荧光碳材料的合成及其在生物硫醇检测中的应用

发布时间：2018-05-27 16:35

本文选题：荧光传感器 + 含碳材料　；参考：《济南大学》2017年硕士论文

【摘要】：生物传感器是分析检测领域的一项重要技术,广泛应用于生命科学、医学、环境及食品检测方面,而且其具有高灵敏度、低成本、快速检测、易于动态监测、操作方便等众多优势。其中,荧光传感器是基于分子识别和荧光技术两者的有机结合,通过荧光信号传导机制将分子结合信息转换为荧光信号,实现分子水平上原位实时检测的一种新型可靠的检测手段。生物硫醇在人体生理活动中发挥重要作用,其浓度与众多人类疾病密切相关,所以生物、环境样品中生物硫醇小分子的检测引起了研究者们的普遍关注和浓厚兴趣。本论文围绕合成含碳无机纳米材料及苯炔类有机材料,构建出多种不同荧光信号传导机制的荧光传感器,以实现对生物硫醇类小分子的检测。具体研究内容如下:1.基于碳点-二氧化锰纳米复合物荧光共振能量转移(FRET)的谷胱甘肽荧光传感分析以有机硅烷作为协同试剂合成一种高荧光量子效率的碳点,与一种花状二氧化锰通过一步合成的简单方法合成该纳米复合物。由于碳点与二氧化锰之间发生荧光共振能量转移,碳点的荧光会被二氧化锰猝灭。当引入谷胱甘肽时,由于二氧化锰被谷胱甘肽还原为二价锰,会导致FRET消失。与其他电解质和生物分子相比,我们发现这个传感器对谷胱甘肽有很好的选择性。在最佳条件下,这种传感器的线性范围为0.03 974.1μmol.L-1,检测限为0.015μmol.L-1。另外,这种荧光传感器有价格低廉,选择性高,生物相容性好等优点。2.基于石墨烯氮化碳(g-C_3N_4)纳米片-发色探针荧光内滤效应(IFE)的谷胱甘肽荧光传感分析通过水热法合成一种超薄g-C_3N_4纳米片和一种对谷胱甘肽有专一吸收响应的发色探针,两者之间分子可通过π-π相互作用构建荧光内滤效应传感器。当硫醇类引入该体系,由于“内滤效应关闭”,会出现明显的荧光恢复现象。我们选择谷胱甘肽作为模型进行检测,发现此IFE传感器线性范围为0.05μM.L-1-1.0μM.L-1,检测限为0.01μmol.L-1。另外,此传感器成功应用在了人类血清样品硫醇含量检测中。3.基于醛基-P酸探针光诱导电子转移(PET)半胱氨酸和同型半胱氨酸荧光传感分析此探针的合成基于引入醛基官能团于稳定的π共轭材料P酸(1,4-二(对乙炔基苯甲酸)-2,5-二甲氧基苯)上。此探针由于其荧光团(P酸)与识别基团(醛基)之间供体光诱导电子转移(d-PET)作用发生荧光猝灭,当遇到硫醇类,特别是半胱氨酸与同型半胱氨酸,d-PET作用发生抑制,荧光恢复,成功构建了一种开关型荧光探针。在最佳条件下,半胱氨酸线性范围为4-95 nM.L-1,最低检测限为3.0 nM.L-1。此探针对半胱氨酸和同型半胱氨酸有良好的选择性,而且成功应用在了细胞荧光成像中。
[Abstract]:Biosensor is an important technology in the field of analysis and detection. It is widely used in life science, medicine, environment and food detection. It has high sensitivity, low cost, rapid detection and easy dynamic monitoring. Easy to operate and many other advantages. Among them, the fluorescence sensor is based on the organic combination of molecular recognition and fluorescence technology, through the fluorescence signal transduction mechanism, the molecular binding information is converted into the fluorescence signal. A novel and reliable method for in situ real-time detection at molecular level. Biological mercaptan plays an important role in human physiological activities, and its concentration is closely related to many human diseases. Therefore, the detection of biological mercaptan small molecules in biological and environmental samples has attracted much attention and interest of researchers. In this paper, a variety of fluorescent sensors with different fluorescence signal transduction mechanisms were constructed around the synthesis of carbon-containing inorganic nano-materials and phenylethynes organic materials to achieve the detection of biological mercaptan small molecules. The specific contents of the study are as follows: 1. Glutathione fluorescence Sensing based on carbon Dot and Manganese dioxide Nano-complex fluorescence Resonance Energy transfer (FRET) Analysis of carbon dots with high fluorescence quantum efficiency using organosilane as a synergist. The nanocomposite was synthesized by a simple method of one step synthesis with a flower-like manganese dioxide. Because of the fluorescence resonance energy transfer between carbon point and manganese dioxide, the fluorescence of carbon point is quenched by manganese dioxide. When glutathione was introduced, FRET disappeared because manganese dioxide was reduced to bivalent manganese by glutathione. Compared with other electrolytes and biomolecules, we found that this sensor is highly selective for glutathione. Under the optimum conditions, the linear range of the sensor is 0.03 渭 mol 路L ~ (-1) and the detection limit is 0.015 渭 mol 路L ~ (-1). In addition, this kind of fluorescence sensor has the advantages of low cost, high selectivity and good biocompatibility. Glutathione fluorescence Sensing Analysis based on graphene nitride carbon nitride and C _ 3N _ 4) Nanoflakes-fluorescence Internal filter effect of Chromogenic probe) Synthesis of an Ultra-thin g-C_3N_4 Nanochip and a Color probe with a specific absorption response to Glutathione by hydrothermal method, The molecular interaction between the two molecules can be used to construct the fluorescence inner filter effect sensor by 蟺-蟺 interaction. When mercaptan is introduced into the system, the fluorescence recovery will be obvious due to the "internal filtration effect". We selected glutathione as the model and found that the linear range of the IFE sensor was 0.05 渭 M.L-1-1.0 渭 M.L-1 and the detection limit was 0.01 渭 mol 路L-1. In addition, the sensor has been successfully applied to the detection of mercaptan in human serum samples. Fluorescence Sensing of cysteine and homocysteine based on the Photo-Induced Electron transfer probe of Aldol -P Acid probe the synthesis of the probe is based on the introduction of a 蟺 -conjugated material, p-acetylbenzoic acid (p-acetylbenzoic acid), 4-bis (p-acetylbenzoic acid) -2o _ 5- (p-acetylbenzoic acid) based on the introduction of functional groups in the stable 蟺 -conjugated material P Dimethoxybenzene). The fluorescence quenching of the probe occurred due to the interaction between the fluorescence group (P acid) and the donor photoinduced electron transfer (d-PET), especially the inhibition of the interaction between cysteine and homocysteine d-PET, and the fluorescence recovered when the interaction of mercaptan, especially cysteine, with homocysteine d-PET was inhibited, the fluorescence of the probe recovered when the interaction between thiols, especially cysteine and homocysteine d-PET, was inhibited. A switched fluorescent probe was successfully constructed. Under the optimum conditions, the linear range of cysteine was 4-95 nM.L-1 and the minimum detection limit was 3.0 nM.L-1. The probe has good selectivity for cysteine and homocysteine, and has been successfully used in cell fluorescence imaging.
【学位授予单位】：济南大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.3;TP212

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