氮杂环、羧酸配体合成MOFs及其药物缓控释研究

发布时间：2018-06-01 10:14

本文选题：配位聚合物 + 氢键　；参考：《西南交通大学》2016年硕士论文

【摘要】：作为配位化学领域的一种新材料,金属有机骨架材料(MOFs)在最近十年内吸引了众多科学家的眼球。这是因为它们不仅拥有新颖的拓扑结构,还有许多潜在的应用,比如载药、催化、生物传感、气体吸附、荧光。为了实现这些应用价值,选择和设计出合适的有机配体构筑基块尤其重要。本论文选用结构中含有氮杂环(吡啶、吡嗪)和羧基的柔性配体Hpypymba、芳香族羧酸刚性配体tta分别与不同种类的过渡金属盐(Cu(II)、Co(II)、Cd(II))合成结构新颖的金属有机骨架材料。随后,通过X-单晶衍射分析配合物的晶体结构,并对其进行热重、红外、荧光、元素分析及相关性质的研究。本论文通过分层扩散法、水热法合成得到了4个结构新颖的配位聚合物：[Cu2(pypymba)3]n (1), [Cu2(pypymba)4]n (2), [Co2(pypymba)4]n (3) {[Cd1.5(tta)(H2O)4.5] · H2O}n (4).X-单晶衍射分析结果表明：配合物1通过Cu-O配位键形成一维螺旋结构,随后在C-H…O氢键和π-π堆积的共同作用下,将配合物的结构扩展成三维网络拓扑结构,孔隙率达21.3%；而配合物2、3只通过氢键和π-π堆积作用就将其结构扩展成1D→3D结构；配合物4的结构中,Cd-O配位键起到了至关重要的作用,它直接完成了配合物结构1D→2D的构筑,随后在配位水分子与晶体骨架间的氢键作用下,形成了具有高孔隙率的三维骨架网络结构,孔隙率为27.3%。此外,本论文对配合物1、2的抗氧化活性、配合物4对布洛芬(Ibu)的药物控释能力作了一定研究。结果表明：(1)配合物1、2均具有良好的抗氧化能力,其半数抑制浓度(IC50)分别为24.2μg/mL、37.5μg/mL。(2)布洛芬与配合物4质量比为1：1时,载药5天后达最大载药量,为0.203 g(Ibu)/g(MOFs);随后,在PBS缓冲溶液中对载药后的配合物作释放研究,其结果表明,布洛芬在72h内释放量为57.6%,表现出了良好的缓释效果。
[Abstract]:As a new material in coordination chemistry, MOFs has attracted the attention of many scientists in recent ten years. This is because they not only have novel topology, but also have many potential applications, such as drug loading, catalysis, biosensor, gas adsorption, fluorescence. In order to realize these applications, it is particularly important to select and design suitable organic ligands for building blocks. In this paper, novel organometallic framework materials were synthesized by using the flexible ligands Hpypymba, aromatic carboxylic acid rigid ligand tta and different kinds of transition metal salts, including pyridine (pyridine, pyrazine) and carboxyl groups, respectively. The crystal structure of the complex was analyzed by X-ray diffraction, and its thermogravimetric, infrared, fluorescence, elemental analysis and related properties were studied. In this paper, four novel coordination polymers, [Cu2(pypymba)3] n, [Cu2(pypymba)4] n ~ (2 +), [Co2(pypymba)4] n ~ (3), {[Cd1.5(tta)(H2O)4.5] H _ 2O} n ~ (4) N ~ (4) O 路X ~ (-), were synthesized by the method of layering diffusion and hydrothermal method. The results show that complex 1 forms one dimensional helical structure by Cu-O coordination bond, and then in C-H _ (2). Under the action of O hydrogen bond and 蟺-蟺 stacking, the structure of the complex was expanded into a 3D network topology with a porosity of 21. 3, while the complex 2 + 3 expanded its structure to 1D / 3D structure only by hydrogen bond and 蟺-蟺 stacking. Cd-O coordination bond plays an important role in the structure of complex 4, which directly completes the construction of the coordination structure 1D ~ (2 D), and then under the interaction of hydrogen bond between the coordination water molecule and the crystal framework. A three-dimensional skeleton network structure with high porosity was formed, with a porosity of 27.3a. In addition, the antioxidant activity of complex 1t2 and the controlled release ability of complex 4 to ibul were studied in this paper. The results showed that both of them had good antioxidant activity, and IC50 was 24.2 渭 g / mL ~ 37.5 渭 g / m ~ (2) when the mass ratio of ibuprofen to complex 4 was 1:1, the maximum drug loading capacity was 0.203 g Ibur / g MOFsN after 5 days of drug loading, then, when the mass ratio of ibuprofen to complex 4 was 1:1, The release of the complex was studied in PBS buffer solution. The results showed that the release of ibuprofen was 57.6 in 72 h, showing a good sustained release effect.
【学位授予单位】：西南交通大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O641.4;TQ460.1

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