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Multielectron Redox in Lithium-Rich, Industrial-Element Sulfides for High Energy Density Lithium-Ion Battery Cathodes

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.))
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)
Research Advisor(s):
  • See, Kimberly A.
Thesis Committee:
  • Chan, Garnet K. (chair)
  • Hadt, Ryan G.
  • Manthiram, Karthish
  • See, Kimberly
Defense Date:30 May 2025
Funders:
Funding AgencyGrant Number
National Science FoundationDMR-2340864
National Science FoundationDGE-2139433
U.S. Department of Energy, Office of Science, Basic Energy SciencesDE-SC0019381
Record Number:CaltechTHESIS:06032025-064811859
Persistent URL:https://resolver.caltech.edu/CaltechTHESIS:06032025-064811859
DOI:10.7907/2pdg-hs94
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.4c18440UNSPECIFIEDArticle adapted for Chapters 2 and 3.
https://doi.org/10.1016/B978-0-12-823144-9.00110-2UNSPECIFIEDBook chapter adapted for Chapter 1.
ORCID:
AuthorORCID
Patheria, Eshaan Salim0000-0002-2761-8498
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

[img] PDF (Redacted thesis. Chapter 4 omitted) - Final Version
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