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Recognition in polymeric media: From molecular imprinting to soluble polymers
The application of polymeric media as sensors, drug delivery agents, chromatographic columns, enzyme mimics, and many other functions is driven by the ability of the polymer to participate in molecular recognition events. The polymer provides a three-dimensional local environment that surrounds the binding site, which is one of the major factors that govern the binding efficiency. The local environment plays a crucial role in both the solid and solution state and will be explored here. The design, synthesis, and characterization of molecularly imprinted polymers (MIPs), highly crosslinked polymers obtained in the presence of host-guest complexes, will be discussed. Using biologically inspired three-point hydrogen-bonding as the recognition motif, a fundamental study to characterize binding pre- and post-polymerization binding, guest molecule transport, and binding site heterogeneity will be presented. The fundamental understanding of the imprinting process obtained will be shown to be necessary for the development of real-time, highly selective MIP-based sensors. Using π-stacking, effective sensing for polychlorinated aromatic contaminants in water will be demonstrated. A modified strategy, surface-templated polymer films, provides an ideal platform for the real-time, selective detection of bacteria at environmentally relevant concentrations. In the solution state, living polymerization methodologies are utilized to systematically explore the factors (molecular weight, backbone composition, chain flexibility) that affect a soluble polymer's ability to bind a guest molecule. ^
"Recognition in polymeric media: From molecular imprinting to soluble polymers"
(January 1, 2003).
Electronic Doctoral Dissertations for UMass Amherst.