: mesoporous silica nanoparticles, stimuli-responsiveness, targeted delivery, drug loading, controlled release, disease treatment
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表1 常见介孔二氧化硅材料的特性汇总
Table 1 A summary of characteristic properties of various mesoporous silica materials
MSNs Surface area (m2/g) Pore volume (cm3/g) Pore diameter (nm) Structure Application ref
MCM-41 610~1157 0.30~0.98 2~10 2D hexagonal,p6mm drug delivery or catalyze 37
MCM-48 604~1480 0.41~0.94 2~10 3D cubic, Ia3d drug delivery and tumor therapy 38
MCM-50 / / / lamellar, p2 / 39
SBA-1 606~1221 0.28~0.67 2~3 3D cubic, Pm3n tumor therapy 40
SBA-2 120~350 0.15~0.60 2~3 3D hexagonal, P63/mmc adsorption 41
SBA-8 944~1022 0.30~0.90 2~3 2D square, c2mm adsorption 42
SBA-11 620~815 0.20~0.86 2~3 3D cubic, Pm3n adsorption or catalyze 43
SBA-15 400~900 0.42~1.08 5~30 2D hexagonal, p6mm tumor therapy or catalyze 44
SBA-16 370~810 0.21~0.72 5~30 3D cubic, Im3m tumor therapy or adsorption 45
AMS 501~963 0.22~0.79 1.3~6.2 3D hexagonal or 2D hexagonal or 3D cubic heterogeneous solid base catalysts 46
IBN 575~821 0.54~0.88 5.3~19.5 3D cubic or 2D hexagonal catalysis and gas adsorption 47
KIT 506~889 0.90~1.36 5.0~9.8 3D cubic or 2D hexagonal adsorption 48
图1 介孔硅的药物装载策略示意图
Fig.1 Schematic of drug loading strategies of MSNs
表2 2019—2021年国内研究人员在介孔二氧化硅基递送体系的构建与应用方面的工作
Table 2 A summary of domestic researchers' works on the construction and application of MSNs-based delivery systems during 2019—2021
Silica frameworks Gatekeepers Stimuli Payloads Treatment model Applications Year ref
MSNs Charge-reversal polymers with acid-labile hydrazone linker pH DOX HepG2 cells Cancer chemotherapy 2019 58
MSNs Succinylated casein Intestinal protease T7E21R-HD5 MDR E. coli Combating intestinal
bacterial infection		 2019 59
MSNs Hyaluronic acid HAase DOX MGC-803 cells Cancer chemotherapy 2019 60
MSNs Poly (L-lysine) &
Hyaluronic acid		 pH GOx, PTX Sub-q
HepG2 cells		 Synergistic cancer starvation-
chemistry therapy		 2019 61
HMSNs Macrocycle-capped CuS Temperature, pH, Competitive binding, light DOX Sub-q
Hela cells		 Synergistic chemo-
photothermal therapy		 2020 62
HMSNs β-cyclodextrin throughdisulfide bond & adamantine-citraconic anhydride-functionalized poly-
l-lysine		 pH, GSH DOX Sub-q
4T1 cells		 Cancer chemotherapy 2020 63
Dendritic large pore MSNs Leukocyte/platelet hybrid membrane NIR laser DOX, IR780 Sub-q
4T1 cells		 Combination of PTT/PDT
and chemotherapy		 2021 64
MSNs Polydopamine manganese
oxide coating		 GSH DOX MCF-7 cells Cancer chemotherapy 2021 65
MSNs Tannic acid/Fe3+ complex pH DOX Sub-q
4T1 cells		 Combined chemo-
photothermal therapy		 2021 66
Dendritic MSNs Thiol-modified poly(methacrylic acid) GSH PTX Sub-q
A549 cells		 Cancer chemotherapy 2021 67
图2 温敏性PNIPAM-PBAPAE分子刷门控的介孔硅纳米载体及其ROS响应释放机制[69]
