Air-Snow exchanges of aldehydes in the Arctic
Snow is a complex multiphase chemical reactor that exchanges many reactive species with the atmosphere. One consequence of such emissions is that snow dramatically impacts the composition and the reactivity of polar the atmosphere. Carbonyl compounds, including aldehydes, are some of theses notewort...
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Other Authors: | , , , , , |
Format: | Doctoral or Postdoctoral Thesis |
Language: | French |
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HAL CCSD
2011
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Online Access: | https://tel.archives-ouvertes.fr/tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978/document https://tel.archives-ouvertes.fr/tel-00609978/file/Barret_ThA_se_Finale-avec-merci.pdf |
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ftccsdartic:oai:HAL:tel-00609978v1 |
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record_format |
openpolar |
institution |
Open Polar |
collection |
Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
op_collection_id |
ftccsdartic |
language |
French |
topic |
Photochemistry Diffusion Phase diagram Carbonyls Composés carbonylés Solution solide Diagramme de phase Photochimie [SDU.STU]Sciences of the Universe [physics]/Earth Sciences |
spellingShingle |
Photochemistry Diffusion Phase diagram Carbonyls Composés carbonylés Solution solide Diagramme de phase Photochimie [SDU.STU]Sciences of the Universe [physics]/Earth Sciences Barret, Manuel Air-Snow exchanges of aldehydes in the Arctic |
topic_facet |
Photochemistry Diffusion Phase diagram Carbonyls Composés carbonylés Solution solide Diagramme de phase Photochimie [SDU.STU]Sciences of the Universe [physics]/Earth Sciences |
description |
Snow is a complex multiphase chemical reactor that exchanges many reactive species with the atmosphere. One consequence of such emissions is that snow dramatically impacts the composition and the reactivity of polar the atmosphere. Carbonyl compounds, including aldehydes, are some of theses noteworthy species emitted by the snowpack. Here, we focus on aldehydes whose photolysis can yield significant amounts of HOx radicals. The knowledge of processes involved in air-snow exchanges is therefore required to understand how snow impacts the oxidative capacity of polar atmospheres. A major part of our work is focused on formaldehyde (HCHO), the most abundant aldehyde in the atmosphere. We first performed an experimental study to measure both the solubility and the diffusivity of HCHO in ice. Our results confirm that the formation of a solid-solution is the process of incorporation of HCHO into snow. We also performed a reanalysis of existing data on the solubility of HCHO in liquid water solutions. Our work made it possible to construct the partial pressure – temperature phase diagram for the H2O-HCHO system. To investigate the processes involved in air-snow exchanges of aldehydes, we monitored their concentration in snow during the OASIS 2009 field campaign which took place at Barrow, Alaska. Our measures were complemented by the monitoring of the snow physical properties and by the measurement of formaldehyde concentration in the gas phase. We developed a numerical code to model HCHO diffusion in and out of ice crystals and showed that it was possible to quantitatively reproduce snow concentrations by considering the equilibration of the H2O-HCHO by solid solution in ice. Our work also focused on other aldehydes that can potentially impact the atmospheric oxidative capacity. Improvements to our analytical method made it possible to measure not only formaldehyde and acetaldehyde, but also glyoxal, methylglyoxal and hydroxyacetaldehyde. This method deployed during the OASIS campaign provided the first measurements of ... |
author2 |
Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG) Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS) Université de Grenoble Florent Dominé Stéphan Houdier |
format |
Doctoral or Postdoctoral Thesis |
author |
Barret, Manuel |
author_facet |
Barret, Manuel |
author_sort |
Barret, Manuel |
title |
Air-Snow exchanges of aldehydes in the Arctic |
title_short |
Air-Snow exchanges of aldehydes in the Arctic |
title_full |
Air-Snow exchanges of aldehydes in the Arctic |
title_fullStr |
