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Degree

Doctor of Philosophy, University of Akron, Chemistry, 2005.

Abstract

The development of new nanostructured optical sensing polymer/nanoparticle composite materials is described. The materials are potentially useful for in vivo sensing of sugars based on the color changes of the plasmon band and Surface Enhanced Raman Scattering of the gold nanoparticles. In the first section, controlled radical polymerization methods including “grafting to” and “grafting from” techniques were studied to synthesize the polymer shell materials on gold nanoparticle surfaces. The controlled radical polymerization techniques were proven to be essential for producing discrete polymer core-shell nanoparticles. In the second section, the preparation of gold nanoparticles with the molecular recognition sites, boronic acids, at the Au nanoparticle/polymer shell interfaces was investigated. A new thiol linker, 1,4-dimercapto-2,3-dimethyl-butane-2,3-diol, designed and synthesized for molecular self-assembling of the boronic acid sensing elements on gold surfaces, was used. The supramolecular assembling of the dioldithiol linker on gold surfaces was studied in detailed with 1D and 2D NMR spectroscopy in solution. This study provided unique opportunities for the investigation of the mechanisms, energetics and dynamics of the thiol/gold surface interactions. In the third section, 3-pyridinylboronic acid, a model sugar sensor that is being incorporated into the polymer shell/Au nanoparticle interfaces, was shown to be useful for quantifying <1 mM adenosine triphosphate (ATP) and differentiating between ATP and AMP in neutral phosphate buffers by a colorimetric assay. The binding constant and the structure of the sensor/analyte complex were determined by NMR spectroscopic methods.

Keywords

biosensors; boronic acid; molecular recognition; SAM on gold; ATP; sugar sensing; dynamic of thiol exchange on gold surface

Advisor

Jun Hu

Pages

141p.

Document number: akron1123637252
Permalink: http://rave.ohiolink.edu/etdc/view?acc_num=akron1123637252

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