气候变化领域集成服务门户(CCPortal): PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study

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DOI	10.1016/j.atmosenv.2020.117939
	PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study
	Hughes D.D.; Christiansen M.B.; Milani A.; Vermeuel M.P.; Novak G.A.; Alwe H.D.; Dickens A.F.; Pierce R.B.; Millet D.B.; Bertram T.H.; Stanier C.O.; Stone E.A.
发表日期	2021
ISSN	1352-2310
卷号	244
英文摘要	The Lake Michigan Ozone Study from 21 May to 23 June 2017 (LMOS 2017) aimed to better understand the anthropogenic and biogenic sources that contribute to ozone and fine particles (PM2.5) along the coast of Lake Michigan. Here, we focus on the chemical composition of daytime and nighttime PM2.5—especially organic carbon, inorganic ions and organosulfates—at a ground-based supersite in Zion, Illinois. PM2.5 mass concentrations ranged from 1.5 to 12.9 μg m−3 with an average (±standard error) of 5.2 ± 0.4 μg m−3. The most significant contributor to PM2.5 mass was organic matter (OM; calculated as 1.7 × organic carbon [OC]; contributing an average of 59 ± 2%), followed by sulfate (17 ± 1%), ammonium (6.3 ± 0.3%), nitrate (3.5 ± 0.4%), and elemental carbon (EC; 3.4 ± 0.2%). During each of the three periods of high ozone, PM2.5 had different regional characteristics. Period A (2–3 June) was impacted by lake breeze and south-easterly air masses that travelled over major urban areas. Period A had the highest daily PM2.5 mass concentrations (11.4 ± 1.5 μg m−3) and EC with a relatively low OC:EC ratio of 7.0, indicating the influence of sources with low OC:EC ratios, which includes the anthropogenic combustion of fossil fuels and biomass. Period B (10–13 June) was impacted by air masses traveling from the southern US. It had a relatively high OC:EC ratio of 18, the highest PM2.5 sulfate concentrations and aerosol acidity, and elevated mixing ratios of isoprene along with its oxidation products methyl vinyl ketone (MVK) and methacrolein (MACR). Peak concentrations of organosulfates, including methyltetrol sulfate (m/z 215; C5H11SO7−), were also observed throughout period B. Period C (13–17 June) followed a change to northerly winds. PM2.5 concentrations decreased along with decreases in sulfate, acidity, and most organosulfates. Throughout the study, organosulfates accounted for an average of 4% of OM and up to 15% of OM in Period B. Organosulfates were largely isoprene-derived, with lessor contributions from monoterpenes (0.3%) and anthropogenic sources (0.5%). Through these measurements of organosulfates in the Great Lakes region, we demonstrate the importance of anthropogenic sulfate emissions and aerosol acidity on SOA formation, and establish that isoprene-derived organosulfates, in particular, contribute significantly to PM2.5. With other LMOS observations, the chemical signatures of PM2.5, and back trajectories show that ozone episodes cooccur with localized lake-breeze meteorology within air masses that vary from episode to episode in chemical history and source region. © 2020 Elsevier Ltd
关键词	Atmospheric aerosols Chemical composition Isoprene Organosulfates PM2.5 Secondary organic aerosol
语种	英语
scopus关键词	Acidity; Aerosols; Fossil fuels; Isoprene; Ketones; Monoterpenes; Organic carbon; Ozone; Sulfur compounds; Anthropogenic sources; Chemical compositions; Chemical signatures; Methyl vinyl ketones; Peak concentrations; Regional characteristics; Secondary organic aerosols; Sulfate concentrations; Lakes; 2 methylerythritol; 2 methylglyceric acid; 2 methylthreitol; ammonia; carbon; cyclohexene derivative; elemental carbon; fossil fuel; glycolic acid sulfate; ion; isoprene; levoglucosan; limonene; methacrolein; methyl vinyl ketone; methylglyceric acid sulfate; methyltetrol sulfate; monoterpene; nitrate; organic carbon; organic compound; organic matter; organosulfate derivative; ozone; pinene; sulfate; unclassified drug; aerosol; air mass; anthropogenic source; chemical composition; elemental carbon; ozone; particulate matter; spatiotemporal analysis; urban area; acidity; air; analytical parameters; Article; biomass; chemical composition; combustion; concentration (parameter); day length; environmental impact; environmental parameters; Illinois; lake; mass; measurement error; meteorology; Michigan; night; organic carbon elemental carbon ratio; oxidation; particulate matter 2.5; priority journal; secondary organic aerosol; United States; urban area; wind; Great Lakes [North America]; Great Lakes [North America]; Illinois; Lake Michigan; United States
来源期刊	ATMOSPHERIC ENVIRONMENT
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/248841
作者单位	Department of Chemistry, University of Iowa, Iowa City, IA, United States; Department of Chemical and Biochemical Engineering, University of Iowa, Iowa City, IA, United States; Department of Chemistry, University of Wisconsin, Madison, WI, United States; Department of Soil, Water, and Climate, University of Minnesota, St. Paul, MN, United States; Wisconsin Department of Natural Resources, Madison, WI, United States; Space Science and Engineering Center, University of Wisconsin, Madison, WI, United States
推荐引用方式 GB/T 7714	Hughes D.D.,Christiansen M.B.,Milani A.,et al. PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study[J],2021,244.
APA	Hughes D.D..,Christiansen M.B..,Milani A..,Vermeuel M.P..,Novak G.A..,...&Stone E.A..(2021).PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study.ATMOSPHERIC ENVIRONMENT,244.
MLA	Hughes D.D.,et al."PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study".ATMOSPHERIC ENVIRONMENT 244(2021).