Air-Snow exchanges of aldehydes in the Arctic |
title_full_unstemmed |
Air-Snow exchanges of aldehydes in the Arctic |
title_sort |
air-snow exchanges of aldehydes in the arctic |
publisher |
HAL CCSD |
publishDate |
2011 |
url |
https://tel.archives-ouvertes.fr/tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978/document https://tel.archives-ouvertes.fr/tel-00609978/file/Barret_ThA_se_Finale-avec-merci.pdf |
geographic |
Arctic |
geographic_facet |
Arctic |
genre |
Arctic Arctique* Barrow Alaska |
genre_facet |
Arctic Arctique* Barrow Alaska |
op_source |
https://tel.archives-ouvertes.fr/tel-00609978 Sciences de la Terre. Université de Grenoble, 2011. Français. ⟨NNT : 2011GRENU019⟩ |
op_relation |
NNT: 2011GRENU019 tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978/document https://tel.archives-ouvertes.fr/tel-00609978/file/Barret_ThA_se_Finale-avec-merci.pdf |
op_rights |
info:eu-repo/semantics/OpenAccess |
_version_ |
1766348632036999168 |
spelling |
ftccsdartic:oai:HAL:tel-00609978v1 2023-05-15T15:18:26+02:00 Air-Snow exchanges of aldehydes in the Arctic Echanges Air-Neige d'aldéhydes en Arctique Barret, Manuel Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG) Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS) Université de Grenoble Florent Dominé Stéphan Houdier 2011-06-21 https://tel.archives-ouvertes.fr/tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978/document https://tel.archives-ouvertes.fr/tel-00609978/file/Barret_ThA_se_Finale-avec-merci.pdf fr fre HAL CCSD NNT: 2011GRENU019 tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978 https://tel.archives-ouvertes.fr/tel-00609978/document https://tel.archives-ouvertes.fr/tel-00609978/file/Barret_ThA_se_Finale-avec-merci.pdf info:eu-repo/semantics/OpenAccess https://tel.archives-ouvertes.fr/tel-00609978 Sciences de la Terre. Université de Grenoble, 2011. Français. ⟨NNT : 2011GRENU019⟩ Photochemistry Diffusion Phase diagram Carbonyls Composés carbonylés Solution solide Diagramme de phase Photochimie [SDU.STU]Sciences of the Universe [physics]/Earth Sciences info:eu-repo/semantics/doctoralThesis Theses 2011 ftccsdartic 2021-10-24T17:39:02Z Snow is a complex multiphase chemical reactor that exchanges many reactive species with the atmosphere. One consequence of such emissions is that snow dramatically impacts the composition and the reactivity of polar the atmosphere. Carbonyl compounds, including aldehydes, are some of theses noteworthy species emitted by the snowpack. Here, we focus on aldehydes whose photolysis can yield significant amounts of HOx radicals. The knowledge of processes involved in air-snow exchanges is therefore required to understand how snow impacts the oxidative capacity of polar atmospheres. A major part of our work is focused on formaldehyde (HCHO), the most abundant aldehyde in the atmosphere. We first performed an experimental study to measure both the solubility and the diffusivity of HCHO in ice. Our results confirm that the formation of a solid-solution is the process of incorporation of HCHO into snow. We also performed a reanalysis of existing data on the solubility of HCHO in liquid water solutions. Our work made it possible to construct the partial pressure – temperature phase diagram for the H2O-HCHO system. To investigate the processes involved in air-snow exchanges of aldehydes, we monitored their concentration in snow during the OASIS 2009 field campaign which took place at Barrow, Alaska. Our measures were complemented by the monitoring of the snow physical properties and by the measurement of formaldehyde concentration in the gas phase. We developed a numerical code to model HCHO diffusion in and out of ice crystals and showed that it was possible to quantitatively reproduce snow concentrations by considering the equilibration of the H2O-HCHO by solid solution in ice. Our work also focused on other aldehydes that can potentially impact the atmospheric oxidative capacity. Improvements to our analytical method made it possible to measure not only formaldehyde and acetaldehyde, but also glyoxal, methylglyoxal and hydroxyacetaldehyde. This method deployed during the OASIS campaign provided the first measurements of ... Doctoral or Postdoctoral Thesis Arctic Arctique* Barrow Alaska Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Arctic |