磺甜菜鹼氮矽三環雙離子自組裝抗污塗層

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姓名

鄭雅云(Ya-Yun Zheng) 查詢紙本館藏

畢業系所

生物醫學工程研究所

論文名稱

磺甜菜鹼氮矽三環雙離子自組裝抗污塗層
(Silatrane-Based Zwitterionic Self-Assembled Coating for Antifouling Properties)

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摘要(中)

植入性醫療器材因長時間與血液及組織接觸，易引發生物分子的非特異性吸附，引發血栓、凝血反應、細菌感染等問題。目前解決之方法為，於材料表面修飾一層抗非特異性吸附之塗層。矽烷 (silane) 官能基常用於修飾氧化矽之自組裝塗層鍵結，然而矽烷易被水解，使得接枝官能基失活，因此增加保存以及修飾上的困難。而氮矽三環 (silatrane) 為以氮矽鍵為軸組成的三環籠狀對稱結構，已被證實於結構上較矽烷穩定。本研究以帶有氧矽三環的磺甜菜鹼兩性雙離子（sulfobetainesilatrane, SBSiT）於氧化矽材料上修飾自組裝抗汙塗層。將以 (1) 核磁共振光譜儀及傅里葉轉換紅外光譜驗證分子結構和水解速度；(2) MTT細胞毒性測試材料生物相容性；(3) 水接觸角測量儀觀察修飾後表面之親水性質；(4) X射線光電子能譜分析表面元素成分；(5)原子力顯微鏡觀察修飾表面粗糙度；(6) 橢圓儀測試表面厚度；(7) 細菌貼附、蛋白質貼附實驗證明此材料具抗非特異性吸附之特性。SBSiT材料不僅突破矽烷官能基容易水解，所造成表面聚集、不均勻之問題，更保有兩性雙離子良好抗非特異性吸附之特性，乃極具潛力之兩性雙離子抗汙塗層，是為生物醫學工程領域上的重大發展。

摘要(英)

Zwitterionic coatings are a new class of antifouling materials for high biocompatibility. Development of the antifouling film has been of great interest over the last decades, particularly for silicon surface modification due to their potential biomedical applications. The most commonly used chemical functionalization of silicon surface is silane. However, silane is very sensitive to moisture which leads to polymerization on the silicon surface. Therefore, silatranes have received attention from the structures features. Because of a strong intramolecular donor-acceptor interaction between nitrogen and silicon atom, silatrane are chemically more stable to hydrolysis than silane. Thus, the formation of large polymer clusters and roughness on silica surface is minimized. In this study, we have developed a superhydrophilic zwitterionic surface by sulfobetaine silatrane ( SBSiT ) coating as an alternative to sulfobetaine silane ( SBSi ) coating. The performance of sulfobetaine silatrane was less sensitive to moisture and more difficult to hydrolyze. SBSiT films offer a significant advantage over SBSi due to its smooth, aggregate free, film formation and also solve homogeneity and reproducibility problems caused by silane. SBSiT suggests its potential role in anti-fouling coatings on silica surface and benefits the development of devices and sonsors based on biomedical applications.

關鍵字(中)

★ 抗非特異性吸附
★ 兩性雙離子材料
★ 自組裝材料
★ 生物界面
★ 氮矽三環材料

關鍵字(英)

★ Antifouling properties
★ zwitterionic material
★ silatrane
★ biointerfaces
★ self-assembly

