基于金属负载型碳纳米管的适体电化学传感器的制备及应用
发布时间：2018-08-25 08:43
【摘要】：自碳纳米管(CNTs)被发现以来,因卓越的性能(如力学性能,电化学性质等),碳纳米管成为了科学领域的一大热点。相比于传统普通材料,碳纳米管电化学活性更高,比表面积更大。金属纳米粒子由于其颗粒体积小,电催化效率高等特点而得到广泛的应用,而负载金属纳米粒子的碳纳米管融合了两者的优势,在催化材料、电化学传感器等领域具有巨大的应用价值。本文将负载金属的碳纳米管修饰到玻碳电极表面,然后将凝血酶适体组装到修饰电极表面制备成适体传感器,并成功应用于凝血酶的分析检测中。所制得的传感器具有选择性好,稳定性高,线性范围宽等优点。本论文研究内容包括以下四个部分。第一章介绍了碳纳米管的概述、性质、制备以及金属负载型碳纳米管的制备和应用；核酸适体的简介、优势及其与凝血酶作用原理；核酸适体传感器的简介、分类、适体的固定方法；基于金属负载型碳纳米管的适体传感器的制备及其应用。第二章采用钯镍金属负载型羧基化碳纳米管(PdNi@CNTs)与季胺化碳纳米管(Q-CNTs)结合,先后修饰到玻碳电极表面,将构建的电化学传感器应用于H_2O_2的检测。通过循环伏安、交流阻抗、扫描电镜等方法对传感器进行了表征。该传感器具有较高的电催化活性,且稳定性和重现性较好。第三章以亚甲基蓝为电化学指示剂,结合Q-CNTs与PdNi@CNTs构建凝血酶适体传感器。将适体互补链(捕获探针)通过静电作用固定到修饰电极表面,让凝血酶适体与其杂交结合,制成凝血酶适体传感器。通过循环伏安、交流阻抗、扫描电镜等方法对传感器进行了表征。该适体传感器制备方法简单,操作简便,具有较宽的线性范围和较低的检出限,且选择性高。第四章制备了钯金属纳米粒子负载型碳纳米管(Pd@CNTs),构建了Pd@CNTs/Q-CNTs/GCE修饰电极。将巯基修饰的适体单链固定到电极表面,通过碱基互补配对形成DNA双链结构,以亚甲基蓝为电化学指示剂与DNA作用,制成凝血酶适体传感器。通过循环伏安、紫外分光光度法、差分脉冲伏安法等方法对传感器进行了表征。该凝血酶适体传感器能够实现对凝血酶的高灵敏检测,具有很好的应用前景。
[Abstract]:Since the discovery of carbon nanotubes (CNTs), carbon nanotubes (CNTs) have become a hot topic in the field of science because of their excellent properties (such as mechanical properties, electrochemical properties, etc.). Compared with conventional materials, carbon nanotubes have higher electrochemical activity and larger specific surface area. Metal nanoparticles have been widely used because of their small size and high electrocatalytic efficiency, while carbon nanotubes loaded with metal nanoparticles have combined the advantages of both in the catalytic materials. Electrochemical sensors and other fields have great application value. In this paper, carbon nanotubes loaded with metal were modified to the surface of glassy carbon electrode, then thrombin aptamer was assembled on the surface of modified electrode to prepare aptamer sensor, and it was successfully applied in the analysis and detection of thrombin. The sensor has the advantages of good selectivity, high stability and wide linear range. This thesis includes the following four parts. The first chapter introduces the overview of carbon nanotubes, properties, preparation, preparation and application of metal-loaded carbon nanotubes, the introduction of nucleic acid aptamers, their advantages and the principle of their interaction with thrombin, the introduction and classification of nucleic acid aptamers, Fixing method of aptamer, fabrication and application of aptamer sensor based on metal-supported carbon nanotubes. In chapter 2, palladium and nickel supported carboxylated carbon nanotubes (PdNi@CNTs) and quaternary amine carbon nanotubes (Q-CNTs) were used to modify the glassy carbon electrode. The electrochemical sensors were applied to the detection of H_2O_2. The sensor was characterized by cyclic voltammetry, AC impedance and scanning electron microscope. The sensor has high electrocatalytic activity and good stability and reproducibility. In chapter 3, using methylene blue as electrochemical indicator, thrombin aptamer sensor was constructed with Q-CNTs and PdNi@CNTs. The aptamer complementary chain (trap probe) was immobilized on the surface of the modified electrode by electrostatic action, and the thrombin aptamer was combined with it to form a thrombin aptamer sensor. The sensor was characterized by cyclic voltammetry, AC impedance and scanning electron microscope. The aptamer sensor has the advantages of simple preparation, simple operation, wide linear range, low detection limit and high selectivity. In chapter 4, palladium metal nanoparticles supported carbon nanotubes (Pd@CNTs) were prepared and Pd@CNTs/Q-CNTs/GCE modified electrodes were constructed. The thiol modified aptamer was immobilized on the electrode surface and the DNA double strand structure was formed by base complementary pairing. The thrombin aptamer sensor was made by using methylene blue as the electrochemical indicator and DNA as the electrochemical indicator. The sensor was characterized by cyclic voltammetry, UV spectrophotometry and differential pulse voltammetry. The thrombin aptamer sensor can be used to detect thrombin with high sensitivity.
