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Discussion papers
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 28 Oct 2019

Submitted as: research article | 28 Oct 2019

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

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative ∆33S-reservoir of sulfate aerosols?

Isabelle Genot1,2, David Au Yang1,3, Erwan Martin2, Pierre Cartigny1, Erwann Legendre2,4, and Marc De Rafelis5 Isabelle Genot et al.
  • 1Institutde physique du globe de Paris, Universitéde Paris, CNRS, 75005 Paris, France
  • 2Sorbonne Université, CNRS-INSU, Institut des Sciences de la Terre de Paris, IsteP UMR7193 Paris, France
  • 3Department of Earth and Planetary Sciences, McGill University, Montréal, Canada
  • 4LATMOS-IPSL - Sorbonne Université-UniversitéVersailles St.-Quentin, Paris, France
  • 5GET, UniversitéPaul Sabatier, Toulouse, France

Abstract. To better understand the formation and the oxidation pathways leading to gypsum-forming “black crusts” and investigate their bearing on the whole atmospheric SO2 cycle, we measured the oxygen (δ17O, δ18O and ∆17O) and sulfur (δ33S, δ34S, δ36S, ∆33S and ∆36S) isotopic compositions of black crust sulfates sampled on carbonate building stones along a NW-SE cross-section in the Parisian basin. The δ18O and δ34S, ranging between 7.5 and 16.7 ± 0.5 ‰ (n = 27, 2σ) and between −2.6 and 13.9 ± 0.2 ‰ respectively, show anthropogenic SO2 as the main sulfur source (from 2 to 81 %, in average ~30 %) with host-rock sulfates making the complement. This is supported by ∆17O-values (up to 2.6 ‰, in average ~0.86 ‰), requiring > 60 % of atmospheric sulfates in black crusts. Both negative ∆33S-∆36S-values between −0.34 and 0.00 ± 0.01 ‰ and between −0.7 and −0.2 ± 0.2 ‰ respectively were measured in black crusts sulfates, that is typical of a magnetic isotope effect that would occur during the SO2 oxidation on the building stone, leading to 33S-depletion in black crust sulfates and subsequent 33S-enrichment in residual SO2. Given that sulfate aerosols have mostly ∆33S > 0 ‰ and no processes can yet explain this enrichment, resulting in a non-consistent S-budget, black crust sulfates could well represent the complementary negative ∆33S-reservoir of the sulfate aerosols solving the atmospheric SO2 budget.

Isabelle Genot et al.
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Isabelle Genot et al.
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Publications Copernicus
Short summary
Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using e.g. their isotope signatures (δ34S, ∆33S, ∆36S, δ18O and ∆17O). A striking observation is their ∆33S > 0 ‰, implying a missing reservoir in the atmospheric sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crusts sulfates (i.e. formed on carbonate walls), that must therefore result from distinct chemical pathway(s) than that for sulfate aerosols and may well represent this complementary reservoir.
Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied...