基于多孔纳米通道的糖超灵敏传感器的研究

发布时间：2018-11-27 18:44

【摘要】：糖作为生命体的三大物质单元之一,在自然界中在广泛存在,在生命活动中起着至关重要的作用。其不仅作为能量物质为维持生命体的活动提供能量来源,还作为结构物质为细胞的构建提供骨架单元,而且它还有许多不为人所熟知的功能,如免疫反应、癌症的转移、细胞之间的沟通、病原体引起的传染病等。糖的检测和识别对研究生命体的生理过程以及疾病的产生与转移有着重要的意义。因此对生物体内各种糖的识别和检测已经成为生命科学领域的重要内容,开发对糖具有高选择性和高灵敏度的传感器有着重要的意义。受自然界中细胞膜上离子通道的启发,通过人工合成的方法之制备出具有选择性、响应性和可控性的传感器件,实现对糖的超灵敏性的检测,对生物、化学和材料学尤其是生物传感领域都有着十分重要的理论和实际意义。本论文以苯硼酸、二肽单元为识别单元、硫脲为协同单元、异丙基丙烯酰胺为功能单元,分别合成对糖具有响应性的二元和三元智能共聚物,将其修饰到多孔阳极氧化铝膜的内壁,并利用皮安计检测的方法,构建一种新型的智能纳米通道,用于多种糖的高灵敏性和高选择性识别。本论文的工作分为以下三个部分:第一章为综述部分。对近年来糖的传感器进行了梳理,分为硼酸类受体和非硼酸类受体的糖传感器。并对多孔阳极氧化铝膜在构建智能纳米通道中的应用做了简要的介绍,进一步介绍了本论文研究的目的和内容。第二章将3-丙烯酰硫脲基苯硼酸(ATPBA)与N-异丙基丙烯酰胺(NIPAAm)通过可逆加成-断裂链转移聚合(RAFT)合成的糖响应性聚合物PNIPAm-co-PATPBA修饰到PAA膜的内壁中,构建对糖具有响应性的智能纳米通道。并对修饰的后的PAA膜进行了扫描电子显微镜(SEM)、X射线光电子能谱(XPS)的表征。利用皮安计对构建的纳米通道对葡萄糖、甘露糖、阿拉伯糖和木糖的响应性进行了表征。结果表明我们构建的传感器对糖具有灵敏的响应性和选择性,当糖浓度为10-7 M时,阿拉伯糖、木糖、甘露糖和葡萄糖的电流变化率分别为50%、25%、60%和90%,从而实现对葡萄糖的高灵敏检测。第三章以具有手性识别作用功能性单元二肽分子(β-Asp-Phe)、响应性单元异丙基丙烯酰胺(PNIPAAm)和起调节作用的苯基硫脲单体合成的三元共聚物(PNI-β-MAP-diTFP)修饰多孔阳极氧化铝薄膜,构建对糖对映体具有不同响应性的智能纳米通道,通过皮安计的测量来苏糖对映体通过纳米通道时电流的变化,实现响应性的信号的传递和放大,用于糖对映体的检测和识别。
[Abstract]:As one of the three major material units of life, sugar exists widely in nature and plays a vital role in life activities. Not only does it provide a source of energy for sustaining the activity of life, but it also provides a skeleton unit for cell construction as a structural substance, and it also has many unknown functions, such as immune responses, cancer metastasis, Communication between cells, infectious diseases caused by pathogens, etc. The detection and recognition of sugar plays an important role in the study of physiological processes of organisms and the generation and transfer of diseases. Therefore, the recognition and detection of sugar in organisms has become an important content in the field of life science, and it is of great significance to develop sensors with high selectivity and sensitivity to sugar. Inspired by ion channels on cell membranes in nature, selective, responsive and controllable sensing devices were prepared by artificial synthesis to detect the hypersensitivity of sugar. Chemistry and material science, especially biosensor, have important theoretical and practical significance. In this paper, binary and ternary intelligent copolymers were synthesized with phenylboric acid and dipeptide units as recognition units, thiourea as synergistic units and isopropyl acrylamide as functional units, respectively. It was modified into the inner wall of porous anodic alumina membrane, and a novel intelligent nanochannel was constructed by using the method of picoammeter detection, which can be used for the high sensitivity and high selectivity recognition of many kinds of sugar. The work of this thesis is divided into three parts: the first chapter is the summary part. The sugar sensors in recent years are sorted into boric acid receptors and non-boric acid receptors. The application of porous anodic alumina membrane in the construction of smart nanochannels is briefly introduced, and the purpose and content of this thesis are further introduced. In chapter 2, the glycosylresponsive polymer (PNIPAm-co-PATPBA) synthesized by reversible addition-break chain transfer polymerization (RAFT) with 3-acryloyl thiourea-phenylborate (ATPBA) and N-isopropylacrylamide (NIPAAm) was modified into the inner wall of PAA film. An intelligent nanochannel responsive to sugar was constructed. The modified PAA films were characterized by scanning electron microscopy (SEM) (SEM), X-ray photoelectron spectroscopy (XPS). The responsiveness of the constructed nanochannels to glucose, mannose, arabinose and xylose was characterized by a picoammeter. The results showed that the sensor was sensitive and selective to sugar. When sugar concentration was 10-7 M, the current change rates of arabinose, xylose, mannose and glucose were 50% and 90%, respectively. In order to achieve the high sensitivity of glucose detection. In Chapter 3, the chiral recognition of functional unit dipeptide molecules (尾-Asp-Phe), Reactive unit isopropyl acrylamide (PNIPAAm) and a terpolymer (PNI- 尾-MAP-diTFP) synthesized by adjusting phenyl thiourea monomer were used to modify porous anodic alumina film. An intelligent nanochannel with different responsiveness to glucose enantiomers was constructed. The changes of electric current of threonose enantiomers through nanowires were measured by a picoammeter to transmit and amplify responsive signals for detection and recognition of sugar enantiomers.
【学位授予单位】：武汉理工大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TB383.1;TP212

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