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Putting the Reversibility of Lithium Batteries Under the Microscope: Dissolved Cathode Species, Water Impurities, and Artificial Protection Layers
Putting the Reversibility of Lithium Batteries Under the Microscope: Dissolved Cathode Spe...
Putting the Reversibility of Lithium Batteries Under the Microscope: Dissolved Cathode Species, Water Impurities, and Artificial Protection Layers

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자료유형  
 학위논문 서양
최종처리일시  
20250211151405
ISBN  
9798382230498
DDC  
541
저자명  
Vila, Rafael.
서명/저자  
Putting the Reversibility of Lithium Batteries Under the Microscope: Dissolved Cathode Species, Water Impurities, and Artificial Protection Layers
발행사항  
[Sl] : Stanford University, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
166 p
주기사항  
Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
주기사항  
Advisor: Cui, Yi.
학위논문주기  
Thesis (Ph.D.)--Stanford University, 2024.
초록/해제  
요약This thesis presents a comprehensive examination of the critical components influencing the performance and longevity of lithium batteries, with a particular focus on the solid-electrolyte interphase (SEI) and its integral role in battery stability and functionality. Through a series of meticulous studies, the thesis leverages advanced characterization and analytical techniques to unravel the complex mechanisms at play within battery anodes and proposes innovative strategies to mitigate performance degradation. In Chapter 1, the thesis begins with a comprehensive introduction to rechargeable lithium battery technology, tracing its evolution from the foundational work of Goodenough, Yoshino, and Whittingham to the latest developments in advanced battery research. This historical perspective encompasses significant innovations like lithium metal, silicon anodes, and sulfur cathodes, illustrating the continuous pursuit of higher energy density, enhanced safety, and cost-effectiveness. The chapter not only introduces fundamental concepts, particularly emphasizing the pivotal role of lithium metal anodes, but also delves into the unique failure mechanisms inherent to different battery chemistries. Highlighting the advanced characterization and analytical tools play in identifying and understanding failure mechanisms of battery materials. This sets the stage for the subsequent in-depth investigations and establishes a framework for understanding the current state, challenges, and future prospects of lithium battery technology, underlining its significance in the broader context of electrification and sustainability efforts. Chapter 2 delves into the detrimental effects of dissolved transition metals, particularly nickel, from high-voltage cathodes on the performance and lifespan of lithium metal anodes. Through the use of cryogenic electron microscopy, the study unveils the intricate process of nickel incorporation into the SEI and its profound impact on the SEI's chemistry and nanostructure. This incorporation is shown to alter the transport properties of lithium ions and electrons within the SEI, expediting electrolyte decomposition, fostering the formation of "dead" lithium, and ultimately triggering battery failure. Chapter 3 shifts the focus to the formation of lithium hydride (LiH) within lithium batteries and its implications on battery efficiency and safety. The chapter presents groundbreaking findings on the formation mechanism of LiH, demonstrating that hydrogen gas, a byproduct of cycling in Li batteries, reacts with deposited lithium metal to form LiH, thus consuming active lithium and diminishing battery capacity. The discovery demonstrates that LiH, a wide-bandgap insulator, electrically isolates metallic lithium from the current collector adds a new dimension to understanding battery degradation. Furthermore, the identification of LiH on various anode chemistries, each with its distinct SEI layer, underscores the significance of this degradation pathway across different lithium battery systems. In Chapter 4, the thesis explores the potential of interfacial coatings, specifically nanometer-scale aluminum oxide (Al2O3) coatings on carbon negative electrodes, to enhance lithium-ion battery performance. The research delineates the transformative changes in the SEI's structure and chemistry induced by Al2O3 coatings during SEI formation at low potentials. The findings illuminate the critical role of the refined SEI structure, chemistry, and uniformity in elevating battery performance, challenging the prevailing notion that performance enhancements are solely attributable to the physical presence of the coatings. Finally, Chapter 5 combines the insights from the preceding chapters, offering a comprehensive summary of the thesis and projecting an outlook for the field. It emphasizes the importance of the interplay between electrolyte composition, SEI structure, and electrode material in determining the performance and durability of lithium batteries. The chapter proposes directions for future research, focusing on understanding failure mechanisms in extreme conditions and emerging battery chemistries. Overall, this thesis contributes significantly to the field of battery technology by providing a deeper understanding of the intricate interactions within lithium battery anodes and paving the way for the development of more robust, efficient, and safer battery systems.
일반주제명  
Physical chemistry
일반주제명  
Electrical engineering
키워드  
Solid-electrolyte interphase
키워드  
Lithium battery technology
키워드  
Lithium hydride
기타저자  
Stanford University.
기본자료저록  
Dissertations Abstracts International. 85-11B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aVila,  Rafael.
■24510▼aPutting  the  Reversibility  of  Lithium  Batteries  Under  the  Microscope:  Dissolved  Cathode  Species,  Water  Impurities,  and  Artificial  Protection  Layers
■260    ▼a[Sl]▼bStanford  University▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a166  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  85-11,  Section:  B.
■500    ▼aAdvisor:  Cui,  Yi.
■5021  ▼aThesis  (Ph.D.)--Stanford  University,  2024.
