Date of Award

5-2021

Document Type

Thesis campus only

Department

Chemistry

First Advisor

Laura Hunsicker-Wang

Second Advisor

Christina B. Cooley

Third Advisor

Jason Shearer

Abstract

In order to generate an efficient detection assay, an analyte’s signal must be amplified to provide a detectable readout in a short time period. Polymerization reactions can be used to amplify a signal, as a single initiator molecule can incite formation of a long polymer chain. Previous research in the Cooley Lab has led to the development of a novel detection assay using an aqueous atom transfer radical polymerization (ATRP) reaction. This assay provides real-time readouts of polymerization progress by using fluorogenic monomers—monomers that are dark in their monomer form but fluoresce under UV light when incorporated into a polymer—to couple the presence of analyte to fluorescence in solution. Though encouraging, the practicality of the originally reported assay was limited by long reaction times and oxygen intolerability. In order to further develop this assay for optimized capabilities of detection, it was necessary to optimize the reaction to achieve the maximum fluorescence possible in the shortest reaction time. A thorough optimization study was conducted, involving the analysis of several fluorogenic ATRP reaction variables and their effects on fluorescence and reaction kinetics. Various surfactants were screened and characterized, the reaction solvent was manipulated, and components of the reaction’s catalyst system were tested. Through the combination of the optimized reaction components, the average reaction time was reduced from 24 hours to 1.5 hours, maximum fluorescence was increased, and the assay was made more tolerant to oxygen. Modifications of this assay— to incorporate enzymatic oxygen scavenging and to apply the method to the analysis of general radical polymerization kinetics— are also explored and are the subject of ongoing study.

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