纳米荧光探针的研究及应用
发布时间：2018-11-09 20:45
【摘要】：纳米荧光探针由于其尺寸与结构的特殊性,表现出与宏观物质截然不同的理化性质,如小尺寸效应、量子效应、表面效应与量子隧道效应等,在医疗、科技、能源、军事等领域具有广阔的应用前景。近年来,将纳米荧光探针应用于化学传感、生物医学等领域一直是科学家研究的热点,其中最关键的是设计合成具有优良性能的荧光纳米材料,如粒径均一、光学性质稳定、细胞毒性低、水溶性及生物相容性良好等。本论文采用简单一步法制得性能优异的银纳米簇、碳点及其复合纳米材料,并基于以上荧光纳米材料构建新的传感平台,实现对S~(2-)、Fe~(3+)、Al~(3+)以及癌细胞的检测。第一章:简述纳米荧光探针的基本性能,对纳米荧光探针(包括量子点、贵金属纳米簇、碳点)的研究及应用进展进行了综述。第二章:常温下,以溶菌酶(Lys)为稳定剂,NaBH_4为还原剂,通过简单的一步法合成溶菌酶稳定的银纳米簇(Lys-Ag NCs)。基于S~(2-)与Ag~+/Ag之间强烈的相互作用,S~(2-)可以显著猝灭Lys-Ag NCs的荧光,进而建立了一种高灵敏、高选择性检测S~(2-)的方法。该方法在5.0×10-6 M-1.0×10-4 M线性范围内对S~(2-)有良好的响应,对应的检出限为1.1×10-6M(S/N=3)。满意的回收率结果(97.0-101.4%)表明该方法具有一定的可行性,可用于环境水样中S~(2-)的检测。此外,对S~(2-)与Lys-Ag NCs之间的作用机理也进行了详细地探讨研究。第三章:以脯氨酸为碳源,乙二胺为氮源,通过简单的一步水热法制备得到发蓝色荧光的CDs。CDs表面的-NH2可以通过经典的EDC/NHS反应与叶酸(FA)表面的-COOH发生反应生成CDs-FA复合物。基于FA与叶酸受体(FR)之间强烈的亲和力以及FR介导的细胞内吞作用,CDs-FA复合物可以特异性识别FR表达的癌细胞并对其完成荧光标记,进而将FR表达的癌细胞与FR不表达的正常细胞区分开来,这为癌症的早期诊断与治疗提供一定的依据。第四章:以环糊精为碳源,通过一步水热法制得发蓝色荧光的CDs。CDs表面丰富的羟基、环氧基等含氧基团使得CDs不仅具有还原剂的特性,而且可以在纳米簇的合成过程中充当保护剂,基于此,将制得的CDs与Ag~+通过简单水热法合成发绿色荧光的CDs-Ag NCs复合物。当Fe~(3+)存在时,该CDs-Ag NCs复合物的荧光发生猝灭,而当Al~(3+)存在时,该CDs-Ag NCs复合物的荧光得到增强,由此,分别构建了“断开式”Fe~(3+)传感体系和“开启式”Al~(3+)传感体系,两个传感体系对应的线性范围分别是5.0×10-6M-3.6×10-4M和2.0×10-5M-1.8×10-4M,检出限分别为2.6×10-6M与4.8×10-7 M(S/N=3)。此外,两者的回收率实验都取得了满意的结果,表明该CDs-Ag NCs复合物在Fe~(3+)与Al~(3+)的分析检测中具有很大的应用潜力。第五章:对本论文中银纳米簇、碳点及其复合物作为荧光探针/标记物,在离子检测和靶向细胞成像方面的研究结果做了总结,并对后续的工作进行了展望。
[Abstract]:Because of the particularity of its size and structure, the nanoscale fluorescent probe has different physicochemical properties from macroscopical materials, such as small size effect, quantum effect, surface effect and quantum tunneling effect, etc., in medical treatment, science and technology, energy, etc. Military and other fields have broad application prospects. In recent years, the application of nano-fluorescent probes in chemical sensing, biomedicine and other fields has been the focus of scientists, the most important is the design and synthesis of fluorescent nanomaterials with excellent properties, such as uniform particle size, stable optical properties. Low cytotoxicity, good water solubility and biocompatibility. In this paper, silver nanoclusters, carbon dots and their composite nanomaterials with excellent performance were obtained by a simple one-step method. Based on the above fluorescent nanomaterials, a new sensing platform was constructed to realize the synthesis of S2-, Fe~ (3). Detection of Al~ (3) and cancer cells. In chapter 1, the basic properties of nano-fluorescent probes are reviewed. The research and application of nano-fluorescent probes (including quantum dots, noble metal nanoclusters and carbon dots) are reviewed. Chapter 2: under normal temperature, using lysozyme (Lys) as stabilizer and NaBH_4 as reducing