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研究生： 徐維隆
Wei-Long Hsu
論文名稱： DNA與陽離子型界面活性劑錯合體奈米結構之研究
Nanostructures from the Electrostatic Complexes of DNA with Cationic Surfactants
指導教授： 陳信龍
Hsin-Lung Chen
口試委員:
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： 2006
畢業學年度： 94
語文別： 英文
論文頁數： 83
中文關鍵詞： DNA 、陽離子型界面活性劑 、錯合體 、自組裝
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    • Polyanionic DNA binds to cationic amphiphiles such as lipids and surfactants to form electrostatic complexes exhibiting rich self-assembled structures. This type of complexes has been considered as a non-viral carrier in gene therapy. Extensive efforts have been dedicated to the relationship between the trnasfection efficiency and the molecular and self-assembled structures of the complexes. In addition to the biomedical application, DNA-cationic amphiphile complexes have also been considered as nanostructured templates due to the characteristic nanostructuring of DNA and the amphiphiles. For non-biomedical applications, cationic surfactant would be a more advantageous complexing agent compared with cationic lipid due to its lower cost and wider availability. However, the self-assembly behavior of the complexes of DNA with cationic surfactants still requires detailed investigations.

    In this dissertation, we systematically studied the lyotropic and thermotropic phase behaviors of the complexes of DNA with a cationic surfactant, dodecyltrimethyl bromide (DTAB), mixed with a neutral lipid, dioleoylphosphatidylethanolamine (DOPE), in fully hydrated state as a function of DTAB-to-DNA base pair molar ratio (x) and DOPE-to-DTAB molar ratio (m). Lyotropically, it was observed that the addition of DOPE induced a phase transition from a condensed multilamellar phase (L□c) to an inverted hexagonal phase (HIIc) at large m (m > ~ 6). The DNA chains confined between the hydrophobic layers in the L□c phase formed ordered arrays with the interhelical distance affected by both x and m. A thermally-induced order-order transition between L□c phase and HIIc phase was found to occur with the transition temperature adjustable by x and m. The stability of L□c phase was enhanced at lower m and x. The suppression of L□c-to-HIIc transition at lower x was attributed to the lower entropic gain from the counterion release due to the presence of uncomplexed DNA in the bulk solution.

    In addition to the self-assembled structure in the bulk state, we also studied the structure of the spin-coated thin film formed by the complex of DNA with a cationic surfactant, cetyltrimethylammonium bromide (CTAB). A highly uniform network structure was fond to develop in the thin film. The formation of the network structure was ascribed to the viscoelastic phase separation complexed with dewetting effect during the solvent evaporation.

    Table of Contents Abstract I Table of Contents III List of Tables V List of Figures VI Abbreviations XII Chapter 1. Introduction and Literature Review 1.1 Preface 1 1.2 Literature Survey 3 1.2.1 A Brief Overview of Amphiphiles 3 1.2.2 Structural Determination for Aggregated Cationic Amphiphiles 4 1.2.3 Structural Determination of DNA-Cationic Amphiphile Complexes 11 1.2.4 Relationship between Structure and Transfection Efficiency 25 1.2.5 Some Examples in Constructing the ordered Nano-Patterned Based on Self-Assembly of DNA-CA Complexes 27 1.3 The Motivations and Objectives of Study 30 1.4 References 31 Chapter 2. Mesomorphic Complexes of DNA with the Mixtures of a Cationic Surfactant and a Neutral Lipid 2.1 Introduction 36 2.2 Experimental Section 38 2.3 Results and Discussion 40 2.4 Conclusions 51 2.5 References and Notes 52 Chapter 3. Thermotropic Structural Changes of DNA-Cationic Surfactant-Neutral Lipid Complexes 3.1 Introduction 55 3.2 Experimental Section 57 3.3 Results and Discussion 59 3.4 Conclusions 70 3.5 References and Notes 72 Chapter 4. Construction of Two-Dimensional Nanopattern From DNA-Cationic Amphiphile Complexes 75

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