Date of Award

12-2024

Document Type

Campus Access Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Chemistry/Physical/Analytical Chemistry

First Advisor

Niya Sa

Second Advisor

Jason Green

Third Advisor

Daniel Dowling, Kimberly Schifferli

Abstract

Magnesium-ion batteries (MIBs) stand out as highly promising candidates for next-generation energy storage solutions, owing to their divalent ion exchange properties, high theoretical volumetric capacity, abundant magnesium resources, and cost-effectiveness. However, the inefficiency of the deposition and dissolution processes at the magnesium metal anode poses a significant challenge to the commercialization of high-energy magnesium batteries. This challenge primarily stems from the lack of a suitable electrolyte compatible with the magnesium anode, the struggle to investigate the instability solid electrolyte interface (SEI), and the incomprehensive understanding of the underlying mechanisms governing magnesium electrodeposition and dissolution. This thesis investigates novel magnesium electrolyte designs and understands the electrolyte/anode interphases. Electroanalytical tools with in situ investigation of the dynamic evolution of the SEI are conducted in different magnesium systems, revealing significant differences in SEI formation and growth during electrochemical cycling. To improve the efficiency of reversible magnesium deposition, a fundamental understanding of the Mg nucleation and growth mechanisms is explored through in-situ diffraction measurements, offering real-time observation of crystal structure evolution at the electrochemically deposited magnesium interface by correlating the electrochemical control with the diffraction patterns. Exploration of multivalent electrochemical systems, SEI evolution, and the mechanisms of magnesium deposition sheds light on valuable insights for advancing high-performance rechargeable battery technologies.

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Signature page_signed.pdf (250 kB)

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