Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets

  • 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.

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Author:Christopher Robert Hoyle, Claudia Fuchs, Emma Järvinen, Harald Saathoff, Antonio Dias, Imad El HaddadORCiDGND, Martin Gysel, Sean C. Coburn, Jasmin Tröstl, Anne-Kathrin Bernhammer, Federico BianchiORCiDGND, Martin BreitenlechnerORCiD, Joel C. Corbin, Jill Craven, Neil McPherson DonahueORCiDGND, Jonathan DuplissyORCiD, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Niko Florian Höppel, Martin HeinritziORCiDGND, Thomas Bjerring Kristensen, Ugo Molteni, Leonid Nichman, Tamara Pinterich, André Stephan Henry Prévôt, Mario SimonORCiD, Jay G. Slowik, Gerhard Steiner, Antonio Tomé, Alexander L. VogelORCiDGND, Rainer VolkamerORCiDGND, Andrea Christine WagnerGND, Robert WagnerORCiDGND, Anthony S. Wexler, Christina Williamson, Paul M. WinklerORCiD, Chao Yan, Antonio AmorimORCiD, Josef Dommen, Joachim CurtiusORCiD, Martin William Gallagher, Richard C. FlaganORCiD, Armin HanselORCiD, Jasper KirkbyORCiD, Markku KulmalaORCiDGND, Ottmar MöhlerORCiDGND, Frank StratmannORCiDGND, Douglas R. WorsnopORCiD, Urs BaltenspergerORCiDGND
Parent Title (English):Atmospheric chemistry and physics
Publisher:European Geosciences Union
Place of publication:Katlenburg-Lindau
Document Type:Article
Date of Publication (online):2016/02/12
Date of first Publication:2016/02/12
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2016/06/14
Page Number:20
First Page:1693
Last Page:1712
Institutes:Geowissenschaften / Geographie / Geowissenschaften
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 55 Geowissenschaften, Geologie / 550 Geowissenschaften
Licence (German):License LogoCreative Commons - Namensnennung 4.0