基于聚苯胺衍生物的肿瘤标志物电化学检测

发布时间：2018-11-18 19:17

【摘要】：聚苯胺及其衍生物由于具有独特的光学和电学性能,为电化学生物传感器和其它化学传感器提供了一个优异的传感平台。本论文基于聚邻巯基苯胺、聚邻苯二胺/金、聚(乙烯基二茂铁-邻巯基苯胺)/金等材料,构建了以聚邻巯基苯胺为基底的癌胚抗原(CEA)电化学免疫传感界面,以及利用聚邻苯二胺/金、聚(乙烯基二茂铁-邻巯基苯胺)/金为电化学活性物质构建了肿瘤标志物双靶标(CEA和甲胎蛋白(AFP))电化学免疫传感器。另外,利用邻巯基苯胺与亚甲基蓝(MB)、Cu2+之间的特殊作用,制备了钴离子的比色检测体系。取得了以下研究成果： 1.通过化学氧化法合成了一种多巯基的共轭聚合物-聚邻巯基苯胺(PATP),其分子链由25个重复单元构成。利用这种导电的长链多巯基聚合物作为基底材料,通过Au-S键吸附金纳米颗粒,构建了一种灵敏的、非标记的CEA电化学免疫传感界面。在CEA的检测过程中,PATP具有良好的电子传递能力,同时分子链上的多巯基与金之间的牢固作用提高了传感界面的稳定性。在最佳条件下,传感器具有线性范围宽(1fg mL-1-10ng mL-1)、检测限低(0.015fg mL-1)、灵敏度高等特点。传感器对血清样品的检测结果与酶联免疫法的检测结果一致。 2.通过一步法合成了新型的聚邻苯二胺/金(POPD/Au)和聚(乙烯基二茂铁-邻巯基苯胺)/金(poly(VFc-ATP)/Au)纳米复合材料。利用这两种纳米复合材料良好的生物相容性、峰电位易区分、易修饰及制备简单等特性,以及POPD和poly(VFc-ATP)优异的电化学活性,制备了新型的肿瘤标志物探针,并以此构建了双靶标电化学免疫传感器,以CEA和AFP为模型检测对象对传感器检测性能进行了研究。对CEA和AFP的检测范围都是0.01-100ng mL-1,检测限分别为0.006ng mL-1和0.003ng mL-1(S/N=3)。对血清样品的检测结果与酶联免疫法的检测结果一致。 3.利用MB、邻巯基苯胺(ATP)和Cu2+之间的相互作用,得到了一种新的Co2+比色检测体系(MB-ATP-Cu2+)。通过调节Co2+的浓度,可以对还原态的MB实现不同程度的氧化,使检测体系呈现不同的颜色,达到对Co2+的可视化检测。其中检测范围为0.1mM-1.1mM,检测限为0.04mM。
[Abstract]:Polyaniline and its derivatives provide an excellent sensing platform for electrochemical biosensors and other chemical sensors due to their unique optical and electrical properties. Based on polymercaptoaniline, poly (o-phenylenediamine / gold), poly (vinylferrocene-o-mercaptoaniline) / gold, the electrochemical immunosensor interface of carcinoembryonic antigen (CEA) was constructed based on poly (o-mercaptoaniline). Using poly (o-phenylenediamine / gold) and poly (vinyl ferrocene-o-mercaptoaniline) / gold as electrochemical active substances, the double target tumor markers (CEA) and alpha-fetoprotein (AFP) electrochemical immunosensors were constructed. In addition, the colorimetric detection system of cobalt ion was prepared by using the special interaction between o-mercaptoaniline and methylene blue (MB), Cu2. Obtained the following research results: 1. A multi-mercapto conjugated polymer, poly (o-mercaptoaniline) (PATP), was synthesized by chemical oxidation. Its molecular chain consists of 25 repeating units. A sensitive, unlabeled CEA electrochemical immunosensor interface was constructed by using this conductive long chain polymercapto polymer as substrate material and gold nanoparticles were adsorbed by Au-S bond. In the process of CEA detection, PATP has good electron transfer ability, and the stability of the sensing interface is improved by the strong interaction between the multiple sulfhydryl groups and gold in the molecular chain. Under the optimum conditions, the sensor has the characteristics of wide linear range (1fg mL-1-10ng mL-1), low detection limit (0.015fg mL-1) and high sensitivity. The results of the detection of serum samples by the sensor were in agreement with the results of enzyme linked immunosorbent assay (Elisa). 2. Novel poly (o-phenylenediamine / gold (POPD/Au) and poly (vinyl ferrocene-o-mercaptoaniline) / gold (poly (VFc-ATP / Au) nanocomposites were synthesized by one-step method. The novel tumor marker probes were prepared by using the good biocompatibility, easy discrimination of peak potential, easy modification and preparation of the two nanocomposites, and the excellent electrochemical activity of POPD and poly (VFc-ATP). A double target electrochemical immunosensor was constructed, and the performance of the sensor was studied by using CEA and AFP as model detection objects. The detection limits of CEA and AFP are 0.006ng mL-1 and 0.003ng mL-1 (S/N=3), respectively. The results of detection of serum samples were consistent with those of enzyme linked immunosorbent assay (Elisa). 3. A new Co2 colorimetry system (MB-ATP-Cu2) was developed by using the interaction between (ATP) and Cu2 of MB, o-mercaptoaniline. By adjusting the concentration of Co2, the reduced MB can be oxidized to different degrees, the detection system presents different colors, and the visual detection of Co2 can be achieved. The detection range is 0.1mM-1.1 mMand the detection limit is 0.04mM.
【学位授予单位】：首都师范大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：R943;O657.1

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