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Ion (De)Solvation, Charge-Transfer, and the Temperature-Dependent Behavior of Li Metal Batteries- [electronic resource]
Ion (De)Solvation, Charge-Transfer, and the Temperature-Dependent Behavior of Li Metal Batteries- [electronic resource]
상세정보
- 자료유형
- 학위논문파일 국외
- 최종처리일시
- 20240214100114
- ISBN
- 9798380382984
- DDC
- 621
- 저자명
- Holoubek, John.
- 서명/저자
- Ion (De)Solvation, Charge-Transfer, and the Temperature-Dependent Behavior of Li Metal Batteries - [electronic resource]
- 발행사항
- [S.l.]: : University of California, San Diego., 2023
- 발행사항
- Ann Arbor : : ProQuest Dissertations & Theses,, 2023
- 형태사항
- 1 online resource(148 p.)
- 주기사항
- Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
- 주기사항
- Advisor: Liu, Ping;Chen, Zheng.
- 학위논문주기
- Thesis (Ph.D.)--University of California, San Diego, 2023.
- 사용제한주기
- This item must not be sold to any third party vendors.
- 초록/해제
- 요약Improving the performance of secondary batteries is crucial to the ubiquity of renewable energy technologies such as electric transport, grid storage, and the operation of advanced portable electronics. To improve the energy density of these systems, significant effort has been made to replace the graphite anode found in conventional Li-ion batteries with lithium metal. Additionally, the electrochemical kinetics of commercial batteries are currently insufficient to provide charging times comparable to standard refueling periods, and to deliver power at reduced operating temperatures. Unfortunately, applying Li metal cells under such conditions compounds these issues due to an increased risk of cell shorting due to dendritic growth and reduced cyclability of Li metal itself. To achieve such operation conditions in high-energy Li metal batteries, the kinetics barriers associated with diffusion of Li+ within the bulk of the electrode materials, migration of Li+ through the solid-electrolyte-interphase (SEI), diffusion of Li+ through the electrolyte bulk, and charge-transfer at the electrode interphase must be enhanced. Though there are well-established strategies developed to optimize the first three of these processes, understanding and designing the charge transfer process remains as a frontier.The following dissertation describes our work to understand the impact of and design the Li+ solvation structure on charge-transfer kinetics and temperature-dependent Li metal anode behavior at reduced temperature. First, we find that Li metal batteries applying conventional electrolytes ultra-low temperatures ( -30 oC) undergo catastrophic shorting events due to charge transfer limitations, which is significantly mitigated in weakly-solvated electrolytes. Second, we develop next-generation computational techniques to probe this behavior at the interface, which reveals that anion coordination of the Li+ ion hastens the desolvation process relative to conventional solvent-dominated structures. Lastly, we employ these insights to demonstrate that the charge-transfer kinetics and low-temperature Li metal performance of cells employing conventional solvents can be significantly improved through the induction of said ion-pairing. This work improves the operating versatility of high-energy Li metal batteries while advancing our understanding of the structure-defined desolvation process crucial to charge-transfer at the electrochemical interface.
- 일반주제명
- Energy.
- 일반주제명
- Chemistry.
- 일반주제명
- Chemical engineering.
- 키워드
- Battery
- 키워드
- Electrolyte
- 키워드
- Solvation
- 기타저자
- University of California, San Diego NanoEngineering
- 기본자료저록
- Dissertations Abstracts International. 85-03B.
- 기본자료저록
- Dissertation Abstract International
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520240214100114
■006m o d
■007cr#unu||||||||
■020 ▼a9798380382984
■035 ▼a(MiAaPQ)AAI30422392
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a621
■1001 ▼aHoloubek, John.
■24510▼aIon (De)Solvation, Charge-Transfer, and the Temperature-Dependent Behavior of Li Metal Batteries▼h[electronic resource]
■260 ▼a[S.l.]:▼bUniversity of California, San Diego. ▼c2023
■260 1▼aAnn Arbor :▼bProQuest Dissertations & Theses, ▼c2023
■300 ▼a1 online resource(148 p.)
■500 ▼aSource: Dissertations Abstracts International, Volume: 85-03, Section: B.
■500 ▼aAdvisor: Liu, Ping;Chen, Zheng.
■5021 ▼aThesis (Ph.D.)--University of California, San Diego, 2023.
■506 ▼aThis item must not be sold to any third party vendors.
■520 ▼aImproving the performance of secondary batteries is crucial to the ubiquity of renewable energy technologies such as electric transport, grid storage, and the operation of advanced portable electronics. To improve the energy density of these systems, significant effort has been made to replace the graphite anode found in conventional Li-ion batteries with lithium metal. Additionally, the electrochemical kinetics of commercial batteries are currently insufficient to provide charging times comparable to standard refueling periods, and to deliver power at reduced operating temperatures. Unfortunately, applying Li metal cells under such conditions compounds these issues due to an increased risk of cell shorting due to dendritic growth and reduced cyclability of Li metal itself. To achieve such operation conditions in high-energy Li metal batteries, the kinetics barriers associated with diffusion of Li+ within the bulk of the electrode materials, migration of Li+ through the solid-electrolyte-interphase (SEI), diffusion of Li+ through the electrolyte bulk, and charge-transfer at the electrode interphase must be enhanced. Though there are well-established strategies developed to optimize the first three of these processes, understanding and designing the charge transfer process remains as a frontier.The following dissertation describes our work to understand the impact of and design the Li+ solvation structure on charge-transfer kinetics and temperature-dependent Li metal anode behavior at reduced temperature. First, we find that Li metal batteries applying conventional electrolytes ultra-low temperatures ( -30 oC) undergo catastrophic shorting events due to charge transfer limitations, which is significantly mitigated in weakly-solvated electrolytes. Second, we develop next-generation computational techniques to probe this behavior at the interface, which reveals that anion coordination of the Li+ ion hastens the desolvation process relative to conventional solvent-dominated structures. Lastly, we employ these insights to demonstrate that the charge-transfer kinetics and low-temperature Li metal performance of cells employing conventional solvents can be significantly improved through the induction of said ion-pairing. This work improves the operating versatility of high-energy Li metal batteries while advancing our understanding of the structure-defined desolvation process crucial to charge-transfer at the electrochemical interface.
■590 ▼aSchool code: 0033.
■650 4▼aEnergy.
■650 4▼aChemistry.
■650 4▼aChemical engineering.
■653 ▼aBattery
■653 ▼aElectrolyte
■653 ▼aSolvation
■653 ▼aElectrochemical interface
■653 ▼aCatastrophic shorting
■690 ▼a0791
■690 ▼a0485
■690 ▼a0542
■71020▼aUniversity of California, San Diego▼bNanoEngineering.
■7730 ▼tDissertations Abstracts International▼g85-03B.
■773 ▼tDissertation Abstract International
■790 ▼a0033
■791 ▼aPh.D.
■792 ▼a2023
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T16931763▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
■980 ▼a202402▼f2024
