| 研究生: |
李蓉 Lee, Jung |
|---|---|
| 論文名稱: |
DNA與離子對雙親分子/雙鏈陽離子型界面活性劑形成之Langmuir單分子層及液胞的交互作用 Interaction of DNA with Langmuir monolayers and vesicles composed of ion pair amphiphile/double-chained cationic surfactant |
| 指導教授: |
張鑑祥
Chang, Chien-Hsiang |
| 學位類別: |
博士 Doctor |
| 系所名稱: |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年: | 2014 |
| 畢業學年度: | 102 |
| 語文別: | 中文 |
| 論文頁數: | 138 |
| 中文關鍵詞: | 陰陽離子液胞 、去氧核醣核酸 、離子對雙親分子 、Langmuir單分子層 、液胞雙層膜 |
| 外文關鍵詞: | catanionic vesicle, DNA, ion pair amphiphile, Langmuir monolayer, vesicular bilayer |
| 相關次數: | 點閱:93 下載:3 |
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本研究探討DNA與離子對雙親分子(ion pair amphiphile, IPA) hexadecyltrimethylammonium-dodecylsulfate (HTMA-DS)及雙鏈陽離子型界面活性劑雙十六烷基二甲基溴化銨(dihexadecyldimethyl- ammonium bromide, DHDAB)於氣/液界面上形成之Langmuir單分子層的結合行為。藉由了解Langmuir單分子層的行為以及單分子層中分子排列的特性,提供對應之液胞系統與DNA交互作用機制的資訊。
在純水環境中,可藉由增加DHDAB的莫耳分率(XDHDAB),提升由HTMA-DS/DHDAB所製備出之陰陽離子液胞的界面電位與物理穩定性,顯示液胞表面帶電特性為液胞物理穩定性的主導因素。當液胞在DNA水溶液中時,液胞的粒徑會增大且界面電位值會降低。在DHDAB添加比率較高的液胞系統中,DNA對液胞的界面電位會造成較大的影響,並觀察到液胞/DNA的複合物較為穩定。然而,實驗結果顯示液胞表面的帶電特性與液胞/DNA複合物之物理穩定性的關聯性不高,因此液胞雙層膜內分子的排列特性或分子間的交互作用在液胞/DNA複合物的物理穩定性中應扮演重要的角色。值得一提的是,隨著水相中DNA濃度的增加,液胞雙層膜表現出規則性較高的分子排列特性,尤其是DHDAB添加比率較高的液胞系統。
對應的Langmuir單分子層行為顯示,在DHDAB添加比率高的單分子層中,水相中DNA對單分子層的行為影響較明顯,表示單分子層的電荷密度或液胞表面的帶電特性可藉由DHDAB的添加來控制。對分子排列特性而言,DNA的吸附使單分子層中的分子表現出較高的規則性。藉由設計的實驗發現,當DNA吸附至單分子層時,能夠減少單分子層中HTMA-DS的HTMA+被DHDA+取代後從氣/液界面上的損失。因而造成界面上單分子層內分子的排列較規則,也進一步影響單分子層的組成。實驗結果顯示DHDAB的添加可提升單分子層內分子間的交互作用,也增加單分子層與DNA間的電性吸引。因此在DHDAB添加比率較高的單分子層系統中,單分子層/DNA複合物具有較佳的穩定性。
根據單分子層系統的行為,針對液胞雙層膜結構於DNA水溶液 中呈現較規則的分子排列特性,以及在DHDAB添加比率較高的液胞系統中發現較穩定的液胞/DNA複合物,都提出適當的解釋,也反應出液胞雙層膜內分子間交互作用在液胞/DNA交互作用中的重要性。整體而言,DNA與HTMA-DS/DHDAB陰陽離子液胞所形成之複合物的穩定性與液胞雙層膜內分子排列特性、雙層膜內分子間的交互作用和液胞與DNA之間的電性作用明顯相關。
Physical stability control of vesicle/DNA complexes is a key issue for the development of catanionic vesicles composed of ion pair amphiphile (IPA) as DNA carriers. In this work, physical stability characteristics of the complexes of DNA with positively charged catanionic vesicles composed of an IPA and a double-chained cationic surfactant, dihexadecyldimethylammonium bromide (DHDAB), were explored. It was found that in pure water, the mixed IPA/DHDAB catanionic vesicles became stable when the molar fraction of DHDAB (XDHDAB) was increased up to 0.5. The improved physical stability of the vesicles with a high XDHDAB could be related to the enhanced electrostatic interaction between the vesicles. When the catanionic vesicles interacted with DNA, excellent physical stability was detected for the vesicle/DNA complexes especially with a high XDHDAB. However, this could not be fully explained by the electrostatic interaction effect, and the role of molecular packing within the vesicular bilayers was apparently important. The corresponding Langmuir monolayer study demonstrated that the molecular packing of mixed IPA/DHDAB layers became ordered with DNA association due to inhibited desorption of the positively charged moiety of the IPA. Moreover, the DNA association-induced improvement in the molecular packing of the mixed IPA/DHDAB layers became pronounced with increased XDHDAB. For the formation of stable HTMA-DS/DHDAB vesicle/DNA complexes, the strong electrostatic interaction of DNA with a vesicle of high charge density and the high vesicle stability characteristic resulting from DHDAB-improved molecular packing/interaction were thus required.
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