{"id":{"repo_id":"alabama","oai_identifier":"oai:ir.ua.edu:123456789/7917"},"canonical_url":"https://search.dev.ndltd.org/etd/alabama/oai:ir.ua.edu:123456789/7917","repository":{"repo_id":"alabama","name":"University of Alabama","base_url":"https://ir-api.ua.edu/oai/request"},"display":{"title":"Investigation of high-performance lithium-ion batteries based on highly conductive Li7La3Zr2O12 solid-state electrolyte and stable electrode-electrolyte interface","abstract":"With the merits of high Li+ conductivity, wide potential window, and electrochemical stability against metallic lithium anode (the highest theoretical capacity: 3,860 mAh g−1), cubic phase garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte has attracted much attention for developing solid-state batteries with increased safety, higher energy density, and longer lifespan. Besides, the solid-state or liquid electrolyte/electrode interface stability and low resistance are important to their optimized electrochemical performance of lithium-ion batteries. The goal of this dissertation is to develop high-performance lithium-ion batteries based on LLZO solid-state electrolyte and stable/low resistance electrode-electrolyte interface via (1) low-temperature synthesis/densification of Al/Bi-doped cubic LLZO electrolytes, (2) surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles, (3) composite polymer electrolytes, and (4) application of plastic-crystal interfacial modification.Chapter 3 explores a low-temperature synthesis strategy to obtain cubic LLZO powders via a combination of sol-gel method and ball milling induced tetragonal to cubic phase transition, which is ~200 °C lower than the thermally induced phase transition temperature. Chapter 4 investigates the role of a facial B2O3 surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles to achieve a stable cathode-electrolyte interface, which enables improved high-rate discharge performance and enhanced cycling stability of the batteries. Chapter 5 reveals the effects of LLZO ceramic filler distribution and doping elements (Al and Bi) on the ambient-temperature ionic conductivity, Li+ transference number, electrochemical stability window, and ability to suppress lithium dendrite growth of poly(vinylidene fluoride) based composite polymer electrolytes, as well as solid-state battery performance based on these composite polymer electrolytes. In Chapter 6, cubic Bi-doped LLZO ceramic pellets with a high relative density (>90%) and ionic conductivity (~1.32×10^(-4) S cm-1 at 20 °C) were achieved with a sintering temperature as low as 900 °C. A succinonitrile-based plastic-crystal interlayer at the Li/LLZO interface was demonstrated to be very effective to reduce interfacial resistance and enable stable cycling of a Li/LLZO/Li symmetric cell. With the help of the plastic-crystal interlayer and a composite cathode, a Li/LLZO/LiCoO2 all-solid-state battery was fabricated, which displayed a stable cycling at 0.1C for 40 times at 20 °C with a discharge capacity of ~115 mAh g-1 and a Coulombic efficiency of ~99%.","abstract_html":"With the merits of high Li+ conductivity, wide potential window, and electrochemical stability against metallic lithium anode (the highest theoretical capacity: 3,860 mAh g−1), cubic phase garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte has attracted much attention for developing solid-state batteries with increased safety, higher energy density, and longer lifespan. Besides, the solid-state or liquid electrolyte/electrode interface stability and low resistance are important to their optimized electrochemical performance of lithium-ion batteries. The goal of this dissertation is to develop high-performance lithium-ion batteries based on LLZO solid-state electrolyte and stable/low resistance electrode-electrolyte interface via (1) low-temperature synthesis/densification of Al/Bi-doped cubic LLZO electrolytes, (2) surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles, (3) composite polymer electrolytes, and (4) application of plastic-crystal interfacial modification.Chapter 3 explores a low-temperature synthesis strategy to obtain cubic LLZO powders via a combination of sol-gel method and ball milling induced tetragonal to cubic phase transition, which is ~200 °C lower than the thermally induced phase transition temperature. Chapter 4 investigates the role of a facial B2O3 surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles to achieve a stable cathode-electrolyte interface, which enables improved high-rate discharge performance and enhanced cycling stability of the batteries. Chapter 5 reveals the effects of LLZO ceramic filler distribution and doping elements (Al and Bi) on the ambient-temperature ionic conductivity, Li+ transference number, electrochemical stability window, and ability to suppress lithium dendrite growth of poly(vinylidene fluoride) based composite polymer electrolytes, as well as solid-state battery performance based on these composite