Citation
Patheria, Eshaan Salim (2025) Multielectron Redox in Lithium-Rich, Industrial-Element Sulfides for High Energy Density Lithium-Ion Battery Cathodes. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/2pdg-hs94. https://resolver.caltech.edu/CaltechTHESIS:06032025-064811859
Abstract
This thesis develops a thermodynamic and electronic framework for lithium-ion battery cathodes and applies it to a new class of high-capacity sulfides composed exclusively of industrially abundant elements. It introduces lithium-rich cathodes composed of aluminum, iron, and sulfur that leverage reversible multielectron anion redox, in which the formation and cleavage of sulfur-sulfur bonds enable especially high extents of charge storage. A core design framework is established linking delithiated-phase stability to accessible electrochemical redox capacity. The chemical space is expanded with copper-substituted phases, in which unique copper-sulfur electronic interactions delocalize charge compensation beyond sulfur-sulfur bonds, thereby improving the reversibility of anion redox. These materials achieve high energy densities using only industrial elements, offering a promising foundation for next-generation lithium-ion cathodes that address both performance and raw materials constraints. Thus, this thesis advances the long-term goal of building more sustainable energy systems and expanding access to electricity worldwide.
Item Type: | Thesis (Dissertation (Ph.D.)) | |||||||||
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Subject Keywords: | lithium-ion batteries; lithium-ion cathodes; multielectron redox; anion redox; sulfide cathodes; energy storage; scalable battery materials; industrially abundant elements; lithium; copper; aluminum; iron; sulfur; high energy density | |||||||||
Degree Grantor: | California Institute of Technology | |||||||||
Division: | Chemistry and Chemical Engineering | |||||||||
Major Option: | Chemistry | |||||||||
Thesis Availability: | Public (worldwide access) | |||||||||
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Defense Date: | 30 May 2025 | |||||||||
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Record Number: | CaltechTHESIS:06032025-064811859 | |||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechTHESIS:06032025-064811859 | |||||||||
DOI: | 10.7907/2pdg-hs94 | |||||||||
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Default Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | |||||||||
ID Code: | 17399 | |||||||||
Collection: | CaltechTHESIS | |||||||||
Deposited By: | Eshaan Patheria | |||||||||
Deposited On: | 06 Jun 2025 22:06 | |||||||||
Last Modified: | 13 Jun 2025 19:34 |
Thesis Files
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PDF (Redacted thesis. Chapter 4 omitted)
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