基于金属石墨烯纳米复合材料构建电化学生物传感器的研究及应用

发布时间：2018-04-19 08:26

本文选题：电化学传感器 + 纳米复合材料　；参考：《济南大学》2017年硕士论文

【摘要】：电化学免疫传感器作为一种新型的检测方法已被广泛应用于不同的领域中。本论文利用不同的方法制备了一系列具有催化性能以及生物相容性较好、导电能力强等优点的纳米复合材料,并将纳米复合材料应用于对电化学免疫传感器的构建中以实现对目标生物分子的定量检测。石墨烯作为一种具有二维结构的纳米材料具有较大的BET比表面积、良好的导电能力、生物相容性好等优点而被广泛应用于电化学免疫传感器中。金属纳米粒子生物相容性好并且具有较好的催化性能,其构建的复合材料较好的保留了金属粒子的相关特性。金属石墨烯复合材料结合了两者的优点有效地改善了传感器的相关性能。本论文主要包括以下五个部分:第一部分,首先对电化学传感器、传感器的类型、纳米材料、生物分子的定义及其基本特性进行了介绍,最后介绍了该论文的研究内容。第二部分,以氨基化石墨烯金(Au-NH_2-rGO)作为基底材料,具有三维结构的石墨烯-碳纳米管-钯(rGO-MWCNT-Pd)作为二抗标记物构建了夹心型免疫传感器实现了对前列腺特异抗原(PSA)的定量检测。以三维结构的rGO-MWCNT-Pd纳米复合材料作为信号放大器,在降低传感器的检出限、拓宽检测范围方面发挥了重要作用。该传感器对PSA的检测范围为0.5 pg/mL至15.0ng/mL,检出限为0.17 pg/mL并将该传感器成功用于对实际样品的检测中。第三部分,通过原位还原的方法将非贵金属镍与贵金属铂、金三种元素进行掺杂制备了镍铂金-还原石墨烯(Ni AuPt-rGO)纳米复合材料,由于三金属之间的协同作用使得NiAuPt-rGO对双氧水(H_2O_2)具有较强的催化能力。以水溶性好识别能力强的环糊精-石墨烯(β-CD@rGO)作为基底材料,NiAuPt-rGO作为二抗标记物催化H_2O_2构建了一种夹心型免疫传感器,实现对癌胚抗原(CEA)的定量检测。该传感器对癌胚抗原的线性检测范围为0.001-100.0 ng/mL,检出限为0.27 pg/mL并展现出良好的重现性、稳定性以及较高的选择性等性能。第四部分,利用原位还原的方法制备了石墨烯-四氧化三铁@金钴(rGO@Fe_3O_4@AuCo)磁性纳米复合材料。具有较大直径的Fe_3O_4纳米粒子的加入防止了rGO的团聚增大了复合材料的比表面积,为AuCo纳米粒子的负载提供了较多的结合位点。基于以上材料构建了检测AFP夹心型免疫传感器,检测范围在0.5 pg/mL-50.0 ng/mL,检出限为0.18 pg/mL,对AFP的临床检测具有重要的应用价值。第五部分,利用1,8-二氨基萘氨基化石墨烯制备了1,8-二氨基萘-石墨烯-金(1,8-DN-rGO-Au)并将其作为传感器的基底材料捕获抗体,以具有三维结构的三维刺状四氧化三铁@二氧化钛@金银@环糊精(Fe_3O_4@TiO_2@AuAg@β-CD)纳米复合材料作为二抗标记物构建了夹心型免疫传感器。该传感器对PSA的检测范围为0.5 pg/mL-100.0 ng/mL,检出限为0.2 pg/mL。并且具有良好的稳定性、选择性以及重现性等优点,该传感器具有临床检测分析的应用前景。
[Abstract]:Electrochemical immunosensor as a new detection method has been widely used in different fields.In this paper, a series of nanocomposites with good catalytic performance, good biocompatibility and strong conductivity were prepared by different methods.Nanocomposites were applied to the construction of electrochemical immunosensors for quantitative detection of target biomolecules.Graphene is widely used in electrochemical immunosensors because of its large BET specific surface area, good conductivity, good biocompatibility and so on.Metal nanoparticles have good biocompatibility and good catalytic performance.Metal graphene composites combine the advantages of the two to improve the performance of the sensor.This thesis mainly includes five parts as follows: in the first part, the electrochemical sensor, the type of sensor, the nanomaterials, the definition of biomolecules and their basic characteristics are introduced. Finally, the research content of this thesis is introduced.In the second part, a sandwich immunosensor was constructed using Au-NH2-rGOA as substrate material and graphene carbon nanotube palladium (PD) as a second antibody marker to realize the quantitative detection of prostate specific antigen (PSAs).Three-dimensional rGO-MWCNT-Pd nanocomposites as signal amplifiers play an important role in reducing the detection limit and widening the detection range of the sensor.The detection range of PSA is 0. 5 pg/mL to 15. 0 ng / mL, and the detection limit is 0. 17 pg/mL. The sensor has been successfully used in the detection of real samples.In the third part, Nickel-platinum / reduced graphene Ni AuPt-rGOA nanocomposites were prepared by doping non-precious metal nickel with precious metal platinum and gold by in-situ reduction.Due to the synergistic effect of trimetals, NiAuPt-rGO has a strong catalytic activity for H _ 2O _ 2 (H _ 2O _ 2).A sandwich immunosensor was constructed by using 尾 -CDDP-graphene (尾 -CDR) as the substrate material and NiAuPt-rGO as the second antibody marker to construct a sandwich immunosensor for the quantitative detection of carcinoembryonic antigen (CEA).The linear detection range of carcinoembryonic antigen was 0.001-100.0 ng / mL, and the detection limit was 0.27 pg/mL. The sensor showed good reproducibility, stability and high selectivity.In the fourth part, in situ reduction method was used to prepare the magnetic nanocomposites of graphene / Fe _ 2O _ 4 @ AuCo _ 2O _ 4 / Co _ (3) O _ (3) O _ (4) O _ (4) O _ (4) O _ (4) AuCoC.The addition of Fe_3O_4 nanoparticles with large diameters prevents the agglomeration of rGO from increasing the specific surface area of the composites and provides more binding sites for the loading of AuCo nanoparticles.Based on the above materials, a sandwich immunosensor for detection of AFP was constructed. The detection range was 0.5 pg/mL-50.0 ng / mL, and the detection limit was 0.18 PG / mL, which has important application value for clinical detection of AFP.In the fifth part, we prepared 1H8-diaminonaphthalene-graphene-Amino-au) and used it as the substrate material of the sensor to capture the antibody.A sandwich immunosensor was constructed using three-dimensional spinned-iron trioxide @ titanium dioxide @ gold and silver @ cyclodextrin / tio _ 3O _ 4tio _ 4tio _ 2d AuAg@ 尾 -CDCD nanocomposite as a second antibody marker.The detection range of PSA is 0.5 pg/mL-100.0 / mL and the detection limit is 0.2 PG / mL.The sensor has the advantages of good stability, selectivity and reproducibility.
【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】：O657.1;TP212

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