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Development of Proton-Conducting Electrolytes with Enhanced Performance and Stability for Reversible Solid Oxide Cells
Development of Proton-Conducting Electrolytes with Enhanced Performance and Stability for ...
Development of Proton-Conducting Electrolytes with Enhanced Performance and Stability for Reversible Solid Oxide Cells

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자료유형  
 학위논문 서양
최종처리일시  
20260209102907
ISBN  
9798265406361
DDC  
621
저자명  
Luo, Zheyu.
서명/저자  
Development of Proton-Conducting Electrolytes with Enhanced Performance and Stability for Reversible Solid Oxide Cells
발행사항  
[Sl] : Georgia Institute of Technology, 2023
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2023
형태사항  
205 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-05, Section: B.
주기사항  
Advisor: Liu, Meilin.
학위논문주기  
Thesis (Ph.D.)--Georgia Institute of Technology, 2023.
초록/해제  
요약Reversible solid oxide cells (ReSOCs) that efficiently operate under both fuel cell (fuel to energy) and electrolysis (energy to fuel) modes in a switchable manner are a promising technology for energy storage and conversion. Proton-conducting electrolytes are attracting increasing attention due to their promising conductivity at intermediate temperatures, enabling operation of ReSOCs with high efficiency. However, one of the reasons that they have not been widely adopted is the lack of an electrolyte material that possesses both high ionic conductivity and sufficient stability, especially against high concentrations of steam and carbon dioxide. This objective of this work is to develop novel proton-conducting electrolyte materials for high-performance ReSOCs.To achieve high proton conductivity, acceptor doping with rare earth elements is a commonly used strategy, which is critical to the formation of protonic defects. The results reveal that conductivity, ionic transference number (tion), chemical stability, and compatibility with NiO (a common fuel-electrode material) are all closely correlated with dopant size. In particular, the reactivity with NiO is found to strongly affect the properties of the electrolytes and hence cell performance. Among all compositions studied, an electrolyte with proper acceptor dopant shows excellent chemical stability and minimal reactivity towards NiO, as predicted from density functional theory (DFT)-based calculations and confirmed by experimental results. In addition, proton-conducting reversible solid oxide cells (P-ReSOCs) based on the optimized electrolyte demonstrate excellent stability and exceptional performance.Donor doping is an effective strategy for improving the chemical stability of BaCeO3-based proton conductors. However, donor-doped materials often exhibit very low conductivity. The enhanced proton conductivity of donor-doped barium cerate is demonstrated by compensating the incorporation of donor dopants with excess acceptor doping, highlighting the potential of defect chemistry engineering for enhancing conductivity and durability simultaneously. When compared to the state-of-the-art proton conductors with similar conductivity, the optimized donor-doped electrolyte materials demonstrate a significantly enhanced chemical stability, especially against high concentrations of steam, which is vital to water electrolysis for hydrogen production.Since the donor dopant needs to be electrically compensated by acceptor dopant, the donor doping concentration should be sufficiently small to ensure chemical compatibility between electrolyte and a Ni-based electrode. Accordingly, to further improve the chemical stability of proton conductors for CO2-involved applications, a promising isovalent dopant is identified by DFT-based computational screening. The results indicate that the new class of electrolytes not only show better chemical stability, but also have much improved tion than conventional Zr-doped counterparts, which may allow the use of hydrocarbon fuels and more efficient CO2-H2O co-electrolysis.While the development of new materials is the focus of this thesis, the technical approach is composed of various electrochemical techniques, surface characterization, and computational modeling to understand the rationale behind the difference in properties. It is hoped that the concepts developed in my studies can offer insights into the rational design of novel materials for chemical and energy transformation technologies.
일반주제명  
Fuel cells
일반주제명  
Transmission electron microscopy
일반주제명  
Electrolytes
일반주제명  
Electrodes
일반주제명  
Spectrum analysis
일반주제명  
Energy consumption
일반주제명  
Conductivity
일반주제명  
Scanning electron microscopy
일반주제명  
Carbon dioxide
일반주제명  
Adsorption
일반주제명  
Electron microscopes
일반주제명  
Alternative energy
일반주제명  
Analytical chemistry
일반주제명  
Chemical engineering
일반주제명  
Optics
기타저자  
Georgia Institute of Technology.
기본자료저록  
Dissertations Abstracts International. 87-05B.
전자적 위치 및 접속  
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MARC

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■006m          o    d                
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■020    ▼a9798265406361
■035    ▼a(MiAaPQ)AAI32315755
■035    ▼a(MiAaPQ)GeorgiaTech75087
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a621
■1001  ▼aLuo,  Zheyu.
■24510▼aDevelopment  of  Proton-Conducting  Electrolytes  with  Enhanced  Performance  and  Stability  for  Reversible  Solid  Oxide  Cells
■260    ▼a[Sl]▼bGeorgia  Institute  of  Technology▼c2023
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2023
■300    ▼a205  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-05,  Section:  B.
■500    ▼aAdvisor:  Liu,  Meilin.
