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NOVEL METHODS AND MECHANISTIC UNDERSTANDING OF BATTERY MATERIALS AND INTERFACES

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Abstract

Since the Industrial Revolution, there has been an ever-climbing demand for energy. Most of this energy comes from the combustion of fossil fuels, which as a side product, generates greenhouse gases. As a result, since 1980, the average global temperature has risen at an average rate of 3 °C/100 years. To mitigate the effects of global warming, we need to reduce our carbon emissions to net zero which requires the transition from fossil fuels to renewable energy sources. However, the intermittency of renewable energy sources makes them non-dispatchable. Electric energy storage systems (EESSs) can aid in the implementation of renewable energy sources by storing energy produced in excess from renewables and supplying it when needed. Rechargeable batteries are the most attractive EESS due to their high energy densities. With a wide variety of potential applications including their widespread use in electric vehicles, we need to develop rechargeable batteries that are less expensive while increasing their energy and power densities. Herein, various rechargeable batteries including lithium metal, sodium metal and sodium-ion batteries were studied as post lithium-ion battery (LIB) alternatives. Lithium and sodium metal anodes can deliver much higher capacities compared to commercial LIBs, albeit with a lower inherent stability. Both metal anodes were studied in various electrolytes to understand and alleviate their dendritic growth. Sodium-ion batteries (SIBs) possess lower energy densities compared to LIBs. However, the reduced costs of Na make SIBs an attractive alternative to the traditional LIB technology. Prussian blue and its nickel analogue were studied as cathode materials for SIBs and spectroscopically investigated to understand the differences in their performances. Along with next-generation batteries, a third electrode was employed to serve as an independent reference electrode. It provides more reliable potentials for the working electrode by monitoring them independently and prevents misleading conclusions. Electrochemical analyses were conducted to evaluate the performance of materials. Synchrotron-based X-ray studies were utilized to investigate chemical changes in materials and understand the mechanisms under the operational conditions. Other techniques such as X-ray photoelectron spectroscopy and scanning/transmission electron microscopy were employed to analyze morphologies, crystal structures and chemical compositions of materials.

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Description

162 pages

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Date Issued

2021-08

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Keywords

Energy storage systems; Next generation rechargeable batteries; Operando measurements

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Union Local

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Committee Chair

Abruna, Hector D.

Committee Co-Chair

Committee Member

Archer, Lynden A.
DiSalvo, Francis J.

Degree Discipline

Chemistry and Chemical Biology

Degree Name

Ph. D., Chemistry and Chemical Biology

Degree Level

Doctor of Philosophy

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Government Document

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Attribution-NonCommercial-NoDerivatives 4.0 International

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dissertation or thesis

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