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Multiphase Chemical Kinetics in Aqueous Microdroplets
Multiphase Chemical Kinetics in Aqueous Microdroplets
Multiphase Chemical Kinetics in Aqueous Microdroplets

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자료유형  
 학위논문 서양
최종처리일시  
20250211152734
ISBN  
9798384455349
DDC  
541
저자명  
Prophet, Alexander M.
서명/저자  
Multiphase Chemical Kinetics in Aqueous Microdroplets
발행사항  
[Sl] : University of California, Berkeley, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
186 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-03, Section: B.
주기사항  
Advisor: Wilson, Kevin R.;Saykally, Richard J.
학위논문주기  
Thesis (Ph.D.)--University of California, Berkeley, 2024.
초록/해제  
요약Multiphase chemistry occurs when reactivity involves two or more distinct phases. Chemical transformations of this kind are ubiquitous in all domains of science, with particular relevance to environmental and biological chemistry. Aerosols, including cloud droplets, sea-spray, smoke, and dust are prime examples of gas-liquid and gas-solid systems that undergo heterogeneous chemical changes while persisting in the atmosphere. A fundamental understanding of how multiphase reactions proceed is critical, then, to the study of our environment and the causal networks between anthropogenic activity, global ecosystems, and atmospheric composition. Moreover, a mechanistic perspective of reactivity in gas-liquid or gas-solid systems provides a useful framework for the study of multiphase interactions more generally, even informing on similar mechanics encountered in liquid-liquid and solid-liquid systems.In this work, experiment and theory are brought together to develop a kinetic framework of multiphase reactivity in aqueous microdroplets with particular focus on the role of the air-water interface. The experiments presented investigate the ozone-oxidation of aqueous sodium iodide contained in levitated microdroplets. This system is not only relevant to oxidation reactions in the environment, but also a compelling platform for studying mass-transfer across the air-water interface due to its unique reactive properties. As explored in Chapters 2 and 3, both I- and O3 possess a unique affinity for the air-water interface relative to their bulk phases, which directly affects the chemical kinetics at the microdroplet surface. This effect is studied by measuring microdroplet-oxidation kinetics while varying the solution pH and the concentration of both reactants. Experiments in Chapter 4 perturb this surface chemistry by the addition of surfactant to the microdroplet solution-effectively suppressing the surface reaction and producing a kinetic signature consistent with a diffusion limited reaction rate in the bulk phase. Insights from the specific systems in Chapters 2-4 provide the basis for a general framework of mass-transport and chemical reactivity in microdroplets which is developed in Chapter 5. This work aims to provide a route to analyzing an array of multiphase experiments from a critical lens by disentangling the underlying physical and chemical phenomena.
일반주제명  
Physical chemistry
일반주제명  
Chemistry
일반주제명  
Analytical chemistry
일반주제명  
Atmospheric chemistry
키워드  
Aerosols
키워드  
Chemical modeling
키워드  
Interfaces
키워드  
Kinetics
키워드  
Multiphase chemistry
키워드  
Surface chemistry
기타저자  
University of California, Berkeley Chemistry
기본자료저록  
Dissertations Abstracts International. 86-03B.
전자적 위치 및 접속  
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MARC

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■040    ▼aMiAaPQ▼cMiAaPQ
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■1001  ▼aProphet,  Alexander  M.
■24510▼aMultiphase  Chemical  Kinetics  in  Aqueous  Microdroplets
■260    ▼a[Sl]▼bUniversity  of  California,  Berkeley▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a186  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-03,  Section:  B.
■500    ▼aAdvisor:  Wilson,  Kevin  R.;Saykally,  Richard  J.
■5021  ▼aThesis  (Ph.D.)--University  of  California,  Berkeley,  2024.
■520    ▼aMultiphase  chemistry  occurs  when  reactivity  involves  two  or  more  distinct  phases.  Chemical  transformations  of  this  kind  are  ubiquitous  in  all  domains  of  science,  with  particular  relevance  to  environmental  and  biological  chemistry.  Aerosols,  including  cloud  droplets,  sea-spray,  smoke,  and  dust  are  prime  examples  of  gas-liquid  and  gas-solid  systems  that  undergo  heterogeneous  chemical  changes  while  persisting  in  the  atmosphere.  A  fundamental  understanding  of  how  multiphase  reactions  proceed  is  critical,  then,  to  the  study  of  our  environment  and  the  causal  networks  between  anthropogenic  activity,  global  ecosystems,  and  atmospheric  composition.  Moreover,  a  mechanistic  perspective  of  reactivity  in  gas-liquid  or  gas-solid  systems  provides  a  useful  framework  for  the  study  of  multiphase  interactions  more  generally,  even  informing  on  similar  mechanics  encountered  in  liquid-liquid  and  solid-liquid  systems.In  this  work,  experiment  and  theory  are  brought  together  to  develop  a  kinetic  framework  of  multiphase  reactivity  in  aqueous  microdroplets  with  particular  focus  on  the  role  of  the  air-water  interface.  The  experiments  presented  investigate  the  ozone-oxidation  of  aqueous  sodium  iodide  contained  in  levitated  microdroplets.  This  system  is  not  only  relevant  to  oxidation  reactions  in  the  environment,  but  also  a  compelling  platform  for  studying  mass-transfer  across  the  air-water  interface  due  to  its  unique  reactive  properties.  As  explored  in  Chapters  2  and  3,  both  I-  and  O3  possess  a  unique  affinity  for  the  air-water  interface  relative  to  their  bulk  phases,  which  directly  affects  the  chemical  kinetics  at  the  microdroplet  surface.  This  effect  is  studied  by  measuring  microdroplet-oxidation  kinetics  while  varying  the  solution  pH  and  the  concentration  of  both  reactants.  Experiments  in  Chapter  4  perturb  this  surface  chemistry  by  the  addition  of  surfactant  to  the  microdroplet  solution-effectively  suppressing  the  surface  reaction  and  producing  a  kinetic  signature  consistent  with  a  diffusion  limited  reaction  rate  in  the  bulk  phase.  Insights  from  the  specific  systems  in  Chapters  2-4  provide  the  basis  for  a  general  framework  of  mass-transport  and  chemical  reactivity  in  microdroplets  which  is  developed  in  Chapter  5.  This  work  aims  to  provide  a  route  to  analyzing  an  array  of  multiphase  experiments  from  a  critical  lens  by  disentangling  the  underlying  physical  and  chemical  phenomena.
■590    ▼aSchool  code:  0028.
■650  4▼aPhysical  chemistry
■650  4▼aChemistry
■650  4▼aAnalytical  chemistry
■650  4▼aAtmospheric  chemistry
■653    ▼aAerosols
■653    ▼aChemical  modeling
■653    ▼aInterfaces
■653    ▼aKinetics
■653    ▼aMultiphase  chemistry
■653    ▼aSurface  chemistry
■690    ▼a0494
■690    ▼a0485
■690    ▼a0486
■690    ▼a0371
■71020▼aUniversity  of  California,  Berkeley▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g86-03B.
■790    ▼a0028
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163635▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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