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Synthesis, modification, and application of siloxane materials for environmental sensing.

机译:用于环境传感的硅氧烷材料的合成,改性和应用。

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摘要

As human populations and resource consumption increase, it is increasingly important to monitor the quality of our environment. While laboratory instruments offer useful information, portable, easy to use sensors would allow environmental analysis to occur on-site, at lower cost, and with minimal operator training. We explore the synthesis, modification, and applications of modified polysiloxane in environmental sensing.;Multiple methods of producing modified siloxanes were investigated. Oligomers were formed by using functionalized monomers, producing siloxane materials containing silicon hydride, methyl, and phenyl side chains. Silicon hydride-functionalized oligomers were further modified by hydrosilylation to incorporate methyl ester and naphthyl side chains. Modifications to the siloxane materials were also carried out using post-curing treatments. Methyl ester-functionalized siloxane was incorporated into the surface of a cured poly(dimethylsiloxane) film by siloxane equilibration. The materials containing methyl esters were hydrolyzed to reveal carboxylic acids, which could later be used for covalent protein immobilization. Finally, the siloxane surfaces were modified to incorporate antibodies by covalent, affinity, and adsorption-based attachment. These modifications were characterized by a variety of methods, including contact angle, attenuated total reflectance Fourier transform infrared spectroscopy, dye labels, and 1H nuclear magnetic resonance spectroscopy.;The modified siloxane materials were employed in a variety of sensing schemes. Volatile organic compounds were detected using methyl, phenyl, and naphthyl-functionalized materials on a Fabry-Perot interferometer and a refractometer. The Fabry-Perot interferometer was found to detect the analytes upon siloxane extraction by deformation of the Bragg reflectors. The refractometer was used to determine that naphthyl-functionalized siloxanes had elevated refractive indices, rendering these materials more sensitive to some analytes.;Antibody-modified siloxanes were used to detect biological analytes through a solid phase microextraction-mediated enzyme linked immunosorbent assay (SPME ELISA). The SPME ELISA was found to have higher analyte sensitivity compared to a conventional ELISA system. The detection scheme was used to detect Escherichia coli at 8500 CFU/mL.;These results demonstrate the variety of methods that can be used to modify siloxanes and the wide range of applications of modified siloxanes has been demonstrated through chemical and biological sensing schemes.
机译:随着人口和资源消耗的增加,监视我们的环境质量变得越来越重要。尽管实验室仪器可提供有用的信息,但便携式,易于使用的传感器将允许以较低的成本在现场进行环境分析,并且只需进行最少的操作人员培训。我们探索了改性聚硅氧烷的合成,改性及其在环境传感中的应用。;研究了多种生产改性硅氧烷的方法。通过使用官能化单体形成低聚物,产生包含氢化硅,甲基和苯基侧链的硅氧烷材料。通过氢化硅烷化将氢化硅官能化的低聚物进一步改性,以结合甲基酯和萘基侧链。还使用后固化处理对硅氧烷材料进行了改性。通过硅氧烷平衡将甲基酯官能化的硅氧烷掺入固化的聚(二甲基硅氧烷)膜的表面中。含有甲酯的材料被水解以显示出羧酸,随后可用于固定共价蛋白。最后,对硅氧烷表面进行修饰以通过共价,亲和力和基于吸附的结合方式掺入抗体。这些修饰通过多种方法进行了表征,包括接触角,衰减全反射傅立叶变换红外光谱,染料标记和1H核磁共振光谱。改性的硅氧烷材料被用于多种传感方案中。使用甲基,苯基和萘基官能化的材料,在Fabry-Perot干涉仪和折光仪上检测到挥发性有机化合物。发现Fabry-Perot干涉仪可通过布拉格反射镜的变形检测硅氧烷萃取后的分析物。折光仪用于确定萘基官能化的硅氧烷具有较高的折光率,从而使这些材料对某些分析物更加敏感;抗体修饰的硅氧烷用于通过固相微萃取介导的酶联免疫吸附测定(SPME ELISA)检测生物分析物)。与常规ELISA系统相比,发现SPME ELISA具有更高的分析物灵敏度。该检测方案用于检测8500 CFU / mL的大肠杆菌。这些结果表明可用于改性硅氧烷的方法多种多样,并且已通过化学和生物传感方案证明了改性硅氧烷的广泛应用。

著录项

  • 作者

    Mackey, Gillian Claire.;

  • 作者单位

    Queen's University (Canada).;

  • 授予单位 Queen's University (Canada).;
  • 学科 Analytical chemistry.;Environmental science.
  • 学位 Ph.D.
  • 年度 2016
  • 页码 296 p.
  • 总页数 296
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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