■5021  ▼aThesis  (Ph.D.)--Georgia  Institute  of  Technology,  2023.
■520    ▼aReversible  solid  oxide  cells  (ReSOCs)  that  efficiently  operate  under  both  fuel  cell  (fuel  to  energy)  and  electrolysis  (energy  to  fuel)  modes  in  a  switchable  manner  are  a  promising  technology  for  energy  storage  and  conversion.  Proton-conducting  electrolytes  are  attracting  increasing  attention  due  to  their  promising  conductivity  at  intermediate  temperatures,  enabling  operation  of  ReSOCs  with  high  efficiency.  However,  one  of  the  reasons  that  they  have  not  been  widely  adopted  is  the  lack  of  an  electrolyte  material  that  possesses  both  high  ionic  conductivity  and  sufficient  stability,  especially  against  high  concentrations  of  steam  and  carbon  dioxide.  This  objective  of  this  work  is  to  develop  novel  proton-conducting  electrolyte  materials  for  high-performance  ReSOCs.To  achieve  high  proton  conductivity,  acceptor  doping  with  rare  earth  elements  is  a  commonly  used  strategy,  which  is  critical  to  the  formation  of  protonic  defects.  The  results  reveal  that  conductivity,  ionic  transference  number  (tion),  chemical  stability,  and  compatibility  with  NiO  (a  common  fuel-electrode  material)  are  all  closely  correlated  with  dopant  size.  In  particular,  the  reactivity  with  NiO  is  found  to  strongly  affect  the  properties  of  the  electrolytes  and  hence  cell  performance.  Among  all  compositions  studied,  an  electrolyte  with  proper  acceptor  dopant  shows  excellent  chemical  stability  and  minimal  reactivity  towards  NiO,  as  predicted  from  density  functional  theory  (DFT)-based  calculations  and  confirmed  by  experimental  results.  In  addition,  proton-conducting  reversible  solid  oxide  cells  (P-ReSOCs)  based  on  the  optimized  electrolyte  demonstrate  excellent  stability  and  exceptional  performance.Donor  doping  is  an  effective  strategy  for  improving  the  chemical  stability  of  BaCeO3-based  proton  conductors.  However,  donor-doped  materials  often  exhibit  very  low  conductivity.  The  enhanced  proton  conductivity  of  donor-doped  barium  cerate  is  demonstrated  by  compensating  the  incorporation  of  donor  dopants  with  excess  acceptor  doping,  highlighting  the  potential  of  defect  chemistry  engineering  for  enhancing  conductivity  and  durability  simultaneously.  When  compared  to  the  state-of-the-art  proton  conductors  with  similar  conductivity,  the  optimized  donor-doped  electrolyte  materials  demonstrate  a  significantly  enhanced  chemical  stability,  especially  against  high  concentrations  of  steam,  which  is  vital  to  water  electrolysis  for  hydrogen  production.Since  the  donor  dopant  needs  to  be  electrically  compensated  by  acceptor  dopant,  the  donor  doping  concentration  should  be  sufficiently  small  to  ensure  chemical  compatibility  between  electrolyte  and  a  Ni-based  electrode.  Accordingly,  to  further  improve  the  chemical  stability  of  proton  conductors  for  CO2-involved  applications,  a  promising  isovalent  dopant  is  identified  by  DFT-based  computational  screening.  The  results  indicate  that  the  new  class  of  electrolytes  not  only  show  better  chemical  stability,  but  also  have  much  improved  tion  than  conventional  Zr-doped  counterparts,  which  may  allow  the  use  of  hydrocarbon  fuels  and  more  efficient  CO2-H2O  co-electrolysis.While  the  development  of  new  materials  is  the  focus  of  this  thesis,  the  technical  approach  is  composed  of  various  electrochemical  techniques,  surface  characterization,  and  computational  modeling  to  understand  the  rationale  behind  the  difference  in  properties.  It  is  hoped  that  the  concepts  developed  in  my  studies  can  offer  insights  into  the  rational  design  of  novel  materials  for  chemical  and  energy  transformation  technologies.
■590    ▼aSchool  code:  0078.
■650  4▼aFuel  cells
■650  4▼aTransmission  electron  microscopy
■650  4▼aElectrolytes
■650  4▼aElectrodes
■650  4▼aSpectrum  analysis
■650  4▼aEnergy  consumption
■650  4▼aConductivity
■650  4▼aScanning  electron  microscopy
■650  4▼aCarbon  dioxide
■650  4▼aAdsorption
■650  4▼aElectron  microscopes
■650  4▼aAlternative  energy
■650  4▼aAnalytical  chemistry
■650  4▼aChemical  engineering
■650  4▼aOptics
■690    ▼a0363
■690    ▼a0486
■690    ▼a0542
■690    ▼a0752
■71020▼aGeorgia  Institute  of  Technology.
■7730  ▼tDissertations  Abstracts  International▼g87-05B.
■790    ▼a0078
■791    ▼aPh.D.
■792    ▼a2023
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17365981▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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