Seasonal variations of fine particulate organosulfates derived from biogenic and anthropogenic hydrocarbons in the mid-Atlantic United States

被引:37
作者
Meade, L. Edward [1 ]
Riva, Matthieu [2 ,3 ]
Blomberg, Max Z. [1 ]
Brock, Amanda K. [1 ]
Qualters, Elisa Marie [1 ]
Siejack, Richard A. [1 ]
Ramakrishnan, Kumar [1 ]
Surratt, Jason D. [2 ]
Kautzman, Kathryn E. [1 ]
机构
[1] Towson Univ, Dept Chem, 8000 York Rd, Towson, MD 21252 USA
[2] Univ North Carolina Chapel Hill, Gillings Sch Global Publ Hlth, Dept Environm Sci & Engn, Chapel Hill, NC 27599 USA
[3] Univ Helsinki, Dept Phys, POB 64, Helsinki 00014, Finland
关键词
Multiphase chemistry; Secondary organic aerosol; HYSPLIT; Acid-catalyzed chemistry; Filter sampling; SECONDARY ORGANIC AEROSOL; 2013 SOUTHERN OXIDANT; PEARL RIVER DELTA; ATMOSPHERIC AEROSOLS; BAY-BREEZE; MOLECULAR CHARACTERIZATION; CHEMICAL-COMPOSITION; ISOPRENE EPOXYDIOLS; MASS-SPECTROMETRY; SOA FORMATION;
D O I
10.1016/j.atmosenv.2016.09.028
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Organosulfates (OSs) are an important and ubiquitous class of organic compounds found in ambient fine particulate matter (PM2.5) that serves as markers for multiphase chemical processes leading to secondary organic aerosol (SOA) formation. In this study, high-volume filter sampling was implemented to collect PM2.5 samples during the August 2012 June 2013 time period in suburban Towson, MD. By utilizing ultra-performance liquid chromatography coupled with high-resolution quadrupole time-of-flight mass spectrometry employing an electrospray ionization source (UPLC/ESI-HR-QTOFMS), 58 OSs were characterized and quantified in PM2.5 collected across all seasons. The selection of the extraction solvent was also found to be important for OS characterization. Seasonal trends demonstrate that the atmospheric oxidation of biogenic volatile organic compounds (VOCs) dominates OS formation in early fall and spring, with substantial contributions from isoprene OS (similar to 15 ng/m(3)), and limonene and alpha-pinene OS (similar to 5 ng/m(3)). From November to March anthropogenic OSs, including polycyclic aromatic hydrocarbon (PAH)- and alkane-derived OSs recently characterized in laboratory-generated SOA, reached their highest levels averaging 4 ng/m(3). Nitrogen-containing OSs derived from terpene chemistry remain consistent over the sampling period averaging 2 ng/m(3) and do not demonstrate strong seasonal fluctuations. Correlations between the identified OSs and known organic acids that arise from either the atmospheric oxidation of biogenic or anthropogenic VOCs assist in source apportionment. Meteorological data coupled with air mass back-trajectory analyses using HYSPLIT provide insight into meteorological and transport conditions that promote the formation/occurrence of OSs within the mid-Atlantic U.S. region. (C) 2016 Elsevier Ltd. All rights reserved.
引用
收藏
页码:405 / 414
页数:10
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