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標題: 側鏈樹枝狀高分子經自組裝製備液胞及其應用
Preparation and Aplications of Vesicles via Self-assembly of Dendritic Side-Chain Polymers
作者: 林茂雄
Lin, Mao-Syong
關鍵字: random copolymer;雜亂共聚物;dendron;self-assembly;vesicles;樹枝狀高分子;自我組裝;液胞
出版社: 化學工程學系所
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本研究以Dendritic side-chain polymer製備出高分子液胞。研究包括了高分子主鏈之合成、Dendron之合成、Dendron接枝於高分子主鏈上、製備高分子液胞,分別討論如下:

(1) 高分子主鏈之合成
以活性聚合法與化學改質,製備雜亂共聚物(Random copolymer),同時得到具較窄分子量分佈之高分子。

(2) Dendron之合成
設計一兼具親疏水性之長烷鏈Waxy type dendron,並以收斂式合成出不同代數的Dendron。

(3) Dendritic side-chain polymer之合成
高分子主鏈在化學改質過程中,採用一步法將[G-1.5]-C18與[G-2.5]-C18接枝於含一級胺官能基的高分子主鏈,得到含不同代數之Dendritic side-chain polymers。

(4) 高分子液胞之製備
利用Double-emulsion程序,將Dendritic side-chain polymer溶液製備出高分子液胞。

(5) 乙醇對製備高分子液胞之影響


A random copolymer, polystyrene-co-poly(vinyl benzyl amine) (r-PS-PVBAm) was synthesized by modifying polystyrene-co-poly (vinyl benzyl chloride)(r-PS-PVBC) via an unique synthetic route.

A dual functional building block, 4-isocyanato-4'(3,3-dimethyl- 2,4-dioxo-azetidino)diphenylmethane (IDD) was selected to prepare waxy type dendrons via a convergent route. The waxy type dendrons of relatively higher generation accompanied with more urea/malonamide linkages at the focal segment, and peripheral alkyl chains would enhance the hydrogen bonding interaction and van der Waals force, respectively.

These waxy type dendrons were grafted onto the amine-containing polystyrene. For the random copolymer with Generation 1.5 dendrons, the polymer vesicles could be easily prepared through self-assembly (pH 5.0) by a double-emulsion process. For the random copolymer with Generation 2.5 dendrons, the multi-emulsions could be easily prepared in the basic conditions. After the emulsion process, these two copolymers exhibited hollow vesticles and multi-vesicles, respectively. This was observed by Laser Scanning Confocal Microscopy (LSCM) after encapsulating hydrophobic fluorescent material into the vesicular walls.

The formation of muti-emulsion was destroyed under pH 7.0 due to the addition of ethanol. The aqueous compartments within multi- emulsion exhibited a strong permeability on the structure formation. However, it was not observed in the range from pH 6.0 to pH 5.0.

The self-assembly behavior of dendritic side-chain polymers was investigated by further addition of ethanol. In these systems, these dendritic side-chain polymers could self-assemble to form spherical vesicles in the presence of different amounts of ethanol. As the amount of ethanol increased from 0 to 5 mL in the first-stage double emulsion, the wall thickness of vesicles increased after double emulsion. According to the fluorescence spectroscopy, the ratio of the intensity of the signal at 384 nm to that at 373.5 nm (I384/I373.5) was equal to 1.01 via encapsulating the fluorescent material of pyrene into the vesicular walls. This indicates that the bilayer of polymeric vesicles was more hydrophobic than H2O (I384/I373.5= 0.55).

Based on the above, the constitution of the vesicle structure was definitely observed. The potential incorporation of a wide range of drugs into the vesicle walls or the center of the vesicle cores will be pursued in the future.
其他識別: U0005-1708200916060300
Appears in Collections:化學工程學系所

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