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Synthesis of Porous Materials and Applications Toward Electrochemical CO2 Reduction
Synthesis of Porous Materials and Applications Toward Electrochemical CO2 Reduction
Synthesis of Porous Materials and Applications Toward Electrochemical CO2 Reduction

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자료유형  
 학위논문 서양
최종처리일시  
20260202104801
ISBN  
9798297600973
DDC  
540
저자명  
Dulovic, Stephanie.
서명/저자  
Synthesis of Porous Materials and Applications Toward Electrochemical CO2 Reduction
발행사항  
[Sl] : Princeton University, 2025
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2025
형태사항  
205 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-04, Section: B.
주기사항  
Advisor: Bocarsly, Andrew.
학위논문주기  
Thesis (Ph.D.)--Princeton University, 2025.
초록/해제  
요약The current global energy landscape is at a critical crossroads defined by an urgent need to transition from environmentally detrimental fossil fuel resources. An attractive alternative is to engineer a closed carbon cycle through the conversion of carbon dioxide into energy-dense fuels. Electrochemical reduction of aqueous CO2 can offer a sustainable approach to achieve these transformation reactions; however, the practical implementation of electrocatalysts is challenged by low efficiency and poor selectivity in product generation. Overcoming these obstacles requires strategic considerations in the structural and functional design of materials. One such focus has centered around porous materials that can enhance the efficiency of C-C bond generation through modification of the local electrochemical environment via confinement effects.This work further explores the synthesis and electrochemical applications of porous materials. Chapter 2 of this dissertation introduces a chromium-gallium oxide mixture that, when in the presence of trace metal, can achieve unprecedented efficiency in the generation of multi-carbon products from CO2. This includes four-carbon products that possess energy densities comparable to conventional fuels. It is concluded that the observed reactivity is enabled by the intrinsic porosity of the metal oxide mixture, which can increase the local concentration of CO2 at the electrode interface and thereby enhance proton/electron transfer rates. Chapter 3 continues the development of this metal oxide system with the adoption of a hard-template technique providing strict synthetic control of the porous morphology. It is found that through the variation of pore diameter, selectivity of CO2-derived products can be altered. Structural characterization of the synthesized metal oxide interfaces is complimented with electroanalytical experiments to evaluate changes in the local electrochemical environment and the relationship to reactivity. Finally, Chapter 4 outlines the synthesis of cyanide coordination polymers from octacyanometallates toward an assortment of materials that include metal carbides, alloys, oxides and phosphides. Similar to a template based syn- thesis, these materials retain their unique morphology, which includes catalytically relevant porous structures.
일반주제명  
Chemistry
일반주제명  
Materials science
일반주제명  
Physical chemistry
키워드  
CO2 reduction
키워드  
Electrocatalysis
키워드  
Porous materials
기타저자  
Princeton University Chemistry
기본자료저록  
Dissertations Abstracts International. 87-04B.
전자적 위치 및 접속  
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■020    ▼a9798297600973
■035    ▼a(MiAaPQ)AAI32164500
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a540
■1001  ▼aDulovic,  Stephanie.▼0(orcid)0000-0003-0921-9714
■24510▼aSynthesis  of  Porous  Materials  and  Applications  Toward  Electrochemical  CO2  Reduction
■260    ▼a[Sl]▼bPrinceton  University▼c2025
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2025
■300    ▼a205  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-04,  Section:  B.
■500    ▼aAdvisor:  Bocarsly,  Andrew.
■5021  ▼aThesis  (Ph.D.)--Princeton  University,  2025.
■520    ▼aThe  current  global  energy  landscape  is  at  a  critical  crossroads  defined  by  an  urgent  need  to  transition  from  environmentally  detrimental  fossil  fuel  resources.  An  attractive  alternative  is  to  engineer  a  closed  carbon  cycle  through  the  conversion  of  carbon  dioxide  into  energy-dense  fuels.  Electrochemical  reduction  of  aqueous  CO2  can  offer  a  sustainable  approach  to  achieve  these  transformation  reactions;  however,  the  practical  implementation  of  electrocatalysts  is  challenged  by  low  efficiency  and  poor  selectivity  in  product  generation.  Overcoming  these  obstacles  requires  strategic  considerations  in  the  structural  and  functional  design  of  materials.  One  such  focus  has  centered  around  porous  materials  that  can  enhance  the  efficiency  of  C-C  bond  generation  through  modification  of  the  local  electrochemical  environment  via  confinement  effects.This  work  further  explores  the  synthesis  and  electrochemical  applications  of  porous  materials.  Chapter  2  of  this  dissertation  introduces  a  chromium-gallium  oxide  mixture  that,  when  in  the  presence  of  trace  metal,  can  achieve  unprecedented  efficiency  in  the  generation  of  multi-carbon  products  from  CO2.  This  includes  four-carbon  products  that  possess  energy  densities  comparable  to  conventional  fuels.  It  is  concluded  that  the  observed  reactivity  is  enabled  by  the  intrinsic  porosity  of  the  metal  oxide  mixture,  which  can  increase  the  local  concentration  of  CO2  at  the  electrode  interface  and  thereby  enhance  proton/electron  transfer  rates.  Chapter  3  continues  the  development  of  this  metal  oxide  system  with  the  adoption  of  a  hard-template  technique  providing  strict  synthetic  control  of  the  porous  morphology.  It  is  found  that  through  the  variation  of  pore  diameter,  selectivity  of  CO2-derived  products  can  be  altered.  Structural  characterization  of  the  synthesized  metal  oxide  interfaces  is  complimented  with  electroanalytical  experiments  to  evaluate  changes  in  the  local  electrochemical  environment  and  the  relationship  to  reactivity.  Finally,  Chapter  4  outlines  the  synthesis  of  cyanide  coordination  polymers  from  octacyanometallates  toward  an  assortment  of  materials  that  include  metal  carbides,  alloys,  oxides  and  phosphides.  Similar  to  a  template  based  syn-  thesis,  these  materials  retain  their  unique  morphology,  which  includes  catalytically  relevant  porous  structures.
■590    ▼aSchool  code:  0181.
■650  4▼aChemistry
■650  4▼aMaterials  science
■650  4▼aPhysical  chemistry
■653    ▼aCO2  reduction
■653    ▼aElectrocatalysis
■653    ▼aPorous  materials
■690    ▼a0485
■690    ▼a0794
■690    ▼a0494
■71020▼aPrinceton  University▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g87-04B.
■790    ▼a0181
■791    ▼aPh.D.
■792    ▼a2025
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17358853▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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