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Enabling Low-Cost Cathodes in All-Solid-State Batteries
Enabling Low-Cost Cathodes in All-Solid-State Batteries
Enabling Low-Cost Cathodes in All-Solid-State Batteries

Detailed Information

자료유형  
 학위논문 서양
최종처리일시  
20250211152807
ISBN  
9798384493471
DDC  
621
저자명  
Cronk, Ashley.
서명/저자  
Enabling Low-Cost Cathodes in All-Solid-State Batteries
발행사항  
[Sl] : University of California, San Diego, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
97 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
주기사항  
Advisor: Meng, Y. Shirley;Kim, H. Alicia.
학위논문주기  
Thesis (Ph.D.)--University of California, San Diego, 2024.
초록/해제  
요약All-solid-state batteries (ASSBs) are one of the most promising systems to enable thermally resilient and high energy dense next-generation energy storage. While lithium-ion batteries (LIB) using layered oxide cathodes have made significant advancements, these cathodes are reaching their limits in terms of cost, capacity, and performance. This necessitates the development of cathode alternatives that are safer, high energy dense, and with lower cost, by reducing reliance on critical materials like cobalt and nickel. Pursuing cobalt- and nickel-free chemistries, like LiFePO4 (LFP) and lithium-sulfur (Li-S) in ASSB architecture is a promising approach to solve some of the current limitations of LIBs. Replacing liquid electrolytes with non-flammable solid-state electrolytes (SSE) can improve both safety and energy density. While SSEs offer many advantages, they often introduce interfacial challenges from resistive solid-solid contact, which can inhibit lithium transport necessary for practical operation. This poses new challenges for LFP and Li-S cathodes, requiring new design strategies due to their unique morphological and material properties.The morphological features of LFP essential for improved electrochemical performance, are highlighted to elucidate the interfacial challenges when implemented in sulfide based ASSBs. For the first study, the compatibility of LFP with two types of solid-state electrolytes, Li6PS5Cl (LPSCl) and Li2ZrCl6 (LZC), are investigated. Irreversible redox products and interfacial degradation from LPSCl were found to be responsible for unstable performance. This work reveals the intrinsic incompatibility of LFP against sulfide-based SSEs. However, employing the chloride-based electrolyte, LZC, high-rate and stable cycling performance for over a thousand cycles is achieved at room temperature. Although LPSCl was found to be incompatible with LFP, it was found to facilitate beneficial properties when paired with Li-S cathodes. Li-S cathodes can realize some of the highest known energy densities. But similar to LFP, its development in ASSBs has been plagued by interfacial and (chemo)mechanical degradation. In the second study, a scalable synthesis method is introduced to overcome the challenges well known for solid-state Li-S batteries. Facilitating interfacial reactions between sulfur and LPSCl, optimizing the cathode/catholyte microstructure, and tuning the redox behavior of LPSCl was found to improve utilization and stability. As a result, this approach enables high loading sulfur cathodes up to 11 mAh cm-2 with stable operation at room temperature. Several high energy density cell architectures are also proposed and demonstrated. These studies establish new design principles for both LFP and Li-S cathodes in ASSBs, potentially transforming the energy storage landscape by enabling safe, low-cost, and high energy dense storage solutions for a wide range of future applications.
일반주제명  
Energy
일반주제명  
Engineering
일반주제명  
Electrical engineering
키워드  
All-solid-state batteries
키워드  
High energy density
키워드  
Lithium iron phosphate
키워드  
Lithium sulfur
키워드  
Low-cost cathodes
키워드  
Solid-state electrolytes
기타저자  
University of California, San Diego Materials Science and Engineering
기본자료저록  
Dissertations Abstracts International. 86-04B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aCronk,  Ashley.
■24510▼aEnabling  Low-Cost  Cathodes  in  All-Solid-State  Batteries
■260    ▼a[Sl]▼bUniversity  of  California,  San  Diego▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a97  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-04,  Section:  B.
■500    ▼aAdvisor:  Meng,  Y.  Shirley;Kim,  H.  Alicia.
■5021  ▼aThesis  (Ph.D.)--University  of  California,  San  Diego,  2024.
