Sources and formation processes of water‐soluble dicarboxylic acids, ω‐oxocarboxylic acids, α‐dicarbonyls, and major ions in summer aerosols from eastern central India

Deshmukh, Dhananjay K.; Kawamura, Kimitaka; Deb, Manas Kanti; Boreddy, Suresh K. R.

doi:10.1002/2016jd026246

Cited by 29 publications

(25 citation statements)

References 110 publications

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“…Tai are largely derived from O 3 and OH radical oxidation of BVOCs such as isoprene and α-pinene, while the nighttime oxalic acid and related SOA might be mostly produced by NO 3 radicals and other oxidizing agents such as H 2 O 2 (Claeys et al, 2004;Herrmann et al, 1999). In addition, the titration of O 3 by the residual NO in the nighttime atmosphere could also be responsible for the lack of correlation between BSOA tracers and O 3 (Edwards et al, 2017).…”

Section: Effects Of Temperature Relative Humidity and O 3 Concentratmentioning

confidence: 99%

Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

et al. 2018

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Abstract. Molecular distributions and stable carbon isotopic (δ13C values) compositions of dicarboxylic acids and related secondary organic aerosols (SOA) in PM2.5 aerosols collected on a day/night basis at the summit of Mt. Tai (1534 m a.s.l.) in the summer of 2016 were analyzed to investigate the sources and photochemical aging process of organic aerosols in the forested highland region of the North China Plain. The molecular distributions of dicarboxylic acids and related SOA are characterized by the dominance of oxalic acid (C2), followed by malonic (C3), succinic (C4) and azelaic (C9) acids. The concentration ratios of C2 ∕ C4, diacid-C ∕ OC and C2 ∕ total diacids are larger in the daytime than in the nighttime, suggesting that the daytime aerosols are more photochemically aged than those in the nighttime due to the higher temperature and stronger solar radiation. Both ratios of C2 ∕ C4 (R2>0.5) and C3 ∕ C4 (R2>0.5) correlated strongly with the ambient temperatures, indicating that SOA in the mountaintop atmosphere are mainly derived from the photochemical oxidation of local emissions rather than long-range transport. The mass ratios of azelaic acid to adipic acid (C9 ∕ C6), azelaic acid to phthalic aid (C9 ∕ Ph) and glyoxal to methylglyoxal (Gly ∕ mGly) and the strong linear correlations of major dicarboxylic acids and related SOA (i.e., C2, C3, C4, ωC2, Pyr, Gly and mGly) with biogenic precursors (SOA tracers derived from isoprene, α/β-pinene and β-caryophyllene) further suggest that aerosols in this region are mainly originated from biogenic sources (i.e., tree emissions). C2 concentrations correlated well with aerosol pH, indicating that particle acidity favors the organic acid formation. The stable carbon isotopic compositions (δ13C) of the dicarboxylic acids are higher in the daytime than in the nighttime, with the highest value (-16.5±1.9 ‰) found for C2 and the lowest value (-25.2±2.7 ‰) found for C9. An increase in δ13C values of C2 along with increases in C2 ∕ Gly and C2 ∕ mGly ratios was observed, largely due to the isotopic fractionation effect during the precursor oxidation process.

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Section: Effects Of Temperature Relative Humidity and O 3 Concentratmentioning

confidence: 99%

Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

et al. 2018

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“…On the other hand, more LWC would lead to increased pH due to dilution. For example, and Duporte et al (2016) found that OS formation decreased with higher RH, which was attributed to increased pH as a result of higher LWC (Duporte et al, 2016;Riva et al, 2016c).…”

Section: Introductionmentioning

confidence: 99%

The secondary formation of organosulfates under interactions between biogenic emissions and anthropogenic pollutants in summer in Beijing

Wang

Guo

et al. 2018

Atmos. Chem. Phys.