Fig.2 Thermosensitive PNIPAM-PBAPAE brush-gated MSNs-based nanocarriers and their ROS-responsive release mechanism[69]
图3 利用缩醛键将AuNPs偶联在介孔硅表面以构筑酸响应型控释体系[77]
Fig.3 Conjugation of AuNPs onto MSNs surfacce by acetal bond for constructing acid-responsive controlled release systems[77]
图4 α-CD/偶氮苯超分子组装体门控的介孔硅纳米载体的构建及UV、酸双重响应释放示意图[90]
Fig.4 Construction of supramolecular assembly (α-CD and azobenzene) gated MSNs-based nanocarriers and their UV/acid dual-responsive cargo release[90]
图5 双链DNA分子门控的介孔硅纳米载体的构建及交变磁场响应示意图[95]
Fig.5 Construction and alternating field responsiveness of double-stranded DNA gated MSNs-based nanocarriers[95]
图6 DOX分子自门控介孔硅纳米载体的构建及其酸响应释放行为[100]
Fig.6 DOX self-gated MSNs-based nanocarriers and their acid- triggered DOX release behavior[100]
图7 (A)FMSNs-DOX超疏水表面蓄积INBs并在超声刺激下诱导气泡空化、ROS生成及药物释放示意图;(B)INBs空化过程中的高速图像和可视化气泡的平均尺寸;(C)使用FMSNs-DOX处理后癌细胞的存活率[109]
Fig.7 (A) Schematic illustrating the superhydrophobic surface of FMSNs-DOX accumulating INBs to induce bubble cavitation, ROS generation, and drug release during US stimulation; (B) High-speed images and the mean size of visualized bubbles during INBs cavitation; (C) Cell viability after treatment with FMSNs-DOX[109]
图8 (A)Amp-MSN@FA@CaP@FA的合成路线及其体内外抑制菌示意图;(B)使用Amp-MSN@FA@CaP@FA和单独Amp处理大肠杆菌和金黄色葡萄球菌后LB-琼脂平板照片;使用Amp-MSN@FA@CaP@FA和单独Amp处理后大肠杆菌(C)和金黄色葡萄球菌(D)的细胞活力[123]
Fig.8 (A) Schematic of the synthesis of Amp-MSN@FA@CaP@FA, the behavior of Amp release in acidic conditions, and inhibition of the drug-resistant bacteria in vitro and in vivo; (B) Viable bacteria remaining in the LB-agar plates of E. coli and S. aureus after being treated with Amp-MSN@FA@CaP@FA and single Amp; Bacterial cell viability of E. coli (C) and S. aureus (D) after treatment with Amp-MSN@FA@CaP@FA and single Amp[123]
图9 (A)SA/CPBA-MSN/INS的制备及其葡萄糖响应控释示意图;药代动力学和药效学评价:(B)不同处理组小鼠的葡萄糖水平-时间曲线;(C)不同处理组糖尿病小鼠的药物浓度-时间曲线;(D)SA/CPBA-MSN/INS,Novolin 30R和Novolin R对葡萄糖水平的影响;(E)治疗4周后不同处理组小鼠的体重[130]
Fig.9 (A) Schematic illustration of the preparation and glucose-responsive controlled release of SA/CPBA-MSN/INS nanoparticles. Pharmacokinetics and pharmacodynamics study: (B) Glucose level-time curves of mice in different groups; (C) drug concentration-time curves of diabetic mice in different groups; (D) effect of SA/CPBA-MSN/INS, Novolin 30R, and Novolin R on glucose level; (E) weight of mice after 4 weeks of treatment[130]
图10 多功能介孔硅递送体系的结构示意图:当注入斑马鱼心衰模型中时,斑马鱼心脏内的ROS促使FL2荧光功能开启,触发卡托普利的释放[138]
Fig.10 Schematic illustration of various components of functional MSNs. When injected into the zebrafish model experiencing heart failure, the ROS within the heart of the zebrafish causes the sensor probe to achieve a “turn-on” fluorescence with a subsequent release of heart failure therapeutic drug, captopril, from functional MSNs[138]
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