polymer electrolytes. In Chapter 6, cubic Bi-doped LLZO ceramic pellets with a high relative density (>90%) and ionic conductivity (~1.32×10^(-4) S cm-1 at 20 °C) were achieved with a sintering temperature as low as 900 °C. A succinonitrile-based plastic-crystal interlayer at the Li/LLZO interface was demonstrated to be very effective to reduce interfacial resistance and enable stable cycling of a Li/LLZO/Li symmetric cell. With the help of the plastic-crystal interlayer and a composite cathode, a Li/LLZO/LiCoO2 all-solid-state battery was fabricated, which displayed a stable cycling at 0.1C for 40 times at 20 °C with a discharge capacity of ~115 mAh g-1 and a Coulombic efficiency of ~99%.","abstract_has_math":false,"creators":["Li, Junhao"],"institution":"University of Alabama Libraries","degree_name":null,"degree_level":null,"degree_discipline":null,"degree_department":null,"school":null,"contributors":["Gupta, Subhadra","Brewer, Luke N.","Huang, Qiang","Mahapatra, Manoj K."],"advisors":["Wang, Ruigang"],"committee_chairs":[],"committee_members":[],"year":2021,"date_issued":"2021","date_published":"2021","updated_at":"2026-07-27T18:44:27Z","subjects":["Engineering","Materials science"],"languages":["en_US","English"],"rights":["All rights reserved by the author unless otherwise indicated."],"rights_urls":[],"identifier_entries":[{"key":"dc:identifier.other","label":"Dc Identifier Other","values":["u0015_0000001_0003838","Li_alatus_0004D_14450"],"render_values":[{"text":"u0015_0000001_0003838","href":null,"code":true},{"text":"Li_alatus_0004D_14450","href":null,"code":true}]}]},"links":{"outbound_url":"http://ir.ua.edu/handle/123456789/7917","outbound_label":"Repository record","outbound_source":"dc:identifier.uri"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Gupta, Subhadra","Brewer, Luke N.","Huang, Qiang","Mahapatra, Manoj K."]},{"key":"dc:contributor.advisor","label":"Advisor","values":["Wang, Ruigang"]},{"key":"dc:contributor.other","label":"Dc Contributor Other","values":["University of Alabama Tuscaloosa"]},{"key":"dc:creator","label":"Author","values":["Li, Junhao"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date.accessioned","label":"Dc Date Accessioned","values":["2021-07-07T14:37:15Z"]},{"key":"dc:date.available","label":"Dc Date Available","values":["2021-07-07T14:37:15Z"]},{"key":"dc:date.issued","label":"Date","values":["2021"]},{"key":"dc:publisher","label":"Institution","values":["University of Alabama Libraries"]},{"key":"dc:type","label":"Dc Type","values":["thesis","text"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["Engineering","Materials science"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["English"]},{"key":"dc:language.iso","label":"Language (ISO)","values":["en_US"]},{"key":"dc:rights","label":"Dc Rights","values":["All rights reserved by the author unless otherwise indicated."]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier.other","label":"Dc Identifier Other","values":["u0015_0000001_0003838","Li_alatus_0004D_14450"]},{"key":"dc:identifier.uri","label":"Identifier URI","values":["http://ir.ua.edu/handle/123456789/7917"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["Electronic Thesis or Dissertation"]},{"key":"dc:description.abstract","label":"Abstract","values":["With the merits of high Li+ conductivity, wide potential window, and electrochemical stability against metallic lithium anode (the highest theoretical capacity: 3,860 mAh g−1), cubic phase garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte has attracted much attention for developing solid-state batteries with increased safety, higher energy density, and longer lifespan. Besides, the solid-state or liquid electrolyte/electrode interface stability and low resistance are important to their optimized electrochemical performance of lithium-ion batteries. The goal of this dissertation is to develop high-performance lithium-ion batteries based on LLZO solid-state electrolyte and stable/low resistance electrode-electrolyte interface via (1) low-temperature synthesis/densification of Al/Bi-doped cubic LLZO electrolytes, (2) surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles, (3) composite polymer electrolytes, and (4) application of plastic-crystal interfacial modification.Chapter 3 explores a low-temperature synthesis strategy to obtain cubic LLZO powders via a combination of sol-gel method and ball milling induced tetragonal to cubic phase transition, which is ~200 °C lower than the thermally induced phase transition temperature. Chapter 4 investigates the role of a facial B2O3 surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles to achieve a stable cathode-electrolyte interface, which enables improved high-rate discharge performance and enhanced cycling stability of the batteries. Chapter 5 reveals the effects of LLZO ceramic filler distribution and doping elements (Al and Bi) on the ambient-temperature ionic conductivity, Li+ transference number, electrochemical