基于氧化石墨烯的光学生化传感检测研究

发布时间：2018-03-10 03:24

本文选题：氧化石墨烯　切入点：生化传感器　出处：《浙江大学》2017年博士论文　论文类型：学位论文

【摘要】：因其异源的化学和电学结构、丰富的生物分子结合位点、良好的水溶性和可调的光电性质等优异特性,氧化石墨烯在光学生物传感检测领域展现出极大的应用前景,已被广泛用于环境监测、医疗健康和食品监管等。但是,目前大多数围绕氧化石墨烯开展的光学生物传感系统都是基于其光致发光和荧光猝灭等特性来构建的。荧光等光学传感技术虽然具有灵敏度高、检测下限低等优点,却也不可避免地存在诸如检测仪器要求高、操作相对复杂、需要额外的标记等问题,因而增加了基于氧化石墨烯的光学生物传感系统的搭建难度,限制了该类系统的实际应用范围。因此,挖掘一种简便、快速、免标记且可定量的光学检测技术,配合其设计基于氧化石墨烯的高灵敏生化传感器,对提升氧化石墨烯在光学生化传感领域的实际应用价值有着重要作用。本文通过不同的修饰方法设计并构建了基于氧化石墨烯的生物传感器、基于氧化石墨烯的仿生传感器,以及基于氧化石墨烯的纳米复合传感器等生化传感平台。根据这些传感器的光学特性,结合操作简单、响应快速、成本低廉且易于便携化的紫外-可见吸收光谱检测技术,搭建了一系列基于氧化石墨烯的免标记光学生化传感检测系统,并探究了其在气味分子检测、甜味物质检测以及生物分子检测等方面的应用。这些研究验证了氧化石墨烯在构建高灵敏生化传感器方面的能力和潜在机理,以及紫外-可见光谱检测技术与基于氧化石墨烯的生化传感器结合构建免标记光学传感平台的潜力,进一步挖掘了氧化石墨烯在光学生化传感领域的应用价值。本文的主要内容和创新点如下:1.设计并实现了基于氧化石墨烯的紫外光谱生物传感检测系统,并验证了其在气味分子检测中的应用。本文合成了对爆炸物气味分子2,4,6-三硝基甲苯(2,4,6-trinitrotoluene,TNT)特异性敏感的多肽,并将其与氧化石墨烯共价交联,构建了一种基于氧化石墨烯的生物传感器。再结合紫外吸收光谱完成了对不同浓度TNT的特异性检测,验证了氧化石墨烯在构建高灵敏生物传感器方面的能力、其作为换能器件将生化信号转化为光学响应的能力、紫外吸收光谱作为光学检测技术与基于氧化石墨烯的生物传感器结合搭建光学生物传感系统的能力,以及该系统在气味分子监测中的应用潜力。2.设计并实现了基于氧化石墨烯的紫外-可见光学仿生传感检测系统,并验证了其在甜味物质检测中的应用。本文设计了一种基于氧化石墨烯的紫外-可见光谱仿生传感系统。先将氧化石墨烯、从血红蛋白活性中心提取的血红素以及与生物味觉受体具有相似糖感受机制的苯硼酸通过非共价及共价结合的方式层层复合,构建了一种类似糖转运蛋白的仿生传感器。再将其与紫外-可见吸收光谱结合,实现了对甜味的检测和对不同种类甜味剂的分辨。该研究验证了氧化石墨烯在构建仿生传感器方面的潜力、紫外-可见吸收光谱与基于氧化石墨烯的仿生传感器结合搭建光学仿生传感系统的潜力,以及基于氧化石墨烯的紫外-可见光谱仿生传感系统在仿生甜味检测中的应用潜能。3.设计并实现了基于氧化石墨烯的可见光谱纳米复合传感系统,并探究了其在生物分子及生物分子间相互作用的检测中的应用。本文通过一步法制备了氧化石墨烯与金纳米颗粒复合的纳米传感器,并将其与可见吸收光谱结合构建了基于氧化石墨烯的纳米复合传感系统。随后探究了该系统在氨基酸、多肽和蛋白等生物分子的检测中的应用。同时,本文还进一步设计并合成了具有凝血酶特异性结合位点的多肽,通过自组装手段使其与氧化石墨烯/纳米金复合,构建了基于氧化石墨烯/纳米金的生物传感器。再结合可见吸收光谱检测技术搭建了基于氧化石墨烯/纳米金的可见光谱生物传感系统,实现了对凝血酶的高灵敏、高特异性检测。这些验证了氧化石墨烯在构建纳米复合生化传感器方面的潜力、可见吸收光谱与基于氧化石墨烯的复合传感器结合搭建纳米光学传感系统的潜力以及该系统在多种生物分子、甚至生物分子间相互作用的检测中的应用潜能。
[Abstract]:Because of the chemical and electrical structure of the heterologous, biological molecules rich binding sites, excellent properties and adjustable optical properties and good water solubility, graphene oxide showed great application prospect in the field of optical biosensing detection, has been widely used in environmental monitoring, medical health and food supervision. But at present. Most around the optical biosensing system of graphene oxide are constructed based on the photoluminescence and fluorescence quenching properties. Fluorescence optical sensing technology has high sensitivity, low detection limit, but inevitably, such as testing equipment requirements, the operation is relatively complex, the need for additional labeling problem thus increasing the optical biosensing system of graphene oxide structures based on the difficulty, limit the system's application scope. Therefore, mining a convenient, fast, Label free optical detection technology and quantitative design, with its high sensitive biochemical sensor based on the graphene oxide, it plays an important role in promoting the graphene oxide in the optical field of biochemical sensing application value. In this paper, through the design of different modification methods and the construction of the biosensor based on graphene oxide, graphite oxide bionic sensor based on graphene, and graphene oxide nano composite sensor based on biochemical sensing platform. According to the optical properties of these sensors, with simple operation, fast response, low cost and easy for UV - visible absorption spectrum of the portable detection technology, set up a series based on label free optical biochemical sensing system of graphene oxide, and explore their application in detection of odor molecules, sweet substance detection and biomolecular detection. These studies validate the oxidation Graphene in the construction of high sensitive biochemical sensor ability and potential mechanism, and