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Uniform, Nitrogen-Doped Carbon Nanospheres and Their Use as Supports for Single-Atom Catalysts
Uniform, Nitrogen-Doped Carbon Nanospheres and Their Use as Supports for Single-Atom Catal...
Uniform, Nitrogen-Doped Carbon Nanospheres and Their Use as Supports for Single-Atom Catalysts

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20260202105327
ISBN  
9798263325077
DDC  
621
저자명  
Jeskey, Jacob.
서명/저자  
Uniform, Nitrogen-Doped Carbon Nanospheres and Their Use as Supports for Single-Atom Catalysts
발행사항  
[Sl] : Georgia Institute of Technology, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
141 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-05, Section: B.
주기사항  
Advisor: Xia, Younan.
학위논문주기  
Thesis (Ph.D.)--Georgia Institute of Technology, 2024.
초록/해제  
요약With the global environmental crisis and ever-increasing demands on energy, development of sustainable systems for energy conversion has become one of the most important challenges today. Currently, electrochemical energy conversion technologies, including fuel cells, water splitting, and metal-air batteries, are considered the most promising means to meet the increasing requirements on energy due to their high-energy densities, high efficiency, and environmental greenness. Unfortunately, their practical use is challenged by the high cost, sluggish kinetics, and long-term stability issues resulting from the use of noble-metal electrocatalysts. Recently, single-atom catalysts (SACs) anchored to carbon nanosphere supports have gained tremendous attention as possible alternatives for noble-metal nanoparticles. However, their preparation typically involves complicated multi-step processes that are not practical for industrial use. In this dissertation, I present a simple yet highly effective chemical-confinement strategy to produce SACs on uniform porous carbon nanospheres with high loadings. Starting from the ground up, the first project was focused on improving the morphology and nitrogen content of carbon nanospheres using an EDTA-assisted synthesis. Without compromising uniformity, the synthesis could be scaled up 10 times to produce colloidal crystals that displayed iridescence across the entire visible spectrum. The synthesis was then modified to produce first-row transition metal SACs on uniform N-doped carbon nanospheres. Utilizing a chemical confinement strategy, a wide range of first-row transition metal SACs with remarkable loadings up to 3.87 wt.% were possible. Finally, I systematically investigated how porosity within the carbon nanospheres affects the activity of Ir-SACs toward formic acid oxidation (FAO). Specifically, we utilized a kinetically-controlled growth strategy to produce Ir-SACs loaded in uniform carbon nanospheres featuring mesoporous, yolk-shell, and hollow structures. The feasible synthesis should be extendible to other metals across the periodic table for the preparation of highly exposed SACs for different catalytic reactions.
일반주제명  
Fuel cells
일반주제명  
Metals
일반주제명  
Adsorption
일반주제명  
Potassium
일반주제명  
Electrocatalysis
일반주제명  
Scanning electron microscopy
일반주제명  
Nitrogen
일반주제명  
Nanotubes
일반주제명  
Polymers
일반주제명  
Transmission electron microscopy
일반주제명  
Electrolytes
일반주제명  
Poisoning
일반주제명  
Energy conversion
일반주제명  
Emulsion polymerization
일반주제명  
Oxidation
일반주제명  
Fourier transforms
일반주제명  
Carbon
일반주제명  
Nanocrystals
일반주제명  
Catalysis
일반주제명  
Atoms & subatomic particles
일반주제명  
Alternative energy
일반주제명  
Analytical chemistry
일반주제명  
Atomic physics
일반주제명  
Chemical engineering
일반주제명  
Mathematics
일반주제명  
Nanotechnology
일반주제명  
Polymer chemistry
기타저자  
Georgia Institute of Technology.
기본자료저록  
Dissertations Abstracts International. 87-05B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aJeskey,  Jacob.
■24510▼aUniform,  Nitrogen-Doped  Carbon  Nanospheres  and  Their  Use  as  Supports  for  Single-Atom  Catalysts
■260    ▼a[Sl]▼bGeorgia  Institute  of  Technology▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a141  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-05,  Section:  B.
