Fisher, Aaron StevenIntellectual Merit: The goal of this dissertation is to investigate the electrochemical properties and microstructure of thin film polymer electrolytes with enhanced electrochemical performance. Solid electrolyte architectures have been produced by blending novel room temperature ionic liquid (RTIL) chemistries with ionically conductive polymer matrices. A variety of microstructure and electrical characterization tools have been employed to understand the hybrid electrolyte's performance. Lithium-ion batteries are limited because of the safety of the electrolyte. The current generation of batteries uses organic solvents to conduct lithium between the electrodes. Occasionally, the low boiling point and high combustibility of these solvents lead to pressure build ups and fires within cells. Additionally, there are issues with electrolyte loss and decreased performance that must be accounted for in daily use. Thus, interest in replacing this system with a solid polymer electrolyte that can match the properties of an organic solvent is of great interest in battery research. However, a polymer electrolyte by itself is incapable of meeting the performance characteristics, and thus by adding an RTIL it has met the necessary threshold values. With the development of the novel sulfur based ionic liquid compounds, improved performance characteristics were realized for the polymer electrolyte. The synthesized RTILs were blended with ionically conductive polymer matrices (polyethylene oxide (PEO) or block copolymers of PEO) to produce solid electrolytes. Such shape-conforming materials could be lead to unique battery morphologies, but more importantly the safety of these new batteries will greatly exceeds those based on traditional organic carbonate electrolytes. Broader Impacts: The broader impact of this research is that it will ultimately help push forward an attractive alternative to carbonate based liquid electrolyte systems. Development of these alternatives has been slow; however bypassing the current commercial options will lead to not only safer and more powerful batteries. The polymer electrolyte system offers flexibility in both mechanical properties and product design. In due course, this will lead to batteries unlike any currently available on the market. RTILs offer quite an attractive option and the electrochemical understanding of novel architectures based upon sulfur will lead to further potential uses for these compounds.DissertationEnergyPolymer chemistryChemical engineeringElectrolyteIonic LiquidLithium BatteriesPolymer