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Abstract. Organosulfates (OSs) with ambiguous formation mechanisms are a potential source of missing secondary organic aerosol (SOA) in current atmospheric models. In this study, we chemically characterized OSs and nitrooxy-OSs (NOSs) formed under the influence of biogenic emissions and anthropogenic pollutants (e.g., NOx, SO42−) in summer in Beijing. An ultrahigh-resolution mass spectrometer equipped with an electrospray ionization source was applied to examine the overall molecular composition of S-containing organics. The number and intensities of S-containing organics, the majority of which could be assigned as OSs and NOSs, increased significantly during pollution episodes, which indicated their importance for SOA accumulation. To further investigate the distribution and formation of OSs and NOSs, high-performance liquid chromatography coupled with mass spectrometry was employed to quantify 10 OSs and 3 NOS species. The total concentrations of quantified OSs and NOSs were 41.4 and 13.8 ng m−3, respectively. Glycolic acid sulfate was the most abundant species among all the quantified species, followed by monoterpene NOSs (C10H16NO7S−). The total concentration of three isoprene OSs was 14.8 ng m−3 and the isoprene OSs formed via the HO2 channel were higher than those formed via the NO ∕ NO2 channel. The OS concentration coincided with the increase in acidic sulfate aerosols, aerosol acidity, and liquid water content (LWC), indicating the acid-catalyzed aqueous-phase formation of OSs in the presence of acidic sulfate aerosols. When sulfate dominated the accumulation of secondary inorganic aerosols (SIAs; sulfate, nitrate, and ammonium; SO42− ∕ SIA > 0.5), OS formation would obviously be promoted as the increasing of acidic sulfate aerosols, aerosol LWC, and acidity (pH < 2.8). Otherwise, acid-catalyzed OS formation would be limited by lower aerosol acidity when nitrate dominated the SIA accumulation. The nighttime enhancement of monoterpene NOSs suggested their formation via the nighttime NO3-initiated oxidation of monoterpene under high-NOx conditions. However, isoprene NOSs are presumed to form via acid-catalyzed chemistry or reactive uptake of oxidation products of isoprene. This study provides direct observational evidence and highlights the secondary formation of OSs and NOSs via the interaction between biogenic precursors and anthropogenic pollutants (NOx, SO2, and SO42−). The results imply that future reduction in anthropogenic emissions can help to reduce the biogenic SOA burden in Beijing or other areas impacted by both biogenic emissions and anthropogenic pollutants.

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“…(iv) Although still limited in their ability to provide direct proof, reports of size-resolved field measurements may miss out on the full story of an aqueous signature if only the submicrometer size range (e.g., droplet mode) is examined, as aqueous processing can influence the composition of aerosol in the coarse mode (e.g., Deshmukh et al, 2017).…”

Section: Caution In Characterizing Air Near Clouds To Detect the Cloumentioning

confidence: 99%

Is there an aerosol signature of cloud processing?

Ervens

Sorooshian

Aldhaif

et al. 2018

Preprint

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15The formation of sulfate and secondary organic aerosol mass in the aqueous phase (aqSOA) of cloud and fog droplets can significantly contribute to ambient aerosol mass. While tracer compounds give evidence that aqueous phase processing occurred, they do not reveal the extent to which particle properties have been modified in terms of mass, chemical composition, hygroscopicity and oxidation state.We analyse data from several field experiments and model studies for six air mass types (urban, biogenic, marine, 20 wild fire biomass burning, agricultural biomass burning and background air). We focus on the trends of changes in mass, hygroscopicity parameter , and oxygen-to-carbon (O/C) ratio due to cloud processing. We find that the modification of these parameters upon cloud-processing is most evident in urban, marine and biogenic air masses, i.e. air masses that are more polluted than very clean air (background air) but cleaner than heavily polluted plumes as encountered during biomass burning. Based on these trends, we suggest that the mass ratio (Rtot) of the potential 25 aerosol sulfate and aqSOA mass to the initial aerosol mass can be used to predict whether cloud processing will be detectable. Scenarios where this ratio exceeds Rtot ~ 2 are the most likely ones where clouds can significantly change aerosol parameters. Comparison to Rtot values as calculated for ambient data at different locations confirm the applicability of the concept to predict a cloud-processing signature in selected air masses.

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Sources and formation processes of water‐soluble dicarboxylic acids, ω‐oxocarboxylic acids, α‐dicarbonyls, and major ions in summer aerosols from eastern central India

Cited by 29 publications

References 110 publications

Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

The secondary formation of organosulfates under interactions between biogenic emissions and anthropogenic pollutants in summer in Beijing

Is there an aerosol signature of cloud processing?

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