{"id":{"repo_id":"texas","oai_identifier":"oai:repositories.lib.utexas.edu:2152/116040"},"canonical_url":"https://search.dev.ndltd.org/etd/texas/oai:repositories.lib.utexas.edu:2152/116040","repository":{"repo_id":"texas","name":"University of Texas","base_url":"https://repositories.lib.utexas.edu/server/oai/request"},"display":{"title":"High-nickel layered oxide cathodes for high-performance lithium-ion batteries","abstract":"The ever-growing market of consumer electronics has been driving surging demand for higher-energy-density lithium-ion batteries (LIBs). Since cathode materials primarily dictate the energy density and cost, extensive investigations have been devoted to exploring advanced cathodes for high-performance LIBs. High-nickel layered oxides LiNi [subscript x] M [subscript 1-x] O₂ (x ≥ 0.6, M = Co, Mn, etc.) are one of the most promising candidates and are being extensively pursued. Unfortunately, the practical applicability of high-Ni cathodes is seriously hampered by their poor cyclability, alarming susceptibility to thermal abuse, and decreased air-stability. This dissertation focuses on enhancing the stability of high-Ni cathodes with diverse strategies and advancing the scientific comprehension of high-Ni cathode materials. First, the effect of pillaring Mg-ion doping in the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂ is investigated. The incorporation of Mg greatly suppresses the anisotropic lattice collapse and maintains the integrity of cathode particles upon high-voltage cycling, significantly enhancing the cyclability. More importantly, the thermal stability of high-Ni cathodes is notably improved by Mg doping. Second, boron-based polyanion is employed to tune high-Ni cathodes. The introduction of boron-based polyanion enables a well-passivated boron/phosphorus-rich cathode-electrolyte interphase, which alleviates electrolyte corrosion on high-Ni cathodes and thus improves the cyclability. Meanwhile, the boron-based polyanion improves the air stability of high-Ni cathodes as well. Third, a well-designed phosphoric acid treatment approach is presented to modify the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂. The implemented treatment not only reduces the detrimental surface residual lithium, but also remarkably improves the electrochemical performance and long-term air-storage stability. Via a range of advanced analytical techniques, the underlying mechanisms involved on the improved performance are disclosed from interphasial and structural perspectives at the nanoscale. Finally, a comparative study is performed to unveil the stabilities of LiNi [subscript 1-x-y] Mn [subscript x] Co [subscript y] O₂ (NMC) cathodes with different Ni contents at identical degrees of delithiation. The overall stabilities of two representative cathodes, LiNi₀.₈Mn₀.₁Co₀.₁O₂ and LiNiO₂, are evaluated with a rigorous control of an identical 70 mol % delithiation. The results suggest that NMC cathodes with higher-Ni contents may have better overall stability than low-Ni NMC cathodes at a given degree of delithiation, disparate from the prevailing belief that high-Ni cathodes with higher-Ni content have inherently reduced stabilities","abstract_html":"The ever-growing market of consumer electronics has been driving surging demand for higher-energy-density lithium-ion batteries (LIBs). Since cathode materials primarily dictate the energy density and cost, extensive investigations have been devoted to exploring advanced cathodes for high-performance LIBs. High-nickel layered oxides LiNi [subscript x] M [subscript 1-x] O₂ (x ≥ 0.6, M = Co, Mn, etc.) are one of the most promising candidates and are being extensively pursued. Unfortunately, the practical applicability of high-Ni cathodes is seriously hampered by their poor cyclability, alarming susceptibility to thermal abuse, and decreased air-stability. This dissertation focuses on enhancing the stability of high-Ni cathodes with diverse strategies and advancing the scientific comprehension of high-Ni cathode materials. First, the effect of pillaring Mg-ion doping in the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂ is investigated. The incorporation of Mg greatly suppresses the anisotropic lattice collapse and maintains the integrity of cathode particles upon high-voltage cycling, significantly enhancing the cyclability. More importantly, the thermal stability of high-Ni cathodes is notably improved by Mg doping. Second, boron-based polyanion is employed to tune high-Ni cathodes. The introduction of boron-based polyanion enables a well-passivated boron/phosphorus-rich cathode-electrolyte interphase, which alleviates electrolyte corrosion on high-Ni cathodes and thus improves the cyclability. Meanwhile, the boron-based polyanion improves the air stability of high-Ni cathodes as well. Third, a well-designed phosphoric acid treatment approach is presented to modify the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂. The implemented treatment not only reduces the detrimental surface residual lithium, but also remarkably improves the electrochemical performance and long-term air-storage stability. Via a range of advanced analytical techniques, the underlying mechanisms involved on the improved performance are disclosed from interphasial and structural perspectives at the nanoscale. Finally, a comparative study is performed to unveil the stabilities of LiNi [subscript 1-x-y] Mn [subscript x] Co [subscript y] O₂ (NMC) cathodes with different Ni contents at identical degrees of delithiation. The overall stabilities of two representative cathodes, LiNi₀.