Date of Award

8-2024

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

School

Polymer Science and Engineering

Committee Chair

Dr. Xiaodan Gu

Committee Chair School

Polymer Science and Engineering

Committee Member 2

Dr. Derek Patton

Committee Member 2 School

Polymer Science and Engineering

Committee Member 3

Dr. Sarah Morgan

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. Yoan Simon

Committee Member 5 School

Polymer Science and Engineering

Abstract

Stretchable semiconductors are pivotal in advancing wearable and implantable electronics, with those boasting both high stretchability and self-healing capabilities being especially significant for a myriad of wearable applications. In this dissertation, we developed an extremely soft, highly stretchable, and self-healing elastomer based on H-bonding crosslinked amide-functionalized polyisobutylene (PIB-amide). When blended with a high-performance conjugated diketopyrrolopyrrole (DPP-T) polymer, the composite exhibits unprecedented stretchability, exceptionally low elastic modulus, and an innate ability to self-heal at room temperature.

The morphology of conjugated polymer/elastomer semiconducting composites have significant impacts on electrical and mechanical properties Further investigations focused on manipulating the phase separation size in CP/elastomer composites by precise placement of H-bonding functional groups within both the CPs and the elastomers. This study elucidates how these strategic modifications influence the composites' mechanical and electrical performance. By introducing amide functional groups to both a DPP-based semiconducting polymer (DPPTVT-A) and a polyisobutylene-based elastomer (PIB-A), we facilitated inter- and intra-phase H-bonding crosslinks. This approach enabled us to fabricate composites with varying crosslinking patterns—dual, uni, and non-H-bonding—thereby allowing a comparative analysis of their phase behaviors and electronic and mechanical properties.

Additionally, an analysis of the mechanical properties of 65 CP thin films challenged the prevailing belief that rigidity and stretchability are mutually exclusive. Our study of rigid deformable CPs reveals their mechanical behavior, electrical properties, and deformation mechanisms.

This dissertation contributes a novel perspective to the development and molecular origin of semiconductive polymers and composites that are stretchable and highly healable, heralding novel applications in the burgeoning field of stretchable electronics.

ORCID ID

0000-0001-7555-5308

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