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Spectroscopic and Electrochemical Characterization of Energy Capture and Storage Materials
Spectroscopic and Electrochemical Characterization of Energy Capture and Storage Materials
Spectroscopic and Electrochemical Characterization of Energy Capture and Storage Materials

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자료유형  
 학위논문 서양
최종처리일시  
20260202103115
ISBN  
9798315712718
DDC  
540
저자명  
Dones Lassalle, Christian Y.
서명/저자  
Spectroscopic and Electrochemical Characterization of Energy Capture and Storage Materials
발행사항  
[Sl] : The University of North Carolina at Chapel Hill, 2025
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2025
형태사항  
252 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-11, Section: B.
주기사항  
Advisor: Dempsey, Jillian L.
학위논문주기  
Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2025.
초록/해제  
요약Quantum confined semiconductor nanocrystals (NCs), such as quantum dots and nanoplatelets, are promising materials for energy capture technologies because of their size-dependent optoelectronic properties that arise from confinement of charge carriers at sizes below the material's exciton Bohr radius. Because of their high surface-to-volume ratios, the NC surface plays a key role in their performance for numerous applications. Surface defects such as undercoordinated surface ions trap charge carriers, hindering NC optoelectronic properties. Although surface modification has been demonstrated to counteract surface defects, the limited understanding of ligand exchange mechanisms and lack of a molecular-level understanding of the NC surface obstructs the optimal performance of NCs.To tackle this conundrum, the work presented in this dissertation outlines efforts to elucidate reactivity at NC surfaces. Two projects focused on enhancing molecular-level understanding of the NC surface are discussed. First, the surface reactivity of oleate-capped PbS NCs with primary amines as non-native L-type ligands is assessed. This work resolves the mechanisms through which primary amines bind to the NC surface and displace native Z-type ligands and identifies the robust electronic structure of PbS NCs that persists through significant surface changes. Ligand binding motifs and thermochemistry at the NC surface are subsequently probed by quantifying the self-exchange of oleic acid ligands in PbS NCs. In a parallel project, electrochemical modulation of the energetics of hybridized states arising from nanoplatelets coupled with light in an optical cavity are investigated, highlighting the versatility of NCs for diverse applications.Coupled with energy capture technologies, redox-flow batteries (RFBs) are a promising alternative for storing large amounts of energy through electrolyte reservoirs. In a final project, the electrochemical properties of quinone and quinone derivatives are investigated as potential RFB electrolytes extracted from naturally occurring fungi. Their electrochemical and chemical reversibility were identified under neutral and buffered conditions, gauging the impact of different conditions in the stability of potential RFB electrolytes. The work described herein serves as a collection of characterization methods to develop design principles for improved energy capture and storage materials, paving the way to combine different systems for a sustainable energy economy.
일반주제명  
Chemistry
일반주제명  
Inorganic chemistry
일반주제명  
Materials science
키워드  
Electrochemistry
키워드  
Exciton-polaritons
키워드  
Nanocrystals
키워드  
Redox flow battery electrolytes
키워드  
Semiconductors
키워드  
Spectroscopy
기타저자  
The University of North Carolina at Chapel Hill Chemistry
기본자료저록  
Dissertations Abstracts International. 86-11B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aDones  Lassalle,  Christian  Y.
■24510▼aSpectroscopic  and  Electrochemical  Characterization  of  Energy  Capture  and  Storage  Materials
■260    ▼a[Sl]▼bThe  University  of  North  Carolina  at  Chapel  Hill▼c2025
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2025
■300    ▼a252  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-11,  Section:  B.
■500    ▼aAdvisor:  Dempsey,  Jillian  L.
■5021  ▼aThesis  (Ph.D.)--The  University  of  North  Carolina  at  Chapel  Hill,  2025.
■520    ▼aQuantum  confined  semiconductor  nanocrystals  (NCs),  such  as  quantum  dots  and  nanoplatelets,  are  promising  materials  for  energy  capture  technologies  because  of  their  size-dependent  optoelectronic  properties  that  arise  from  confinement  of  charge  carriers  at  sizes  below  the  material's  exciton  Bohr  radius.  Because  of  their  high  surface-to-volume  ratios,  the  NC  surface  plays  a  key  role  in  their  performance  for  numerous  applications.  Surface  defects  such  as  undercoordinated  surface  ions  trap  charge  carriers,  hindering  NC  optoelectronic  properties.  Although  surface  modification  has  been  demonstrated  to  counteract  surface  defects,  the  limited  understanding  of  ligand  exchange  mechanisms  and  lack  of  a  molecular-level  understanding  of  the  NC  surface  obstructs  the  optimal  performance  of  NCs.To  tackle  this  conundrum,  the  work  presented  in  this  dissertation  outlines  efforts  to  elucidate  reactivity  at  NC  surfaces.  Two  projects  focused  on  enhancing  molecular-level  understanding  of  the  NC  surface  are  discussed.  First,  the  surface  reactivity  of  oleate-capped  PbS  NCs  with  primary  amines  as  non-native  L-type  ligands  is  assessed.  This  work  resolves  the  mechanisms  through  which  primary  amines  bind  to  the  NC  surface  and  displace  native  Z-type  ligands  and  identifies  the  robust  electronic  structure  of  PbS  NCs  that  persists  through  significant  surface  changes.  Ligand  binding  motifs  and  thermochemistry  at  the  NC  surface  are  subsequently  probed  by  quantifying  the  self-exchange  of  oleic  acid  ligands  in  PbS  NCs.  In  a  parallel  project,  electrochemical  modulation  of  the  energetics  of  hybridized  states  arising  from  nanoplatelets  coupled  with  light  in  an  optical  cavity  are  investigated,  highlighting  the  versatility  of  NCs  for  diverse  applications.Coupled  with  energy  capture  technologies,  redox-flow  batteries  (RFBs)  are  a  promising  alternative  for  storing  large  amounts  of  energy  through  electrolyte  reservoirs.  In  a  final  project,  the  electrochemical  properties  of  quinone  and  quinone  derivatives  are  investigated  as  potential  RFB  electrolytes  extracted  from  naturally  occurring  fungi.  Their  electrochemical  and  chemical  reversibility  were  identified  under  neutral  and  buffered  conditions,  gauging  the  impact  of  different  conditions  in  the  stability  of  potential  RFB  electrolytes.  The  work  described  herein  serves  as  a  collection  of  characterization  methods  to  develop  design  principles  for  improved  energy  capture  and  storage  materials,  paving  the  way  to  combine  different  systems  for  a  sustainable  energy  economy.
■590    ▼aSchool  code:  0153.
■650  4▼aChemistry
■650  4▼aInorganic  chemistry
■650  4▼aMaterials  science
■653    ▼aElectrochemistry
■653    ▼aExciton-polaritons
■653    ▼aNanocrystals
■653    ▼aRedox  flow  battery  electrolytes
■653    ▼aSemiconductors
■653    ▼aSpectroscopy
■690    ▼a0485
■690    ▼a0488
■690    ▼a0794
■71020▼aThe  University  of  North  Carolina  at  Chapel  Hill▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g86-11B.
■790    ▼a0153
■791    ▼aPh.D.
■792    ▼a2025
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17357008▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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