Organosulfates in cloud water above the Ozarks' isoprene source region

Pratt, Kerri A.; Fiddler, Marc N.; Shepson, P. B.; Carlton, Annmarie G.; Surratt, Jason D.

doi:10.1016/j.atmosenv.2013.05.011

Cited by 59 publications

(79 citation statements)

References 69 publications

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“…During wildfire influence, the cloud water showed evidence of aqueous SOA formation, including oligomer formation involving methylglyoxal Yasmeen et al, 2010) and aqueousphase reactions of syringol and guaiacol (Yu et al, 2014(Yu et al, , 2016. Monoterpene-derived organosulfates and organonitrates (Surratt et al, 2008) were observed in the cloud water during all air mass influences, similar to previous cloud water studies (Boone et al, 2015;Pratt et al, 2013). Notably, long-chain, alkane-derived organosulfates (Riva et al, 2016) were observed in cloud water when urban influence was present.…”

Section: Conclusion and Atmospheric Implicationssupporting

confidence: 70%

“…In the Amazon, Kourtchev et al (2016) previously found a similar subset of these unidentified CHOS compounds in SOA samples, suggesting a biogenic influence. Many organosulfates and nitrooxy-organosulfates, previously reported in laboratory studies, ambient aerosols, and cloud water as derived from monoterpene oxidation (Boone et al, 2015;Hamilton et al, 2013;Iinuma et al, 2007aIinuma et al, , b, 2009Kristensen et al, 2016;Kristensen and Glasius, 2011;Lin et al, 2012;Mazzoleni et al, 2012;Nguyen et al, 2012b;Nozière et al, 2010;O'Brien et al, 2014;Pratt et al, 2013;Stone et al, 2012;Surratt et al, 2008), were detected in the biogenic-influenced cloud water samples (Table 2), also consistent with monoterpene emissions along the air mass trajectories (Guenther et al, 2006). In this study, the required solid-phase extraction step precluded the detection of isoprene-derived organosulfates, which would have been removed prior to analysis.…”

Section: Biogenic Influencesupporting

confidence: 66%

“…Potential products of aqueous processing include carboxylic acids, esters, organosulfur compounds, polyols, amines, amino acids, and highly oxygenated oligomeric species (Blando and Turpin, 2000;Ervens et al, 2011). However, only limited ambient evidence of cloud processing involving high molecular weight organic compounds has been reported (Boone et al, 2015;Feng and Möller, 2004;Lee et al, 2011Lee et al, , 2012Pratt et al, 2013;Sagona et al, 2014;van Pinxteren et al, 2016;Zhao et al, 2013). A recent review found that more than 50 % of organic matter in fog and cloud water remains unspeciated (Herckes et al, 2013).…”

mentioning

confidence: 99%

“…Organosulfates are suggested to be formed from acidcatalyzed reactive uptake of epoxides onto sulfate aerosol (Surratt et al, 2010), as well as in-cloud radical-radical reactions involving sulfate radicals (Nozière et al, 2010;Perri et al, 2010;Schindelka et al, 2013). Isoprene-and monoterpene-derived organosulfates have been observed in cloud water over the southeastern US (Boone et al, 2015;Pratt et al, 2013). Modeling suggests that organosulfate formation most commonly occurs in aqueous aerosol rather than in cloud droplets (McNeill et al, 2012).…”

mentioning

confidence: 99%

“…Laboratory studies have shown the production of oligomers in bulk aqueous solutions from the photochemical oxidation of glyoxal, methylglyoxal, pyruvic acid, and methacrolein (Ervens et al, 2011). Oligomers have been observed in ambient cloud water (Boone et al, 2015;Pratt et al, 2013;Zhao et al, 2013); however, oligomer formation is expected to be favored in aqueous aerosol, compared to cloud droplets, due to increased self-reaction rates (Ervens et al, 2011). Yet, with few studies reporting the molecular composition of high molecular weight compounds, it is difficult to assess the potential importance of these aqueous-phase derived compounds and their impacts on SOA composition and wet deposition to ecosystems (Hallquist et al, 2009).…”

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confidence: 99%

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Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

Cook¹,

Lin²,

Peng³

et al. 2017

Atmos. Chem. Phys.

