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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 Measurements
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211151125
- ISBN
- 9798382718224
- DDC
- 551.5
- 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
- 기타저자
- University of Colorado at Boulder Chemistry
- 기본자료저록
- Dissertations Abstracts International. 85-11B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520250211151125
■006m o d
■007cr#unu||||||||
■020 ▼a9798382718224
■035 ▼a(MiAaPQ)AAI31146959
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a551.5
■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.


