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Characterization and Fate of Isoprene Epoxydiol Isomerization Products in Atmospheric Secondary Organic Aerosol
Characterization and Fate of Isoprene Epoxydiol Isomerization Products in Atmospheric Secondary Organic Aerosol
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152131
- ISBN
- 9798383688199
- DDC
- 551.5
- 서명/저자
- Characterization and Fate of Isoprene Epoxydiol Isomerization Products in Atmospheric Secondary Organic Aerosol
- 발행사항
- [Sl] : The University of North Carolina at Chapel Hill, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 152 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
- 주기사항
- Advisor: Gold, Avram;Surratt, Jason.
- 학위논문주기
- Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2024.
- 초록/해제
- 요약Isoprene, the largest atmospheric emission of a non-methane volatile organic compound derived from terrestrial vegetation, is oxidized to secondary organic aerosol (SOA), contributing a significant fraction of global ambient fine particulate matter (PM2.5, or aerosol with aerodynamic diameter 2.5 μm). PM2.5 are a significant factor in Earth's radiative balance and adversely affect human health. Large uncertainties in atmospheric chemistry model predictions of global SOA levels arise from lack of authentic standards, causing inaccurate identification and quantitation of SOA species. This dissertation involves the synthesis of novel authentic standards to identify and quantitate major isoprene SOA components observed in low-nitrogen oxide (NOx) environments designated as "C5-alkene triols", which are now fully identified as 3- methylenebutane-1,2,4-triol and isomeric 3-methyletrahydrofuran-2,4-diols. This class of neutral, polar, hydrophilic polyols, hereafter described as IEPOX-derived C5H10O3 isomerization products for structural accuracy, present an analytical challenge for traditional chromatographymass spectrometry techniques, and in the absence of authentic standards, have likely been underestimated in atmospheric aerosols. Using novel authentic standards in combination with indoor smog chamber generation of SOA and subsequent chemical speciation with hydrophilic interaction liquid chromatography-high-resolution tandem mass spectrometry equipped with electrospray ionization (HILIC/ESI-HRMS/MS), the formation mechanisms of 3- methylenebutane-1,2,4-triol and 3-methyletrahydrofuran-2,4-diols are shown to be through particle-phase isomerization of isoprene-epoxydiol (IEPOX) under acidic conditions. Particle-togas partitioning with subsequent gas phase oxidation to non-volatile products is further demonstrated as a currently unrecognized SOA source. Findings suggest that the substantial atmospheric contribution of IEPOX-derived C5H10O3 isomerization products and resultant oxidation products must be considered in future chemically-explicit atmospheric modeling of isoprene oxidation for a more accurate depiction of SOA composition and mass within PM2.5. The dissertation represents an important advance in understanding the atmospheric chemistry of isoprene, particularly as NOx pollution control policies are implemented and this low-NOx oxidation pathway is projected to become increasingly dominant.
- 일반주제명
- Atmospheric chemistry
- 일반주제명
- Atmospheric sciences
- 일반주제명
- Chemistry
- 키워드
- Alkene triols
- 키워드
- Isomerization
- 키워드
- Isoprene
- 기타저자
- The University of North Carolina at Chapel Hill Environmental Sciences and Engineering
- 기본자료저록
- Dissertations Abstracts International. 86-02B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520250211152131
■006m o d
■007cr#unu||||||||
■020 ▼a9798383688199
■035 ▼a(MiAaPQ)AAI31483309
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a551.5
■1001 ▼aFrauenheim, Molly.
■24510▼aCharacterization and Fate of Isoprene Epoxydiol Isomerization Products in Atmospheric Secondary Organic Aerosol
■260 ▼a[Sl]▼bThe University of North Carolina at Chapel Hill▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a152 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-02, Section: B.
■500 ▼aAdvisor: Gold, Avram;Surratt, Jason.
■5021 ▼aThesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2024.
■520 ▼aIsoprene, the largest atmospheric emission of a non-methane volatile organic compound derived from terrestrial vegetation, is oxidized to secondary organic aerosol (SOA), contributing a significant fraction of global ambient fine particulate matter (PM2.5, or aerosol with aerodynamic diameter 2.5 μm). PM2.5 are a significant factor in Earth's radiative balance and adversely affect human health. Large uncertainties in atmospheric chemistry model predictions of global SOA levels arise from lack of authentic standards, causing inaccurate identification and quantitation of SOA species. This dissertation involves the synthesis of novel authentic standards to identify and quantitate major isoprene SOA components observed in low-nitrogen oxide (NOx) environments designated as "C5-alkene triols", which are now fully identified as 3- methylenebutane-1,2,4-triol and isomeric 3-methyletrahydrofuran-2,4-diols. This class of neutral, polar, hydrophilic polyols, hereafter described as IEPOX-derived C5H10O3 isomerization products for structural accuracy, present an analytical challenge for traditional chromatographymass spectrometry techniques, and in the absence of authentic standards, have likely been underestimated in atmospheric aerosols. Using novel authentic standards in combination with indoor smog chamber generation of SOA and subsequent chemical speciation with hydrophilic interaction liquid chromatography-high-resolution tandem mass spectrometry equipped with electrospray ionization (HILIC/ESI-HRMS/MS), the formation mechanisms of 3- methylenebutane-1,2,4-triol and 3-methyletrahydrofuran-2,4-diols are shown to be through particle-phase isomerization of isoprene-epoxydiol (IEPOX) under acidic conditions. Particle-togas partitioning with subsequent gas phase oxidation to non-volatile products is further demonstrated as a currently unrecognized SOA source. Findings suggest that the substantial atmospheric contribution of IEPOX-derived C5H10O3 isomerization products and resultant oxidation products must be considered in future chemically-explicit atmospheric modeling of isoprene oxidation for a more accurate depiction of SOA composition and mass within PM2.5. The dissertation represents an important advance in understanding the atmospheric chemistry of isoprene, particularly as NOx pollution control policies are implemented and this low-NOx oxidation pathway is projected to become increasingly dominant.
■590 ▼aSchool code: 0153.
■650 4▼aAtmospheric chemistry
■650 4▼aAtmospheric sciences
■650 4▼aChemistry
■653 ▼aAlkene triols
■653 ▼aIsomerization
■653 ▼aIsoprene
■653 ▼aMultiphase chemistry
■653 ▼aOrganic synthesis
■690 ▼a0371
■690 ▼a0725
■690 ▼a0485
■71020▼aThe University of North Carolina at Chapel Hill▼bEnvironmental Sciences and Engineering.
■7730 ▼tDissertations Abstracts International▼g86-02B.
■790 ▼a0153
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163067▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
