Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Lukács, H.; Gelencsér, András; Hoffer, András; Kiss, Gyula; Horváth, Krisztián; Hartyáni, Zsuzsanna

doi:10.5194/acp-9-231-2009

Cited by 86 publications

(69 citation statements)

References 41 publications

(48 reference statements)

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“…For the site of K-puszta, Hungary, and a 2003 summer period, which was very dry and warm (Ion et al, 2005), the calculations indicated that organosulfates could be responsible for 20% of the total PM 10 sulfur concentration and 30% of the PM 10 OM Surratt et al, 2008). Using a similar approach, it was estimated that organosulfates accounted for 6-14% of the total PM 2.5 sulfur concentration at the same site during summer 2006 (Lukács et al, 2009). …”

Section: Organosulfates and Nitrooxy Organosulfates From α-/β-Pinene Soamentioning

confidence: 77%

The formation, properties and impact of secondary organic aerosol: current and emerging issues

et al. 2009

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Abstract. Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.

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Section: Organosulfates and Nitrooxy Organosulfates From α-/β-Pinene Soamentioning

confidence: 77%

The formation, properties and impact of secondary organic aerosol: current and emerging issues

et al. 2009

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“…Although their prevalence in ambient aerosol remains unclear, further evidence for substantial OS contributions to SOA come from rainwater studies (21). Similar to ON, OS have been quantified as the difference between total particulate S and sulfate plus methylsulfonic acid (MSA); studies in rural Hungary estimated OS accounted for 6-14% of sulfate (22) and up to 30% of the total organic matter (23). OS fractions of this order would cause an error in the evaluation of acidity using nominally inorganic ions (24) and constitute a fraction of OA that is not accounted for in current models.…”

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confidence: 99%

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry

Farmer

Matsunaga

Docherty

et al. 2010

Proc. Natl. Acad. Sci. U.S.A.

527

562

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Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ONnitrogen appears as NO þ x ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using NO þ x fragment ratios, organonitrogen ions, HNO þ 3 ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species.atmospheric chemistry | organic aerosol | organic nitrate | organic sulfate | SOA O rganonitrates (ON, i.e., RONO 2 ) and organosulfates (OS, i.e., ROSO 3 H) are known to be present in secondary organic aerosol (SOA) (1-4), and are a nearly unexplored but potentially important aspect of atmospheric chemistry. The mechanisms behind ON and OS production and aging are poorly understood and generally ignored in models due in part to a lack of measurement approaches. ON have recently been identified as significant components (15-35%) of NO y in the gas-phase (5, 6) and serve as indicators of ozone production (7). Oceans and certain industrial processes directly emit ON, but these are generally short-chain alkyl nitrates that exist only in the gas-phase and constitute a minor fraction of atmospheric ON (6,8). Most atmospheric ON are produced either by photochemical (OH-initiated) or nocturnal (NO 3 -initiated) oxidation reactions of anthropogenic and biogenic volatile organic compounds (VOCs). These reactions can produce large, multifunctional ON with vapor pressures potentially low enough to condense and form SOA. During photochemical oxidation of VOCs in the presence of nitrogen oxides, ON are minor products of peroxy radical ðRO 2 Þ þ NO reactions. These reactions produce ON with yields of ...

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“…Moreover, methanesulfonic acid (MSA) was found at the forest site, and its possible sources are discussed. MSA is formed by the photooxidation of dimethylsulfide (DMS) and is typically found in marinebiologically influenced aerosols; measurements of MSA in terrestrial regions are limited (e.g., Lukács et al, 2009). On the basis of these data sets, we discuss the relative importance of the forest floor in WSOC formation at a deciduous forest site.…”

Section: Introductionmentioning

confidence: 99%

Seasonal variations of stable carbon isotopic composition and biogenic tracer compounds of water-soluble organic aerosols in a deciduous forest

et al. 2012

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Abstract. To investigate the seasonal changes in biogenic water-soluble organic carbon (WSOC) aerosols in a boreal forest, aerosol samples were collected continuously in the canopy of a deciduous forest in northern Japan during 2009–2010. Stable carbon isotopic composition of WSOC (δ13CWSOC) in total suspended particulate matter (TSP) exhibited a distinct seasonal cycle, with lower values from June through September (−25.5±0.5 ‰). This cycle follows the net CO2 exchange between the forest ecosystem and the atmosphere, indicating that δ13CWSOC likely reflects the biological activity at the forest site. WSOC concentrations showed the highest values in early summer and autumn. Positive matrix factorization (PMF) analysis indicated that the factor in which biogenic secondary organic aerosols (BSOAs) dominated accounted for ~40 % of the highest concentrations of WSOC, where BSOAs mostly consisted of α-/β-pinene SOA. In addition, primary biological aerosol particles (PBAPs) made similar contributions (~57 %) to the WSOC near the forest floor in early summer. This finding indicates that the production of both primary and secondary WSOC aerosols is important during the growing season in a deciduous forest. The methanesulfonic acid (MSA) maximum was also found in early summer and had a distinct vertical gradient with larger concentrations near the forest floor. Together with the similar vertical gradients found for WSOC and δ13CWSOC as well as the α-/β-pinene SOA tracers, our results indicate that the forest floor, including ground vegetation and soil, acts as a significant source of WSOC in TSP within a forest canopy at the study site.

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Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Cited by 86 publications

References 41 publications

The formation, properties and impact of secondary organic aerosol: current and emerging issues

The formation, properties and impact of secondary organic aerosol: current and emerging issues

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry

Seasonal variations of stable carbon isotopic composition and biogenic tracer compounds of water-soluble organic aerosols in a deciduous forest

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