UV Vis spectroscopy detection technology and biochemical sensor based on the graphene oxide paper label free optical sensing platform to further tap the potential application value of graphene oxide in optical and biochemical sensing field. The main contents and innovations of this paper are as follows 1.: the design and implementation of UV biosensor based on graphene oxide, and verified its application in odorant detection. The synthesis of explosives odor molecules 2,4,6- three nitro - toluene (2,4,6-trinitrotoluene, TNT) - sensitive specific peptides, and the graphene oxide covalent crosslinking, built a biosensor based on graphene oxide. Combined with UV finish specific detection of different TNT concentrations on the absorption spectra, verify oxygen graphite In the presence of high sensitive biosensors construction ability, as the transducer biochemical signal into optical response ability, UV absorption spectrum as optical detection technology and biosensor based on graphene oxide with the ability to build optical bio sensing system, and the potential application of.2. in the design of the system in the monitoring of odor molecules and the UV - visible optical graphene oxide based on bionic sensing detection system, and verify its application in sweet substance detection. This paper describes the design of a UV - graphene oxide based on visible light spectrum of bionic sensor system. First graphene oxide layers, compound extracted from heme hemoglobin activity the center and biological taste receptors with similar sugar boronic acid receptor mechanism through noncovalent and covalent binding, construct a similar sugar transporter And the biomimetic sensor. The UV Vis absorption spectroscopy, the detection of sweet and of different sweeteners resolution. The study verified the potential of graphene oxide in the biomimetic sensor, UV Vis absorption spectroscopy and biomimetic sensor graphene oxide based on building bionic sensing system the optical potential, and UV - graphene oxide based on the potential application of.3. in the design of bionic sweet detection in the visible spectrum of bionic sensing system and the realization of the visible spectrum of nano composite sensing system based on graphene oxide, and explore its application in the interaction of biological molecules and biological molecules through detection. Nano sensors, graphene oxide and gold nanoparticles composite prepared by one-step method, and combined with the construction of the visible absorption spectrum of graphene oxide based nano composite Sensing system. Then explores the system in the application of detection of amino acids, peptides and proteins and other biological molecules in. At the same time, this paper also further design and has the specific binding sites of thrombin peptides were synthesized by self-assembly method makes it with graphene oxide / gold nanoparticles composite, constructed biosensor of graphene oxide / based on gold nanoparticles. Then build a visible spectrum biosensing system of graphene oxide / gold nanoparticles based on visible absorption spectroscopy detection technology, the realization of thrombin with high sensitivity and high specificity detection. These verified graphene oxide in constructing nano composite biochemical sensor potential, visible absorption spectra and composite the sensor based on the graphene oxide nano optical sensing system to build the system and potential in a variety of biological molecules, and detection of biomolecular interactions. The potential of application.

【学位授予单位】：浙江大学
【学位级别】：博士
【学位授予年份】：2017
【分类号】：TP212

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