Lithium batteries have powered portable electronics for two decades and are emerging as a leading power source for sustainable transportation. Lithium batteries include various categories defined by their electrode materials and electrolytes. In each category, there are demands for improved energy, power, lifespan, safety, and cost. To address these demands, new materials are needed. In this dissertation, computational research is presented based on density functional theory and a variety of thermodynamic models to build knowledge about the behavior of existing materials and also predict new materials for improved performance. Electrode coatings can limit reactivity at electrode-electrolyte interfaces. We study coatings for phosphate cathodes, oxide cathodes, and lithium metal anodes to determine reactivity during material processing and battery operation. Coatings are identified with exceptional stability including LiNiPO4 for LiMnPO4 cathodes, Li3PO 4 for oxide cathodes, and a variety of new coatings for lithium metal anodes. Oxygen evolution contributes to thermal runaway and jeopardizes safety. We explore delithiated phosphate cathodes to determine the relationship between cathode transition metal composition and oxygen evolution behavior. Ion exchange materials can help lithium producers deliver a secure supply of lithium needed for the battery industry. We identify new ion exchange materials to absorb lithium with high selectivity from various brine resources and then release the lithium in acid. Experimental work is proposed to validate new insights into existing materials and to test new materials for improved performance.
|Advisor:||Wolverton, Chris M.|
|Commitee:||Haile, Sossina M., Hersam, Mark C., Thackeray, Michael M.|
|Department:||Materials Science and Engineering|
|School Location:||United States -- Illinois|
|Source:||DAI-B 78/02(E), Dissertation Abstracts International|
|Subjects:||Chemistry, Energy, Materials science|
|Keywords:||Batteries, Chemistry, DFT, Lithium, Materials, Thermodynamics|
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