Date of Award

12-2025

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

School

Polymer Science and Engineering

Committee Chair

Dr. Jeffrey Wiggins

Committee Chair School

Polymer Science and Engineering

Committee Member 2

Dr. Andrea Browning

Committee Member 3

Dr. Derek Patton

Committee Member 3 School

Polymer Science and Engineering

Committee Member 4

Dr. Sergei Nazarenko

Committee Member 4 School

Polymer Science and Engineering

Committee Member 5

Dr. James Rawlins

Committee Member 5 School

Polymer Science and Engineering

Abstract

This dissertation aims to expand the fundamental understanding of diamine-based benzoxazine chemistry by examining how synthesis influences the network properties of 4,4’-ddm and phenol-based (P-ddm) benzoxazine, compared to the constitutionally isomeric bisphenol-F and aniline-based (BF-a) benzoxazine. While bisphenol-based benzoxazines such as BF-a have been studied more extensively, diamine-based benzoxazines are still relatively unexplored due to the competition with the formation of 1,3,5-hexahydrotriazine intermediates and the inconsistent thermal and mechanical properties reported in the literature. These inconsistencies stem from factors including synthetic methods, curing conditions, and degradation during polymerization that have been overlooked.

To address these issues, this dissertation is organized into three main experimental sections. Firstly, new synthetic methods for P-ddm were developed and evaluated, and the resultant networks were characterized to assess the influence of triazine formation and monomer purity on network development and properties. Secondly, networks of BF-a prepared through melt- and solution-based methods were compared to a commercial equivalent, with particular focus on the overlap of curing and degradation at high temperatures. Finally, the impact of cure environment was examined by comparing Poly(P-ddm) and Poly(BF-a) networks polymerized in oxidative and inert conditions. Throughout, molecular dynamics (MD) simulations were used to explore atomistic differences in bond dissociation, triazine incorporation, and structure-property relationships.

Collectively, these results demonstrate that synthetic pathways, cure environment, and molecular connectivity govern polymerization behavior and network performance, providing a framework for reproducible, high-performance polybenzoxazines.

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