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Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets

Hoyle, C. R. ; Fuchs, C. ; Jarvinen, E. ; Saathoff, H. ; Dias, A. ; El Haddad, I. ; Gysel, M. ; Coburn, S. C. ; Trostl, J. and Hansel, A. , et al. (2016) In Atmospheric Chemistry and Physics 16(3). p.1693-1712
Abstract

The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and-10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion-pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that... (More)

The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and-10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion-pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and-10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, supercooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.

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published
in
Atmospheric Chemistry and Physics
volume
16
issue
3
pages
20 pages
publisher
Copernicus Gesellschaft mbH
external identifiers
  • scopus:84958279188
ISSN
1680-7316
DOI
10.5194/acp-16-1693-2016
language
English
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no
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be214b3d-340c-47c6-88da-8d98fc39a4e8
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2018-10-09 14:24:24
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2020-01-16 03:33:17
@article{be214b3d-340c-47c6-88da-8d98fc39a4e8,
  abstract     = {<p>The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and-10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion-pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and-10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO<sub>2</sub> in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, supercooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.</p>},
  author       = {Hoyle, C. R. and Fuchs, C. and Jarvinen, E. and Saathoff, H. and Dias, A. and El Haddad, I. and Gysel, M. and Coburn, S. C. and Trostl, J. and Hansel, A. and Bianchi, F. and Breitenlechner, M. and Corbin, J. C. and Craven, J. and Donahue, N. M. and Duplissy, J. and Ehrhart, S. and Frege, C. and Gordon, H. and Hoppel, N. and Heinritzi, M. and Kristensen, T. B. and Molteni, U. and Nichman, L. and Pinterich, T. and Prevôt, A. S.H. and Simon, M. and Slowik, J. G. and Steiner, G. and Tome, A. and Vogel, A. L. and Volkamer, R. and Wagner, A. C. and Wagner, R. and Wexler, A. S. and Williamson, C. and Winkler, P. M. and Yan, C. and Amorim, A. and Dommen, J. and Curtius, J. and Gallagher, M. W. and Flagan, R. C. and Hansel, A. and Kirkby, J. and Kulmala, M. and Mohler, O. and Stratmann, F. and Worsnop, D. R. and Baltensperger, U.},
  issn         = {1680-7316},
  language     = {eng},
  month        = {02},
  number       = {3},
  pages        = {1693--1712},
  publisher    = {Copernicus Gesellschaft mbH},
  series       = {Atmospheric Chemistry and Physics},
  title        = {Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets},
  url          = {http://dx.doi.org/10.5194/acp-16-1693-2016},
  doi          = {10.5194/acp-16-1693-2016},
  volume       = {16},
  year         = {2016},
}