【学位授予单位】：浙江大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1
[Abstract]:Since the discovery of carbon nanotubes (CNTs), carbon nanotubes (CNTs) have become a hot topic in the field of science because of their excellent properties (such as mechanical properties, electrochemical properties, etc.). Compared with conventional materials, carbon nanotubes have higher electrochemical activity and larger specific surface area. Metal nanoparticles have been widely used because of their small size and high electrocatalytic efficiency, while carbon nanotubes loaded with metal nanoparticles have combined the advantages of both in the catalytic materials. Electrochemical sensors and other fields have great application value. In this paper, carbon nanotubes loaded with metal were modified to the surface of glassy carbon electrode, then thrombin aptamer was assembled on the surface of modified electrode to prepare aptamer sensor, and it was successfully applied in the analysis and detection of thrombin. The sensor has the advantages of good selectivity, high stability and wide linear range. This thesis includes the following four parts. The first chapter introduces the overview of carbon nanotubes, properties, preparation, preparation and application of metal-loaded carbon nanotubes, the introduction of nucleic acid aptamers, their advantages and the principle of their interaction with thrombin, the introduction and classification of nucleic acid aptamers, Fixing method of aptamer, fabrication and application of aptamer sensor based on metal-supported carbon nanotubes. In chapter 2, palladium and nickel supported carboxylated carbon nanotubes (PdNi@CNTs) and quaternary amine carbon nanotubes (Q-CNTs) were used to modify the glassy carbon electrode. The electrochemical sensors were applied to the detection of H_2O_2. The sensor was characterized by cyclic voltammetry, AC impedance and scanning electron microscope. The sensor has high electrocatalytic activity and good stability and reproducibility. In chapter 3, using methylene blue as electrochemical indicator, thrombin aptamer sensor was constructed with Q-CNTs and PdNi@CNTs. The aptamer complementary chain (trap probe) was immobilized on the surface of the modified electrode by electrostatic action, and the thrombin aptamer was combined with it to form a thrombin aptamer sensor. The sensor was characterized by cyclic voltammetry, AC impedance and scanning electron microscope. The aptamer sensor has the advantages of simple preparation, simple operation, wide linear range, low detection limit and high selectivity. In chapter 4, palladium metal nanoparticles supported carbon nanotubes (Pd@CNTs) were prepared and Pd@CNTs/Q-CNTs/GCE modified electrodes were constructed. The thiol modified aptamer was immobilized on the electrode surface and the DNA double strand structure was formed by base complementary pairing. The thrombin aptamer sensor was made by using methylene blue as the electrochemical indicator and DNA as the electrochemical indicator. The sensor was characterized by cyclic voltammetry, UV spectrophotometry and differential pulse voltammetry. The thrombin aptamer sensor can be used to detect thrombin with high sensitivity.
【学位授予单位】：浙江大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1
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