agent, a simple one-step method was used to synthesize lysozyme stabilized silver nanoclusters (Lys-Ag NCs). Based on the strong interaction between S2- and Ag~ / Ag, S2- can significantly quench the fluorescence of Lys-Ag NCs and establish a highly sensitive and selective method for the detection of S2-. The method has a good response to S2- in the linear range of 5.0 脳 10-6 M-1.0 脳 10-4 M and the detection limit is 1.1 脳 10-6 M (S/N=3). The satisfactory recovery (97.0-101.4%) showed that the method was feasible and could be applied to the determination of S2- in environmental water samples. In addition, the interaction mechanism between S2- and Lys-Ag NCs is also studied in detail. Chapter III: proline as carbon source, ethylenediamine as nitrogen source, The-NH2 of the blue fluorescent CDs.CDs surface was prepared by a simple one step hydrothermal method. The CDs-FA complex can be formed by classical EDC/NHS reaction with-COOH on the (FA) surface of folate. Based on the strong affinity between FA and folate receptor (FR) and the intracellular endocytosis mediated by FR, the CDs-FA complex can specifically recognize and label FR expressed cancer cells. Furthermore, the FR expressed cancer cells were distinguished from the normal cells not expressed by FR, which provided a basis for the early diagnosis and treatment of cancer. Chapter 4: using cyclodextrin as carbon source, the blue fluorescent CDs.CDs surface with abundant hydroxyl, epoxy and other oxygen-containing groups can be prepared by one-step hydrothermal method, which makes CDs not only have the properties of reductant. And it can be used as a protective agent in the synthesis of nanoclusters. Based on this, CDs and Ag~ were synthesized by a simple hydrothermal method to synthesize green fluorescent CDs-Ag NCs complexes. In the presence of Fe~ (3), the fluorescence of the CDs-Ag NCs complex is quenched, and when Al~ (3) exists, the fluorescence of the CDs-Ag NCs complex is enhanced. The "open" Fe~ (3) sensing system and the "open" Al~ (3) sensing system are constructed respectively. The linear ranges of the two sensing systems are 5.0 脳 10-6M-3.6 脳 10-4M and 2.0 脳 10-5M-1.8 脳 10-4M, respectively. The detection limits were 2.6 脳 10 ~ (-6) M and 4.8 脳 10 ~ (-7) M (S/N=3), respectively. In addition, satisfactory results have been obtained in both the recovery experiments, indicating that the CDs-Ag NCs complex has great potential for application in the analysis and detection of Fe~ (3) and Al~ (3). Chapter 5: the research results of silver nanoclusters, carbon spots and their complexes as fluorescent probes / markers in this thesis are summarized in ion detection and targeted cell imaging, and the future work is prospected.
