氧化锌纳米材料基生物传感器的构建及性能研究

发布时间：2018-08-29 16:56

【摘要】：纳米生物传感器是在生物传感器件领域引入纳米材料与技术以期获得灵敏度高、抗干扰性强、长效稳定、分析实时迅速、简单便携和成本低廉的检测器件。氧化锌(ZnO)纳米材料具有大的比表面积、高的等电点、优良的电子输运性能、较强的生物相容性,被广泛应用于纳米器件的构建及性能研究中。而贵金属金纳米颗粒也具有良好的导电性、生物兼容性和电催化活性等。因此,本文围绕ZnO纳米材料及其贵金属Au纳米颗粒复合物的制备、电催化性能和相应生物传感器件的性能方面开展了系统性的研究,主要内容如下：分别采用化学气相沉积法和水热法,可控制备ZnO微/纳线、ZnO纳米线及Al掺杂的ZnO纳米片,利用光还原法结合静电自组装技术成功地在纳米片上修饰Au纳米颗粒。通过场发射扫描电镜、能谱分析仪、X射线衍射仪、共聚焦拉曼光谱仪、X射线光电子能谱技术、透射电镜等仪器手段对形貌、成分和结构进行表征。优化ZnO线和纳米Au颗粒修饰Al掺杂ZnO纳米片的制备工艺参数。设计构筑了单根ZnO微/纳线基酶电极电化学尿酸生物传感器,采用循环伏安法和计时电流法标定器件的灵敏度高达89.74μA cm-2mM-1,线性检测范围宽为100μM～0.59mM(人体血尿酸的正常含量范围为90μM～0.42mM).并研究了器件的抗干扰性优劣,分析器件的实际应用前景。构建了大面积ZnO纳米线生物酶电极,该酶电极传感器对乳酸溶液的线性检测范围宽12μM～1.2mM,灵敏度15.6μAcm-2mM-1,探测下限12μM,米氏常数低至0.85mM。探究了器件性能的影响因素,分析如何进一步改善其性能。设计并构建了Al掺ZnO纳米片电化学乳酸生物传感器,其灵敏度为33.46μA cm-2mM-1,线性探测范围宽1.2μM～0.12mM,米氏常数为0.25mM,这是通过Al的掺杂和ZnO的垂直纳米片结构提高了材料的导电性和酶电极的电子传输特性而得以实现的。该传感器性能相对优于纯ZnO纳米线等乳酸传感器。对比研究了引入纳米Au颗粒后,Al掺ZnO纳米片乳酸生物传感器的性能,发现其灵敏度提高至115.65μAcm-2mM-,线性检测范围展宽为0.6μM～0.18mM,米氏常数降低至0.2mM。Au纳米颗粒优异的电催化活性、电子传输特性和生物兼容性以及Au颗粒引入的更大材料表面积便得器件的性能得以明显改善。
[Abstract]:Nano-biosensor is a kind of detection device with high sensitivity, strong anti-interference, long-term effect and stability, rapid analysis, simple portability and low cost, which is introduced into the field of biosensor devices. Zinc oxide (ZnO) nanomaterials have been widely used in the construction and study of nanodevices for their large specific surface area, high isoelectric point, excellent electronic transport performance and strong biocompatibility. The noble metal gold nanoparticles also have good electrical conductivity, biological compatibility and electrocatalytic activity. Therefore, the preparation of ZnO nanomaterials and their noble metal Au nanoparticles composites, the electrocatalytic properties and the properties of the corresponding biosensor devices have been systematically studied in this paper. The main contents are as follows: ZnO micro / nanowire ZnO nanowires and Al doped ZnO nanowires were prepared by chemical vapor deposition and hydrothermal method respectively. Au nanoparticles were successfully modified by photoreduction method and electrostatic self-assembly technique. The morphology, composition and structure were characterized by means of field emission scanning electron microscope, energy spectrum analyzer, confocal Raman spectrometer, X-ray photoelectron spectroscopy and transmission electron microscope. The preparation parameters of Al doped ZnO nanoparticles modified by ZnO wire and Au nanoparticles were optimized. A single ZnO micro/ nanowire enzyme electrode electrochemical uric acid biosensor was designed and constructed. The sensitivity of calibrating device by cyclic voltammetry and chronoamperometric method is as high as 89.74 渭 A cm-2mM-1,. The linear detection range is 100 渭 M~0.59mM (the normal content range of human serum uric acid is 90 渭 M~0.42mM). The merits and demerits of the device are studied, and the practical application prospect of the device is analyzed. A large area of ZnO nanowire bioenzyme electrode was constructed. The linear detection range of the enzyme electrode sensor for lactic acid solution was 12 渭 m ~ (-1) mm, the sensitivity was 15.6 渭 Acm-2mM-1, the detection limit was 12 渭 M, and the Michaelis constant was as low as 0.85 mm. The influencing factors of device performance are discussed, and how to further improve its performance is analyzed. An electrochemical lactate biosensor with Al doped ZnO nanoparticles was designed and constructed. The sensitivity is 33.46 渭 A cm-2mM-1, with a linear detection range of 1.2 渭 MN 0.12 mm and a Michaelis constant of 0.25 mm. This is achieved through the doping of Al and the enhancement of the electrical conductivity of the material and the electron transport characteristics of the enzyme electrode by the doping of Al and the vertical nanochip structure of ZnO. The performance of the sensor is better than that of pure ZnO nanowires. The performance of lactic acid biosensor with Al doped ZnO nanoparticles after the introduction of nanometer Au particles was compared. It was found that the sensitivity of the biosensor was increased to 115.65 渭 Acm-2mM-, and the linear detection range was expanded to 0. 18 mm, and the Michaelis constant was reduced to the excellent electrocatalytic activity of 0.2mM.Au nanoparticles. The properties of the device can be improved obviously by electron transport characteristics and biological compatibility, as well as by the introduction of larger surface area of Au particles.
【学位授予单位】：北京科技大学
【学位级别】：博士
【学位授予年份】：2015
【分类号】：TB383.1;O614.241

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