Date of Award
Campus Access Dissertation
Doctor of Philosophy (PhD)
Multivalent ion batteries offer transformative potential for meeting escalating energy demands and the transition from fossil fuels to renewables. This dissertation delves into divalent chemistries as alternatives to lithium-ion chemistry, examining the intertwined nature of solution structures and charge transfer mechanisms. By investigating the electrochemistry of nonaqueous Magnesium, Zinc, and Calcium divalent electrolytes, a foundational understanding is established to design high-performance electrolyte systems for future energy storage applications. In this work, the functionality of novel cosolvent-facilitated nonaqueous electrolytes was systematically investigated. Hydrodynamic studies illuminated charge transfer mechanisms of electrochemical deposition and dissolution of divalent magnesium, revealing underlying challenges facing these electrolyte systems. Solvation structure was studied across different cations, connecting to the electrochemistry and stability characteristics, and emphasizing the potential benefits of a tailored solvation environment for optimizing electrochemical properties. Incorporating studies on coordination, ionic interactions, and kinetic constraints becomes imperative, and contributes to the understanding of solvation structure's profound impact on the electrochemistry of divalent ions in rechargeable batteries. By revealing the interplay between electrolyte composition, cations, and solvation environments, a foundation is laid for high-performance electrolyte design. Fundamental exploration of multivalent electrochemical systems helps propel the advancement of novel rechargeable battery technologies, ultimately facilitating a greener, more sustainable energy landscape.
Asselin, Genevieve M., "Multivalent Electrolyte Insights: Bridging Structure and Electrochemistry" (2023). Graduate Doctoral Dissertations. 880.