二硫化钼纳米片及石墨烯功能材料的生物传感应用

发布时间：2018-06-02 05:23

本文选题：二硫化钼纳米片 + 石墨烯功能化　；参考：《吉林大学》2017年硕士论文

【摘要】：二维片层材料,特别是二维二硫化钼和石墨烯材料,近年来受到广泛关注。二维二硫化钼材料因具有大的比表面积、可调的带隙、独特的物理和化学性质而备受青睐,在光电领域应用得到越来越多的关注。而纯石墨烯缺陷少、成本高、零带隙等特点,使其在实际应用过程中受到诸多限制。因此,通过掺杂、负载等手段,改善石墨烯的性能并扩展其应用范围,已成为当前研究者亟待解决的重要问题。本文的第一部分通过模板导向的高温裂解法制备了具有窄带隙、高光电活性的超薄二硫化钼(Mo S_2)纳米片层材料,并以二维Mo S_2纳米片为光电活性材料,制备了高可见光敏感的光电化学葡萄糖传感器。首先,通过系列物理化学手段,对二维材料的微观结构和形貌进行了详细的表征和研究,结果表明,Mo S_2超薄纳米片呈三维网状结构,具有大的比表面积。其次,以葡萄糖氧化酶为例,基于三维网状结构对酶的优良吸附性能,构建了新型高可见光敏感的光电化学葡萄糖传感器。上述三维孔状结构设计不仅有效提高了传感器的光电化学催化活性,而且利于缩短光电极表面与酶活性中心之间的电子传输距离,在实现对葡萄糖进行快速、超灵敏检测的同时,也显著提高了对目标物质检测的选择性。本文所构筑的基于二维Mo S_2光电活性材料的新型光电化学生物传感器,为二维片层材料在光电化学检测领域的可能应用提供了支持。本文的第二部分采用原位热解法,获得了三维多孔氮掺杂石墨烯(NGr)负载的超小碳化铁(Fe_3C)纳米粒子,系统研究其过氧化物模拟酶性能。研究发现,在H2O2存在下,所制备的Fe_3C/NGr能够催化氧化3,3',5,5'-四甲基联苯胺(TMB),而使溶液呈现蓝色,这种变色变化证明了Fe_3C/NGr具有本征过氧化物酶活性。基于Fe_3C/NGr和TMB的显色反应,本文系统研究了通过目视比色法进行葡萄糖检测的可行性。其检测原理如下:首先,葡萄糖氧化酶催化氧化葡萄糖生成葡萄糖酸和H2O2;其次,通过测量Fe_3C/NGr催化TMB和H2O2反应体系的吸光度值(溶液颜色与反应生成的H2O2浓度呈正比),实现了对葡萄糖的目视比色测定。目视觉比色法具有快速检测、成本低廉、过程简单、易于操作和普适性等优点,有利于规模化生成和推广使用。
[Abstract]:Two-dimensional lamellar materials, especially two-dimensional molybdenum disulfide and graphene materials, have attracted wide attention in recent years. Due to its large specific surface area, adjustable band gap and unique physical and chemical properties, two-dimensional molybdenum disulfide has attracted more and more attention in the field of photoelectricity. However, the defects of pure graphene are low, the cost is high and the band gap is zero, so it is limited in practical application. Therefore, improving the properties of graphene and extending its application range by doping and loading has become an important problem to be solved. In the first part of this paper, ultrathin molybdenum disulfide (MoS _ 2) nanolamellae with narrow band gap and high photoactivity was prepared by template-oriented high-temperature pyrolysis method, and two dimensional molybdenum disulfide (MoS) _ 2 nanocrystals were used as photoactive materials. A photoelectrochemical glucose sensor with high visible light sensitivity was prepared. Firstly, the microstructure and morphology of the two-dimensional materials were characterized and studied by a series of physical and chemical methods. The results show that the ultrathin MOS _ 2 nanostructures have a three-dimensional reticular structure and a large specific surface area. Secondly, taking glucose oxidase as an example, a novel photochemical glucose sensor with high visible light sensitivity was constructed based on the excellent adsorption performance of the three-dimensional reticular structure on the enzyme. The above three-dimensional pore structure design not only improves the photochemical catalytic activity of the sensor, but also shortens the electron transport distance between the photoelectrode surface and the enzyme active center. In addition to hypersensitive detection, the selectivity of target substance detection is improved significantly. In this paper, a novel photochemical biosensor based on 2-D MoS _ 2 photoactive material is constructed, which provides support for the possible application of two-dimensional lamellar material in photochemical detection. In the second part of this paper, in situ pyrolysis method was used to obtain ultrasmall Fe _ 3C _ 3C _ 3 nanoparticles loaded with three dimensional porous nitrogen-doped graphene (NGR), and their peroxide-mimic enzyme properties were systematically studied. It was found that in the presence of H2O2, the prepared Fe_3C/NGr could catalyze the oxidation of TMBs in the presence of 3H 3N, 5N, 5N and tetramethyl benzidine, and make the solution blue. This discoloration indicates that the Fe_3C/NGr has intrinsic peroxidase activity. Based on the color reaction of Fe_3C/NGr and TMB, the feasibility of glucose detection by visual colorimetry was studied systematically. The detection principle is as follows: firstly, glucose oxidase catalyzes the oxidation of glucose to form gluconic acid and H _ 2O _ 2; secondly, The visual colorimetric determination of glucose was achieved by measuring the absorbance of TMB and H2O2 catalyzed by Fe_3C/NGr (the color of solution was proportional to the concentration of H2O2 produced by the reaction). Eye vision colorimetry has the advantages of rapid detection, low cost, simple process, easy operation and universality.
【学位授予单位】：吉林大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB34;TP212.3

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