功能化碳纳米管与介孔硅修饰电极对AA、DA和UA同时测定的研究
发布时间：2018-10-09 07:38
【摘要】：多巴胺(DA)、抗坏血酸(AA)、尿酸(UA)是人体新陈代谢中三种重要的生物小分子。人体中这些物质含量的高低直接影响人的身体健康。如,缺乏多巴胺可导致精神分裂、帕金森病等,缺乏抗坏血酸可导致坏血病,尿酸代谢紊乱则是引起痛风的原因。能够对三种物质进行精确检测,对这些疾病的诊断和预防具有重要意义。但三者氧化峰电位却十分接近,使用普通的电极会互相干扰,因此各种修饰电极应运而生。本文制备了三种新型修饰电极,利用循环伏安法(CV)和微分脉冲伏安法(DPV)对DA、AA和UA在三种修饰电极上的电化学响应进行分析:(1)通过非共价修饰的方法将聚合离子液体修饰于多壁碳纳米管上,不仅可以使易发生缠绕的多壁碳纳米管在水溶液中分散,还可以保留碳纳米管的优良特性,聚合离子液体的引入也增强了电子转移速率。基于此将聚合离子液体(聚(1-乙烯基-3-乙基咪唑溴代盐))和多壁碳纳米管结合,利用该复合物制备出聚合离子液体-多壁碳纳米管修饰电极(Poly(ViEt Im~+Br~-)/MWCNTs/GCE),并采用红外光谱(FT-IR)和透射电镜(TEM)等手段对Poly(ViEt Im~+Br~-)/MWCNTs复合物进行了表征。Poly(Vi Et Im~+Br~-)与MWCNTs实现了复合,而且多壁碳纳米管在形成复合物后未发生缠绕,可稳定分散于水溶液中。此外,碳纳米管的催化作用与复合物的协同作用使得Poly(ViEtIm~+Br~-)/MWCNTs/GCE与MWCNTs/GCE相比,对DA、AA和UA具有更好的电化学响应信号。在pH=7.4的PBS中,DA,AA和UA的检测范围分别为2-180μM,40-5000μM和4-50μM。同时可实现维生素C注射剂和盐酸多巴胺注射剂中AA和DA的检测。(2)介孔硅(MCF)具有大比表面积,孔径大小可调等介孔材料特性,此外,其互通的三维孔道结构还可增强物质在MCF孔道中的传输和扩散。基于该优势,本文以介孔硅(MCF)为修饰材料,与石墨等材料混合制备出介孔硅-碳糊电极(MCF/CPE)。实验结果显示,MCF/CPE在p H=6的PBS中,可以在AA、DA和UA共存条件下选择性测定DA和UA。在三者同时存在下,DA和UA的检测范围分别为2-220μM和1-120μM。(3)以离子液体修饰介孔硅(MCF-IL)为电极修饰材料,在MCF优良特性的基础上引入离子液体,制备出碳糊电极(MCF-IL/CPE)。相比MCF/CPE对AA、UA具有更好的响应。MCF-IL(17%)/CPE在p H=6的PBS中,可以在三者共存条件下选择性测定DA和UA。DA、UA的检测范围为5-160μM和1-160μM。MCF-IL(25%)/CPE在pH=6的PBS中,实现了AA、DA、UA的同时测定。AA的检测范围为50-3000μM,DA的检测范围为2-180μM,UA的检测范围为1-150μM,并应用于样品中AA和DA的检测。
[Abstract]:Dopamine (DA), ascorbic acid (AA), uric acid (UA) is one of the three important biomolecules in human metabolism. The content of these substances in the human body directly affects the health of the human body. For example, lack of dopamine can lead to schizophrenia, Parkinson's disease, lack of ascorbic acid can lead to scurvy, uric acid metabolism disorder is the cause of gout. It is important to diagnose and prevent these diseases by accurate detection of three kinds of substances. However, the oxidation peak potentials of the three kinds of electrodes are very close, and the common electrodes interfere with each other, so all kinds of modified electrodes emerge as the times require. In this paper, three novel modified electrodes were prepared. The electrochemical responses of DA,AA and UA on three modified electrodes were analyzed by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). (1) Polymeric ionic liquids were modified onto multi-walled carbon nanotubes by non-covalent modification. It can not only disperse the multi-walled carbon nanotubes in aqueous solution, but also retain the excellent properties of carbon nanotubes. The introduction of polymeric ionic liquids also increases the electron transfer rate. Based on this, polymeric ionic liquids (poly (1-vinyl-3-ethylimidazolium bromide) and multi-walled carbon nanotubes were combined, The polymeric ionic liquid-multi-wall carbon nanotube modified electrode (Poly (ViEt Im~ Br~-) / MWCNTs / GCE) was prepared. The composite of Poly (ViEt Im~ Br~-) / MWCNTs was characterized by IR (FT-IR) and transmission electron microscopy (TEM). Moreover, the multiwalled carbon nanotubes were not wound after the formation of the complex, and could be dispersed stably in aqueous solution. In addition, Poly (ViEtIm~ Br~-) / MWCNTs / GCE has better electrochemical response to DA,AA and UA than MWCNTs/GCE. In the PBS of pH=7.4, the detection ranges of DAA AA and UA were 2-180 渭 M 40-5000 渭 M and 4-50 渭 M, respectively. At the same time, the detection of AA and DA in vitamin C injection and dopamine hydrochloride injection can be realized. (2) Mesoporous silicon (MCF) has large specific surface area, adjustable pore size and other mesoporous materials. The interworking 3D pore structure can also enhance the transport and diffusion of matter in MCF channels. Based on this advantage, mesoporous silicon-carbon paste electrode (MCF/CPE) was prepared by mixing mesoporous silicon (MCF) with graphite and other materials. The experimental results show that MCFR / CPE can selectively determine DA and UA. under the condition of coexistence of AA,DA and UA in the PBS of pHf6. The detection ranges of DA and UA were 2-220 渭 M and 1-120 渭 M respectively. (3) carbon paste electrode (MCF-IL/CPE) was prepared by using ionic liquid modified mesoporous silicon (MCF-IL) as electrode modification material and introducing ionic liquid on the basis of the excellent properties of MCF. MCF-IL (17%) / CPE can selectively determine the detection range of DA and UA.DA,UA between 5-160 渭 M and 1-160 渭 M.MCF-IL (25%) / CPE in pH=6 PBS. The detection range of AA,DA,UA for simultaneous determination of .AA is 50-3000 渭 m ~ (-1) DA. The detection range is 2-180 渭 M ~ (-1) 渭 m ~ (-1), and it is applied to the detection of AA and DA in the sample.