論文目次

中文摘要------------------------------------------------------------------------------------------V
Abstract-------------------------------------------------------------------------------------------VI
致謝----------------------------------------------------------------------------------------------VII
目錄---------------------------------------------------------------------------------------------VIII
圖目錄-------------------------------------------------------------------------------------------XI
表目錄------------------------------------------------------------------------------------------XIII
第一章文獻回顧-------------------------------------------------------------------------------01
1-1生物汙染-------------------------------------------------------------------------------------01
1-1-1 生物膜的形成------------------------------------------------------------------02
1-1-2 抵抗生物汙染之機制---------------------------------------------------------03
1-2 抗生物沾黏材料--------------------------------------------------------------------------05
1-2-1 聚乙二醇材料------------------------------------------------------------------06
1-2-2 兩性雙離子材料---------------------------------------------------------------08
1-2-2-1 兩性雙離子材料抗非特異性吸附機制----------------------------10
1-3 自組裝抗汙塗層---------------------------------------------------------------------------11
1-4 矽烷官能基---------------------------------------------------------------------------------12
1-4-1矽烷官能基修飾原理----------------------------------------------------------13
1-4-2矽烷官能基修飾衍生之問題------------------------------------------------15
1-5氮矽三環類化合物------------------------------------------------------------------------18
1-5-1氮矽三環類化合物修飾機制-------------------------------------------------19
1-5-2氮矽三環類化合物修飾優勢-------------------------------------------------21
第二章、研究目的-----------------------------------------------------------------------------23
第三章、材料與方法--------------------------------------------------------------------------24
3-1實驗藥品-------------------------------------------------------------------------------------24
3-2實驗儀器-------------------------------------------------------------------------------------25
3-3材料合成-------------------------------------------------------------------------------------26
3-3-1磺甜菜鹼氮矽三環兩性雙離子 (SBSiT) ----------------------------------26
3-3-2帶矽烷官能基磺甜菜鹼兩性雙離子 (SBSi) ------------------------------27
3-3-3無水乙醇製備-------------------------------------------------------------------27
3-4實驗方法-------------------------------------------------------------------------------------28
3-4-1 SBSi、SBSiT自組裝抗汙塗層製備----------------------------------------28
3-4-2 接觸角測量---------------------------------------------------------------------29
3-4-3 橢圓偏振儀厚度量測---------------------------------------------------------29
3-4-4 高解析電子能譜儀 (XPS) --------------------------------------------------29
3-4-5 傅立葉轉換紅外光譜 (FTIR) ----------------------------------------------30
3-4-6 SBSi、SBSiT對於酸鹼值不同的UV-VIS吸收光譜分析------------30
3-4-7 SBSi、SBSiT對於酸鹼值不同的粒徑分析 (DLS) ---------------------30
3-4-8 SBSi、SBSiT與不同酸鹼值的粗糙度分析 (AFM) --------------------31
3-4-9 細菌貼附實驗------------------------------------------------------------------31
3-4-10 石英晶體微天平對牛血清蛋白吸附試驗 (QCM-D) -----------------32
3-4-10 毒性試驗 (MTT) ------------------------------------------------------------32
第四章、結果與討論------------------------------------------------------------------33
4-1 SBSi以及SBSiT材料分析-------------------------------------------------------------33
4-1-1 磺甜菜鹼氮矽三環兩性雙離子 (SBSiT) 之NMR頻譜分析--------33
4-1-2 利用 NMR頻譜分析比較SBSi以及SBSiT水解速度---------------34
4-1-3 利用FTIR分析比較SBSi以及SBSiT水解----------------------------36
4-1-4 SBSi以及SBSiT材料之保存性-------------------------------------------37
4-1-5 SBSi以及SBSiT材料之生物相容性 (MTT) --------------------------38
4-2 SBSi以及SBSiT表面修飾--------------------------------------------------------------39
4-2-1 SBSiT自組裝抗汙塗層對於不同修飾方法以及溶劑之選擇--------39
4-2-2 SBSiT 自組裝抗汙塗層對於不同修飾時間之水接觸角-------------41
4-2-3 SBSiT 自組裝抗汙塗層表面元素分析 (XPS) ------------------------43
4-2-4 SBSiT 自組裝抗汙塗層粗糙度測試 (AFM) --------------------------46
4-2-5 SBSiT 自組裝抗汙塗層厚度測試 (Ellipsometry) --------------------48
4-2-6 SBSiT 自組裝抗汙塗層之抗細菌貼附----------------------------------49
4-2-7 SBSiT 自組裝抗汙塗層之抗蛋白質貼附 (QCM-D) -----------------51
第五章、討論-------------------------------------------------------------------------------------52
5-1 SBSiT於酸性條件之水解開環--------------------------------------------------------52
5-2 SBSiT表面修飾機制--------------------------------------------------------------------53
5-3 SBSi以及SBSiT之溶膠凝膠化 (Sol-gel) ------------------------------------------55
第六章、結論------------------------------------------------------------------------------------58
第七章、未來展望-------------------------------------------------------------------------------59
第八章、參考文獻------------------------------------------------------------------------------60

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指導教授

黃俊仁(Chun-Jen Huang)

審核日期

2017-6-26

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