Grantee Research Project Results
Final Report: Sources and Radiative Properties of Organosulfates in the Atmosphere
EPA Grant Number: R835401Title: Sources and Radiative Properties of Organosulfates in the Atmosphere
Investigators: Stone, Elizabeth A
Institution: University of Iowa
EPA Project Officer: Chung, Serena
Project Period: April 1, 2013 through March 31, 2016
Project Amount: $300,000
RFA: Anthropogenic Influences on Organic Aerosol Formation and Regional Climate Implications (2012) RFA Text | Recipients Lists
Research Category: Air Quality and Air Toxics , Climate Change , Air , Early Career Awards
Objective:
This project focuses on the measurement of organosulfates in the 2013 Southern Oxidant & Aerosol Study (SOAS) with the aim of identifying the biogenic and anthropogenic emissions sources that lead to formation of organosulfates and understanding how mixtures of biogenic and anthropogenic emissions lead to secondary organic aerosol formation. Specific objectives include developing organosulfate standards, evaluating their climate-relevant properties, developing an accurate method for their quantification in ambient aerosol, detailed chemical characterization of ambient aerosol in Centreville, AL, during the Southeast Atmosphere Study (SAS), and apportionment of ambient particulate matter to its biogenic and/or anthropogenic sources.
Summary/Accomplishments (Outputs/Outcomes):
Within this project, we have developed an efficient method for the synthesis of organosulfates as high-purity potassium salts for use as organosulfate quantification standards (Hettiyadura, et al., 2015). With the newly developed organosulfate standards, an ultra-performance liquid chromatography (UPLC) and tandem mass spectrometry (MS/MS) method was developed and validated for the extraction, separation, identification, and quantification of atmospheric organosulfates in ambient aerosol (Hettiyadura, et al., 2015). This method now has been applied to more than 60 fine particle (PM2.5) samples collected in Centreville during SAS. The three most abundant species quantified—glycolic acid sulfate, lactic acid sulfate, and hydroxyacetone sulfate—accounted for <0.3% of organic carbon (OC) in PM2.5. Qualitative methods in MS/MS revealed strong signals for isoprene-derived organosulfates, particularly 2-methyltetrol sulfate.
The hygroscopic properties of organosulfate were evaluated for their hygroscopic water uptake as described by Estillore, et al. (2016). In contrast to ammonium sulfate, potassium salts of organosulfates showed gradual deliquescence with continuous growth in size upon hydration with growth factors ranging from 1.29-1.50. Consequently, organosulfate molecules are hygroscopic even at low relative humidity and are expected to extend the range of environmental conditions that water is taken up onto aerosol particles. Further, organosulfates have the ability to modify the water uptake of inorganic salts, like sodium chloride.
Complementary measurements of PM2.5, including OC, elemental carbon, water-soluble organic carbon, and molecular markers of primary and secondary aerosol sources have been completed. These measurements have supported a better understanding of the sources of brown carbon in the Southeastern United States (Washenfelder, et al., 2015) and aerosol composition at other SAS sites (Rattanavaraha, et al., 2016; Budisulistiorini, et al., 2015). These data have been used in preliminary source apportionment of OC using chemical mass balance (CMB) modeling, which indicates a very small role for primary sources relative to secondary sources.
Journal Articles on this Report : 8 Displayed | Download in RIS Format
| Other project views: | All 24 publications | 8 publications in selected types | All 8 journal articles |
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Budisulistiorini SH, Li X, Bairai ST, Renfro J, Liu Y, Liu YJ, McKinney KA, Martin ST, McNeill VF, Pye HOT, Nenes A, Neff ME, Stone EA, Mueller S, Knote C, Shaw SL, Zhang Z, Gold A, Surratt JD. Examining the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol formation during the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee ground site. Atmospheric Chemistry and Physics 2015;15(15):8871-8888. |
R835401 (2014) R835401 (Final) R835404 (2014) R835404 (2015) R835404 (Final) R835410 (2013) R835410 (2014) R835410 (2015) R835410 (Final) |
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Estillore AD, Hettiyadura AP, Qin Z, Leckrone E, Wombacher B, Humphry T, Stone EA, Grassian VH. Water uptake and hygroscopic growth of organosulfate aerosol. Environmental Science & Technology 2016;50(8):4259-4268. |
R835401 (Final) |
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Hettiyadura APS, Stone EA, Kundu S, Baker Z, Geddes E, Richards K, Humphry T. Determination of atmospheric organosulfates using HILIC chromatography with MS detection. Atmospheric Measurement Techniques 2015;8(6):2347-2358. |
R835401 (2014) R835401 (Final) |
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Hettiyadura APS, Jayarathne T, Baumann K, Goldstein AH, de Gouw JA, Koss A, Keutsch FN, Skog K, Stone EA. Qualitative and quantitative analysis of atmospheric organosulfates in Centreville, Alabama. Atmospheric Chemistry & Physics 2017;17(2):1343-1359. |
R835401 (Final) |
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Hettiyadura APS, Xu L, Jayarathne T, Skog K, Guo H, Weber RJ, Nenes A, Keutsch FN, Ng NL, Stone EA. Source apportionment of organic carbon in Centreville, AL using organosulfates in organic tracer-based positive matrix factorization. Atmospheric Environment 2018;186:74-88. |
R835401 (Final) R835403 (Final) |
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Rattanavaraha W, Chu K, Budisulistiorini SH, Riva M, Lin Y-H, Edgerton ES, Baumann K, Shaw SL, Guo H, King L, Weber RJ, Neff ME, Stone EA, Offenberg JH, Zhang Z, Gold A, Surratt JD. Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study. Atmospheric Chemistry and Physics 2016;16(8):4897-4914. |
R835401 (Final) R835404 (2014) R835404 (2015) R835404 (Final) R835410 (2013) |
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Washenfelder RA, Attwood AR, Brock CA, Guo H, Xu L, Weber RJ, Ng NL, Allen HM, Ayres BR, Baumann K, Cohen RC, Draper DC, Duffey KC, Edgerton E, Fry JL, Hu WW, Jimenez JL, Palm BB, Romer P, Stone EA, Wooldridge PJ, Brown SS. Biomass burning dominates brown carbon absorption in the rural southeastern United States. Geophysical Research Letters 2015;42(2):653-664. |
R835401 (2014) R835401 (Final) R835399 (2014) R835399 (Final) |
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Zhang J, Liu J, Ding X, He X, Zhang T, Zheng M, Choi M, Isaacman-VanWertz G, Yee L, Zhang H, Miztal P, Goldstein A, Guenther A, Budisulistiorini S, Surratt J, Stone E, Shrivastava M, Wu D, Yu J, Ying Q. New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling. NJP CLIMATE AND ATMOSPHERIC SCIENCE 2023;6(1):69 |
R835401 (Final) |
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Supplemental Keywords:
air quality, global climate, troposphere, analytical chemistry, Southern Oxidant & Aerosol Study, SOASRelevant Websites:
Stone Research Group at the University of Iowa Department of Chemistry ExitProgress and Final Reports:
Original AbstractThe perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.