Preprints
https://doi.org/10.5194/acp-2021-1025
https://doi.org/10.5194/acp-2021-1025
 
12 Jan 2022
12 Jan 2022
Status: this preprint is currently under review for the journal ACP.

Modelling SO2 conversion into sulphates in the mid-troposphere with a 3D chemistry-transport model: the case of Mount Etna's eruption on April 12, 2012

Mathieu Lachatre1,a, Sylvain Mailler1,2, Laurent Menut1, Arineh Cholakian1, Pasquale Sellitto3, Guillaume Siour3, Henda Guermazi3, Giuseppe Salerno4, and Salvatore Giammanco4 Mathieu Lachatre et al.
  • 1LMD/IPSL, École Polytechnique, Institut Polytechnique de Paris, ENS, PSL Université, Sorbonne Université, CNRS, Palaiseau, France
  • 2École des Ponts, Université Paris-Est, 77455 Champs-sur-Marne, France
  • 3Univ Paris Est Creteil and Université de Paris, CNRS, LISA, F-94010 Créteil, France
  • 4Istituto Nazionale di Geofisica e Vulcanologia, Osservatorio Etneo, Catania, Italy
  • apresently at: ARIA is now SUEZ, 8-10 rue de la Ferme 92100 Boulogne-Billancourt France

Abstract. Volcanic activity is an important source of atmospheric sulphur dioxide (SO2), which, after conversion into sulphuric acid, induces impacts on, among others, rain acidity, human health, meteorology and the radiative balance of the atmosphere. This work focuses on the conversion of SO2 into sulphates (, S(+VI)) in the mid-tropospheric volcanic plume emitted by the explosive eruption of Mount Etna (Italy) on Apr. 12, 2012, using the CHIMERE chemistry-transport model. Since volcanic plume location and composition depend on several often poorly constrained parameters, using a chemistry-transport model allows us to study the sensitivity of SO2 oxidation to multiple aspects such as volcanic water emissions, transition metal emissions, plume diffusion and plume altitude. Our results show that in the mid-troposphere, two pathways contribute to sulphate production, the oxidation of SO2 by OH in the gaseous phase (70 %), and the aqueous oxidation by O2 catalyzed by Mn2+ and Fe3+ ions (25 %). The oxidation in aqueous phase is the faster process, but in the mid-troposphere, liquid water is scarce, therefore the relative share of gaseous oxidation can be important. After one day in the mid-troposphere, about 0.5 % of the volcanic SO2 was converted to sulphates through the gaseous process. Because of the nonlinear dependency of the kinetics in the aqueous phase to the amount of volcanic water emitted and on the availability of transition metals in the aqueous phase, several experiments have been designed to determine the prominence of different parameters. Our simulations show that during the short time that liquid water remains in the plume, around 0.4 % of sulphates manage to quickly enter the liquid phase. Sensitivity tests regarding the advection scheme have shown that this scheme must be chosen wisely, as dispersion will impact both oxidation pathways explained above.

Mathieu Lachatre et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-1025', Anonymous Referee #1, 22 Apr 2022
    • AC1: 'Reply on RC1', Mathieu Lachatre, 22 Apr 2022
  • RC2: 'Comment on acp-2021-1025', Anonymous Referee #2, 24 Jun 2022

Mathieu Lachatre et al.

Mathieu Lachatre et al.

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Short summary
In this study we have mostly evaluate the predominance of various pathways of volcanic SO2 conversion to sulphates. It was shown that if the main pathway of conversion was the gaseous oxydation with OH, although the liquid pathways was exepected to be predominant. These results are interesting for a better understanding of sulphates formation in the mid and upper troposphere, an important component to evaluate PM radiative forcing.
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