有机电化学晶体管在酶生物传感器中的应用研究

发布时间：2018-03-17 18:35

本文选题：有机电化学晶体管　切入点：酶生物传感器　出处：《深圳大学》2017年硕士论文　论文类型：学位论文

【摘要】：由于具有低成本、容易制备、工作电压低(1 V)、电化学活性强、可制备成柔性器件、环境稳定性优异、生物兼容性好等诸多优点,有机电化学晶体管(Organic Electrochemical Transistors,OECTs)在生物化学传感领域受到了广泛的关注。而基于OECT的酶生物传感器具有检测灵敏度高及检测极限低等特点,在一些重大疾病的预防及监测诊断等方面具有非常好的应用前景。本论文主要以基于OECT的酶生物传感器为研究对象,围绕优化OECT的器件制备工艺、利用OECT肌氨酸传感器实现对肌氨酸的高灵敏检测、基于OECT的无创唾液血糖试纸及血糖仪的应用研究初步探索等三个方面展开探讨。研究并优化了OECT的器件制备工艺。结果表明,器件在PBS溶液中可以稳定工作,且沟道电流可调范围大于1个数量级(VGS1 V),有利于其在酶生物传感器中的应用。当VGS大于或等于0.7 V时,IDS达到相对平衡状态时间较短,所需时间为20 s左右,说明器件能够快速达到稳定状态。利用碳纳米管、铂纳米颗粒及阳极多孔氧化铝等修饰并改进OECT传感器的栅电极,实现了对肌氨酸检测性能的提高。结果表明,利用碳纳米管修饰栅电极、铂纳米颗粒修饰栅电极、及镀铂AAO栅电极的OECT肌氨酸传感器的最低检测极限分别为50 nM、5 nM、50 nM,比不修饰纳米材料的传感器检测极限降低了1-3个数量级。由于纳米材料可以增加栅电极的比表面积,使有效肌氨酸氧化酶的负载量增大,同时碳纳米管和铂纳米颗粒等具有较好的电催化能力,因此OECT传感器对肌氨酸的检测性能得到有效提高。由于对肌氨酸5 nM的检测极限低于正常人和前列腺癌患者尿液中的肌氨酸浓度(2×10-8~5×10-6 M),因此可以满足对尿液中的肌氨酸检测的实际应用要求。研究了基于OECT的无创唾液血糖试纸及血糖仪。由于铂电极的电催化能力较强,导电性好且性能稳定,对葡萄糖的检测性能较好,因此是OECT无创血糖试纸的一种理想电极。同时,OECT无创血糖仪可以实现对无创血糖试纸的配套使用,对糖尿病患者唾液样本的检测读数可以反映出血液中的血糖浓度,并得到一定的线性关系。其中对早晨空腹唾液样本检测得到的线性关系较好,说明早晨空腹状态下对患者唾液取样得到的样本受到的干扰较小,是比较理想的唾液取样时机。初步探索表明,利用OECT的高灵敏检测特性可以实现对唾液葡萄糖浓度(3-210μM)的检测。
[Abstract]:Due to its advantages of low cost, easy preparation, low working voltage, high electrochemical activity, excellent environmental stability, good biocompatibility and so on, it can be made into flexible devices. Organic Electrochemical transistors have attracted wide attention in the field of biochemical sensing. The enzyme biosensor based on OECT has the characteristics of high detection sensitivity and low detection limit. In this paper, the enzyme biosensor based on OECT is taken as the research object, and the fabrication technology of OECT device is optimized. The high sensitivity detection of sarcosine was realized by using OECT sarcosine sensor, the application of non-invasive salivary blood glucose test paper based on OECT and the application of blood glucose instrument were discussed in three aspects. The fabrication process of OECT device was studied and optimized. The device can work stably in PBS solution, and the channel current adjustable range is more than 1 order of magnitude, which is beneficial to its application in enzyme biosensor. When VGS is greater than or equal to 0.7 V, the relative equilibrium time is relatively short. The time required is about 20 s, which shows that the device can reach stable state quickly. The gate electrode of OECT sensor is modified and improved by carbon nanotubes, platinum nanoparticles and porous anodic alumina, etc. The results showed that the gate electrode was modified by carbon nanotubes and the gate electrode modified by platinum nanoparticles. The lowest detection limit of OECT sarcosine sensor with platinum plated AAO gate electrode is 50 nm M5 nm M, which is 1 ~ 3 orders of magnitude lower than that of unmodified nanomaterials. Because nanometer material can increase the specific surface area of gate electrode, The loading amount of effective sarcosine oxidase was increased, and carbon nanotubes and platinum nanoparticles had good electrocatalytic ability. Therefore, the detection performance of sarcosine by OECT sensor has been improved effectively. Because the detection limit of 5 nm of sarcosine is lower than that of urine of normal people and prostate cancer patients, the detection limit is 2 脳 10 ~ (-8) ~ 5 脳 10 ~ (-6) M ~ (-1), so it can satisfy the value of muscle in urine. The paper studies the non-invasive saliva blood glucose test paper and blood sugar instrument based on OECT. Because of the strong electrocatalytic ability of platinum electrode, It is an ideal electrode for OECT noninvasive blood glucose test paper. At the same time, it can realize the complete use of noninvasive blood glucose test paper. The detection readings of saliva samples from diabetic patients can reflect the blood glucose concentration and obtain a certain linear relationship, among which the linear relationship is better for the fasting saliva samples in the morning. The results showed that the sample taken from saliva in the morning was less disturbed, and it was an ideal time to sample saliva. The preliminary exploration showed that the detection of salivary glucose concentration 3-210 渭 M could be realized by using the highly sensitive detection characteristic of OECT.
【学位授予单位】：深圳大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：R446.1;TP212.3

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