{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/130178"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/130178","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Interfacial electrochemo-mechanical studies of nano/microstructures in lithium-ion batteries","abstract":"Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2027-08-01","abstract_html":"Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2027-08-01","abstract_has_math":false,"creators":["Jeong, Hyewon"],"institution":"University of Illinois Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Materials Science & Engr","degree_department":null,"school":null,"contributors":["Braun, Paul","Zuo, Jian-Min","Krogstad, Jessica Anne","Wang, Pingfeng"],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2025,"date_issued":"2025-07-18","date_published":"2025-07-18","updated_at":"2026-07-22T22:25:06Z","subjects":["Electrochemo-mechanics","Silicon Anodes","Solid-state Batteries","Engineering Cei (cathode-electrolyte Interphase)","Scanning Transmission Electron Microscopy (stem)"],"languages":["en","eng"],"rights":["Copyright 2025 Hyewon Jeong"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"https://hdl.handle.net/2142/130178","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Braun, Paul","Zuo, Jian-Min","Krogstad, Jessica Anne","Wang, Pingfeng"]},{"key":"dc:creator","label":"Author","values":["Jeong, Hyewon"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2025-07-18","2025-08"]},{"key":"dc:type","label":"Dc Type","values":["text"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Materials Science & Engr"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Dissertation"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph.D."]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["University of Illinois Urbana-Champaign"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["Electrochemo-mechanics","Silicon Anodes","Solid-state Batteries","Engineering Cei (cathode-electrolyte Interphase)","Scanning Transmission Electron Microscopy (stem)"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["en","eng"]},{"key":"dc:rights","label":"Dc Rights","values":["Copyright 2025 Hyewon Jeong"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["https://hdl.handle.net/2142/130178"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2027-08-01","The student, Hyewon Jeong, accepted the attached license on 2025-07-13 at 14:31.","The student, Hyewon Jeong, submitted this Dissertation for approval on 2025-07-13 at 14:51.","This Dissertation was approved for publication on 2025-07-18 at 11:33.","DSpace SAF Submission Ingestion Package generated from Vireo submission #22536 on 2025-10-25 at 15:53:52","1. Nickel current collector | Silicon (anode) Silicon has emerged as a promising anode material due to its high lithium storage capacity. While commercial batteries may now include silicon particles, porous three-dimensional (3D) scaffolded silicon electrodes may enable higher silicon loading by providing space to accommodate the silicon volume expansion during alloying with lithium without significant electrode swelling. However, the electrochemo-mechanical response of silicon film on a metal scaffold is not well understood due to the complex morphology of the scaffold. Here we explore the role of scaffold curvature on the cycling behavior of silicon films and show that different curvatures exhibit distinctive silicon failure modes. Negative curvature shows tensile and compressive stress driven-crack opening failure. Positive curvature is correlated with tensile stress driven buckling. Zero curvatures (a flat surface) exhibit fragmentation. The detailed electrode morphology and chemistry for these systems is evaluated via scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy (STEM-EDS). COMSOL Multiphysics simulations also show the electrochemo-mechanics of silicon are curvature-dependent. These findings point the way towards design strategies for next-generation 3D architected silicon anodes with improved cycling integrity. 2. Lithium cobalt oxide, LiCoO2 (cathode) | Lithium indium chloride, Li3InCl6 (LIC, solid-electrolyte) All-solid-state batteries (ASSBs) are emerging as a promising energy storage solution due to their enhanced safety, high energy density, and improved performance over conventional lithium-ion batteries (LIBs). The use of solid electrolytes, such as sulfides, oxides, or halides, helps mitigate issues like leakage, flammability, and dendrite formation typically associated with liquid-electrolyte systems. In this thesis, layered LiCoO2 (LCO) cathodes and Li3InCl6 (LIC) solid-electrolytes were selected for their high energy density and oxidation stability. Our study via scanning transmission electron microscopy (STEM) reveals that a spinel structure forms uniformly (~15 nm) on the LCO surface over extended cycling at high temperatures, leading to performance degradation. Through various testing conditions—including voltage holding, resting, and different charge rates—we identified that the spinel phase nucleates under electrochemical influence at high temperatures, during fast charging at room temperature, and at high states of charge. This phenomenon is corroborated by electrochemical impedance spectroscopy (EIS), which shows a growth in interfacial resistance in the presence of the spinel phase. These findings provide valuable insights into the origins of spinel formation and its role in the accelerated degradation of solid-state batteries."]