Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012
<p>Volcanic activity is an important source of atmospheric sulfur dioxide (<span class="inline-formula">SO<sub>2</sub></span>), which, after conversion into sulfuric acid, induces impacts on rain acidity, human health, meteorology and the radiative balance of...
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2022-10-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/22/13861/2022/acp-22-13861-2022.pdf |
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| author | M. Lachatre M. Lachatre S. Mailler S. Mailler L. Menut A. Cholakian P. Sellitto P. Sellitto G. Siour H. Guermazi G. Salerno S. Giammanco |
| author_facet | M. Lachatre M. Lachatre S. Mailler S. Mailler L. Menut A. Cholakian P. Sellitto P. Sellitto G. Siour H. Guermazi G. Salerno S. Giammanco |
| author_sort | M. Lachatre |
| collection | DOAJ |
| description | <p>Volcanic activity is an important source of atmospheric sulfur dioxide (<span class="inline-formula">SO<sub>2</sub></span>), which, after conversion into sulfuric acid, induces impacts on rain acidity, human health, meteorology and the radiative balance of the atmosphere, among others. This work focuses on the conversion of <span class="inline-formula">SO<sub>2</sub></span> into sulfates (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M5" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msubsup><mi mathvariant="normal">SO</mi><mrow><mn mathvariant="normal">4</mn><mo>(</mo><mi mathvariant="normal">p</mi><mo>)</mo></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="32pt" height="19pt" class="svg-formula" dspmath="mathimg" md5hash="f4e7c7b964b267bf11d8b72059e023c8"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-13861-2022-ie00001.svg" width="32pt" height="19pt" src="acp-22-13861-2022-ie00001.png"/></svg:svg></span></span>, <span class="inline-formula">S(+VI)</span>) in the mid-tropospheric volcanic plume emitted by the explosive eruption of Mount Etna (Italy) on 12 April 2012, using the CHIMERE chemistry transport model. As the volcanic plume location and composition depend on several often poorly constrained parameters, using a chemistry transport model allows us to study the sensitivity of <span class="inline-formula">SO<sub>2</sub></span> oxidation to multiple aspects, such as volcanic water emissions, transition metal emissions, plume diffusion and plume altitude. Our results show that two pathways contribute to sulfate production in the mid-troposphere: (1) the oxidation of <span class="inline-formula">SO<sub>2</sub></span> by <span class="inline-formula">OH</span> in the gaseous phase (70 %) and (2) aqueous oxidation by <span class="inline-formula">O<sub>2</sub></span> catalysed by <span class="inline-formula">Mn<sup>2+</sup></span> and <span class="inline-formula">Fe<sup>3+</sup></span> ions (25 %). Oxidation in the aqueous phase is the faster process, but liquid water is scarce in the mid-troposphere; therefore, the relative share of gaseous oxidation can be important. After 1 d in the mid-troposphere, about 0.5 % of the volcanic <span class="inline-formula">SO<sub>2</sub></span> was converted to sulfates via the gaseous process. Because of the nonlinear dependency of the kinetics in the aqueous phase on 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 sulfates 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 of the oxidation pathways explained above.</p> |
| first_indexed | 2024-04-11T08:24:02Z |
| format | Article |
| id | doaj.art-e89b6ae97ade492fb1a2602e9d4cee27 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-04-11T08:24:02Z |
| publishDate | 2022-10-01 |
| publisher | Copernicus Publications |
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| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-e89b6ae97ade492fb1a2602e9d4cee272022-12-22T04:34:49ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242022-10-0122138611387910.5194/acp-22-13861-2022Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012M. Lachatre0M. Lachatre1S. Mailler2S. Mailler3L. Menut4A. Cholakian5P. Sellitto6P. Sellitto7G. Siour8H. Guermazi9G. Salerno10S. Giammanco11LMD/IPSL, École Polytechnique, Institut Polytechnique de Paris, ENS, PSL Université, Sorbonne Université, CNRS, 91120 Palaiseau, Francecurrently at: ARIA is now SUEZ, 8-10 rue de la Ferme, 92100 Boulogne-Billancourt, FranceLMD/IPSL, École Polytechnique, Institut Polytechnique de