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

Artikel i vetenskaplig tidskrift
Författare Y. J. Wang
M. Hu
S. Guo
Y. C. Wang
J. Zheng
Y. D. Yang
W. F. Zhu
R. Z. Tang
X. Li
Y. Liu
Michael Le Breton
Z. F. Du
D. J. Shang
Y. S. Wu
Z. J. Wu
Y. Song
S. R. Lou
Mattias Hallquist
J. Z. Yu
Publicerad i Atmospheric Chemistry and Physics
Volym 18
Nummer/häfte 14
Sidor 10693-10713
ISSN 1680-7316
Publiceringsår 2018
Publicerad vid Institutionen för kemi och molekylärbiologi
Sidor 10693-10713
Språk en
Länkar dx.doi.org/10.5194/acp-18-10693-201...
Ämnesord organic aerosol formation, southeastern united-states, isoprene-derived, organosulfates, resolution mass-spectrometry, 2013 southern oxidant, atmospheric aerosols, molecular characterization, particulate, organosulfates, ambient aerosol, chemical-characterization, Meteorology & Atmospheric Sciences
Ämneskategorier Miljökemi, Miljövetenskap, Geovetenskap och miljövetenskap, Spektroskopi, Organisk kemi, Fysikalisk kemi, Analytisk kemi, Kemi, Meteorologi och atmosfärforskning

Sammanfattning

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 aqueousphase 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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Utskriftsdatum: 2019-09-17