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Discussion papers
https://doi.org/10.5194/acp-2018-1091
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1091
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 17 Oct 2018

Research article | 17 Oct 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2

David Au Yang1,2, Pierre Cartigny1, Karine Desboeufs3, and David Wîdory2 David Au Yang et al.
  • 1Laboratoire de Géochimie des Isotopes Stables, Institut de Physique du Globe de Paris, Université Paris Diderot, CNRS UMR 7154, Sorbonne Paris-Cité, 1 rue de Jussieu, 75005 Paris, France
  • 2GEOTOP/Université du Québec à Montreal, Montreal H3C 3P8, Canada
  • 3Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), UMR7583 CNRS, Université Paris 7 Denis Diderot, Université Paris-Est Créteil, Institut Pierre-Simon Laplace, Créteil, 94010, France

Abstract. Sulfates present in urban aerosols collected worldwide usually exhibit significant non-zero Δ33S signatures (from −0.6 to 0.5‰) whose origin still remains unclear. To better address this issue, we recorded the seasonal variations of the multiple sulfur isotope compositions of PM10 aerosols collected over the year 2013 at five stations within the Montreal Island (Canada), each characterized by distinct types and levels of pollution. The δ34S-values (n=155) vary from 2.0 to 11.3‰ (± 0.2‰, 2σ), the Δ33S-values from −0.080 to 0.341‰ (± 0.01‰, 2σ) and the Δ36S-values from −1.082 to 1.751‰ (± 0.2‰, 2σ). Our study evidences a seasonality for both the δ34S and Δ33S, which can be observed either when considering all monitoring stations or, to a lesser degree, when considering them individually. Among them, the monitoring station located at the most western end of the island, upstream of local emissions, yields the lowest mean δ34S coupled to the highest mean Δ33S-values. The Δ33S-values are higher during both summer and winter, and are <0.1‰ during both spring and autumn. As these higher Δ33S-values are measured in "upstream" aerosols, we conclude that the mechanism responsible for these highly positive S-MIF also occurs outside and not within the city, at odds with common assumptions. While the origin of such variability in the Δ33S-values of urban aerosols (i.e. −0.6 to 0.5‰) is still subject to debate, we suggest that oxidation by Criegee radicals and/or photooxidation of atmospheric SO2 in presence of mineral dust may play a role in generating such large ranges of S-MIF.

David Au Yang et al.
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David Au Yang et al.
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Short summary
Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two possible others oxidation pathways.
Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose...
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