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首页> 外文学位 >Detection strategies with membrane-based electrochemical sensing systems and mechanistic studies of ethanol oxidation at ordered electrode surfaces.
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Detection strategies with membrane-based electrochemical sensing systems and mechanistic studies of ethanol oxidation at ordered electrode surfaces.

机译：基于膜的电化学传感系统的检测策略以及有序电极表面乙醇氧化的机理研究。

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摘要

The first part of this dissertation describes the use of surface refunctionalized fluorinated ethylene propylene (FEP) membranes in biosensors based on the Clark-type oxygen sensor. FEP membranes, partially hydroxylated by exposure to a radio frequency glow discharge plasma, were aminated by treatment with ({dollar}gamma{dollar}-aminopropyl)triethoxysilane. Measurement of the permeability and diffusion coefficients for oxygen in non-modified, hydroxylated, and aminated FEP showed that modifications did not alter the oxygen transport characteristics of the membranes. In subsequent experiments, biosensors were constructed by using aminated FEP as the gas-permeable membrane of a Clark-type oxygen sensor. The respiration of mouse neuroblastoma cells (NB2a) was monitored with an oxygen sensor following cell attachment to the sensor membrane through natural growth processes. Another biosensor was constructed by linking glucose oxidase to an aminated oxygen sensor membrane with albumin and glutaraldehyde. Sensor response to glucose was linear between 0.1 mM and 6.5 mM.; In a second study, a sensing system for ethanol was developed. The sensor was designed to extract ethanol vapor through an expanded poly(tetrafluoroethylene) detection schemes were used to monitor ethanol levels. Cyclic voltammograms and pulsed amperometric detection response curves recorded with a rotated platinum disk electrode were used to optimize pulsed potential waveforms employed in a static electrolyte drop behind a membrane. A four step waveform was insensitive to solution hydrodynamics and sensitive to ethanol concentration between 0.02 mM and 1.7 M. Response characteristics of this sensing system enabled the direct determination of ethanol in non-diluted alcoholic beverages.; In concluding studies, platinum single crystal electrodes with (111), (557), and (335) surface orientations were used to probe the effects of electrode surface step density on ethanol electrooxidation to acetic acid. Cyclic voltammetry demonstrated the sensitivity of ethanol voltammetry to electrode surface structure. Chronocoulometry was coupled with ion chromatography to quantify acetic acid produced during ethanol oxidation as a function of electrolysis potential and electrode surface step density. Results showed increased surface step density inhibits ethanol oxidation to acetic acid and promotes carbon-carbon bond cleavage pathways.
机译：本文的第一部分描述了基于克拉克型氧传感器的生物传感器中表面再官能化氟化乙烯丙烯（FEP）膜的使用。通过暴露于射频辉光放电等离子体而部分羟基化的FEP膜通过用（{gamma} {gamma {dollar}-氨丙基}）三乙氧基硅烷处理而被胺化。在未改性的，羟基化的和胺化的FEP中，氧气的渗透性和扩散系数的测量结果表明，改性不会改变膜的氧气传输特性。在随后的实验中，通过使用胺化FEP作为Clark型氧气传感器的透气膜来构建生物传感器。细胞通过自然生长过程附着在传感器膜上后，用氧传感器监测小鼠神经母细胞瘤细胞（NB2a）的呼吸。通过将葡萄糖氧化酶与白蛋白和戊二醛连接到胺化的氧传感器膜上，构建了另一个生物传感器。传感器对葡萄糖的响应在0.1 mM和6.5 mM之间呈线性关系。在第二项研究中，开发了乙醇传感系统。该传感器设计用于通过扩展的聚四氟乙烯提取乙醇蒸气，检测方案用于监测乙醇水平。用旋转的铂圆盘电极记录的循环伏安图和脉冲安培检测响应曲线用于优化膜后的静态电解质液滴中使用的脉冲电势波形。四步波形对溶液的流体动力学不敏感，对乙醇浓度在0.02 mM至1.7 M之间不敏感。该传感系统的响应特性使得可以直接测定非稀释酒精饮料中的乙醇。在最后的研究中，使用具有（111），（557）和（335）表面取向的铂单晶电极来探测电极表面步长密度对乙醇电氧化为乙酸的影响。循环伏安法证明了乙醇伏安法对电极表面结构的敏感性。计时容量分析法与离子色谱法结合使用，以量化乙醇氧化过程中产生的乙酸与电解电位和电极表面步长密度的关系。结果表明，增加的表面台阶密度抑制了乙醇氧化为乙酸，并促进了碳-碳键的裂解途径。

著录项

  • 作者

    Tarnowski, David John.;

  • 作者单位

    University of Michigan.;

  • 授予单位 University of Michigan.;
  • 学科 Chemistry Analytical.
  • 学位 Ph.D.
  • 年度 1996
  • 页码 133 p.
  • 总页数 133
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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