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https://doi.org/10.5194/acp-2020-484
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-484
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 10 Jun 2020

Submitted as: research article | 10 Jun 2020

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This preprint is currently under review for the journal ACP.

Kinetics of dimethyl sulfide (DMS) reactions with isoprene-derived Criegee intermediates studied with direct UV absorption

Mei-Tsan Kuo1, Isabelle Weber2,a, Christa Fittschen2, Luc Vereecken3,4, and Jim Jr-Min Lin1,5 Mei-Tsan Kuo et al.
  • 1Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan
  • 2Univ. Lille, CNRS, UMR 8522 – PC2A – Physicochimie des Processus de Combustion et de l'Atmosphère, F-59000 Lille, France
  • 3Max Planck Institute for Chemistry, Hahn-Meitner-Weg 1, 55128 Mainz, Germany
  • 4Institute for Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, 52428 Jülich, Germany
  • 5Department of Chemistry, National Taiwan University, Taipei 10617, Taiwan
  • apresent address: Department of Applied Chemistry and Institute of Molecular Science, National Chiao Tung University, Hsinchu 30010, Taiwan

Abstract. Criegee intermediates (CIs) are formed in the ozonolysis of unsaturated hydrocarbons and play a role in atmospheric chemistry as a non-photolytic OH source or a strong oxidant. Using a relative rate method in an ozonolysis experiment, Newland et al. (2015) reported high reactivity of isoprene-derived Criegee intermediates towards dimethyl sulfide (DMS) relative to that towards SO2 with the ratio of the rate coefficients kDMS+CI/kSO2+CI = 3.5 ± 1.8. Here we reinvestigated the kinetics of DMS reactions with two major Criegee intermediates formed in isoprene ozonolysis, CH2OO and methyl vinyl ketone oxide (MVKO). The individual CI was prepared following reported photolytic method with suitable (diiodo) precursors in the presence of O2. The concentration of CH2OO or MVKO was monitored directly in real time through their intense UV-visible absorption. Our results indicate the reactions of DMS with CH2OO and MVKO are both very slow; the upper limits of the rate coefficients are 4 orders of magnitude smaller than that reported by Newland et al. These results suggest that the ozonolysis experiment could be complicated such that interpretation should be careful and these CIs would not oxidize atmospheric DMS at any substantial level.

Mei-Tsan Kuo et al.

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Short summary
Dimethyl sulfide (DMS) is the major sulfur-containing species in the troposphere. Previous work by Newland et al. (2015) reported very high reactivity of isoprene-derived Criegee intermediates (CIs) towards DMS. By monitoring CIs with direct UV absorption, we found CI + DMS reactions are very slow, in contrast to the results of Newland et al., suggesting these CIs would not oxidize atmospheric DMS at any substantial level.
Dimethyl sulfide (DMS) is the major sulfur-containing species in the troposphere. Previous work...
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