本文選題：熱力學 + 膽酸鈉　； 參考：《河南師范大學》2016年碩士論文

【摘要】：超分子聚集體囊泡為具有可調(diào)控性的軟納米粒子,由于其與細胞類似的雙分子層膜結(jié)構(gòu),為細胞仿生研究提供了模型體系。小分子表面活性劑囊泡作為仿生研究及實際應(yīng)用的系統(tǒng),如緩釋或定向釋放的藥物載體,在保持軟材料性質(zhì)的前提下提高雙分子層穩(wěn)定性是關(guān)鍵課題之一。本工作的目的是采用膽酸鈉改性的葡聚糖聚合物對表面活性劑囊泡的修飾,提高囊泡的穩(wěn)定性。本論文以等溫滴定量熱(ITC)為主要研究手段,結(jié)合冷凍透射電鏡(cryo-TEM)、濁度、電導和動態(tài)光散射(DLS)等分析技術(shù),以膽酸鈉(NaCA)和含膽酸鈉側(cè)鏈的改性聚合物為研究主線,探討它們與陰、陽離子表面活性劑的混合體系和陰陽離子混合囊泡之間的一系列分子自組裝熱力學和相行為。詳細分析了雙親分子疏水側(cè)鏈性質(zhì)、電荷、溶液的組成和濃度等因素對復雜體系中分子聚集過程的影響,討論了各種雙親分子間的協(xié)同效應(yīng)。由此從宏觀熱力學特性和分子結(jié)構(gòu)方面,解釋膽酸鈉組分對囊泡聚集體轉(zhuǎn)變的調(diào)控作用以及此類復雜體系中分子間相互作用的熱力學行為。論文工作包含以下主要內(nèi)容:1.膽酸鈉在水溶液中的膠束化熱力學以等溫滴定量熱和電導率測定方法,研究了膽酸鈉的濃度變化對其膠束化過程的影響。測量了膽酸鈉的臨界預膠束濃度和臨界膠束濃度及其相應(yīng)過程的相變焓。尤其是對于膽酸鈉的預膠束形成,首次得到了有明確定義的預膠束化焓。2.建立了相同電荷的表面活性劑混合體系——NaCA/十二烷基硫酸鈉(SDS)得到了在不同SDS初始濃度下相同電荷的NaCA和SDS之間的相互作用能。結(jié)果表明ITC對于相同電荷混合表面活性劑非常弱的協(xié)同效應(yīng)以及疏水作用能量研究是最為直接準確的手段。3.建立了相反電荷的表面活性劑混合體系—NaCA/雙子表面活性劑(12-10-12Br2)深入研究了這類混合體系從膠束到液晶,再到混合膠束的轉(zhuǎn)變過程熱力學和相行為。得到了混合體系膠束相與液晶相的濃度范圍,詳細討論了雙子表面活性劑濃度對混合體系聚集行為的影響。4.NaCA對于陰陽離子混合表面活性劑囊泡聚集行為的調(diào)控作用建立了含有三種表面活性劑分子的復雜體系。通過等溫滴定量熱與濁度、動態(tài)光散射、低溫透射電鏡等手段結(jié)合,研究了NaCA誘導的囊泡從溶脹到破裂過程的形態(tài)變化及聚集熱力學,并得到了囊泡破裂的臨界濃度和焓變。5.含有NaCA側(cè)鏈的改性聚合物(Dex-xCACOONa)與囊泡的相互作用基于前面工作的基礎(chǔ),論文工作進一步在混合表面活性劑囊泡體系中加入側(cè)鏈帶有膽酸鈉的改性聚合物,旨在調(diào)控囊泡的穩(wěn)定性和聚集行為。首先利用ITC方法表征了雙親聚合物在水溶液中的自組裝熱力學性質(zhì)和聚集能力。進而建立疏水聚合物與囊泡的混合體系,聚合物的NaCA改性側(cè)鏈及替代度對囊泡聚集行為的影響被詳細地討論。這些結(jié)果對于我們進一步深入擴展此類復雜體系的研究和應(yīng)用,有著重要的指導意義。論文工作得到國家自然科學基金項目(No.21273061和No.21327003)的支持。研究生期間關(guān)于同電荷表面活性劑體系的工作已經(jīng)發(fā)表在國際專業(yè)雜志J.Chem.Thermodynamics,(100(2016)131-139)上。發(fā)表國內(nèi)外會議論文(3篇)。兩篇工作在整理中,一篇為膽酸鈉與混合囊泡的相互作用,另一篇為疏水改性聚合物對囊泡聚集行為的調(diào)控及其相互作用熱力學。
[Abstract]:The supramolecular aggregate vesicle is a controllable soft nanoparticle, which provides a model system for biomimetic research due to its similar bimolecular membrane structure. Small molecular surface active agent vesicles are used as biomimetic research and practical applications, such as sustained release or directional release drug carriers, before maintaining the properties of soft materials. It is one of the key issues to improve the stability of the biolecular layer. The aim of this work is to improve the stability of the vesicles by using sodium cholate modified glucan polymer to modify the vesicles of the surfactant. In this paper, the isothermal drop quantitative heat (ITC) is used as the main research method, combined with the cryopreservation transmission electron microscopy (cryo-TEM), turbidity, conductivity and dynamic dispersion. A series of molecular self-assembly thermodynamics and phase behaviors between the mixed systems of anion and cationic surfactant and the mixed vesicles of yin and yang ions are discussed with DLS and other analytical techniques. The properties of the hydrophobic side chain of the parents, charge and solution are detailed and analyzed. The effects of composition and concentration on the molecular aggregation process in complex systems are discussed, and the synergistic effects of various parents are discussed. From the macroscopic thermodynamic properties and molecular structures, the regulation of the sodium cholate component to the vesicle aggregates transformation and the thermodynamic behavior of intermolecular interaction in such complex systems are explained. The work includes the following main contents: 