Hankins, Kie Scott (2022-04). Reactivity, Morphology, and Solvation Phenomena Over Electrode Interfaces in Battery Systems. Doctoral Dissertation.
Thesis
The global shift towards renewable energy resources and electric vehicles has generated an unprecedented demand for robust energy storage technology. Lithium-ion batteries with graphitic anodes are the current standard of energy storage, but they are insufficient to meet this demand, and are quickly approaching the theoretical limit of their energy density. In order to meet the energy storage requirements of the future, new chemistries beyond the standard lithium-ion formulation are needed. Many new battery chemistries are being researched, but they face substantial challenges in stability and durability that must be overcome before they can replace current technology. These challenges are strongly influenced by the reactivity and morphological behavior of the electrode surfaces, and the ion solvation and transport phenomena that occur in the electrolyte. The reactivity and morphology of the electrode can play both a beneficial or a catastrophic role in battery function, these behaviors are related to the chemical and mechanical properties of the electrode material and the electrolyte. The solvation and transport phenomena of ions control the stability and charging rate, as well as affect the surface behavior of the battery electrodes. These phenomena are influenced by the ion, electrode, and electrolyte chemistries. Much work is being done to understand and mitigate these challenges, but the nanoscale mechanisms that drive them are complex and not well-understood. In this work, I present several projects where I have used primarily-computational methods to elucidate the atom-scale phenomena that occur at electrode surfaces and in the electrolyte, in order to develop a broader understanding of the mechanisms that inhibit future battery chemistries.
