葫芦脲化学传感器的制备及其分子识别作用的研究
发布时间：2018-11-03 08:13
【摘要】：超分子化学是一个发展迅速的领域。它在分子识别,分子自组装和分子器件等方面取得了很大进展。超分子的结构是通过几个分子(所谓的“分子亚单位”)聚集形成,因此它们不仅具有“分子亚单位”的功能,而且由于超分子结构而具有了新的功能。化学传感器一直是一个不断发展的研究领域,并且在过去三十年中已经在该领域取得了许多成果。其中,光化学传感器是研究最为广泛的,因为通过识别客体分子的光学变化,如颜色或荧光,可以快速、方便地观察到现象。通常发色团观察到的变化被用作传感器的输出信号。随着超分子化学,生物化学和纳米技术的发展,基于超分子化学传感器以及纳米碳和纳米颗粒的新型化学传感器得到了了广泛的研究。本论文中研究了基于超分子主体葫芦脲的均相传感器法测定药物分子奥沙利铂,探究了药物分子奥沙利铂与超分子主体葫芦脲的相互作用机理,形成稳定包合物的条件(包括pH,温度,时间)以及在药物分析方面的应用。同时也探究了基于葫芦脲衍生物薄膜传感器的制备,通过荧光显微镜对其进行表征,将其初步应用于某些药物小分子的识别。本论文主要阐述了以下四个方面:1.首先简单的概括了超分子化学的发展,以及超分子主体的结构特征。对第一、二、三代超分子主体化合物的合成方法和结构做了简单的描述,通过对它们结构的分析得出其在化学领域中的实际应用。根据它们结构特点,详细地介绍了第四代超分子主体葫芦脲及其衍生物的结构,合成途径以及应用,为本论文后续的研究提供了理论依据。2.通过以葫芦[7]脲为主体的均相荧光传感器法测定抗癌药物奥沙利铂。由于巴马汀/小檗碱/黄连碱和葫芦[7]脲的水溶液本身无荧光,二者混合后体系荧光显著增强,但当加入无荧光的奥沙利铂后,体系的荧光又显著猝灭。且分别在0.05~1.75,0.010~1.50和0.020~1.05μg mL-1的范围内奥沙利铂的浓度与荧光猝灭值呈良好的线性关系,检测限分别为2,3和7 ng m L 1,并可应用于血浆中奥沙利铂的测定。通过核磁共振和密度泛函理论对其作用机理进行了探究。葫芦[7]脲将是一种潜在的转运和监测奥沙利铂的良好药物载体,同时可以降低药物毒性提高药物的疗效。3.通过光聚合法制备了基于葫芦脲的薄膜荧光传感器。尝试用三种不同的制备方法来制备,且对这三种方法制备的薄膜传感器的优缺点进行比较,用荧光素异硫氰酸酯衍生化精胺和荧光显微镜对其进行表征,探究其相互作用的机理,并初步用制备好的薄膜传感器识别一些药物小分子,预测了其在许多领域中的应用。4.通过化学键合法制备了基于葫芦脲的薄膜荧光传感器。采用两种不同的键合方法来制备,并对这两种方法制备好的薄膜传感器进行表征,且初步探索了它们与客体小分子甲基橙的相互作用,为后续的研究提供了理论基础和实验依据。
[Abstract]:Supramolecular chemistry is a rapidly developing field. It has made great progress in molecular recognition, molecular self-assembly and molecular devices. Supramolecular structures are formed by aggregation of several molecules (so-called "molecular subunits"), so they not only have the function of "molecular subunits", but also have new functions due to their supramolecular structures. Chemical sensors have been a developing field of research, and many achievements have been made in this field in the past 30 years. Among them photochemical sensors are the most widely studied because the phenomena can be observed quickly and conveniently by recognizing the optical changes of guest molecules such as color or fluorescence. Usually the changes observed in the chromophore are used as the output signal of the sensor. With the development of supramolecular chemistry, biochemistry and nanotechnology, new chemical sensors based on supramolecular chemical sensors, carbon nanoparticles and nanoparticles have been widely studied. In this paper, the homogenous sensor method based on supramolecular host cucurbituron was studied for the determination of oxaliplatin, and the interaction mechanism between the drug molecule oxaliplatin and supramolecular cucurbituron was investigated. Conditions for the formation of stable inclusion complexes (including pH, temperature, time) and their application in drug analysis. At the same time, the preparation of hyacinarbazone derivatives based on thin film sensor was investigated, and characterized by fluorescence microscope, which was applied to the recognition of some small drug molecules. This paper mainly expounds the following four aspects: 1. Firstly, the development of supramolecular chemistry and the structural characteristics of supramolecular host are briefly summarized. The synthesis methods and structures of the first, second and third generation supramolecular host compounds are briefly described, and their practical applications in the field of chemistry are obtained through the analysis of their structures. According to their structural characteristics, the structure, synthesis and application of the fourth generation supramolecular main body cucurbituron and its derivatives are introduced in detail, which provides a theoretical basis for further research in this paper. 2. The anticancer drug oxaliplatin was determined by homogeneous fluorescence sensor with gourd [7] urea as the main body. Since there is no fluorescence in the aqueous solution of palmatine / berberine / Coptis and gourd [7] urea, the fluorescence of the system increases significantly after mixing, but the fluorescence of the system is significantly quenched after the addition of oxaliplatin without fluorescence. There was a good linear relationship between the concentration of oxaliplatin and the fluorescence quenching value in the range of 0.05 渭 g mL-1 and 0.020 渭 g mL-1, respectively. The detection limits of oxaliplatin were 2m3 and 7 ng m L ~ (-1), respectively. It can be applied to the determination of oxaliplatin in plasma. The mechanism of nuclear magnetic resonance (NMR) and density functional theory (DFT) was studied. Gourd [7] urea will be a potential drug carrier for the transport and monitoring of oxaliplatin. A thin film fluorescence sensor based on cucurbituron was prepared by photopolymerization. The advantages and disadvantages of the three kinds of thin film sensors were compared and characterized by fluorescein isothiocyanate derivative spermine and fluorescence microscope. The mechanism of its interaction is explored, and some small drug molecules are identified by the prepared thin film sensors, and their applications in many fields are forecasted. 4. A thin film fluorescence sensor based on cucurbituron was prepared by chemical bond method. Two different bonding methods were used to prepare and characterize the thin film sensors prepared by these two methods, and the interaction between them and the guest small molecule methyl orange was preliminarily explored. It provides theoretical basis and experimental basis for further research.