■520    ▼aThis  thesis  presents  a  comprehensive  examination  of  the  critical  components  influencing  the  performance  and  longevity  of  lithium  batteries,  with  a  particular  focus  on  the  solid-electrolyte  interphase  (SEI)  and  its  integral  role  in  battery  stability  and  functionality.  Through  a  series  of  meticulous  studies,  the  thesis  leverages  advanced  characterization  and  analytical  techniques  to  unravel  the  complex  mechanisms  at  play  within  battery  anodes  and  proposes  innovative  strategies  to  mitigate  performance  degradation.  In  Chapter  1,  the  thesis  begins  with  a  comprehensive  introduction  to  rechargeable  lithium  battery  technology,  tracing  its  evolution  from  the  foundational  work  of  Goodenough,  Yoshino,  and  Whittingham  to  the  latest  developments  in  advanced  battery  research.  This  historical  perspective  encompasses  significant  innovations  like  lithium  metal,  silicon  anodes,  and  sulfur  cathodes,  illustrating  the  continuous  pursuit  of  higher  energy  density,  enhanced  safety,  and  cost-effectiveness.  The  chapter  not  only  introduces  fundamental  concepts,  particularly  emphasizing  the  pivotal  role  of  lithium  metal  anodes,  but  also  delves  into  the  unique  failure  mechanisms  inherent  to  different  battery  chemistries.  Highlighting  the  advanced  characterization  and  analytical  tools  play  in  identifying  and  understanding  failure  mechanisms  of  battery  materials.  This  sets  the  stage  for  the  subsequent  in-depth  investigations  and  establishes  a  framework  for  understanding  the  current  state,  challenges,  and  future  prospects  of  lithium  battery  technology,  underlining  its  significance  in  the  broader  context  of  electrification  and  sustainability  efforts.  Chapter  2  delves  into  the  detrimental  effects  of  dissolved  transition  metals,  particularly  nickel,  from  high-voltage  cathodes  on  the  performance  and  lifespan  of  lithium  metal  anodes.  Through  the  use  of  cryogenic  electron  microscopy,  the  study  unveils  the  intricate  process  of  nickel  incorporation  into  the  SEI  and  its  profound  impact  on  the  SEI's  chemistry  and  nanostructure.  This  incorporation  is  shown  to  alter  the  transport  properties  of  lithium  ions  and  electrons  within  the  SEI,  expediting  electrolyte  decomposition,  fostering  the  formation  of  "dead"  lithium,  and  ultimately  triggering  battery  failure.  Chapter  3  shifts  the  focus  to  the  formation  of  lithium  hydride  (LiH)  within  lithium  batteries  and  its  implications  on  battery  efficiency  and  safety.  The  chapter  presents  groundbreaking  findings  on  the  formation  mechanism  of  LiH,  demonstrating  that  hydrogen  gas,  a  byproduct  of  cycling  in  Li  batteries,  reacts  with  deposited  lithium  metal  to  form  LiH,  thus  consuming  active  lithium  and  diminishing  battery  capacity.  The  discovery  demonstrates  that  LiH,  a  wide-bandgap  insulator,  electrically  isolates  metallic  lithium  from  the  current  collector  adds  a  new  dimension  to  understanding  battery  degradation.  Furthermore,  the  identification  of  LiH  on  various  anode  chemistries,  each  with  its  distinct  SEI  layer,  underscores  the  significance  of  this  degradation  pathway  across  different  lithium  battery  systems.  In  Chapter  4,  the  thesis  explores  the  potential  of  interfacial  coatings,  specifically  nanometer-scale  aluminum  oxide  (Al2O3)  coatings  on  carbon  negative  electrodes,  to  enhance  lithium-ion  battery  performance.  The  research  delineates  the  transformative  changes  in  the  SEI's  structure  and  chemistry  induced  by  Al2O3  coatings  during  SEI  formation  at  low  potentials.  The  findings  illuminate  the  critical  role  of  the  refined  SEI  structure,  chemistry,  and  uniformity  in  elevating  battery  performance,  challenging  the  prevailing  notion  that  performance  enhancements  are  solely  attributable  to  the  physical  presence  of  the  coatings.  Finally,  Chapter  5  combines  the  insights  from  the  preceding  chapters,  offering  a  comprehensive  summary  of  the  thesis  and  projecting  an  outlook  for  the  field.  It  emphasizes  the  importance  of  the  interplay  between  electrolyte  composition,  SEI  structure,  and  electrode  material  in  determining  the  performance  and  durability  of  lithium  batteries.  The  chapter  proposes  directions  for  future  research,  focusing  on  understanding  failure  mechanisms  in  extreme  conditions  and  emerging  battery  chemistries.  Overall,  this  thesis  contributes  significantly  to  the  field  of  battery  technology  by  providing  a  deeper  understanding  of  the  intricate  interactions  within  lithium  battery  anodes  and  paving  the  way  for  the  development  of  more  robust,  efficient,  and  safer  battery  systems.
■590    ▼aSchool  code:  0212.
■650  4▼aPhysical  chemistry
■650  4▼aElectrical  engineering
■653    ▼aSolid-electrolyte  interphase
■653    ▼aLithium  battery  technology
■653    ▼aLithium  hydride
■690    ▼a0544
■690    ▼a0494
■71020▼aStanford  University.
■7730  ▼tDissertations  Abstracts  International▼g85-11B.
■790    ▼a0212
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17161506▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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