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有機電化學晶體管在酶生物傳感器中的應用研究

發(fā)布時間:2018-03-17 18:35

  本文選題:有機電化學晶體管 切入點:酶生物傳感器 出處:《深圳大學》2017年碩士論文 論文類型:學位論文


【摘要】:由于具有低成本、容易制備、工作電壓低(1 V)、電化學活性強、可制備成柔性器件、環(huán)境穩(wěn)定性優(yōu)異、生物兼容性好等諸多優(yōu)點,有機電化學晶體管(Organic Electrochemical Transistors,OECTs)在生物化學傳感領(lǐng)域受到了廣泛的關(guān)注。而基于OECT的酶生物傳感器具有檢測靈敏度高及檢測極限低等特點,在一些重大疾病的預防及監(jiān)測診斷等方面具有非常好的應用前景。本論文主要以基于OECT的酶生物傳感器為研究對象,圍繞優(yōu)化OECT的器件制備工藝、利用OECT肌氨酸傳感器實現(xiàn)對肌氨酸的高靈敏檢測、基于OECT的無創(chuàng)唾液血糖試紙及血糖儀的應用研究初步探索等三個方面展開探討。研究并優(yōu)化了OECT的器件制備工藝。結(jié)果表明,器件在PBS溶液中可以穩(wěn)定工作,且溝道電流可調(diào)范圍大于1個數(shù)量級(VGS1 V),有利于其在酶生物傳感器中的應用。當VGS大于或等于0.7 V時,IDS達到相對平衡狀態(tài)時間較短,所需時間為20 s左右,說明器件能夠快速達到穩(wěn)定狀態(tài)。利用碳納米管、鉑納米顆粒及陽極多孔氧化鋁等修飾并改進OECT傳感器的柵電極,實現(xiàn)了對肌氨酸檢測性能的提高。結(jié)果表明,利用碳納米管修飾柵電極、鉑納米顆粒修飾柵電極、及鍍鉑AAO柵電極的OECT肌氨酸傳感器的最低檢測極限分別為50 nM、5 nM、50 nM,比不修飾納米材料的傳感器檢測極限降低了1-3個數(shù)量級。由于納米材料可以增加柵電極的比表面積,使有效肌氨酸氧化酶的負載量增大,同時碳納米管和鉑納米顆粒等具有較好的電催化能力,因此OECT傳感器對肌氨酸的檢測性能得到有效提高。由于對肌氨酸5 nM的檢測極限低于正常人和前列腺癌患者尿液中的肌氨酸濃度(2×10-8~5×10-6 M),因此可以滿足對尿液中的肌氨酸檢測的實際應用要求。研究了基于OECT的無創(chuàng)唾液血糖試紙及血糖儀。由于鉑電極的電催化能力較強,導電性好且性能穩(wěn)定,對葡萄糖的檢測性能較好,因此是OECT無創(chuàng)血糖試紙的一種理想電極。同時,OECT無創(chuàng)血糖儀可以實現(xiàn)對無創(chuàng)血糖試紙的配套使用,對糖尿病患者唾液樣本的檢測讀數(shù)可以反映出血液中的血糖濃度,并得到一定的線性關(guān)系。其中對早晨空腹唾液樣本檢測得到的線性關(guān)系較好,說明早晨空腹狀態(tài)下對患者唾液取樣得到的樣本受到的干擾較小,是比較理想的唾液取樣時機。初步探索表明,利用OECT的高靈敏檢測特性可以實現(xiàn)對唾液葡萄糖濃度(3-210μM)的檢測。
[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.
【學位授予單位】:深圳大學
【學位級別】:碩士
【學位授予年份】:2017
【分類號】:R446.1;TP212.3

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