DOI: 10.1016/j.atmosenv.2015.09.038
Scopus记录号: 2-s2.0-84942326702
论文题名: Control of ozonolysis kinetics and aerosol yield by nuances in the molecular structure of volatile organic compounds
作者: Harvey R ; M ; , Petrucci G ; A
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2015
卷: 122 起始页码: 188
结束页码: 195
语种: 英语
英文关键词: Alkene
; Green leaf volatile
; Oxygenated alkene
; Ozonolysis
; SOA yield
; Structure activity relationships (SARs)
Scopus关键词: Aerosols
; Atmospheric chemistry
; Carbon
; Chemical bonds
; Hydrocarbons
; Kinetics
; Molecular structure
; Molecules
; Olefins
; Ozone
; Rate constants
; Volatile organic compounds
; Green leaf volatiles
; Molecular level interactions
; Ozonolysis
; Ozonolysis reactions
; Secondary organic aerosols
; SOA yield
; Structural differences
; Structure activity relationships
; Atmospheric structure
; alkene
; carbon
; functional group
; oxygen
; volatile organic compound
; aerosol composition
; aerosol formation
; alkene
; carbon
; chemical bonding
; chemical reaction
; environmental fate
; kinetics
; laboratory method
; oxygenation
; ozone
; volatile organic compound
; Article
; chemical bond
; chemical reaction kinetics
; chemical structure
; environmental impact
; ozonolysis
; priority journal
; secondary organic aerosol
; stereochemistry
Scopus学科分类: Environmental Science: Water Science and Technology
; Earth and Planetary Sciences: Earth-Surface Processes
; Environmental Science: Environmental Chemistry
英文摘要: Secondary organic aerosol (SOA) plays integral roles in climate and human health, yet there remains a limited understanding of the mechanisms that lead to its formation and ultimate fate, as evidenced by a disparity between modeled atmospheric SOA loadings and field measurements. This disparity highlights the need for a more accurate representation of the molecular-level interactions between SOA sources and oxidative pathways. Due to the paucity of detailed chemical data for most SOA precursors of atmospheric relevance, models generally predict SOA loadings using structure activity relationships generalized to classes of SOA precursors. However, the kinetics and SOA forming potential of molecules are nuanced by seemingly minor structural differences in parent molecules that may be neglected in models. Laboratory chamber studies were used to measure SOA yields and rate constants for the ozonolysis of several linear, cyclic and oxygenated C5-C7 alkenes whose molecular structure vary in the site of unsaturation and/or the presence/position of functional groups and that represent atmospherically relevant classes of molecules. For the alkenes studied in this work, we found greater SOA yields for cyclic compounds compared to their linear analogs. For 1-alkenes, SOA yield increased with carbon number but was also dependent on the position of the double bond (internal vs terminal). Both the identity and position of oxygenated functional groups influenced SOA yield and kinetics through steric and electronic effects. Additionally, terminal alkenes generally resulted in a greater SOA yield than analogous internal alkenes, indicating that the position of the double bond in alkenes plays an important role in its atmospheric fate. Herein, we demonstrate the nuanced behavior of these ozonolysis reactions and discuss relationships between parent compound molecular structure and SOA yield and kinetics. © 2015 Elsevier Ltd. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/81438
Appears in Collections: 气候变化事实与影响
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作者单位: University of Vermont, Cook Physical Sciences, Burlington, VT, United States
Recommended Citation:
Harvey R,M,, Petrucci G,et al. Control of ozonolysis kinetics and aerosol yield by nuances in the molecular structure of volatile organic compounds[J]. Atmospheric Environment,2015-01-01,122