Date of Award

12-2025

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

School

Polymer Science and Engineering

Committee Chair

Zhe Qiang

Committee Chair School

Polymer Science and Engineering

Committee Member 2

Xiaodan Gu

Committee Member 2 School

Polymer Science and Engineering

Committee Member 3

Boran Ma

Committee Member 3 School

Polymer Science and Engineering

Committee Member 4

Sergei Nazarenko

Committee Member 4 School

Polymer Science and Engineering

Committee Member 5

Derek Patton

Committee Member 5 School

Polymer Science and Engineering

Abstract

Synthetic polymers play an essential role in nearly every aspect of our lives. Extending beyond single-use packaging, polymeric material design has progressed to attain tailorable architectures granting exceptional performance across advanced applications, including carbon-fiber reinforced polymer composites for aerospace, conductive materials for soft electronics, and drug carriers for biomedicine. While highly promising, intricately designed polymers needed to achieve excellent performance often have limited processability, complex synthetic methods, and expensive precursors. Furthermore, due to a lack of recyclability, commodity polymer waste streams result in both environmental impacts and a substantial loss of economic value. This dissertation focuses on developing robust strategies for elevating commercial polymers into functional, high-performance materials with an emphasis on simple processing steps and scalability. In the first portion of this work, complex plastic waste streams, including polyolefin-based textiles and mixed polyolefin wastes, were leveraged to prepare three-dimensionally (3D) structured carbon monoliths through a two-step process involving sulfonation-induced crosslinking and pyrolysis. This process was then extended to additively-manufactured (AM) structures, employing fused filament fabrication (FFF) and powder bed fusion (PBF) to expand structural complexity and elevate material properties. Due to their high conductivity and resistivity, structured carbons were utilized as resistive heating devices for electrified chemical synthesis and electrodes for electrochemical energy storage. The second portion of this work focuses on establishing manufacturing methods for the preparation of ordered mesoporous materials (OMMs) through process and precursor design. Accelerated OMM synthesis was enabled through a plasma reactor to facilitate high-throughput materials development. Additionally, commodity styrenic thermoplastic elastomers (TPEs), containing self-assembled nanostructures, were leveraged to prepare OMMs with a wide range of matrix chemistries, including polymers, ceramics, metal oxides, carbons, and carbon-metal/ceramic nanocomposites, which were implemented as low-cost anodes for high-performance sodium-ion batteries. Fabrication of OMMs with complex macroscopic structures was also enabled through simple AM techniques to expand the OMM utility. Moreover, OMM synthesis could be further simplified through the inclusion of a radical generator during sulfonation, which resulted in selective cleavage of polystyrene and mesopore formation in one-step, leading to excellent ion exchange sorbents. Overall, this dissertation offers several routes for upcycling commodity polymers into high-performance advanced materials.

ORCID ID

0000-0003-0526-194X

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