₈Mn₀.₁Co₀.₁O₂ and LiNiO₂, are evaluated with a rigorous control of an identical 70 mol % delithiation. The results suggest that NMC cathodes with higher-Ni contents may have better overall stability than low-Ni NMC cathodes at a given degree of delithiation, disparate from the prevailing belief that high-Ni cathodes with higher-Ni content have inherently reduced stabilities","abstract_has_math":false,"creators":["Xie, Qiang, Ph. D."],"institution":"The University of Texas at Austin","degree_name":"Doctor of Philosophy","degree_level":"Doctoral","degree_discipline":"Materials Science and Engineering","degree_department":null,"school":null,"contributors":[],"advisors":["Manthiram, Arumugam"],"committee_chairs":[],"committee_members":["Goodenough, John B","Hwang, Gyeong S","Yu, Guihua"],"year":2020,"date_issued":"2020-11-09","date_published":"2020-11-09","updated_at":"2026-07-24T05:01:18Z","subjects":["High-nickel layered oxide cathodes","Lithium-ion batteries","Electrode-electrolyte interphase","Thermal stability"],"languages":["en"],"rights":[],"rights_urls":[],"identifier_entries":[{"key":"dc:identifier.uri","label":"Identifier URI","values":["http://dx.doi.org/10.26153/tsw/42936"],"render_values":[{"text":"http://dx.doi.org/10.26153/tsw/42936","href":"http://dx.doi.org/10.26153/tsw/42936","code":true}]}]},"links":{"outbound_url":"https://hdl.handle.net/2152/116040","outbound_label":"Handle","outbound_source":"dc:identifier.uri"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor.advisor","label":"Advisor","values":["Manthiram, Arumugam"]},{"key":"dc:contributor.committeemember","label":"Committee Member","values":["Goodenough, John B","Hwang, Gyeong S","Yu, Guihua"]},{"key":"dc:creator","label":"Author","values":["Xie, Qiang, Ph. D."]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date.accessioned","label":"Dc Date Accessioned","values":["2022-10-01T22:19:03Z"]},{"key":"dc:date.available","label":"Dc Date Available","values":["2022-10-01T22:19:03Z"]},{"key":"dc:date.issued","label":"Date","values":["2020-11-09"]},{"key":"dc:type","label":"Dc Type","values":["Thesis"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Materials Science and Engineering"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Doctoral"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Doctor of Philosophy"]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["The University of Texas at Austin"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["High-nickel layered oxide cathodes","Lithium-ion batteries","Electrode-electrolyte interphase","Thermal stability"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language.iso","label":"Language (ISO)","values":["en"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier.uri","label":"Identifier URI","values":["https://hdl.handle.net/2152/116040","http://dx.doi.org/10.26153/tsw/42936"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description.abstract","label":"Abstract","values":["The ever-growing market of consumer electronics has been driving surging demand for higher-energy-density lithium-ion batteries (LIBs). Since cathode materials primarily dictate the energy density and cost, extensive investigations have been devoted to exploring advanced cathodes for high-performance LIBs. High-nickel layered oxides LiNi [subscript x] M [subscript 1-x] O₂ (x ≥ 0.6, M = Co, Mn, etc.) are one of the most promising candidates and are being extensively pursued. Unfortunately, the practical applicability of high-Ni cathodes is seriously hampered by their poor cyclability, alarming susceptibility to thermal abuse, and decreased air-stability. This dissertation focuses on enhancing the stability of high-Ni cathodes with diverse strategies and advancing the scientific comprehension of high-Ni cathode materials. First, the effect of pillaring Mg-ion doping in the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂ is investigated. The incorporation of Mg greatly suppresses the anisotropic lattice collapse and maintains the integrity of cathode particles upon high-voltage cycling, significantly enhancing the cyclability. More importantly, the thermal stability of high-Ni cathodes is notably improved by Mg doping. Second, boron-based polyanion is employed to tune high-Ni cathodes. The introduction of boron-based polyanion enables a well-passivated boron/phosphorus-rich cathode-electrolyte interphase, which alleviates electrolyte corrosion on high-Ni cathodes and thus improves the cyclability. Meanwhile, the boron-based polyanion improves the air stability of high-Ni cathodes as well. Third, a