■500    ▼aAdvisor:  Xia,  Younan.
■5021  ▼aThesis  (Ph.D.)--Georgia  Institute  of  Technology,  2024.
■520    ▼aWith  the  global  environmental  crisis  and  ever-increasing  demands  on  energy,  development  of  sustainable  systems  for  energy  conversion  has  become  one  of  the  most  important  challenges  today.  Currently,  electrochemical  energy  conversion  technologies,  including  fuel  cells,  water  splitting,  and  metal-air  batteries,  are  considered  the  most  promising  means  to  meet  the  increasing  requirements  on  energy  due  to  their  high-energy  densities,  high  efficiency,  and  environmental  greenness.  Unfortunately,  their  practical  use  is  challenged  by  the  high  cost,  sluggish  kinetics,  and  long-term  stability  issues  resulting  from  the  use  of  noble-metal  electrocatalysts.  Recently,  single-atom  catalysts  (SACs)  anchored  to  carbon  nanosphere  supports  have  gained  tremendous  attention  as  possible  alternatives  for  noble-metal  nanoparticles.  However,  their  preparation  typically  involves  complicated  multi-step  processes  that  are  not  practical  for  industrial  use.  In  this  dissertation,  I  present  a  simple  yet  highly  effective  chemical-confinement  strategy  to  produce  SACs  on  uniform  porous  carbon  nanospheres  with  high  loadings.  Starting  from  the  ground  up,  the  first  project  was  focused  on  improving  the  morphology  and  nitrogen  content  of  carbon  nanospheres  using  an  EDTA-assisted  synthesis.  Without  compromising  uniformity,  the  synthesis  could  be  scaled  up  10  times  to  produce  colloidal  crystals  that  displayed  iridescence  across  the  entire  visible  spectrum.  The  synthesis  was  then  modified  to  produce  first-row  transition  metal  SACs  on  uniform  N-doped  carbon  nanospheres.  Utilizing  a  chemical  confinement  strategy,  a  wide  range  of  first-row  transition  metal  SACs  with  remarkable  loadings  up  to  3.87  wt.%  were  possible.  Finally,  I  systematically  investigated  how  porosity  within  the  carbon  nanospheres  affects  the  activity  of  Ir-SACs  toward  formic  acid  oxidation  (FAO).  Specifically,  we  utilized  a  kinetically-controlled  growth  strategy  to  produce  Ir-SACs  loaded  in  uniform  carbon  nanospheres  featuring  mesoporous,  yolk-shell,  and  hollow  structures.  The  feasible  synthesis  should  be  extendible  to  other  metals  across  the  periodic  table  for  the  preparation  of  highly  exposed  SACs  for  different  catalytic  reactions.
■590    ▼aSchool  code:  0078.
■650  4▼aFuel  cells
■650  4▼aMetals
■650  4▼aAdsorption
■650  4▼aPotassium
■650  4▼aElectrocatalysis
■650  4▼aScanning  electron  microscopy
■650  4▼aNitrogen
■650  4▼aNanotubes
■650  4▼aPolymers
■650  4▼aTransmission  electron  microscopy
■650  4▼aElectrolytes
■650  4▼aPoisoning
■650  4▼aEnergy  conversion
■650  4▼aEmulsion  polymerization
■650  4▼aOxidation
■650  4▼aFourier  transforms
■650  4▼aCarbon
■650  4▼aNanocrystals
■650  4▼aCatalysis
■650  4▼aAtoms  &  subatomic  particles
■650  4▼aAlternative  energy
■650  4▼aAnalytical  chemistry
■650  4▼aAtomic  physics
■650  4▼aChemical  engineering
■650  4▼aMathematics
■650  4▼aNanotechnology
■650  4▼aPolymer  chemistry
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■71020▼aGeorgia  Institute  of  Technology.
■7730  ▼tDissertations  Abstracts  International▼g87-05B.
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■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17360248▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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