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Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets

Hoyle, C. R. and Craven, J. and Flagan, R. C. (2016) Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets. Atmospheric Chemistry and Physics, 16 (3). pp. 1693-1712. ISSN 1680-7324. http://resolver.caltech.edu/CaltechAUTHORS:20160325-080400747

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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 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, super-cooled 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.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.5194/acp-16-1693-2016DOIArticle
http://www.atmos-chem-phys.net/16/1693/2016/PublisherArticle
ORCID:
AuthorORCID
Flagan, R. C.0000-0001-5690-770X
Additional Information:© 2016 Author(s). Published by Copernicus Publications on behalf of the European Geosciences Union. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 30 October 2015. Published in Atmos. Chem. Phys. Discuss.: 1 December 2015. Revised: 28 January 2016. Accepted: 29 January 2016. Published: 12 February 2016. We thank Martin Schnaiter for his assistance with the SIMONE and PPD-2K data interpretation. The PPD-2K was made available by funding from the Deutsche Forschungsgemeinschaft under grant SCHN 1140/2-1. C. R. Hoyle was supported by the Swiss National Science Foundation (SNSF) (grant number 200021_140663). T. B. Kristensen gratefully acknowledges funding from the German Federal Ministry of Education and Research (BMBF) through the CLOUD12 project. J. Craven received funding through the Dreyfus Award EP-11-117. N. M. Donahue received funding through US National Science Foundation Grants AGS-1447056 and AGS-1439551. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network “CLOUD-TRAIN” grant no. 316662, and the German Federal Ministry of Education and Research (project no. 01LK1222A and B). Edited by: V.-M. Kerminen.
Funders:
Funding AgencyGrant Number
Deutsche ForschungsgemeinschaftSCHN 1140/2-1
Swiss National Science Foundation (SNSF)200021_140663
German Federal Ministry of Education and Research (BMBF)UNSPECIFIED
Camille and Henry Dreyfus FoundationEP-11-117
NSFAGS-1447056
NSFAGS-1439551
Marie Curie Initial Training Network316662
German Federal Ministry of Education and Research01LK1222A
German Federal Ministry of Education and Research01LK1222B
Record Number:CaltechAUTHORS:20160325-080400747
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160325-080400747
Official Citation:Hoyle, C. R., Fuchs, C., Järvinen, E., Saathoff, H., Dias, A., El Haddad, I., Gysel, M., Coburn, S. C., Tröstl, J., Bernhammer, A.-K., Bianchi, F., Breitenlechner, M., Corbin, J. C., Craven, J., Donahue, N. M., Duplissy, J., Ehrhart, S., Frege, C., Gordon, H., Höppel, N., Heinritzi, M., Kristensen, T. B., Molteni, U., Nichman, L., Pinterich, T., Prévôt, A. S. H., Simon, M., Slowik, J. G., Steiner, G., Tomé, A., Vogel, A. L., Volkamer, R., Wagner, A. C., Wagner, R., Wexler, A. S., Williamson, C., Winkler, P. M., Yan, C., Amorim, A., Dommen, J., Curtius, J., Gallagher, M. W., Flagan, R. C., Hansel, A., Kirkby, J., Kulmala, M., Möhler, O., Stratmann, F., Worsnop, D. R., and Baltensperger, U.: Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets, Atmos. Chem. Phys., 16, 1693-1712, doi:10.5194/acp-16-1693-2016, 2016.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:65666
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:25 Mar 2016 15:32
Last Modified:25 Mar 2016 15:32

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