在矽樹脂上建構磺甜菜鹼雙離子自組裝薄膜 以提升其生物相容性

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姓名

葉修邦(Shiou-bang Yeh) 查詢紙本館藏

畢業系所

生物醫學工程研究所

論文名稱

在矽樹脂上建構磺甜菜鹼雙離子自組裝薄膜以提升其生物相容性
(Sulfobetainesilane Modified Silicone Elastomers for Durable Enhanced Biocompatibility)

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摘要(中)

醫療器材表面的蛋白質及微生物的非特異性吸附容易引發諸如凝血反應、微生物感染以及組織鈣化等生物自發性的各項負面效應。過去研究證明表面電中性的親水性修飾能有效降低非特異性吸附。然而在矽利康（silicone）材料方面，由於其本身的高度疏水再生性質（hydrophobic regeneration），造成難以在材料表面上進行穩定的親水性修飾。本研究以帶有矽烷官能基的磺甜菜鹼兩性離子分子（sulfobetainesilane, SBSi）在聚二甲基矽烷（polydimethylsiloxane, PDMS）矽利康材料進行自組裝單層膜（self-assembled monolayers, SAMs）修飾，已獲得親水性表面修飾的矽利康基材並進一步證明能抵抗非特異性吸附。以X光光電子能譜儀（X-ray photoelectron spectroscopy, XPS）分析表面原素成分。以接觸角側角儀（contact angle goniometer）判斷親水材料修飾的效果以及隨著時間在空氣中保存的材料表面親水修飾之穩定性。修飾後的矽利康基材對於表皮葡萄球菌（Staphylococcus epidermidis）和綠膿桿菌（Pseudomonas aeruginosa）有顯著的抗細菌吸附效果。抵抗蛋白質貼附的方面本研究也成功測試了修飾後的矽利康基材對於牛血清白蛋白（bovine-serum-albumin, BSA），黏蛋白（mucin）以及溶菌.（lysozyme）有良好的抵抗效果。以包覆磺酸羅丹明B （Sulforhodamine B，SRB）的微酯體證明抵抗酯質貼附能力。並成功使磺甜菜鹼兩性離子分子修飾後的矽利康水膠軟式隱形眼鏡（silicone hydrogel soft contact lens）抵抗綠膿桿菌之黏附。利用本研究的成果，可以將矽利康在醫療照護上更安全且更有效發揮其功能。最後，我們利用SBSi超親水的特性，使表面具有抗霧、自潔的功能，並成功製備油水分離系統，以快速回收純水。

摘要(英)

Biofouling on biomaterials causes adverse consequences to health, such as thrombosis, infection, and pathogenic calcification. Hydrophilic and charge-balanced surface is proved to resist the nonspecific absorption. Unfortunately, the state-of-art technology for silicone modification cannot provide a stable and effective coating for the long-term applications under complex conditions. In this study, we aim to modify the silicone surfaces with a zwitterionic surface ligand to resist nonspecific adsorption of protein and bacteria. We synthesized a silanized surface ligand conjugated with a head residue of zwitterionic sulfobetaine (SBSi) that bears positively charged quaternary amine and negatively charged sulfonate. Surface elemental composition was confirmed by X-ray photoelectron spectroscopy (XPS) and the stability of hydrophilicity modification was tested by contact angle goniometer. The tests for adsorption of bacteria, protein, and liposome revealed the excellent antifouling properties of modified silicones. For the real-world application, we modified commercially available silicone hydrogel contact lenses with developed zwitterionic ligands and showed their capability of anti-bacterial adhesion. The strategy of surface engineering in this work can be applied to other silicone-based medical devices in facile and effective fashion. Moreover, we employed the super hydrophilicity of SBSi for preparing anti-fogging, self-cleaning surfaces. We accomplished a water-oil separation system for effective recovery of fresh water.

關鍵字(中)

★ 生物相容性
★ 矽樹脂
★ 磺甜菜鹼
★ 雙離子
★ 自組裝

關鍵字(英)

★ Biocompatibility
★ Anti-fouling
★ Sulfobetaine
★ Zwitterionic
★ Self-assembling

論文目次

摘要 i
Abstract iii
ACKNOWLEDGEMENTS v
TABLE OF CONTENTS vi
LIST OF FIGURES x
LIST OF TABLES xiv
CHAPTER 1. Introduction 1
1.1. Biomolecule Adsorption on Surface 1
1.2. Biofouling at Medical Devices 2
1.3. Development of Nonfouling Materials 4
1.4. Medical Applications of Silicones 5
1.5. Poly(dimethylsiloxane) (PDMS) Silicone Elastomer 6
1.6. Silicone Hydrogel Soft Contact Lenses 7
1.7. Surface Modification of silicones 8
1.8. Approach of “Grafting-onto” to Graft Polymers on Surface 9
1.9. Surface Modification by Silanization 10
CHAPTER 2. Research Objectives 12
CHAPTER 3. Materials and Methods 14
3.1. Materials 14
3.2. SBSi Synthesis 14
3.3. PDMS Preparation and SBSi Modification. 15
3.4. Surface Elemental Composition Analysis by X-ray Photoelectron Spectroscopy (XPS) 16
3.5. Surface Wettability and Water Contact Angle Measurement 18
3.6. Observation and Analysis of Bacterial adhesion 19
3.7. Protein Fouling Evaluation by Enzyme-Linked Immunosorbent Assay (ELISA) 20
3.8. Observation of SRB-Encapsulated Liposome Adsorption Using Microarray Scanner 21
3.9. Cytotoxicity of SBSi Tested by MTT Assay 22
3.10. Oil-Water Separation with SBSi Modified 304 Stainless Steel Mesh 22
CHAPTER 4. Results 24
4.1. NMR Spectrum Analysis of SBSi Molecules 24
4.2. Surface Hydrophobicity Regeneration of Oxygen Plasma Treated PDMS Induced by Mechanical Bending 25
4.3. Effect of Working Solvents on PDMS Silanization 25
4.4. Surface Elemental Composition Analysis of SBSi Modified PDMS 26
4.5. Surface Wettability of Oxygen Plasma Treated/SBSi Modified PDMS 28
4.6. Resistance of SBSi Modified PDMS against P. aeruginosa and S. epidermidis Adhesion 29
4.7. BSA, Mucin and Lysozyme Fouling Resistibility 32
4.8. Resistance of SBSi Modified PDMS against Liposome Adsorption 33
4.9. SBSi Modified Silicone Hydrogel Soft Contact Lenses Resist P. aeruginosa Adhesion 34
4.10. The Cytotoxicity of SBSi to NIH-3T3 Cells 35
4.11. Anti-Fogging and Self-Cleaning Properties of SBSi Modified Silica 36
4.12Oil-Water Separation by SBSi Modified 304 Stainless Steel Meshes 37
CHAPTER 5. Discussion 39
5.1. PDMS Surface Modification with SBSi 39
5.2. Biocompatibility of SBSi Modified PDMS 42
5.3. The Other Applications beyond Antifouling properties 46
CHAPTER 6. Conclusion 50
CHAPTER 7. Suggestions for Future Work 51
7.1. Storage Condition of PDMS-SBSi for Long-term Stability 51
7.2. Biofilm Formation on PDMS-SBSi 52
7.3. Screening of the Most Adhesive Human Microbiome to SBSi Modified Materials 52
7.4. Hemocompatibility of SBSi Modified Surfaces 53
7.5. Improvement of Oil-water Separation Device 53
Bibliography 54

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指導教授

黃俊仁(Chun-jen Huang)

審核日期

2014-7-25

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