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Abstract. Organic aerosol formation and transformation occurs within aqueous aerosol and cloud droplets, yet little is known about the composition of high molecular weight organic compounds in cloud water. Cloud water samples collected at Whiteface Mountain, New York, during AugustSeptember 2014 were analyzed by ultra-high-resolution mass spectrometry to investigate the molecular composition of dissolved organic carbon, with a focus on sulfur-and nitrogen-containing compounds. Organic molecular composition was evaluated in the context of cloud water inorganic ion concentrations, pH, and total organic carbon concentrations to gain insights into the sources and aqueous-phase processes of the observed high molecular weight organic compounds. Cloud water acidity was positively correlated with the average oxygen : carbon ratio of the organic constituents, suggesting the possibility for aqueous acid-catalyzed (prior to cloud droplet activation or during/after cloud droplet evaporation) and/or radical (within cloud droplets) oxidation processes. Many tracer compounds recently identified in laboratory studies of bulk aqueous-phase reactions were identified in the cloud water. Organosulfate compounds, with both biogenic and anthropogenic volatile organic compound precursors, were detected for cloud water samples influenced by air masses that had traveled over forested and populated areas. Oxidation products of long-chain (C 10−12 ) alkane precursors were detected during urban influence. Influence of Canadian wildfires resulted in increased numbers of identified sulfur-containing compounds and oligomeric species, including those formed through aqueous-phase reactions involving methylglyoxal. Light-absorbing aqueous-phase products of syringol and guaiacol oxidation were observed in the wildfire-influenced samples, and dinitroaromatic compounds were observed in all cloud water samples (wildfire, biogenic, and urban-influenced). Overall, the cloud water molecular composition depended on air mass source influence and reflected aqueous-phase reactions involving biogenic, urban, and biomass burning precursors.

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Section: Conclusion and Atmospheric Implicationssupporting

confidence: 70%

Section: Biogenic Influencesupporting

confidence: 66%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

Cook¹,

Lin²,

Peng³

et al. 2017

Atmos. Chem. Phys.

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Airborne measurements of organosulfates over the continental U.S.

et al. 2015

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Organosulfates are important secondary organic aerosol (SOA) components and good tracers for aerosol heterogeneous reactions. However, the knowledge of their spatial distribution, formation conditions, and environmental impact is limited. In this study, we report two organosulfates, an isoprene-derived isoprene epoxydiols (IEPOX) (2,3-epoxy-2-methyl-1,4-butanediol) sulfate and a glycolic acid (GA) sulfate, measured using the NOAA Particle Analysis Laser Mass Spectrometer (PALMS) on board the NASA DC8 aircraft over the continental U.S. during the Deep Convective Clouds and Chemistry Experiment (DC3) and the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS). During these campaigns, IEPOX sulfate was estimated to account for 1.4% of submicron aerosol mass (or 2.2% of organic aerosol mass) on average near the ground in the southeast U.S., with lower concentrations in the western U.S. (0.2–0.4%) and at high altitudes (<0.2%). Compared to IEPOX sulfate, GA sulfate was more uniformly distributed, accounting for about 0.5% aerosol mass on average, and may be more abundant globally. A number of other organosulfates were detected; none were as abundant as these two. Ambient measurements confirmed that IEPOX sulfate is formed from isoprene oxidation and is a tracer for isoprene SOA formation. The organic precursors of GA sulfate may include glycolic acid and likely have both biogenic and anthropogenic sources. Higher aerosol acidity as measured by PALMS and relative humidity tend to promote IEPOX sulfate formation, and aerosol acidity largely drives in situ GA sulfate formation at high altitudes. This study suggests that the formation of aerosol organosulfates depends not only on the appropriate organic precursors but also on emissions of anthropogenic sulfur dioxide (SO2), which contributes to aerosol acidity.Key PointsIEPOX sulfate is an isoprene SOA tracer at acidic and low NO conditions Glycolic acid sulfate may be more abundant than IEPOX sulfate globally SO2 impacts IEPOX sulfate by increasing aerosol acidity and water uptake

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Surface and airborne measurements of organosulfur and methanesulfonate over the western United States and coastal areas

et al. 2015

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This study reports on ambient measurements of organosulfur (OS) and methanesulfonate (MSA) over the western United States and coastal areas. Particulate OS levels are highest in summertime, and generally increase as a function of sulfate (a precursor) and sodium (a marine tracer) with peak levels at coastal sites. The ratio of OS to total sulfur (TS) is also highest at coastal sites, with increasing values as a function of Normalized Difference Vegetation Index (NDVI) and the ratio of organic carbon to elemental carbon. Correlative analysis points to significant relationships between OS and biogenic emissions from marine and continental sources, factors that coincide with secondary production, and vanadium due to a suspected catalytic role. A major OS species, methanesulfonate (MSA), was examined with intensive field measurements and the resulting data support the case for vanadium’s catalytic influence. Mass size distributions reveal a dominant MSA peak between aerodynamic diameters of 0.32—0.56 μm at a desert and coastal site with nearly all MSA mass (≥ 84%) in sub-micrometer sizes; MSA:non-sea salt sulfate ratios vary widely as a function of particle size and proximity to the ocean. Airborne data indicate that relative to the marine boundary layer, particulate MSA levels are enhanced in urban and agricultural areas, and also the free troposphere when impacted by biomass burning. Some combination of fires and marine-derived emissions leads to higher MSA levels than either source alone. Finally, MSA differences in cloud water and out-of-cloud aerosol are discussed.

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Organosulfates in cloud water above the Ozarks' isoprene source region

Cited by 59 publications

References 69 publications

Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

Airborne measurements of organosulfates over the continental U.S.

Surface and airborne measurements of organosulfur and methanesulfonate over the western United States and coastal areas

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