},{"key":"dc:format","label":"Dc Format","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Interfacial electrochemo-mechanical studies of nano/microstructures in lithium-ion batteries"]}]}],"canonical_facts":{"dc:contributor":["Braun, Paul","Zuo, Jian-Min","Krogstad, Jessica Anne","Wang, Pingfeng"],"dc:creator":["Jeong, Hyewon"],"dc:date":["2025-07-18","2025-08"],"dc:description":["Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2027-08-01","The student, Hyewon Jeong, accepted the attached license on 2025-07-13 at 14:31.","The student, Hyewon Jeong, submitted this Dissertation for approval on 2025-07-13 at 14:51.","This Dissertation was approved for publication on 2025-07-18 at 11:33.","DSpace SAF Submission Ingestion Package generated from Vireo submission #22536 on 2025-10-25 at 15:53:52","1. Nickel current collector | Silicon (anode) Silicon has emerged as a promising anode material due to its high lithium storage capacity. While commercial batteries may now include silicon particles, porous three-dimensional (3D) scaffolded silicon electrodes may enable higher silicon loading by providing space to accommodate the silicon volume expansion during alloying with lithium without significant electrode swelling. However, the electrochemo-mechanical response of silicon film on a metal scaffold is not well understood due to the complex morphology of the scaffold. Here we explore the role of scaffold curvature on the cycling behavior of silicon films and show that different curvatures exhibit distinctive silicon failure modes. Negative curvature shows tensile and compressive stress driven-crack opening failure. Positive curvature is correlated with tensile stress driven buckling. Zero curvatures (a flat surface) exhibit fragmentation. The detailed electrode morphology and chemistry for these systems is evaluated via scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy (STEM-EDS). COMSOL Multiphysics simulations also show the electrochemo-mechanics of silicon are curvature-dependent. These findings point the way towards design strategies for next-generation 3D architected silicon anodes with improved cycling integrity. 2. Lithium cobalt oxide, LiCoO2 (cathode) | Lithium indium chloride, Li3InCl6 (LIC, solid-electrolyte) All-solid-state batteries (ASSBs) are emerging as a promising energy storage solution due to their enhanced safety, high energy density, and improved performance over conventional lithium-ion batteries (LIBs). The use of solid electrolytes, such as sulfides, oxides, or halides, helps mitigate issues like leakage, flammability, and dendrite formation typically associated with liquid-electrolyte systems. In this thesis, layered LiCoO2 (LCO) cathodes and Li3InCl6 (LIC) solid-electrolytes were selected for their high energy density and oxidation stability. Our study via scanning transmission electron microscopy (STEM) reveals that a spinel structure forms uniformly (~15 nm) on the LCO surface over extended cycling at high temperatures, leading to performance degradation. Through various testing conditions—including voltage holding, resting, and different charge rates—we identified that the spinel phase nucleates under electrochemical influence at high temperatures, during fast charging at room temperature, and at high states of charge. This phenomenon is corroborated by electrochemical impedance spectroscopy (EIS), which shows a growth in interfacial resistance in the presence of the spinel phase. These findings provide valuable insights into the origins of spinel formation and its role in the accelerated degradation of solid-state batteries."],"dc:format":["application/pdf"],"dc:identifier":["https://hdl.handle.net/2142/130178"],"dc:language":["en","eng"],"dc:rights":["Copyright 2025 Hyewon Jeong"],"dc:subject":["Electrochemo-mechanics","Silicon Anodes","Solid-state Batteries","Engineering Cei (cathode-electrolyte Interphase)","Scanning Transmission Electron Microscopy (stem)"],"dc:title":["Interfacial electrochemo-mechanical studies of nano/microstructures in lithium-ion batteries"],"dc:type":["text"],"thesis:degree_discipline":["Materials Science & Engr"],"thesis:degree_level":["Dissertation"],"thesis:degree_name":["Ph.D."],"thesis:institution_name":["University of Illinois Urbana-Champaign"]},"updated_at":"2026-07-22T22:25:06Z"}