■520    ▼aAll-solid-state  batteries  (ASSBs)  are  one  of  the  most  promising  systems  to  enable  thermally  resilient  and  high  energy  dense  next-generation  energy  storage.  While  lithium-ion  batteries  (LIB)  using  layered  oxide  cathodes  have  made  significant  advancements,  these  cathodes  are  reaching  their  limits  in  terms  of  cost,  capacity,  and  performance.  This  necessitates  the  development  of  cathode  alternatives  that  are  safer,  high  energy  dense,  and  with  lower  cost,  by  reducing  reliance  on  critical  materials  like  cobalt  and  nickel.  Pursuing  cobalt-  and  nickel-free  chemistries,  like  LiFePO4  (LFP)  and  lithium-sulfur  (Li-S)  in  ASSB  architecture  is  a  promising  approach  to  solve  some  of  the  current  limitations  of  LIBs.  Replacing  liquid  electrolytes  with  non-flammable  solid-state  electrolytes  (SSE)  can  improve  both  safety  and  energy  density.  While  SSEs  offer  many  advantages,  they  often  introduce  interfacial  challenges  from  resistive  solid-solid  contact,  which  can  inhibit  lithium  transport  necessary  for  practical  operation.  This  poses  new  challenges  for  LFP  and  Li-S  cathodes,  requiring  new  design  strategies  due  to  their  unique  morphological  and  material  properties.The  morphological  features  of  LFP  essential  for  improved  electrochemical  performance,  are  highlighted  to  elucidate  the  interfacial  challenges  when  implemented  in  sulfide  based  ASSBs.  For  the  first  study,  the  compatibility  of  LFP  with  two  types  of  solid-state  electrolytes,  Li6PS5Cl  (LPSCl)  and  Li2ZrCl6  (LZC),  are  investigated.  Irreversible  redox  products  and  interfacial  degradation  from  LPSCl  were  found  to  be  responsible  for  unstable  performance.  This  work  reveals  the  intrinsic  incompatibility  of  LFP  against  sulfide-based  SSEs.  However,  employing  the  chloride-based  electrolyte,  LZC,  high-rate  and  stable  cycling  performance  for  over  a  thousand  cycles  is  achieved  at  room  temperature.  Although  LPSCl  was  found  to  be  incompatible  with  LFP,  it  was  found  to  facilitate  beneficial  properties  when  paired  with  Li-S  cathodes.  Li-S  cathodes  can  realize  some  of  the  highest  known  energy  densities.  But  similar  to  LFP,  its  development  in  ASSBs  has  been  plagued  by  interfacial  and  (chemo)mechanical  degradation.  In  the  second  study,  a  scalable  synthesis  method  is  introduced  to  overcome  the  challenges  well  known  for  solid-state  Li-S  batteries.  Facilitating  interfacial  reactions  between  sulfur  and  LPSCl,  optimizing  the  cathode/catholyte  microstructure,  and  tuning  the  redox  behavior  of  LPSCl  was  found  to  improve  utilization  and  stability.  As  a  result,  this  approach  enables  high  loading  sulfur  cathodes  up  to  11  mAh  cm-2  with  stable  operation  at  room  temperature.  Several  high  energy  density  cell  architectures  are  also  proposed  and  demonstrated.  These  studies  establish  new  design  principles  for  both  LFP and  Li-S  cathodes  in  ASSBs,  potentially  transforming  the  energy  storage  landscape  by  enabling  safe,  low-cost,  and  high  energy  dense  storage  solutions  for  a  wide  range  of  future  applications.
■590    ▼aSchool  code:  0033.
■650  4▼aEnergy
■650  4▼aEngineering
■650  4▼aElectrical  engineering
■653    ▼aAll-solid-state  batteries
■653    ▼aHigh  energy  density
■653    ▼aLithium  iron  phosphate
■653    ▼aLithium  sulfur
■653    ▼aLow-cost  cathodes
■653    ▼aSolid-state  electrolytes
■690    ▼a0791
■690    ▼a0537
■690    ▼a0544
■71020▼aUniversity  of  California,  San  Diego▼bMaterials  Science  and  Engineering.
■7730  ▼tDissertations  Abstracts  International▼g86-04B.
■790    ▼a0033
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163899▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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