well-designed phosphoric acid treatment approach is presented to modify the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂. The implemented treatment not only reduces the detrimental surface residual lithium, but also remarkably improves the electrochemical performance and long-term air-storage stability. Via a range of advanced analytical techniques, the underlying mechanisms involved on the improved performance are disclosed from interphasial and structural perspectives at the nanoscale. Finally, a comparative study is performed to unveil the stabilities of LiNi [subscript 1-x-y] Mn [subscript x] Co [subscript y] O₂ (NMC) cathodes with different Ni contents at identical degrees of delithiation. The overall stabilities of two representative cathodes, LiNi₀.₈Mn₀.₁Co₀.₁O₂ and LiNiO₂, are evaluated with a rigorous control of an identical 70 mol % delithiation. The results suggest that NMC cathodes with higher-Ni contents may have better overall stability than low-Ni NMC cathodes at a given degree of delithiation, disparate from the prevailing belief that high-Ni cathodes with higher-Ni content have inherently reduced stabilities"]},{"key":"dc:format.mimetype","label":"Dc Format Mimetype","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["High-nickel layered oxide cathodes for high-performance lithium-ion batteries"]}]}],"canonical_facts":{"dc:contributor.advisor":["Manthiram, Arumugam"],"dc:contributor.committeemember":["Goodenough, John B","Hwang, Gyeong S","Yu, Guihua"],"dc:creator":["Xie, Qiang, Ph. D."],"dc:date.accessioned":["2022-10-01T22:19:03Z"],"dc:date.available":["2022-10-01T22:19:03Z"],"dc:date.issued":["2020-11-09"],"dc:description.abstract":["The ever-growing market of consumer electronics has been driving surging demand for higher-energy-density lithium-ion batteries (LIBs). Since cathode materials primarily dictate the energy density and cost, extensive investigations have been devoted to exploring advanced cathodes for high-performance LIBs. High-nickel layered oxides LiNi [subscript x] M [subscript 1-x] O₂ (x ≥ 0.6, M = Co, Mn, etc.) are one of the most promising candidates and are being extensively pursued. Unfortunately, the practical applicability of high-Ni cathodes is seriously hampered by their poor cyclability, alarming susceptibility to thermal abuse, and decreased air-stability. This dissertation focuses on enhancing the stability of high-Ni cathodes with diverse strategies and advancing the scientific comprehension of high-Ni cathode materials. First, the effect of pillaring Mg-ion doping in the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂ is investigated. The incorporation of Mg greatly suppresses the anisotropic lattice collapse and maintains the integrity of cathode particles upon high-voltage cycling, significantly enhancing the cyclability. More importantly, the thermal stability of high-Ni cathodes is notably improved by Mg doping. Second, boron-based polyanion is employed to tune high-Ni cathodes. The introduction of boron-based polyanion enables a well-passivated boron/phosphorus-rich cathode-electrolyte interphase, which alleviates electrolyte corrosion on high-Ni cathodes and thus improves the cyclability. Meanwhile, the boron-based polyanion improves the air stability of high-Ni cathodes as well. Third, a well-designed phosphoric acid treatment approach is presented to modify the high-Ni cathode LiNi₀.₉₄Co₀.₀₆O₂. The implemented treatment not only reduces the detrimental surface residual lithium, but also remarkably improves the electrochemical performance and long-term air-storage stability. Via a range of advanced analytical techniques, the underlying mechanisms involved on the improved performance are disclosed from interphasial and structural perspectives at the nanoscale. Finally, a comparative study is performed to unveil the stabilities of LiNi [subscript 1-x-y] Mn [subscript x] Co [subscript y] O₂ (NMC) cathodes with different Ni contents at identical degrees of delithiation. The overall stabilities of two representative cathodes, LiNi₀.₈Mn₀.₁Co₀.₁O₂ and LiNiO₂, are evaluated with a rigorous control of an identical 70 mol % delithiation. The results suggest that NMC cathodes with higher-Ni contents may have better overall stability than low-Ni NMC cathodes at a given degree of delithiation, disparate from the prevailing belief that high-Ni cathodes with higher-Ni content have inherently reduced stabilities"],"dc:format.mimetype":["application/pdf"],"dc:identifier.uri":["https://hdl.handle.net/2152/116040","http://dx.doi.org/10.26153/tsw/42936"],"dc:language.iso":["en"],"dc:subject":["High-nickel layered oxide cathodes","Lithium-ion batteries","Electrode-electrolyte interphase","Thermal stability"],"dc:title":["High-nickel layered oxide cathodes for high-performance lithium-ion batteries"],"dc:type":["Thesis"],"thesis:degree_discipline":["Materials Science and Engineering"],"thesis:degree_level":["Doctoral"],"thesis:degree_name":["Doctor of Philosophy"],"thesis:institution_name":["The University of Texas at Austin"]},"updated_at":"2026-07-24T05:01:18Z"}