Paris, ENS, PSL Université, Sorbonne Université, CNRS, 91120 Palaiseau, FranceÉcole des Ponts, Université Paris-Est, 77455 Champs-sur-Marne, FranceLMD/IPSL, École Polytechnique, Institut Polytechnique de Paris, ENS, PSL Université, Sorbonne Université, CNRS, 91120 Palaiseau, FranceLMD/IPSL, École Polytechnique, Institut Polytechnique de Paris, ENS, PSL Université, Sorbonne Université, CNRS, 91120 Palaiseau, FranceUniv Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, FranceIstituto Nazionale di Geofisica e Vulcanologia, Osservatorio Etneo, 95125 Catania, ItalyUniv Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, FranceUniv Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, FranceIstituto Nazionale di Geofisica e Vulcanologia, Osservatorio Etneo, 95125 Catania, ItalyIstituto Nazionale di Geofisica e Vulcanologia, Osservatorio Etneo, 95125 Catania, Italy<p>Volcanic activity is an important source of atmospheric sulfur dioxide (<span class="inline-formula">SO<sub>2</sub></span>), which, after conversion into sulfuric acid, induces impacts on rain acidity, human health, meteorology and the radiative balance of the atmosphere, among others. This work focuses on the conversion of <span class="inline-formula">SO<sub>2</sub></span> into sulfates (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M5" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msubsup><mi mathvariant="normal">SO</mi><mrow><mn mathvariant="normal">4</mn><mo>(</mo><mi mathvariant="normal">p</mi><mo>)</mo></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="32pt" height="19pt" class="svg-formula" dspmath="mathimg" md5hash="f4e7c7b964b267bf11d8b72059e023c8"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-13861-2022-ie00001.svg" width="32pt" height="19pt" src="acp-22-13861-2022-ie00001.png"/></svg:svg></span></span>, <span class="inline-formula">S(+VI)</span>) in the mid-tropospheric volcanic plume emitted by the explosive eruption of Mount Etna (Italy) on 12 April 2012, using the CHIMERE chemistry transport model. As the volcanic plume location and composition depend on several often poorly constrained parameters, using a chemistry transport model allows us to study the sensitivity of <span class="inline-formula">SO<sub>2</sub></span> oxidation to multiple aspects, such as volcanic water emissions, transition metal emissions, plume diffusion and plume altitude. Our results show that two pathways contribute to sulfate production in the mid-troposphere: (1) the oxidation of <span class="inline-formula">SO<sub>2</sub></span> by <span class="inline-formula">OH</span> in the gaseous phase (70 %) and (2) aqueous oxidation by <span class="inline-formula">O<sub>2</sub></span> catalysed by <span class="inline-formula">Mn<sup>2+</sup></span> and <span class="inline-formula">Fe<sup>3+</sup></span> ions (25 %). Oxidation in the aqueous phase is the faster process, but liquid water is scarce in the mid-troposphere; therefore, the relative share of gaseous oxidation can be important. After 1 d in the mid-troposphere, about 0.5 % of the volcanic <span class="inline-formula">SO<sub>2</sub></span> was converted to sulfates via the gaseous process. Because of the nonlinear dependency of the kinetics in the aqueous phase on 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 sulfates 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 of the oxidation pathways explained above.</p>https://acp.copernicus.org/articles/22/13861/2022/acp-22-13861-2022.pdf |
| spellingShingle | M. Lachatre M. Lachatre S. Mailler S. Mailler L. Menut A. Cholakian P. Sellitto P. Sellitto G. Siour H. Guermazi G. Salerno S. Giammanco Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 Atmospheric Chemistry and Physics |
| title | Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 |
| title_full | Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 |
| title_fullStr | Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 |
| title_full_unstemmed | Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 |
| title_short | Modelling SO<sub>2</sub> conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012 |
| title_sort | modelling so sub 2 sub conversion into sulfates in the mid troposphere with a 3d chemistry transport model the case of mount etna s eruption on 12 april 2012 |
| url | https://acp.copernicus.org/articles/22/13861/2022/acp-22-13861-2022.pdf |
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