Title:
Molecularly Imprinted Polymers: Towards a Rational Understanding of Biomimetic Materials

Simple item page
dc.contributor.advisor Mizaikoff, Boris
dc.contributor.author Molinelli, Alexandra Lidia en_US
dc.contributor.committeeMember Huang, Ching-Hua
dc.contributor.committeeMember Janata, Jiri
dc.contributor.committeeMember Josowicz, Mira
dc.contributor.committeeMember Weck, Marcus
dc.contributor.department Chemistry and Biochemistry en_US
dc.date.accessioned 2005-03-01T19:31:05Z
dc.date.available 2005-03-01T19:31:05Z
dc.date.issued 2004-11-22 en_US
dc.description.abstract The research described in this thesis contributes to the development of new strategies facilitating advanced understanding of the fundamental principles governing selective recognition of molecularly imprinted polymers (MIPs) at a molecular level for the rational optimization of biomimetic materials. The nature of non-covalent interactions involved in the templating process of molecularly imprinted polymers based on the self-assembly approach were investigated with a variety of analytical techniques addressing molecular level interactions. For this purpose, the concerted application of IR and 1H-NMR spectroscopy enabled studying the complexation of the template molecules 2,4-dichlorophenoxyacetic acid, quercetin, and o-, m-, and p-nitrophenol with a variety of functional monomers in the pre-polymerization solution by systematically varying the ratio of the involved components. In aqueous and non protic porogenic solvents, information on the interaction types, thermodynamics, and complex stoichiometry was applied toward predicting the optimum imprinting building blocks and ratios. Molecular dynamics simulations of 2,4-dichlorophenoxyacetic acid and its interactions with the functional monomer 4-vinylpyridine in aqueous and aprotic explicit solvent allowed demonstrating the fundamental potential of computer MD simulations for predicting optimized pre-polymerization ratios and the involved interaction types. The obtained results clearly demonstrate that the application of rapid IR/NMR pre-screening methods in combination with molecular modeling strategies is a promising strategy towards optimized imprinting protocols in lieu of the conventionally applied labor intensive and time-consuming trial-and-error approach. Furthermore, HPLC characterization of the produced MIPs compared to control polymers enabled a systematic approach to imprinting based on advanced understanding of the factors governing the formation of high-affinity binding sites during the polymerization. In addition, the importance of the combination of size, shape, and molecular functionalities for the selective recognition properties of MIPs was investigated. MIPs for the mycotoxins deoxynivalenol and zearalenone and for the antioxidant quercetin were applied as separation materials for advanced sample preparation in beverage analysis. The obtained results demonstrated the potential of MIPs for rapid one-step sample clean-up and pre-concentration from beverages such as wine and beer. en_US
dc.description.degree Ph.D. en_US
dc.format.extent 3836309 bytes
dc.format.mimetype application/pdf
dc.identifier.uri http://hdl.handle.net/1853/4837
dc.language.iso en_US
dc.publisher Georgia Institute of Technology en_US
dc.subject Beverage analysis en_US
dc.subject Solid phase extraction
dc.subject NMR spectroscopy
dc.subject IR spectroscopy
dc.subject Non-covalent imprinting
dc.subject Molecularly imprinted polymers
dc.subject.lcsh Molecular imprinting en_US
dc.subject.lcsh Nuclear magnetic resonance spectroscopy en_US
dc.subject.lcsh Imprinted polymers en_US
dc.subject.lcsh Infrared spectroscopy en_US
dc.title Molecularly Imprinted Polymers: Towards a Rational Understanding of Biomimetic Materials en_US
dc.type Text
dc.type.genre Dissertation
dspace.entity.type Publication
local.contributor.corporatename School of Chemistry and Biochemistry
local.contributor.corporatename College of Sciences
relation.isOrgUnitOfPublication f1725b93-3ab8-4c47-a4c3-3596c03d6f1e
relation.isOrgUnitOfPublication 85042be6-2d68-4e07-b384-e1f908fae48a
Files
Original bundle
Now showing 1 - 1 of 1
Thumbnail Image
Name:
molinelli_alexandra_l_200412_phd.pdf
Size:
3.66 MB
Format:
Adobe Portable Document Format
Description:
Download
Collections
Theses and Dissertations