qualitative and quantitative analysis of atmospheric organosulfates in centreville, alabama
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2017
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Abstract
Organosulfates are components of secondary organic aerosols (SOA) that form
from oxidation of volatile organic compounds (VOCs) in the presence of
sulfate. In this study, the composition and abundance of organosulfates were
determined in fine particulate matter (PM2.5) collected from
Centreville, AL, during the Southern Oxidant and Aerosol Study (SOAS) in
summer 2013. Six organosulfates were quantified using hydrophilic interaction
liquid chromatography (HILIC) with triple quadrupole mass spectrometry (TQD)
against authentic standards. Among these, the three most abundant species
were glycolic acid sulfate (0.5–52.5 ng m−3), lactic acid sulfate
(0.5–36.7 ng m−3), and hydroxyacetone sulfate
(0.5–14.3 ng m−3). These three species were strongly
inter-correlated, suggesting similar precursors and/or formation pathways.
Further correlations with sulfate, isoprene, and isoprene oxidation products
indicate important roles for these precursors in organosulfate formation in
Centreville. Positive filter sampling artifacts associated with these
organosulfates due to gas adsorption or reaction of gas phase precursors of
organosulfates with sulfuric acid were assessed for a subset of samples and
were less than 7.8 % of their PM2.5 concentrations. Together, the
quantified organosulfates accounted for < 0.3 % of organic carbon mass
in PM2.5. To gain insights into other organosulfates in PM2.5
collected from Centreville, semi-quantitative analysis was employed by way of
monitoring characteristic product ions of organosulfates (HSO4− at
m∕z 97 and SO4− ⋅ at m∕z 96) and evaluating relative signal
strength by HILIC–TQD. Molecular formulas of organosulfates were determined
by high-resolution time-of-flight (TOF) mass spectrometry. The major
organosulfate signal across all samples corresponded to 2-methyltetrol
sulfates, which accounted for 42–62 % of the total bisulfate ion signal.
Conversely, glycolic acid sulfate, the most abundant organosulfate quantified
in this study, was 0.13–0.57 % of the total bisulfate ion signal.
Precursors of m∕z 96 mainly consisted of nitro-oxy organosulfates.
Organosulfates identified were mainly associated with biogenic VOC
precursors, particularly isoprene and to a lesser extent monoterpenes and
2-methyl-3-buten-2-ol (MBO). While a small number of molecules dominated the
total organosulfate signal, a large number of minor species were also
present. This study provides insights into the major organosulfate species in
the southeastern US, as measured by tandem mass spectrometry that should
be targets for future standard
development and quantitative analysis.
| Reference Key |
hettiyadura2017atmosphericqualitative
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|---|---|
| Authors | ;A. P. S. Hettiyadura;T. Jayarathne;K. Baumann;A. H. Goldstein;J. A. de Gouw;A. Koss;F. N. Keutsch;K. Skog;E. A. Stone |
| Journal | Journal of agricultural and food chemistry |
| Year | 2017 |
| DOI |
10.5194/acp-17-1343-2017
|
| URL | |
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