Date of Award

Summer 2025

Document Type

Open Access Dissertation

Department

Chemistry and Biochemistry

First Advisor

Morgan Stefik

Second Advisor

Michael L. Myrick

Abstract

The initial commercialization and subsequent development of the lithium-ion battery (LIB) in 1991 has revolutionized the way that humans power devices, cars, and homes and led to the advent of many technologies that seemed impossible just half a century ago. As LIBs are integrated into more of daily life through handheld devices, wearable medical devices, transportation, and grid-level energy storage, the demand for fast charging and high energy density increases rapidly. To design a battery with these favorable qualities, an understanding of the effect of electrode crystal structure and electrode morphology on the ionic/electronic transport and failure modes must be developed. However, cause and effect relationships between material structure and material performance are traditionally hard to derive due to the convolution of many concurrent, rapid processes during battery charging in addition to the wide variety of materials and lack of direct comparisons between similar materials and methods in literature.

These challenges may be resolved with the comparison of lithiation behavior in isomorphic structures, which allows for an extraction of the effect of specific material dimensions such as crystallographic channel size and metal polyhedra size on transport properties. Similarly, different lithiation conditions with the same material allow for isolation of favorable charging conditions that improve capacity retention over unprecedented cycling lifetime. Additionally, the development of nanostructured oxides with tunable defect states allows identification of specific crystalline defects in electrodes which may be beneficial for LIB application. These insights allow for selection of ideal crystal features (structures and defects) and charging conditions for new, high-performance batteries.

Rights

© 2025, Sean Cade Wechsler

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