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The Characterization, Synthesis, and Optimization of Metalated Nitrogen-Doped Carbon Active Sites for Aerobic Oxidation Reactions
The Characterization, Synthesis, and Optimization of Metalated Nitrogen-Doped Carbon Activ...
The Characterization, Synthesis, and Optimization of Metalated Nitrogen-Doped Carbon Active Sites for Aerobic Oxidation Reactions

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자료유형  
 학위논문 서양
최종처리일시  
20260202105135
ISBN  
9798291577325
DDC  
540
저자명  
Martinez, Jesse J.
서명/저자  
The Characterization, Synthesis, and Optimization of Metalated Nitrogen-Doped Carbon Active Sites for Aerobic Oxidation Reactions
발행사항  
[Sl] : The University of Wisconsin - Madison, 2025
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2025
형태사항  
94 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-02, Section: B.
주기사항  
Advisor: Stahl, Shannon S.
학위논문주기  
Thesis (Ph.D.)--The University of Wisconsin - Madison, 2025.
초록/해제  
요약Metalated nitrogen-doped carbon (M-N-C) materials are an important class of catalysts that feature isolated metal ions dispersed within a conductive nitrogen-doped graphitic support. Fe-N-C variants of these materials have gained prominence as electrocatalysts for the oxygen reduction reaction (ORR) in fuel cells. The catalytic active sites consist of single-atom Fe ions coordinated by nitrogen atoms within the graphitic material (FeNx), resembling Fe-porphyrins (i.e., x = 4) and related Fe-macrocycles commonly encountered in molecular and biological catalysts. The same class of M-N-C materials have been identified as effective catalysts for aerobic oxidation of organic molecules. The latter reactions are conceptually similar to the electrochemical ORR, using protons and electrons from chemical bonds in the organic molecules to reduce O2 to water, but their mechanisms have received much less attention. The present study of aerobic oxidation reactions with an array of different Fe-N-C catalysts reveals that catalytic activity does not depend on the FeNx site density but, instead, the basicity of nitrogen atoms within the catalyst. This conclusion is supported by kinetic and spectroscopic data and observation of similar behavior across three different liquid-phase aerobic oxidation reactions.
일반주제명  
Chemistry
일반주제명  
Inorganic chemistry
일반주제명  
Materials science
키워드  
Aerobic oxidation
키워드  
Heterogeneous catalysis
키워드  
Metalated nitrogen-doped carbon
기타저자  
The University of Wisconsin - Madison Chemistry
기본자료저록  
Dissertations Abstracts International. 87-02B.
전자적 위치 및 접속  
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■035    ▼a(MiAaPQ)AAI32239790
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a540
■1001  ▼aMartinez,  Jesse  J.
■24510▼aThe  Characterization,  Synthesis,  and  Optimization  of  Metalated  Nitrogen-Doped  Carbon  Active  Sites  for  Aerobic  Oxidation  Reactions
■260    ▼a[Sl]▼bThe  University  of  Wisconsin  -  Madison▼c2025
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2025
■300    ▼a94  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-02,  Section:  B.
■500    ▼aAdvisor:  Stahl,  Shannon  S.
■5021  ▼aThesis  (Ph.D.)--The  University  of  Wisconsin  -  Madison,  2025.
■520    ▼aMetalated  nitrogen-doped  carbon  (M-N-C)  materials  are  an  important  class  of  catalysts  that  feature  isolated  metal  ions  dispersed  within  a  conductive  nitrogen-doped  graphitic  support.  Fe-N-C  variants  of  these  materials  have  gained  prominence  as  electrocatalysts  for  the  oxygen  reduction  reaction  (ORR)  in  fuel  cells.  The  catalytic  active  sites  consist  of  single-atom  Fe  ions  coordinated  by  nitrogen  atoms  within  the  graphitic  material  (FeNx),  resembling  Fe-porphyrins  (i.e.,  x  =  4)  and  related  Fe-macrocycles  commonly  encountered  in  molecular  and  biological  catalysts.  The  same  class  of  M-N-C  materials  have  been  identified  as  effective  catalysts  for  aerobic  oxidation  of  organic  molecules.  The  latter  reactions  are  conceptually  similar  to  the  electrochemical  ORR,  using  protons  and  electrons  from  chemical  bonds  in  the  organic  molecules  to  reduce  O2  to  water,  but  their  mechanisms  have  received  much  less  attention.  The  present  study  of  aerobic  oxidation  reactions  with  an  array  of  different  Fe-N-C  catalysts  reveals  that  catalytic  activity  does  not  depend  on  the  FeNx  site  density  but,  instead,  the  basicity  of  nitrogen  atoms  within  the  catalyst.  This  conclusion  is  supported  by  kinetic  and  spectroscopic  data  and  observation  of  similar  behavior  across  three  different  liquid-phase  aerobic  oxidation  reactions.
■590    ▼aSchool  code:  0262.
■650  4▼aChemistry
■650  4▼aInorganic  chemistry
■650  4▼aMaterials  science
■653    ▼aAerobic  oxidation
■653    ▼aHeterogeneous  catalysis
■653    ▼aMetalated  nitrogen-doped  carbon
■690    ▼a0485
■690    ▼a0794
■690    ▼a0488
■71020▼aThe  University  of  Wisconsin  -  Madison▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g87-02B.
■790    ▼a0262
■791    ▼aPh.D.
■792    ▼a2025
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17359545▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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