基于低维碳纳米材料的电化学生物传感器的研究

发布时间：2018-05-30 09:15

本文选题：电化学生物传感器 + 修饰电极　；参考：《西南科技大学》2017年硕士论文

【摘要】：电化学传感器具有良好选择性、较高灵敏度、易于操作、低成本且分析快速等特点,被广泛应用于环境评测、食品检验和生物医学等领域。碳纳米材料有着优异的物理及化学特性,能够有效改善电极表面的微结构,是电化学传感器领域的研究热点。通过将碳纳米材料和其他材料相结合,达到进一步改善和提高电化学传感器性能的目的。本论文通过将碳纳米角、碳量子点等低维碳纳米材料与其他材料复合,设计制备了四种复合材料,分别构建了四种电化学传感器,并研究了复合材料对生物分子的电化学催化性能。本论文开展的主要工作如下:(1)通过电聚合方法制备了聚2-氨基吡啶(PAP)/单壁碳纳米角(SWCNH)修饰玻碳电极(GCE),在循环伏安法、交流阻抗法和计时电流等电化学方法下对所制备电极进行性能的测试。研究表明,通过PAP和SWCNH之间良好的协同效应,PAP/SWCNH/GCE对过氧化氢表现出良好的电催化作用。在5.0×10-5~8.0×1 0-3 m o l L-1范围内响应电流与浓度呈现良好的线性关系,检出限为3.6×10-6m o l L-1(S/N=3)。(2)采用电聚合的方式在SWCNH基质上固定磷钼酸(PMo1 2),合成PMo1 2/S W C N H复合材料。P M o1 2/S W C N H/G C E可在较低氧化电位下催化葡萄糖的氧化。在葡萄糖浓度为3.5×10-5~4.0×1 0-3m o l L-1的范围内,呈现良好的线性电流响应,检出限为2.4×10-6m o l L-1(S/N=3)。(3)采用一锅法对Cu2+和硫钼酸铵进行同步还原并自然干燥,合成二硫化钼-氧化亚铜(Mo S2-C u 2 O)复合材料,并基于碳量子点(CQDs)较大的比表面积和良好的导电性等特点,制备Mo S2-C u 2 O/C Q D s/G C E修饰电极。M o S2-C u 2 O/C Q D s/G C E对亚硝酸根表现出良好的电催化氧化作用,在1.0×10-5~6.0×1 0-3 m o l L-1范围内响应电流与亚硝酸根浓度呈现良好的线性关系,检出限为1.8×10-6 m o l L-1(S/N=3)。(4)采用电聚合的方式在CQDs基质上固定聚(β-环糊精)(β-CD),合成β-CD/CQDs复合材料。β-CD/CQDs/GCE分别在0.16、0.3 1和0.7 3 V处催化多巴胺(D A)、尿酸(U A)和色氨酸(Tr p)的氧化,并成功实现三者的同时测定。在UA和Trp共存的条件下,D A检测的线性范围为4.0×1 0-6~2.2×1 0-4 m o l L-1,检出限低至1.4×1 0-7 m o l L-1(S/N=3)。在DA和Trp共存的条件下,UA检测的线性范围为3.0×10-7~2.0×1 0-4 m o l L-1,检出限低至1.0×10-8m o l L-1(S/N=3)。在DA和UA共存的条件下,Trp检测的线性范围为5.0×10-6~2.7×1 0-4 m o l L-1,检出限低至1.6×10-7 m o l L-1(S/N=3)。综上所述,本论文制备PAP/SWCNH/GCE、PMo1 2/S W C N H/G C E、M o S 2-C u 2 O/C Q D s/G C E和β-C D/C Q D s/G C E四种复合电极,并将其用于构建生物小分子的电化学传感器。结果表明,所制备的四种修饰电极呈现较高的电催化活性、良好的选择性和稳定性等优点,具有较好的应用前景。
[Abstract]:Electrochemical sensors with good selectivity, high sensitivity, easy operation, low cost and fast analysis are widely used in environmental assessment, food testing and biomedicine. Carbon nanomaterials have excellent physical and chemical properties and can effectively improve the microstructure of electrode surface. It is a hot research topic in the field of electrochemical sensors. By combining carbon nanomaterials with other materials, the performance of electrochemical sensors can be further improved. In this paper, four kinds of composite materials are designed and fabricated by combining low dimensional carbon nanomaterials such as carbon nanometers, carbon quantum dots and other materials, and four kinds of electrochemical sensors are constructed respectively. The electrochemical catalytic performance of the composite to biomolecules was also studied. The main work of this thesis is as follows: (1) Poly (2-aminopyridine) PAPP / SWCNH modified glassy carbon electrode was prepared by electropolymerization. Electrochemical methods, such as AC impedance method and chronoelectric current, were used to test the performance of the prepared electrode. The results showed that PAP / SWCNH / GCE had a good electrocatalytic effect on hydrogen peroxide through the good synergistic effect between SWCNH and PAP. In the range of 5.0 脳 