【学位授予单位】：山西大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.3
本文编号：2321514
[Abstract]:Because of the particularity of its size and structure, the nanoscale fluorescent probe has different physicochemical properties from macroscopical materials, such as small size effect, quantum effect, surface effect and quantum tunneling effect, etc., in medical treatment, science and technology, energy, etc. Military and other fields have broad application prospects. In recent years, the application of nano-fluorescent probes in chemical sensing, biomedicine and other fields has been the focus of scientists, the most important is the design and synthesis of fluorescent nanomaterials with excellent properties, such as uniform particle size, stable optical properties. Low cytotoxicity, good water solubility and biocompatibility. In this paper, silver nanoclusters, carbon dots and their composite nanomaterials with excellent performance were obtained by a simple one-step method. Based on the above fluorescent nanomaterials, a new sensing platform was constructed to realize the synthesis of S2-, Fe~ (3). Detection of Al~ (3) and cancer cells. In chapter 1, the basic properties of nano-fluorescent probes are reviewed. The research and application of nano-fluorescent probes (including quantum dots, noble metal nanoclusters and carbon dots) are reviewed. Chapter 2: under normal temperature, using lysozyme (Lys) as stabilizer and NaBH_4 as reducing agent, a simple one-step method was used to synthesize lysozyme stabilized silver nanoclusters (Lys-Ag NCs). Based on the strong interaction between S2- and Ag~ / Ag, S2- can significantly quench the fluorescence of Lys-Ag NCs and establish a highly sensitive and selective method for the detection of S2-. The method has a good response to S2- in the linear range of 5.0 脳 10-6 M-1.0 脳 10-4 M and the detection limit is 1.1 脳 10-6 M (S/N=3). The satisfactory recovery (97.0-101.4%) showed that the method was feasible and could be applied to the determination of S2- in environmental water samples. In addition, the interaction mechanism between S2- and Lys-Ag NCs is also studied in detail. Chapter III: proline as carbon source, ethylenediamine as nitrogen source, The-NH2 of the blue fluorescent CDs.CDs surface was prepared by a simple one step hydrothermal method. The CDs-FA complex can be formed by classical EDC/NHS reaction with-COOH on the (FA) surface of folate. Based on the strong affinity between FA and folate receptor (FR) and the intracellular endocytosis mediated by FR, the CDs-FA complex can specifically recognize and label FR expressed cancer cells. Furthermore, the FR expressed cancer cells were distinguished from the normal cells not expressed by FR, which provided a basis for the early diagnosis and treatment of cancer. Chapter 4: using cyclodextrin as carbon source, the blue fluorescent CDs.CDs surface with abundant hydroxyl, epoxy and other oxygen-containing groups can be prepared by one-step hydrothermal method, which makes CDs not only have the properties of reductant. And it can be used as a protective agent in the synthesis of nanoclusters. Based on this, CDs and Ag~ were synthesized by a simple hydrothermal method to synthesize green fluorescent CDs-Ag NCs complexes. In the presence of Fe~ (3), the fluorescence of the CDs-Ag NCs complex is quenched, and when Al~ (3) exists, the fluorescence of the CDs-Ag NCs complex is enhanced. The "open" Fe~ (3) sensing system and the "open" Al~ (3) sensing system are constructed respectively. The linear ranges of the two sensing systems are 5.0 脳 10-6M-3.6 脳 10-4M and 2.0 脳 10-5M-1.8 脳 10-4M, respectively. The detection limits were 2.6 脳 10 ~ (-6) M and 4.8 脳 10 ~ (-7) M (S/N=3), respectively. In addition, satisfactory results have been obtained in both the recovery experiments, indicating that the CDs-Ag NCs complex has great potential for application in the analysis and detection of Fe~ (3) and Al~ (3). Chapter 5: the research results of silver nanoclusters, carbon spots and their complexes as fluorescent probes / markers in this thesis are summarized in ion detection and targeted cell imaging, and the future work is prospected.
【学位授予单位】：山西大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.3
【参考文献】
相关期刊论文 前2条
1 Taotao Li;Jingjing Yang;Zeeshan Ali;Zunliang Wang;Xianbo Mou;Nongyue He;Zhifei Wang;;Synthesis of aptamer-functionalized Ag nanoclusters for MCF-7 breast cancer cells imaging[J];Science China(Chemistry);2017年03期
2 方静美;刘利芹;赵希娟;李原芳;;铝离子与羟基功能化荧光碳点的相互作用[J];应用化学;2013年10期
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