【摘要】：隨著材料科學(xué)和電化學(xué)傳感器的深入發(fā)展,運(yùn)用單一材料制備的常規(guī)電化學(xué)傳感器已經(jīng)不能滿足研究者們的要求�？茖W(xué)家們嘗試將具有不同特性的材料組合在一起形成新的復(fù)合材料對(duì)電極進(jìn)行修飾,期望復(fù)合材料各組分之間的協(xié)同作用帶給電極新的電化學(xué)特性。溫敏性聚合物表現(xiàn)出溫度控制的分子構(gòu)型轉(zhuǎn)變,納米碳材料具有優(yōu)良的電子傳導(dǎo)能力和電催化性能。將二者混合制備納米復(fù)合材料,用來直接修飾電極或者在電極表面固定氧化還原蛋白質(zhì),能得到具備溫度響應(yīng)特性的電化學(xué)傳感器。通過調(diào)節(jié)環(huán)境溫度實(shí)現(xiàn)對(duì)傳感器電化學(xué)性能的智能調(diào)控,為電化學(xué)傳感領(lǐng)域開辟了新的研究方向。本論文的主要工作概括如下:(1)用沉淀聚合方法合成了具有溫敏性的聚N-乙烯基己內(nèi)酰胺均聚物(PVCL),通過變溫紫外測試證實(shí):合成的PVCL具有溫敏性質(zhì),低臨界溶解溫度(LCST)為30℃。(2)用氧化石墨烯(GO)和PVCL在玻碳電極表面修飾一層“夾心式”的溫敏性GO/PVCL/GO復(fù)合膜。以PVCL的LCST溫度(30℃)為界,復(fù)合膜修飾電極檢測鄰苯二酚(1,2-Benzenediol,CC)與對(duì)苯二酚(Hydroquinone,HQ)時(shí)表現(xiàn)出明顯的溫度響應(yīng)電化學(xué)“開-關(guān)”效應(yīng),并且具有可逆性。電極在高溫“開”狀態(tài)下能對(duì)溶液中的CC和HQ進(jìn)行同時(shí)檢測,且具有較寬的線性范圍。(3)用羧基化多壁碳納米管(MWCNT(COOH))、GO和PVCL混合修飾玻碳電極,制備了具有溫度響應(yīng)特性的PSG電極。以30℃為界,對(duì)乙酰氨基苯酚(4-Acetamino phenol,AP)在PSG電極上的電化學(xué)響應(yīng)信號(hào)具有明顯的溫度響應(yīng)“開-關(guān)”特性。在26℃和36℃之間反復(fù)改變?nèi)芤簻囟?AP在36℃的峰電流衰減小,溫度開關(guān)具有可逆性。“開”狀態(tài)下,PSG電極能在較寬的線性范圍和低檢出限下檢測溶液中的AP。(4)將葡萄糖氧化酶(GOD)包覆于還原型氧化石墨烯(rGO)與PVCL復(fù)合膜中,固定在玻碳電極表面,構(gòu)筑了具有溫度響應(yīng)特性的GOD生物傳感器。rGO-PVCL復(fù)合膜能為GOD提供一個(gè)良好的生物微環(huán)境,保持GOD的生物活性。溫度低于30℃,GOD活性低;當(dāng)溫度高于30℃時(shí),GOD在電極表面進(jìn)行快速的直接電子轉(zhuǎn)移,對(duì)溶液中葡萄糖的電催化活性高。高溫時(shí)檢測葡萄糖的精密度好并且靈敏度高。
[Abstract]:With the development of materials science and electrochemical sensors, conventional electrochemical sensors based on a single material can no longer meet the requirements of researchers. Scientists try to combine materials with different characteristics to form new composite materials to modify electrodes, expecting synergy between the components of composite materials. Temperature-sensitive polymers exhibit temperature-controlled molecular configurations and nano-carbon materials exhibit excellent electronic conductivity and electrocatalytic properties. Nanocomposites prepared by mixing the two materials can be used to modify the electrode directly or to immobilize redox proteins on the surface of the electrode. The main work of this paper is summarized as follows: (1) Poly (N-vinylcaprolactam) homopolymer (PVCL) with thermo-sensitivity was synthesized by precipitation polymerization method, and its electrochemical properties were controlled intelligently by adjusting ambient temperature. Temperature-sensitive properties of PVCL were confirmed by UV-Vis spectroscopy. Low critical solution temperature (LCST) of PVCL was 30. (2) Graphite oxide (GO) and PVCL were used to modify a "sandwich" thermosensitive GO/PVCL/GO composite film on the surface of glassy carbon electrode. Hydroquinone (HQ) exhibits an obvious "on-off" effect in temperature-responsive electrochemistry and is reversible. The electrode can simultaneously detect C and HQ in solution at high temperature and has a wide linear range. (3) Carboxylated multi-walled carbon nanotubes (MWCNT (COOH), GO and PVCL are used to modify glassy carbon. A PSG electrode with temperature response characteristics was prepared. The electrochemical response signal of 4-Acetamino phenol (AP) on the PSG electrode has a distinct "on-off" temperature response at the temperature range of 30 C. The peak current attenuation of AP at 36 C is small and the temperature switch is feasible when the solution temperature is changed repeatedly between 26 C and 36 C. In the "open" state, the PSG electrode can detect AP in solution in a wide linear range and a low detection limit. (4) Glucose oxidase (GOD) is coated on the composite film of reduced graphene oxide (rGO) and PVCL, fixed on the surface of glassy carbon electrode, and a GOD biosensor with temperature response characteristics is constructed. Provide a good biological micro-environment to maintain the biological activity of GOD. Temperature below 30 C, GOD activity is low; when temperature above 30 C, GOD on the electrode surface for rapid direct electron transfer, the electrocatalytic activity of glucose in solution is high.
【學(xué)位授予單位】：湘潭大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O657.1;TP212.2

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本文編號(hào)：2210375