10 ~ (-5) ~ 8.0 脳 10 ~ (-3) m o l L ~ (-1), there is a good linear relationship between the response current and the concentration. The detection limit was 3.6 脳 10-6 mol / L -1 / N ~ (3 +) N ~ (3 +) C ~ (2) the PMo1 _ 2 / S / S W C N / H _ (G) C _ E composite was synthesized by electropolymerization of PMO _ (12) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) O _ (2) S W C N / H _ (G) C _ (E). In the range of 3.5 脳 10 ~ (-5) 渭 m ~ (-1) 脳 10 ~ (-3) mol ~ (-1) L ~ (-1) of glucose, the linear current response was good, and the detection limit was 2.4 脳 10 ~ (-6) mmol / L ~ (-1) S / N _ (3) O _ (3) the simultaneous reduction and natural drying of Cu2 and ammonium molybdate were carried out by one-pot method. The molybdenum disulfide / cuprous oxide Mo S2-C u 2O) composite was synthesized and based on the characteristics of large specific surface area and good electrical conductivity of carbon quantum dots (CQDs). The Mo S 2-C u 2 O / C Q D / G C E modified electrode, M o S 2-C u 2 O 2 O / C Q D / G C E, showed a good electrocatalytic effect on nitrite oxidation. The response current showed a good linear relationship with the concentration of nitrite in the range of 1.0 脳 10 ~ (-5) ~ 6.0 脳 10 ~ (-3) m o l 路L ~ (-1). The detection limit was 1.8 脳 10 ~ (-6) m o l / L ~ (-1) S / N ~ (3) N ~ (3 +). The polymer was immobilized on the CQDs substrate by electropolymerization (尾 -CD ~ (2 +) (尾 -CD ~ (2 +) to synthesize 尾 -CD _ (-C) / C _ (QDs) composites. 尾 -CD / C _ (1) / C ~ (2 +) / GCE catalyzed the oxidation of dopamine D anion (U A) and tryptophan at 0.160.3 V and 0.73 V, respectively. The simultaneous determination of the three was successfully realized. Under the condition of coexistence of UA and Trp, the linear range was 4.0 脳 10 ~ (-6) m o l ~ (-1) 脳 10 ~ (-4) m o l / L ~ (-1), and the detection limit was as low as 1.4 脳 10 ~ (-7) m o l / L ~ (-1) S / N ~ (-1). Under the condition of co-existence of DA and Trp, a linear range of 3.0 脳 10 ~ (-7) 渭 m ~ (-1) 脳 10 ~ (4) m o l / L ~ (-1) was obtained, and the detection limit was as low as 1.0 脳 10 ~ (-8) mol ~ (-1) L ~ (-1) S / N ~ (-1). Under the condition of the coexistence of DA and UA, the linear range of TRP detection was 5.0 脳 10 ~ (-6) 渭 m ~ (2.7 脳 10 ~ (-4) m o l / L ~ (-1), and the detection limit was as low as 1.6 脳 10 ~ (-7) m o l / L ~ (-1) S / N ~ (-1). To sum up, four kinds of composite electrodes, PAP / SWCNH / GCEP, PMO / SWCNH / S / S W C N / H / G / C, M o S 2-C u 2 O, Q D / G / C E and 尾 -C D / C D / S / G / C E composite electrodes, were prepared and used to construct electrochemical sensors for small biomolecules. The results show that the four modified electrodes have high electrocatalytic activity, good selectivity and stability, and have a good prospect of application.
【学位授予单位】：西南科技大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1

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