臺灣博碩士論文加值系統

本研究利用同步輻射X光還原法(Synchrotron X-rays irradiation method)，成功地以一步驟合成聚苯乙烯微球(PS spheres)、奈米銀修飾聚苯乙烯微球(Ag-PS) 和奈米銀修飾生物活性玻璃(Ag-BG)之奈米複合材料。以苯乙烯、球型/多孔型生物活性玻璃和硝酸銀(AgNO3)為前驅物，並且加入聚乙烯吡咯烷酮（Polyvinylpyrrolidone，PVP）當作表面活性劑，合成複合材料。Ag-PS奈米複合材料的合成機制包含乙醇溶液中的自由基生成，苯乙烯的聚合，以及金屬銀的還原。以調整曝光時間、苯乙烯濃度、表面活性劑量，系統性地檢測聚苯乙烯的大小分佈與分子量。
實驗結果顯示，聚苯乙烯微球具有狹窄的分子量分佈(PDI)、均勻的球狀形貌和對人體細胞的低毒性。在乙醇溶液中合成多晶的奈米銀顆粒得到直徑範圍約4至12 nm的顆粒大小。在Ag-PS奈米複合材料中，調整Ag離子對苯乙烯單體之體積比比例(5/1~10/1)可獲得更多奈米顆粒量修飾於聚苯乙烯微球表面上。由於聚苯乙烯微球擁有負值之界面電位(Zeta potential)，奈米銀顆粒的分佈位置接近或附著於聚苯乙烯微球表面。另外，以噴霧熱解法製備之球型或多孔型生物活性玻璃作為銀修飾複合材料之基板，其生物相容性之特質令其為生醫應用上具潛力之奈米材料。在Ag-BG奈米複合材料中，奈米銀顆粒的分佈和直徑大小與Ag-PS奈米複合材料中的差異不大。
陽離子苄乙基三甲基铵單體經過光聚合形成低毒性的正性TMA-PS微球作為基因傳遞。以Ag-PS奈米複合材料抵抗革蘭氏陰性與革蘭氏陰性陽性之菌體(大腸桿菌和金黃色葡萄糖球)展現極佳的抗菌效果。此外，Ag-BG奈米複合材料只對於大腸桿菌具有抗菌能力。

In this research, polystyrene spheres, silver nanoparticles decorated polystyrene nanocomposites and silver nanoparticles decorated bioactive glass nanocomposites have been successfully synthesized using synchrotron X-rays irradiation method in a one-step process. Styrene monomer, spherical/mesoporous bioactive glass, and silver nitrate were used as precursors. Polyvinylpyrrolidone was included as surfactant for all samples. The proposed mechanism of the formation of the Ag-PS nanocomposite spheres involves the generation of radicals in the aqueous solution to induce PS polymerization and the reduction of Ag. The distribution of the sizes and the molecular weight of the core PS spheres in the Ag-PS nanocomposite spheres were systematically examined as a function of irradiation time, concentration of styrene, and amount of PVP.
Experimental results show that PS spheres exhibited low polydiversity value, uniformly spherical shapes and low cytotoxicity to human cells. Polycrystalline silver nanoparticles were synthesized in aqueous solution with particle size range from 4 to 12 nm in diameter. In Ag-PS nanocomposites, increasing Ag+-to-styrene volume ratios (5/1~10/1) enabled the increase of silver nanoparticles amount decorated around PS spheres. The silver nanoparticles were either close or on the surface of PS spheres due to negative zeta potential values. Furthermore, spherical and mesoporous bioactive glass produced by spray pyrolysis method were selected as templates in silver decorated nanocomposites as potential biocompatible nanomaterials in biomedical applications. The distribution and size of the silver nanoparticles decorated on Ag-BG nanocomposites have little differences compared with the ones in Ag-PS nanocomposites.
The cationic (vinylbenzyl)trimethylammonium (TMA) monomer was photopolymerized to form positively charged TMA-PS spheres as gene carriers with uniquely low cytotoxicity. Ag-PS nanocomposites demonstrated excellent antimicrobial ability when challenged against Gram negative and Gram positive bacteria (Escherichia coli and Staphylococcus aureus). Additionally, Ag-BG nanocomposites exhibited antimicrobial activity only against Escherichia coli.

ACKNOWLEDGEMENTS I
中文摘要 III
ABSTRACT V
CONTENTS VII
List of Tables IX
List of Figures X
Chapter 1 INTRODUCTION 1
Chapter 2 LITERATURE REVIEW 3
2.1 Polystyrene synthesis techniques 3
2.2 Bioactive glass synthesis techniques 8
2.3 Silver nanoparticles reduction techniques 12
2.4 Photoinitiated synthesis by synchrotron X-rays 15
2.5 Biomedical applications for PS spheres, Ag-PS and Ag-bioactive glass 17
Chapter 3 EXPERIMENTAL PROCEDURES 22
3.1 Experimental preparation 22
3.2 Preparation of polystyrene spheres 27
3.3 Preparation of silver-polystyrene nanocomposites 28
3.4 Preparation of silver-bioactive glass nanocomposites 29
3.5 Cell culture 30
3.6 Materials characterization 30
3.6.1 Transmission electron microscopy (TEM) 30
3.6.2 Dynamic light scattering (DLS) and zeta-potential analysis 31
3.6.3 Gel permeation chromatography (GPC) 32
3.6.4 Thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) 32
3.6.5 Cytotoxicity tests 33
3.6.6 Ultraviolet-visible spectroscopy (UV-Vis) 34
3.6.7 Fourier transformed infrared spectroscopy (FT-IR) and nuclear magnetic resonance (NMR) 34
3.6.8 X-ray related analysis - X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD) and selected-area diffraction (SAD) 36
3.7 Transgene delivery test 39
3.8 Antibacterial assay 40
Chapter 4 RESULTS AND DISCUSSIONS 42
4.1 Polystyrene spheres, PS 42
4.1.1 Morphology observation of PS 44
4.1.2 Size identification and molecular weight of PS 46
4.1.3 Thermal analysis of PS 50
4.1.4 Zeta potential and Cytotoxicity of PS 52
4.1.5 Transgene delivery of PS 54
4.2 Silver-polystyrene nanocomposites, Ag-PS 57
4.2.1 Morphology observation of Ag-PS 59
4.2.2 UV-Vis spectroscopy of Ag-PS 65
4.2.3 XAS analysis of Ag-PS 69
4.2.4 Structural investigation of Ag-PS 70
4.2.5 Antibacterial assay of Ag-PS 80
4.3 Silver-bioactive glass nanocomposites, Ag-BG 83
4.3.1 Morphology observation of Ag-BG 83
4.3.2 UV-Vis spectroscopy of Ag-BG 88
4.3.3 Structural investigation of Ag-BG 91
4.3.4 Antibacterial assay of Ag-BG 94
Chapter 5 CONCLUSIONS 97
Chapter 6 FUTURE WORKS 99
REFERENCES 102

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