基于聚N-乙烯基己内酰胺的温度响应型电化学传感器研究
发布时间：2018-08-28 19:24
【摘要】：随着材料科学和电化学传感器的深入发展,运用单一材料制备的常规电化学传感器已经不能满足研究者们的要求。科学家们尝试将具有不同特性的材料组合在一起形成新的复合材料对电极进行修饰,期望复合材料各组分之间的协同作用带给电极新的电化学特性。温敏性聚合物表现出温度控制的分子构型转变,纳米碳材料具有优良的电子传导能力和电催化性能。将二者混合制备纳米复合材料,用来直接修饰电极或者在电极表面固定氧化还原蛋白质,能得到具备温度响应特性的电化学传感器。通过调节环境温度实现对传感器电化学性能的智能调控,为电化学传感领域开辟了新的研究方向。本论文的主要工作概括如下:(1)用沉淀聚合方法合成了具有温敏性的聚N-乙烯基己内酰胺均聚物(PVCL),通过变温紫外测试证实:合成的PVCL具有温敏性质,低临界溶解温度(LCST)为30℃。(2)用氧化石墨烯(GO)和PVCL在玻碳电极表面修饰一层“夹心式”的温敏性GO/PVCL/GO复合膜。以PVCL的LCST温度(30℃)为界,复合膜修饰电极检测邻苯二酚(1,2-Benzenediol,CC)与对苯二酚(Hydroquinone,HQ)时表现出明显的温度响应电化学“开-关”效应,并且具有可逆性。电极在高温“开”状态下能对溶液中的CC和HQ进行同时检测,且具有较宽的线性范围。(3)用羧基化多壁碳纳米管(MWCNT(COOH))、GO和PVCL混合修饰玻碳电极,制备了具有温度响应特性的PSG电极。以30℃为界,对乙酰氨基苯酚(4-Acetamino phenol,AP)在PSG电极上的电化学响应信号具有明显的温度响应“开-关”特性。在26℃和36℃之间反复改变溶液温度,AP在36℃的峰电流衰减小,温度开关具有可逆性。“开”状态下,PSG电极能在较宽的线性范围和低检出限下检测溶液中的AP。(4)将葡萄糖氧化酶(GOD)包覆于还原型氧化石墨烯(rGO)与PVCL复合膜中,固定在玻碳电极表面,构筑了具有温度响应特性的GOD生物传感器。rGO-PVCL复合膜能为GOD提供一个良好的生物微环境,保持GOD的生物活性。温度低于30℃,GOD活性低;当温度高于30℃时,GOD在电极表面进行快速的直接电子转移,对溶液中葡萄糖的电催化活性高。高温时检测葡萄糖的精密度好并且灵敏度高。
[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.
【学位授予单位】：湘潭大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1;TP212.2
[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.
【学位授予单位】：湘潭大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1;TP212.2
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