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Title page for ETD etd-11232015-131924

Type of Document Dissertation
Author Spears, Benjamin Russell
URN etd-11232015-131924
Title Precise Polymer Networks: An Investigation Encompassing Hydrogels, Proteins, and Nanoparticles
Degree PhD
Department Chemistry
Advisory Committee
Advisor Name Title
Eva M. Harth, Ph.D. Committee Chair
David W. Wright, Ph.D. Committee Member
Scott A. Guelcher, Ph.D. Committee Member
Timothy P. Hanusa, Ph.D. Committee Member
  • formulation
  • nanoparticle
  • carbonate
  • ester
  • PEG
  • drug delivery
  • polymer
  • glycidol
Date of Defense 2015-11-04
Availability unrestricted
The polymerization of glycidol has been studied for some time due to the numerous uses for the product polymer species, including the transportation of drug molecules and biological cargo, biomineralization, and even solid catalyst supports in organic synthesis. Hitherto, the entirety of research performed has been restrained to the formation of either hyperbranched dendrimer-like structures through either cationic or anionic polymerization mechanisms, or solely linear species through the polymerization of protected derivatives with subsequent deprotection steps. The product structures are limited in their post-modification potential to reactions based around the functionalization of the numerous pendant hydroxyl groups. The dendrimer-like structures are limited to implementation of the products in problems previously treated by dendrimer species, while the rigorous reaction conditions and numerous protection and deprotection steps that facilitate the formation of the linear species are far from what could be considered facile. The advent of novel synthetic routes to take advantage of the inherent water solubility of poly(glycidol) systems and development of methodologies to prepare poly(glycidol)s that address the need for controlled semibranched structures for implementation in the study of diverse biomedical research targets is presented. The newly synthesized structures afford a polymerization pathway that can be performed on the bench top with little extraneous concern for reaction conditions. The utilization of a previously studied tin catalyst provides a reproducible and facile method for the formation of semi-branched polyglycerol structures. Further investigation has also led to the formulation of a completely green synthetic route that can be utilized in the formation of poly(glycidol) and the functionalization of biological proteins such as BSA and LYZ. The synthesis routes utilized allow for the introduction of functional groups during the polymerization process, which leads to the ability for inclusion of the newly formed polymer structures, in conjunction with polymers previously pioneered in the lab, for the development of a novel pathway for the formation of monodisperse microgel structures, using a readily available materials printer system, capable of delivering both hydrophobic and hydrophilic therapeutic cargo.
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