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Atmospheric Aerosols: Quantification and Method Development Using Field and Laboratory Measurements
Atmospheric Aerosols: Quantification and Method Development Using Field and Laboratory Mea...
Atmospheric Aerosols: Quantification and Method Development Using Field and Laboratory Measurements

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자료유형  
 학위논문 서양
최종처리일시  
20250211151125
ISBN  
9798382718224
DDC  
551.5
저자명  
Schueneman, Melinda Kaye.
서명/저자  
Atmospheric Aerosols: Quantification and Method Development Using Field and Laboratory Measurements
발행사항  
[Sl] : University of Colorado at Boulder, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
231 p
주기사항  
Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
주기사항  
Advisor: Jimenez, Jose L.
학위논문주기  
Thesis (Ph.D.)--University of Colorado at Boulder, 2024.
초록/해제  
요약The composition of atmospheric aerosols is influenced by the source/atmospheric conditions (e.g. rural, polluted, and/or biomass burning) as well as gas (g)↔particle (p) partitioning in an air mass. There are several analytical techniques used to measure aerosols, including Extractive Electrospray Ionization Mass Spectrometers (e.g. EESI, molecular ions of components of aerosols); Aerosol Mass Spectrometers (AMSs, typically bulk aerosol composition), and Scanning Mobility Particle Sizers (SMPSs, aerosol number density and size). Here, aerosol data from: 1. airborne atmospheric field studies that span a wide range of sources, including remote, urban, biomass burning, and air mass ages, 2. laboratory experiments for either sulfate aerosol or organic aerosol g↔p partitioning and quantification, and 3. kinetic modeling are used to quantify aerosol sulfate detection using an AMS across multiple field studies, calibrate molecular species present in the aerosol phase, and quantify secondary organic aerosol (SOA) formation and g↔p partitioning for known Volatile Organic Compound (VOC) precursors. In part I, a method for classifying total measured aerosol sulfate (~20% of global aerosol mass) into either ammonium sulfate (AS) or organosulfate (OS) was tested with the AMS. I identified four chemical regimes in the atmosphere, each of which has distinct properties impacting the ability of the AMS to classify OS vs. AS. I found that ambient conditions in two of these regimes allow for an estimation of aerosol pH in real-time. In part II, I designed a new calibration technique which combines High Performance Liquid Chromatography (HPLC), aerosolization, SMPS, and Positive Matrix Factorization (PMF) to calibrate the EESI and AMS. I showed that species in complex aerosol mixtures (like SOA) can be separated and calibrated for in the absence of reference standards. In part III, I quantified the SOA formation potential of different biomass burning VOC precursors with OH. I designed an iterative solver within a kinetic model that calculates the effect of vapor wall loss (VWL) in atmospheric chambers, which allowed me to constrain g↔p partitioning for the reaction products of each VOC. I compared the volatility of SOA to that of primary OA (POA) in a simulated wildfire and found that POA appears to be less volatile, thus more likely to be retained in the p phase as wildfire smoke ages.
일반주제명  
Atmospheric chemistry
일반주제명  
Analytical chemistry
일반주제명  
Environmental studies
키워드  
Aerosols
키워드  
Calibration
키워드  
Mass spectrometry
키워드  
Partitioning process
키워드  
Secondary organic aerosols
기타저자  
University of Colorado at Boulder Chemistry
기본자료저록  
Dissertations Abstracts International. 85-11B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aSchueneman,  Melinda  Kaye.▼0(orcid)0000-0003-4359-1472
■24510▼aAtmospheric  Aerosols:  Quantification  and  Method  Development  Using  Field  and  Laboratory  Measurements
■260    ▼a[Sl]▼bUniversity  of  Colorado  at  Boulder▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a231  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  85-11,  Section:  B.
■500    ▼aAdvisor:  Jimenez,  Jose  L.
■5021  ▼aThesis  (Ph.D.)--University  of  Colorado  at  Boulder,  2024.
■520    ▼aThe  composition  of  atmospheric  aerosols  is  influenced  by  the  source/atmospheric  conditions  (e.g.  rural,  polluted,  and/or  biomass  burning)  as  well  as  gas  (g)↔particle  (p)  partitioning  in  an  air  mass.  There  are  several  analytical  techniques  used  to  measure  aerosols,  including  Extractive  Electrospray  Ionization  Mass  Spectrometers  (e.g.  EESI,  molecular  ions  of  components  of  aerosols);  Aerosol  Mass  Spectrometers  (AMSs,  typically  bulk  aerosol  composition),  and  Scanning  Mobility  Particle  Sizers  (SMPSs,  aerosol  number  density  and  size).  Here,  aerosol  data  from:  1.  airborne  atmospheric  field  studies  that  span  a  wide  range  of  sources,  including  remote,  urban,  biomass  burning,  and  air  mass  ages,  2.  laboratory  experiments  for  either  sulfate  aerosol  or  organic  aerosol  g↔p  partitioning  and  quantification,  and  3.  kinetic  modeling  are  used  to  quantify  aerosol  sulfate  detection  using  an  AMS  across  multiple  field  studies,  calibrate  molecular  species  present  in  the  aerosol  phase,  and  quantify  secondary  organic  aerosol  (SOA)  formation  and  g↔p  partitioning  for  known  Volatile  Organic  Compound  (VOC)  precursors.  In  part  I,  a  method  for  classifying  total  measured  aerosol  sulfate  (~20%  of  global  aerosol  mass)  into  either  ammonium  sulfate  (AS)  or  organosulfate  (OS)  was  tested  with  the  AMS.  I  identified  four  chemical  regimes  in  the  atmosphere,  each  of  which  has  distinct  properties  impacting  the  ability  of  the  AMS  to  classify  OS  vs.  AS.  I  found  that  ambient  conditions  in  two  of  these  regimes  allow  for  an  estimation  of  aerosol  pH  in  real-time.  In  part  II,  I  designed  a  new  calibration  technique  which  combines  High  Performance  Liquid  Chromatography  (HPLC),  aerosolization,  SMPS,  and  Positive  Matrix  Factorization  (PMF)  to  calibrate  the  EESI  and  AMS.  I  showed  that  species  in  complex  aerosol  mixtures  (like  SOA)  can  be  separated  and  calibrated  for  in  the  absence  of  reference  standards.  In  part  III,  I  quantified  the  SOA  formation  potential  of  different  biomass  burning  VOC  precursors  with  OH.  I  designed  an  iterative  solver  within  a  kinetic  model  that  calculates  the  effect  of  vapor  wall  loss  (VWL)  in  atmospheric  chambers,  which  allowed  me  to  constrain  g↔p  partitioning  for  the  reaction  products  of  each  VOC.  I  compared  the  volatility  of  SOA  to  that  of  primary  OA  (POA)  in  a  simulated  wildfire  and  found  that  POA  appears  to  be  less  volatile,  thus  more  likely  to  be  retained  in  the  p  phase  as  wildfire  smoke  ages.
■590    ▼aSchool  code:  0051.
■650  4▼aAtmospheric  chemistry
■650  4▼aAnalytical  chemistry
■650  4▼aEnvironmental  studies
■653    ▼aAerosols
■653    ▼aCalibration
■653    ▼aMass  spectrometry
■653    ▼aPartitioning  process
■653    ▼aSecondary  organic  aerosols
■690    ▼a0371
■690    ▼a0486
■690    ▼a0477
■71020▼aUniversity  of  Colorado  at  Boulder▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g85-11B.
■790    ▼a0051
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17160844▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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