葫蘆脲化學傳感器的制備及其分子識別作用的研究
發(fā)布時間：2018-11-03 08:13
【摘要】：超分子化學是一個發(fā)展迅速的領(lǐng)域。它在分子識別,分子自組裝和分子器件等方面取得了很大進展。超分子的結(jié)構(gòu)是通過幾個分子(所謂的“分子亞單位”)聚集形成,因此它們不僅具有“分子亞單位”的功能,而且由于超分子結(jié)構(gòu)而具有了新的功能。化學傳感器一直是一個不斷發(fā)展的研究領(lǐng)域,并且在過去三十年中已經(jīng)在該領(lǐng)域取得了許多成果。其中,光化學傳感器是研究最為廣泛的,因為通過識別客體分子的光學變化,如顏色或熒光,可以快速、方便地觀察到現(xiàn)象。通常發(fā)色團觀察到的變化被用作傳感器的輸出信號。隨著超分子化學,生物化學和納米技術(shù)的發(fā)展,基于超分子化學傳感器以及納米碳和納米顆粒的新型化學傳感器得到了了廣泛的研究。本論文中研究了基于超分子主體葫蘆脲的均相傳感器法測定藥物分子奧沙利鉑,探究了藥物分子奧沙利鉑與超分子主體葫蘆脲的相互作用機理,形成穩(wěn)定包合物的條件(包括pH,溫度,時間)以及在藥物分析方面的應(yīng)用。同時也探究了基于葫蘆脲衍生物薄膜傳感器的制備,通過熒光顯微鏡對其進行表征,將其初步應(yīng)用于某些藥物小分子的識別。本論文主要闡述了以下四個方面:1.首先簡單的概括了超分子化學的發(fā)展,以及超分子主體的結(jié)構(gòu)特征。對第一、二、三代超分子主體化合物的合成方法和結(jié)構(gòu)做了簡單的描述,通過對它們結(jié)構(gòu)的分析得出其在化學領(lǐng)域中的實際應(yīng)用。根據(jù)它們結(jié)構(gòu)特點,詳細地介紹了第四代超分子主體葫蘆脲及其衍生物的結(jié)構(gòu),合成途徑以及應(yīng)用,為本論文后續(xù)的研究提供了理論依據(jù)。2.通過以葫蘆[7]脲為主體的均相熒光傳感器法測定抗癌藥物奧沙利鉑。由于巴馬汀/小檗堿/黃連堿和葫蘆[7]脲的水溶液本身無熒光,二者混合后體系熒光顯著增強,但當加入無熒光的奧沙利鉑后,體系的熒光又顯著猝滅。且分別在0.05~1.75,0.010~1.50和0.020~1.05μg mL-1的范圍內(nèi)奧沙利鉑的濃度與熒光猝滅值呈良好的線性關(guān)系,檢測限分別為2,3和7 ng m L 1,并可應(yīng)用于血漿中奧沙利鉑的測定。通過核磁共振和密度泛函理論對其作用機理進行了探究。葫蘆[7]脲將是一種潛在的轉(zhuǎn)運和監(jiān)測奧沙利鉑的良好藥物載體,同時可以降低藥物毒性提高藥物的療效。3.通過光聚合法制備了基于葫蘆脲的薄膜熒光傳感器。嘗試用三種不同的制備方法來制備,且對這三種方法制備的薄膜傳感器的優(yōu)缺點進行比較,用熒光素異硫氰酸酯衍生化精胺和熒光顯微鏡對其進行表征,探究其相互作用的機理,并初步用制備好的薄膜傳感器識別一些藥物小分子,預(yù)測了其在許多領(lǐng)域中的應(yīng)用。4.通過化學鍵合法制備了基于葫蘆脲的薄膜熒光傳感器。采用兩種不同的鍵合方法來制備,并對這兩種方法制備好的薄膜傳感器進行表征,且初步探索了它們與客體小分子甲基橙的相互作用,為后續(xù)的研究提供了理論基礎(chǔ)和實驗依據(jù)。
[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.
【學位授予單位】：山西師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TP212.2;O641.3
本文編號：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.
【學位授予單位】：山西師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TP212.2;O641.3
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