1. the micellization thermodynamics of sodium cholate in aqueous solution, the influence of the concentration change of sodium cholate on the micellization process of the isothermal drop quantitative heat and electrical conductivity. The critical Premicelle concentration and critical micelle concentration of sodium cholate and the enthalpy of the corresponding process are measured. In the formation of pre micelle of sodium cholate, a clearly defined premicellar enthalpy.2. has been obtained for the first time to establish a mixed system of surfactants with the same charge - NaCA/ twelve alkyl sulfate (SDS). The interaction energy between NaCA and SDS at the same charge at different initial SDS concentrations is obtained. The results show that ITC is the same charge mixing table. The very weak synergistic effect and the study of hydrophobic energy are the most direct and accurate means for.3. to establish a surface active agent, NaCA/ Gemini Surfactants (12-10-12Br2), to study the thermodynamics and phase behavior of the transition process from micelles to liquid crystals and then to mixed micelles. The concentration range of the micell phase and liquid crystal phase of the mixed system was obtained. The effect of the concentration of Gemini Surfactant on the aggregation behavior of the mixed system was discussed in detail. The complex system containing three kinds of surfactant molecules was established in the regulation of the aggregation behavior of the mixed surfactant in the mixture of yin and Yang. By the isothermal titration calorimetry (.4.NaCA) Combined with turbidity, dynamic light scattering and low temperature transmission electron microscopy, the morphological changes and aggregation thermodynamics of NaCA induced vesicles from swelling to rupture were studied. The interaction between the critical concentration and enthalpy of the vesicle rupture and the interaction of the modified polymer (Dex-xCACOONa) with the NaCA side chain (Dex-xCACOONa) with the vesicle was obtained based on the previous work. In this paper, a modified polymer of side chain with sodium cholate was added to the mixed surfactant vesicle system to regulate the stability and aggregation behavior of the vesicles. First, the ITC method was used to characterize the self assembly thermodynamic properties and the aggregation energy of the amphiphilic polymer in aqueous solution. The effects of the NaCA modified side chain and the substitution degree of the polymer on the vesicle aggregation are discussed in detail. These results have important guiding significance for us to further expand the research and application of such complex systems. The work has been supported by the National Natural Science Foundation Project (No.21273061 and No.21327003). The work on the same charge surface active agent system was published in the international professional journal J.Chem.Thermodynamics, (100 (2016) 131-139). Published in the domestic and foreign Conference Papers (3). Two work was in the arrangement, one for the interaction between sodium cholate and mixed vesicles, and the other for the aggregation of the vesicles by the hydrophobic modified polymer. Regulation and interaction thermodynamics.
【學位授予單位】：河南師范大學
【學位級別】：碩士
【學位授予年份】：2016
【分類號】：O647.2

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