烷基苯磺酸钆—聚酰胺—胺树状大分子亲水胶束聚集体的构建及钆离子释放的调控

发布时间：2018-10-30 12:34

【摘要】：以水合氯化钆(GdCl3·6H2O)和直链十二烷基苯磺酸钠为初始原料合成难溶于水的直链十二烷基苯磺酸钆(Gd)。使用增溶物质脂肪醇聚氧乙烯醚—平平加(AEO-25)将其分散于水中,形成混合增溶胶束。当AEO-25与Gd的质量比大于1.5时,溶液透明且稳定,冷冻干燥后得到白色雪花状固体。将增溶混合胶束与四代聚酰胺-胺树状大分子(4G-PAMAM)溶液混合,通过分子间的弱相互作用及其协同效应自组装成具有有序高级结构的超分子聚集体(4G-PAMAM/AEO-25/LASGd)。通过元素分析、热重、红外、核磁、透射电子显微镜、电感耦合等离子体原子发射光谱等方法对十二烷基苯磺酸钆、混合胶束及其增溶方式以及聚集体的结构和性质进行表征。结果表明:混合胶束以非极性分子在内核的方式增溶。该聚集体以烷基苯磺酸钆处于胶束核心部位,树状分子围绕在混合胶束周围的形式存在于水溶液中;将该聚集体冷冻干燥后的产物溶于水,加入酸或碱调节不同的pH值后透析,相同时间后测量透析液中钆元素的含量,发现钆含量逐渐降低,说明pH的改变可以控制聚集体中钆离子的释放;同理,实验还发现通过改变4G-PAMAM与增溶混合胶束的质量配比和聚集体水溶液体系的温度也可以达到控释钆离子的目的。本论文制备了一种水溶性好的聚集体,并通过改变溶液的pH值、配料比和体系温度调控了该聚集体中钆离子的释放行为。该聚集体有望用于pH敏感型核磁共振成像(MRI)造影剂。
[Abstract]:Synthesis of water-insoluble gadolinium dodecyl benzene sulfonate gadolinium chloride (GdCl3 6H2O) and straight chain sodium dodecylbenzene sulfonate (Gd).) The solubilized fatty alcohol polyoxyethylene ether (AEO-25) was dispersed in water to form a mixed sol beam. When the mass ratio of AEO-25 to Gd is greater than 1.5, the solution is transparent and stable, and the white snowflake solid is obtained after freeze-drying. The solubilized mixed micelles were mixed with the fourth generation polyamide-amine dendrimer (4G-PAMAM) solution. Supramolecular aggregates (4G-PAMAM/AEO-25/LASGd) with ordered and advanced structures are self-assembled by weak intermolecular interactions and their synergistic effects. The structure and properties of dodecyl benzenesulfonate gadolinium sulfonate mixed micelles and their solubilized aggregates were characterized by elemental analysis thermogravimetry IR NMR transmission electron microscopy and inductively coupled plasma atomic emission spectrometry. The results show that the mixed micelles are solubilized by nonpolar molecules in the core. The aggregate is in the core of the micelle as gadolinium alkyl benzenesulfonate and the dendrimer is surrounded by the mixed micelle in the form of aqueous solution. The product of freeze-drying was dissolved in water, then dialyzed by adding acid or alkali to adjust different pH value, the content of gadolinium in dialysate was measured after the same time, it was found that the content of gadolinium decreased gradually. It shows that the change of pH can control the release of gadolinium ion in aggregates. Similarly, it was also found that the controlled release of gadolinium ion could be achieved by changing the mass ratio of 4G-PAMAM and solubilized micelles and the temperature of the aqueous solution system of aggregates. In this paper, a water-soluble aggregate was prepared, and the release behavior of gadolinium ion was regulated by changing the pH value of the solution, the ratio of the mixture and the temperature of the system. The aggregates are expected to be used as pH sensitive (MRI) contrast agents.
【学位授予单位】：温州大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ421;O641.3

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