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DOI | 10.5194/acp-19-7255-2019 |
Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions | |
Schwantes R.H.; Charan S.M.; Bates K.H.; Huang Y.; Nguyen T.B.; Mai H.; Kong W.; Flagan R.C.; Seinfeld J.H. | |
发表日期 | 2019 |
ISSN | 16807316 |
起始页码 | 7255 |
结束页码 | 7278 |
卷号 | 19期号:11 |
英文摘要 | Recent advances in our knowledge of the gas-phase oxidation of isoprene, the impact of chamber walls on secondary organic aerosol (SOA) mass yields, and aerosol measurement analysis techniques warrant reevaluating SOA yields from isoprene. In particular, SOA from isoprene oxidation under high-NOx conditions forms via two major pathways: (1) low-volatility nitrates and dinitrates (LV pathway) and (2) hydroxymethyl-methyl-α-lactone (HMML) reaction on a surface or the condensed phase of particles to form 2-methyl glyceric acid and its oligomers (2MGA pathway). These SOA production pathways respond differently to reaction conditions. Past chamber experiments generated SOA with varying contributions from these two unique pathways, leading to results that are difficult to interpret. This study examines the SOA yields from these two pathways independently, which improves the interpretation of previous results and provides further understanding of the relevance of chamber SOA yields to the atmosphere and regional or global modeling. Results suggest that low-volatility nitrates and dinitrates produce significantly more aerosol than previously thought; the experimentally measured SOA mass yield from the LV pathway is ∼0.15. Sufficient seed surface area at the start of the reaction is needed to limit the effects of vapor wall losses of low-volatility compounds and accurately measure the complete SOA mass yield. Under dry conditions, substantial amounts of SOA are formed from HMML ring-opening reactions with inorganic ions and HMML organic oligomerization processes. However, the lactone organic oligomerization reactions are suppressed under more atmospherically relevant humidity levels, where hydration of the lactone is more competitive. This limits the SOA formation potential from the 2MGA pathway to HMML ring-opening reactions with water or inorganic ions under typical atmospheric conditions. The isoprene SOA mass yield from the LV pathway measured in this work is significantly higher than previous studies have reported, suggesting that low-volatility compounds such as organic nitrates and dinitrates may contribute to isoprene SOA under high-NOx conditions significantly more than previously thought and thus deserve continued study. © Author(s) 2019. |
语种 | 英语 |
scopus关键词 | aerosol composition; isoprene; modeling; nitrogen oxides; oxidation; reaction kinetics; volatile substance |
来源期刊 | Atmospheric Chemistry and Physics
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/144368 |
作者单位 | Division of Geological and Planetary Sciences, California Institute of Technology, 1200 East California Boulevard, Pasadena, CA 91125, United States; Division of Chemistry and Chemical Engineering, California Institute of Technology, 1200 East California Boulevard, Pasadena, CA 91125, United States; Department of Environmental Toxicology, University of California - Davis, Davis, CA 95616, United States; Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125, United States; National Center for Atmospheric Research, Boulder, CO 80307, United States; Faculty of Arts and Sciences, Harvard University, Cambridge, MA 02138, United States |
推荐引用方式 GB/T 7714 | Schwantes R.H.,Charan S.M.,Bates K.H.,et al. Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions[J],2019,19(11). |
APA | Schwantes R.H..,Charan S.M..,Bates K.H..,Huang Y..,Nguyen T.B..,...&Seinfeld J.H..(2019).Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions.Atmospheric Chemistry and Physics,19(11). |
MLA | Schwantes R.H.,et al."Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions".Atmospheric Chemistry and Physics 19.11(2019). |
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