论文总字数：20989字

摘 要

在药物输送体系中，水滑石和有序介孔硅材料是具有代表性的载体材料，有序介孔硅材料具有低毒性、良好的生物相容性、优良的孔道结构、易于修饰的表面性质和可设计的结构特征等等，这些特征使得其被广泛运用在生物医药领域。核壳复合材料可以同时具有核心与外壳的优良的性质，也可以规避任何一方可能存在的缺点，赋予材料多重的结构的特征与物理化学性质，开拓了药物输送体系的发展领域，使其应用更加具有研究意义。本文以镁铝水滑石为核心，合成水滑石酪氨酸有序介孔有机硅核壳复合材料，主要介绍了酪氨酸有机硅前驱体的合成、水滑石酪氨酸有序介孔有机硅核壳复合材料的构建与表征以及核壳复合材料的性能研究。

本文采用共沉淀法合成了镁铝水滑石核心材料。酪氨酸有机硅前驱体的合成是以酪氨酸为底物，经过酯化反应后与水合肼进行偶联得到酪氨酸甲酰肼，然后与3-异氰酸酯基丙基三乙氧基硅烷反应得到酪氨酸有机硅前驱体，经表征确定结构与目标分子一致。核壳复合材料是利用软模板法，在模板剂的作用下，核壳质量比为1:1.7合成水滑石酪氨酸有序介孔有机硅核壳材料（LDH@Tyr-PMO）。通过红外、XRD和BET的表征方式确定了酪氨酸分子被引进了核壳材料，且确定了存在水滑石，验证了核壳复合材料的合成。以依诺沙星为药物模型研究LDH@Tyr-PMO的药物释放性能研究，12 h的吸附量为0.0412 mg/g，而12 h的释放量为33.39 %，呈现缓慢释放的现象。

水滑石有序介孔硅核壳复合材料可以被应用在了药物输送领域之中，存在诸多的优势，而且可以被应用在吸附等相关领域之中，这为核壳复合材料的诸多应用打下了基础，本文合成了LDH@Tyr-PMO，为有序介孔有机硅应用在不同核心结构的复合材料中奠定了基础。

关键词：水滑石 有序介孔有机硅 核壳复合材料 药物输送

Abstract

In drug delivery system, hydrotalcite and ordered mesoporous silica materials is representative of the carrier materials, ordered mesoporous silica materials with low toxicity and good biological compatibility, excellent open-framework structure, easy to modify the surface properties of porous and can design the structure characteristics and so on, these characteristics make it widely used in biomedical field. Core-shell composite materials can have the excellent properties of both the core and the shell at the same time, and can also avoid the possible shortcomings of either side, endowing the material with the characteristics of multiple structures and physical and chemical properties, thus opening up the development field of drug delivery system and making its application more meaningful. In this paper, the synthesis of hydrotalcite tyrosine ordered mesoporous organosiloxane core-shell composite materials was carried out with magnesium aluminum hydrotalcite as the core. The synthesis of the precursor, the construction and characterization of the hydrotalcite tyrosine ordered mesoporous organosiloxane core-shell composite materials and the properties of the core-shell composite materials were introduced.

The core material of magnesium-aluminum hydrotalcite was synthesized by coprecipitation method. The synthesis of tyrosine organosilicone precursor was based on tyrosine as the substrate. After the esterification reaction, it was coupled with hydrazine hydrate to get tyrosine formyl hydrazine, and then reacted with 3-isocyanate propyl triethoxysilane to get tyrosine organosilicone precursor. The structure was consistent with the target molecule after characterization. Core-shell composite material was synthesized by the method of soft template. Under the action of template agent, the core-shell mass ratio was 1:1.7 to synthesize hydrocite tyrosine ordered mesoporous organosiloxane core-shell material (LDH@Tyr-PMO). Through the characterization methods of FTIR, XRD and BET, it was confirmed that tyrosine molecules were introduced into the core-shell material, and the existence of hydrotalcite was confirmed, which verified the synthesis of the core-shell composite material. The drug release performance of LDH@Tyr-PMO was studied with enoxacin as the drug model. The adsorption capacity of 12 h was 0.0412 mg/g, while the release capacity of 12 h was 33.39 %, showing a phenomenon of slow release.

Hydrotalcite ordered mesoporous silica core-shell composite material can be applied in the field of drug delivery, has many advantages, but also can be applied in the related fields of adsorption, etc, for the core-shell composite laid the foundation of application, this paper synthesized LDH@Tyr-PMO, as ordered mesoporous silicon application in different core structure of composite material laid a foundation.

Keywords: layered double hydroxide；ordered mesoporous material；core-shell composite；drug deliver

目 录

摘要 I

ABSTRACT II

第一章 绪论 1

1.1水滑石的简介及应用 1

1.2有序介孔有机硅材料简介及应用 2

1.3水滑石有序介孔硅核壳复合材料 3

1.3.1核壳复合材料的合成方法 4

1.3.2核壳复合材料的应用 4

1.4本课题意义与目的 5

第二章 实验部分 6

2.1实验试剂及仪器 6

2.2水滑石的合成 7

2.3酪氨酸有机硅前驱体的合成 7

2.3.1酪氨酸甲酯盐酸盐的合成 7

2.3.2酪氨酸甲酯的合成 8

2.3.3酪氨酸甲酯与水合肼的偶联 8

2.3.4酪氨酸双桥联有机硅前驱体的合成 8

2.4水滑石有序介孔有机硅核壳材料（LDH@Tyr-PMO）的合成 9

2.5 LDH@Tyr-PMO材料对依诺沙星的吸附 9

2.6 有序介孔有机硅材料的表征方式 10

第三章 结果与讨论 11

3.1酪氨酸有机硅前驱体表征 11

3.1.1核磁氢谱表征结果 11

3.1.2红外表征结果 11

3.1.3质谱表征结果 11

3.2水滑石有序介孔有机硅核壳材料表征 11

3.2.1水滑石有序介孔有机硅核壳材料的红外光谱表征 11

3.2.2水滑石有序介孔有机硅核壳材料的XRD分析 12

3.2.3水滑石有序介孔有机硅核壳材料的比表面积分析 13

3.3 LDH@Tyr-PMO对依诺沙星的性能研究 14

3.3.1依诺沙星的标准曲线 14

3.3.2不同pH值条件下LDH@Tyr-PMO对依诺沙星的吸附 15

3.3.3 LDH@Tyr-PMO材料对依诺沙星的释放 16

第四章 结论与展望 18

4.1实验结论 18

4.2展望 18

参考文献 20

附录 23

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