【学位授予单位】：沈阳师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1
本文编号：2258517
[Abstract]:Dopamine (DA), ascorbic acid (AA), uric acid (UA) is one of the three important biomolecules in human metabolism. The content of these substances in the human body directly affects the health of the human body. For example, lack of dopamine can lead to schizophrenia, Parkinson's disease, lack of ascorbic acid can lead to scurvy, uric acid metabolism disorder is the cause of gout. It is important to diagnose and prevent these diseases by accurate detection of three kinds of substances. However, the oxidation peak potentials of the three kinds of electrodes are very close, and the common electrodes interfere with each other, so all kinds of modified electrodes emerge as the times require. In this paper, three novel modified electrodes were prepared. The electrochemical responses of DA,AA and UA on three modified electrodes were analyzed by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). (1) Polymeric ionic liquids were modified onto multi-walled carbon nanotubes by non-covalent modification. It can not only disperse the multi-walled carbon nanotubes in aqueous solution, but also retain the excellent properties of carbon nanotubes. The introduction of polymeric ionic liquids also increases the electron transfer rate. Based on this, polymeric ionic liquids (poly (1-vinyl-3-ethylimidazolium bromide) and multi-walled carbon nanotubes were combined, The polymeric ionic liquid-multi-wall carbon nanotube modified electrode (Poly (ViEt Im~ Br~-) / MWCNTs / GCE) was prepared. The composite of Poly (ViEt Im~ Br~-) / MWCNTs was characterized by IR (FT-IR) and transmission electron microscopy (TEM). Moreover, the multiwalled carbon nanotubes were not wound after the formation of the complex, and could be dispersed stably in aqueous solution. In addition, Poly (ViEtIm~ Br~-) / MWCNTs / GCE has better electrochemical response to DA,AA and UA than MWCNTs/GCE. In the PBS of pH=7.4, the detection ranges of DAA AA and UA were 2-180 渭 M 40-5000 渭 M and 4-50 渭 M, respectively. At the same time, the detection of AA and DA in vitamin C injection and dopamine hydrochloride injection can be realized. (2) Mesoporous silicon (MCF) has large specific surface area, adjustable pore size and other mesoporous materials. The interworking 3D pore structure can also enhance the transport and diffusion of matter in MCF channels. Based on this advantage, mesoporous silicon-carbon paste electrode (MCF/CPE) was prepared by mixing mesoporous silicon (MCF) with graphite and other materials. The experimental results show that MCFR / CPE can selectively determine DA and UA. under the condition of coexistence of AA,DA and UA in the PBS of pHf6. The detection ranges of DA and UA were 2-220 渭 M and 1-120 渭 M respectively. (3) carbon paste electrode (MCF-IL/CPE) was prepared by using ionic liquid modified mesoporous silicon (MCF-IL) as electrode modification material and introducing ionic liquid on the basis of the excellent properties of MCF. MCF-IL (17%) / CPE can selectively determine the detection range of DA and UA.DA,UA between 5-160 渭 M and 1-160 渭 M.MCF-IL (25%) / CPE in pH=6 PBS. The detection range of AA,DA,UA for simultaneous determination of .AA is 50-3000 渭 m ~ (-1) DA. The detection range is 2-180 渭 M ~ (-1) 渭 m ~ (-1), and it is applied to the detection of AA and DA in the sample.
【学位授予单位】：沈阳师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1
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