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Source apportionment of organic carbon in Centreville, AL using organosulfates in organic tracer-based positive matrix factorization

Hettiyadura, Anusha P. S. and Xu, Lu and Jayarathne, Thilina and Skog, Kate and Guo, Hongyu and Weber, Rodney J. and Nenes, Athanasios and Keutsch, Frank N. and Ng, Nga Lee and Stone, Elizabeth A. (2018) Source apportionment of organic carbon in Centreville, AL using organosulfates in organic tracer-based positive matrix factorization. Atmospheric Environment, 186 . pp. 74-88. ISSN 1352-2310. https://resolver.caltech.edu/CaltechAUTHORS:20180711-160223298

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Abstract

Organic tracer-based positive matrix factorization (PMF) was used to apportion fine particulate (PM_(2.5)) organic carbon (OC) to its sources in Centreville, AL, USA, a rural forested site influenced by anthropogenic emissions, during the Southern Oxidant and Aerosol Study (SOAS) in the summer of 2013. Model inputs included organosulfates, a group of organic compounds that are tracers of anthropogenically-influenced biogenic secondary organic aerosols (SOA), as well as, OC, elemental carbon, water-soluble organic carbon, and other organic tracers for primary and secondary sources measured during day and night. The organic tracer-based PMF resolved eight factors that were identified as biomass burning (11%, average contribution to PM_(2.5) OC), vehicle emissions (8%), isoprene SOC formed under low-NO_x conditions (13%), isoprene SOC formed under high-NO_x conditions (11%), SOC formed by photochemical reactions (9%), oxidatively aged biogenic SOC (6%), sulfuric acid-influenced SOC (21%, that also includes isoprene and monoterpene SOC), and monoterpene SOC formed under high-NO_x conditions (21%). These results indicate that OC in Centreville during summer is mainly secondary in origin (81%). Fossil fuel combustion is the major source of NO_x, ozone, and sulfuric acid that play a key role in SOA formation in the southeastern US. Fossil fuel was found to influence 61–76% of OC through vehicle emissions and SOA formation. Together with prescribed burns, which were the major type of biomass burning during this study, the OC influenced by anthropogenic activities reached 87%. The organic tracer-based PMF results were further compared with two complementary source apportionment techniques: PMF factors resolved for submicron organic aerosols measured using aerosol mass spectrometry (AMS) by Xu et al. (2015a) in Centreville during SOAS; biomass burning organic aerosols (BBOA, 11% of OC), isoprene-derived organic aerosols (isoprene-OA, 20% of OC), more-oxidized oxygenated organic aerosols (MO-OOA, 34% of OC), and less-oxidized oxygenated organic aerosols (LO-OOA, 35% of OC); and PM_(2.5) OC apportioned by chemical-mass balance model (CMB), considering the same chemical species as this study, save for organosulfates; biomass burning (5%), diesel engines (2%), gasoline smokers (3%), vegetative detritus (1%), isoprene SOC (23%) and monoterpene SOC (34%), and other (likely biogenic secondary) sources (33%). Overall, this study indicates the primary and secondary sources resolved by the organic tracer-based PMF are in good agreement with CMB and AMS-PMF results, while the organic tracer-based PMF provides additional insight to the SOC formation pathways through the inclusion of organosulfates and other organic tracers measured during day and night.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.atmosenv.2018.05.007DOIArticle
ORCID:
AuthorORCID
Xu, Lu0000-0002-0021-9876
Nenes, Athanasios0000-0003-3873-9970
Ng, Nga Lee0000-0001-8460-4765
Additional Information:© 2018 Elsevier. Received 30 January 2018, Revised 27 April 2018, Accepted 7 May 2018, Available online 8 May 2018. The authors would like to thank E. Geddes, K. Richards, and T. Humphrey at the Truman State University for synthesizing standards of hydroxyacetone sulfate and glycolic acid sulfate; S. Staudt at the University of Wisconsin, Madison for synthesizing the lactic acid sulfate standard; J. D. Surratt, A. Gold and Z. Zhang at the University of North Carolina at Chapel Hill for providing 2-methyltetrol sulfate standard; L. Teesch and V. Parcell for their assistance in the University of Iowa High Resolution Mass Spectrometry Facility (HRMSF); J. Crounse, A. Teng, J. St. Clair, T. Nguyen (now at UC-Davis), and P. Wennberg from the California Institute of Technology for access to glycolaldehyde, hydroxyacetone, IEPOX, ISPOOH, and ISOPN measurements; K. F. Olson and A. H. Goldstein from the University of California, Berkeley, and A. Koss and J. A. de Gouw from the National Oceanic and Atmospheric Administration (NOAA) and the University of Colorado, Boulder, for access to isoprene, MACR, and MVK measurements; R. J. Wild (now at UIBK, Austria) and S. S. Brown from NOAA and the University of Colorado, Boulder, for access to ozone measurements; K. Baumann (now at UNC Department for Environmental Sciences and Engineering at Chapel Hill and MPI for Chemistry at Mainz, Germany) and E. Edgerton from the Atmospheric Research and Analysis for access to solar radiation, sulfate and BLH measurements; A. Carlton from Rutgers University (now at UC-Irvine), A. H. Goldstein from the University of California, Berkeley, J. Jimenez from the University of Colorado, Boulder, and A. Guenther from the National Center for Atmospheric Research (now at UC-Irvine) for organizing the SOAS component of the Southeast Atmosphere Study; and A. Charles at the department of Chemistry at the University of Iowa for copy editing. A. P. S. Hettiyadura, T. Jayarathne, and E. A. Stone were supported by the US Environmental Protection Agency (EPA) Science To Achieve Results (STAR) program (grant number 83540101). H. Guo, L. Xu, N. L. Ng, A. Nenes, and R. Weber were supported by the National Science Foundation (NSF) (grant number 1242258). L. Xu and N. L. Ng were also supported by the US EPA STAR program (grant number RD-83540301). K. Skog and F. N. Keutsch were supported by the NSF (grant numbers AGS-1247421 and 1628530). Data availability: The SOAS research data used in this publication are available at http://esrl.noaa.gov/csd/groups/csd7/measurements/2013senex/Ground/DataDownload Disclaimer: The content of this article is solely the response of the authors and do not necessarily represent the official views of the US EPA. Further, US EPA does not endorse the purchase of any commercial products or services mentioned in the publication.
Funders:
Funding AgencyGrant Number
Environmental Protection Agency (EPA)83540101
NSFAGS-1242258
Environmental Protection Agency (EPA)RD-83540301
NSFAGS-1247421
NSFAGS-1628530
Subject Keywords:PM2.5; Isoprene; Monoterpene; Primary; Secondary; Anthropogenic
Record Number:CaltechAUTHORS:20180711-160223298
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180711-160223298
Official Citation:Anusha P.S. Hettiyadura, Lu Xu, Thilina Jayarathne, Kate Skog, Hongyu Guo, Rodney J. Weber, Athanasios Nenes, Frank N. Keutsch, Nga Lee Ng, Elizabeth A. Stone, Source apportionment of organic carbon in Centreville, AL using organosulfates in organic tracer-based positive matrix factorization, Atmospheric Environment, Volume 186, 2018, Pages 74-88, ISSN 1352-2310, https://doi.org/10.1016/j.atmosenv.2018.05.007. (http://www.sciencedirect.com/science/article/pii/S1352231018303108)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:87781
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:12 Jul 2018 13:55
Last Modified:09 Mar 2020 13:19

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