【学位授予单位】：山西师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TP212.2;O641.3
本文编号：2307219
[Abstract]:Supramolecular chemistry is a rapidly developing field. It has made great progress in molecular recognition, molecular self-assembly and molecular devices. Supramolecular structures are formed by aggregation of several molecules (so-called "molecular subunits"), so they not only have the function of "molecular subunits", but also have new functions due to their supramolecular structures. Chemical sensors have been a developing field of research, and many achievements have been made in this field in the past 30 years. Among them photochemical sensors are the most widely studied because the phenomena can be observed quickly and conveniently by recognizing the optical changes of guest molecules such as color or fluorescence. Usually the changes observed in the chromophore are used as the output signal of the sensor. With the development of supramolecular chemistry, biochemistry and nanotechnology, new chemical sensors based on supramolecular chemical sensors, carbon nanoparticles and nanoparticles have been widely studied. In this paper, the homogenous sensor method based on supramolecular host cucurbituron was studied for the determination of oxaliplatin, and the interaction mechanism between the drug molecule oxaliplatin and supramolecular cucurbituron was investigated. Conditions for the formation of stable inclusion complexes (including pH, temperature, time) and their application in drug analysis. At the same time, the preparation of hyacinarbazone derivatives based on thin film sensor was investigated, and characterized by fluorescence microscope, which was applied to the recognition of some small drug molecules. This paper mainly expounds the following four aspects: 1. Firstly, the development of supramolecular chemistry and the structural characteristics of supramolecular host are briefly summarized. The synthesis methods and structures of the first, second and third generation supramolecular host compounds are briefly described, and their practical applications in the field of chemistry are obtained through the analysis of their structures. According to their structural characteristics, the structure, synthesis and application of the fourth generation supramolecular main body cucurbituron and its derivatives are introduced in detail, which provides a theoretical basis for further research in this paper. 2. The anticancer drug oxaliplatin was determined by homogeneous fluorescence sensor with gourd [7] urea as the main body. Since there is no fluorescence in the aqueous solution of palmatine / berberine / Coptis and gourd [7] urea, the fluorescence of the system increases significantly after mixing, but the fluorescence of the system is significantly quenched after the addition of oxaliplatin without fluorescence. There was a good linear relationship between the concentration of oxaliplatin and the fluorescence quenching value in the range of 0.05 渭 g mL-1 and 0.020 渭 g mL-1, respectively. The detection limits of oxaliplatin were 2m3 and 7 ng m L ~ (-1), respectively. It can be applied to the determination of oxaliplatin in plasma. The mechanism of nuclear magnetic resonance (NMR) and density functional theory (DFT) was studied. Gourd [7] urea will be a potential drug carrier for the transport and monitoring of oxaliplatin. A thin film fluorescence sensor based on cucurbituron was prepared by photopolymerization. The advantages and disadvantages of the three kinds of thin film sensors were compared and characterized by fluorescein isothiocyanate derivative spermine and fluorescence microscope. The mechanism of its interaction is explored, and some small drug molecules are identified by the prepared thin film sensors, and their applications in many fields are forecasted. 4. A thin film fluorescence sensor based on cucurbituron was prepared by chemical bond method. Two different bonding methods were used to prepare and characterize the thin film sensors prepared by these two methods, and the interaction between them and the guest small molecule methyl orange was preliminarily explored. It provides theoretical basis and experimental basis for further research.
【学位授予单位】：山西师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TP212.2;O641.3
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