stability window, and ability to suppress lithium dendrite growth of poly(vinylidene fluoride) based composite polymer electrolytes, as well as solid-state battery performance based on these composite polymer electrolytes. In Chapter 6, cubic Bi-doped LLZO ceramic pellets with a high relative density (>90%) and ionic conductivity (~1.32×10^(-4) S cm-1 at 20 °C) were achieved with a sintering temperature as low as 900 °C. A succinonitrile-based plastic-crystal interlayer at the Li/LLZO interface was demonstrated to be very effective to reduce interfacial resistance and enable stable cycling of a Li/LLZO/Li symmetric cell. With the help of the plastic-crystal interlayer and a composite cathode, a Li/LLZO/LiCoO2 all-solid-state battery was fabricated, which displayed a stable cycling at 0.1C for 40 times at 20 °C with a discharge capacity of ~115 mAh g-1 and a Coulombic efficiency of ~99%."]},{"key":"dc:format.medium","label":"Dc Format Medium","values":["electronic"]},{"key":"dc:format.mimetype","label":"Dc Format Mimetype","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Investigation of high-performance lithium-ion batteries based on highly conductive Li7La3Zr2O12 solid-state electrolyte and stable electrode-electrolyte interface"]}]}],"canonical_facts":{"dc:contributor":["Gupta, Subhadra","Brewer, Luke N.","Huang, Qiang","Mahapatra, Manoj K."],"dc:contributor.advisor":["Wang, Ruigang"],"dc:contributor.other":["University of Alabama Tuscaloosa"],"dc:creator":["Li, Junhao"],"dc:date.accessioned":["2021-07-07T14:37:15Z"],"dc:date.available":["2021-07-07T14:37:15Z"],"dc:date.issued":["2021"],"dc:description":["Electronic Thesis or Dissertation"],"dc:description.abstract":["With the merits of high Li+ conductivity, wide potential window, and electrochemical stability against metallic lithium anode (the highest theoretical capacity: 3,860 mAh g−1), cubic phase garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte has attracted much attention for developing solid-state batteries with increased safety, higher energy density, and longer lifespan. Besides, the solid-state or liquid electrolyte/electrode interface stability and low resistance are important to their optimized electrochemical performance of lithium-ion batteries. The goal of this dissertation is to develop high-performance lithium-ion batteries based on LLZO solid-state electrolyte and stable/low resistance electrode-electrolyte interface via (1) low-temperature synthesis/densification of Al/Bi-doped cubic LLZO electrolytes, (2) surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles, (3) composite polymer electrolytes, and (4) application of plastic-crystal interfacial modification.Chapter 3 explores a low-temperature synthesis strategy to obtain cubic LLZO powders via a combination of sol-gel method and ball milling induced tetragonal to cubic phase transition, which is ~200 °C lower than the thermally induced phase transition temperature. Chapter 4 investigates the role of a facial B2O3 surface modification of LiNi1/3Co1/3Mn1/3O2 cathode particles to achieve a stable cathode-electrolyte interface, which enables improved high-rate discharge performance and enhanced cycling stability of the batteries. Chapter 5 reveals the effects of LLZO ceramic filler distribution and doping elements (Al and Bi) on the ambient-temperature ionic conductivity, Li+ transference number, electrochemical stability window, and ability to suppress lithium dendrite growth of poly(vinylidene fluoride) based composite polymer electrolytes, as well as solid-state battery performance based on these composite polymer electrolytes. In Chapter 6, cubic Bi-doped LLZO ceramic pellets with a high relative density (>90%) and ionic conductivity (~1.32×10^(-4) S cm-1 at 20 °C) were achieved with a sintering temperature as low as 900 °C. A succinonitrile-based plastic-crystal interlayer at the Li/LLZO interface was demonstrated to be very effective to reduce interfacial resistance and enable stable cycling of a Li/LLZO/Li symmetric cell. With the help of the plastic-crystal interlayer and a composite cathode, a Li/LLZO/LiCoO2 all-solid-state battery was fabricated, which displayed a stable cycling at 0.1C for 40 times at 20 °C with a discharge capacity of ~115 mAh g-1 and a Coulombic efficiency of ~99%."],"dc:format.medium":["electronic"],"dc:format.mimetype":["application/pdf"],"dc:identifier.other":["u0015_0000001_0003838","Li_alatus_0004D_14450"],"dc:identifier.uri":["http://ir.ua.edu/handle/123456789/7917"],"dc:language":["English"],"dc:language.iso":["en_US"],"dc:publisher":["University of Alabama Libraries"],"dc:rights":["All rights reserved by the author unless otherwise indicated."],"dc:subject":["Engineering","Materials science"],"dc:title":["Investigation of high-performance lithium-ion batteries based on highly conductive Li7La3Zr2O12 solid-state electrolyte and stable electrode-electrolyte interface"],"dc:type":["thesis","text"]},"updated_at":"2026-07-27T18:44:27Z"}