dc.contributor.author	Zanelotti, Curt Joseph	en
dc.contributor.committeechair	Madsen, Louis A.	en
dc.contributor.committeemember	Qiao, Rui	en
dc.contributor.committeemember	Moore, Robert Bowen	en
dc.contributor.committeemember	Morris, John R.	en
dc.contributor.department	Chemistry	en
dc.date.accessioned	2022-01-29T09:00:29Z	en
dc.date.available	2022-01-29T09:00:29Z	en
dc.date.issued	2022-01-28	en
dc.description.abstract	This dissertation aims to develop, characterize, and fundamentally understand a new class of materials termed "molecular ionic composites" (MICs). MICs show promise as next-generation solid electrolytes for batteries. MICs form when mixing a rigid polyanion with purely ionic fluids, and they behave mechanically as a solid but contain a high density of ions that move nearly as in a neat liquid. Specifically, prototypical MICs are based on solutions of the rigid-rod polyelectrolyte poly(2,2'-disulfonyl-4,4'-benzideneterephthalamide) (PBDT), which forms a double helix, combined with imidazolium-based ionic liquids (ILs). The IL comprises 75-97 wt% of the final solid, even though the Young's modulus can reach ~ 2 GPa at 80 wt% IL. We propose that these properties are driven by a biphasic internal structure in MICs corresponding to IL-rich "puddles" (an interconnected liquid phase) and PBDT-IL associated "bundles" where IL ions form the collective electrostatic associations that cause the MICs to be a solid. Through this dissertation I will discuss a wide variety of MICs that have been created through the use of two different formation processes, the "ingot" method and the "solvent casting" method, which allow for the use of many different ionic fluid sources to further tune MIC properties. The following chapters build to the fundamental knowledge and our current understanding of the wide variety of materials that can be created from PBDT and IL.	en
dc.description.abstractgeneral	Battery electrolytes, biosensors, and hydrogels all depend on new materials for next-generation applications. For these new materials to be used characterization on the interactions, morphological restrictions, and/or what unique internal structures used to generate their properties must be performed. Through This analysis using common polymeric characterization techniques these materials can be further optimized. This dissertation highlights a new class of materials termed "molecular ionic composites" (MICs) which are formed from a rigid double helical polymer, poly(2,2'-disulfonyl-4,4'-benzideneterephthalamide) (PBDT), and fluids composed entirely of ions, including ionic liquids (ILs). These composite systems feature a unique combination of properties including high thermal stability, mechanical stability, and excellent ionic conductivity, all of which are highly tunable through the amount of PBDT incorporated or the fluid ion types. Chapters 3, 4, 5, and 6 present fundamental investigations of MICs to determine how tunable they are, the processes by which they form, and the various ways we can fabricate them. Chapter 7 describes the creation of another impressive material formed from PBDT-low-polymer-content hydrogels. These studies are intended to provide deeper understanding of the behaviors of these unique materials and how they may be used in the future.	en
dc.description.degree	Doctor of Philosophy	en
dc.format.medium	ETD	en
dc.identifier.other	vt_gsexam:33681	en
dc.identifier.uri	http://hdl.handle.net/10919/107997	en
dc.language.iso	en	en
dc.publisher	Virginia Tech	en
dc.rights	In Copyright	en
dc.rights.uri	http://rightsstatements.org/vocab/InC/1.0/	en
dc.subject	Polymer Electrolytes	en
dc.subject	Ion Gels	en
dc.subject	Rigid-rod Polyelectrolytes	en
dc.subject	NMR	en
dc.subject	Self-diffusion	en
dc.subject	Variable Temperature Ion Transport	en
dc.subject	Hydrogel	en
dc.subject	Self-assembly	en
dc.title	Development, Characterization, and Fundamental Studies on Molecular Ionic Composites and PBDT Hydrogels	en
dc.type	Dissertation	en
thesis.degree.discipline	Chemistry	en
thesis.degree.grantor	Virginia Polytechnic Institute and State University	en
thesis.degree.level	doctoral	en
thesis.degree.name	Doctor of Philosophy	en

Development, Characterization, and Fundamental Studies on Molecular Ionic Composites and PBDT Hydrogels

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