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| Titel |
Oxidation of SO2 by stabilized Criegee intermediate (sCI) radicals as a crucial source for atmospheric sulfuric acid concentrations |
| VerfasserIn |
M. Boy, D. Mogensen, S. Smolander, L. Zhou, T. Nieminen, P. Paasonen, C. Plass-Dülmer, M. Sipilä, T. Petäjä, L. Mauldin, H. Berresheim, M. Kulmala  |
| Medientyp |
Artikel
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| Sprache |
Englisch
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| ISSN |
1680-7316
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| Digitales Dokument |
URL |
| Erschienen |
In: Atmospheric Chemistry and Physics ; 13, no. 7 ; Nr. 13, no. 7 (2013-04-12), S.3865-3879 |
| Datensatznummer |
250018584
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| Publikation (Nr.) |
 copernicus.org/acp-13-3865-2013.pdf |
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| Zusammenfassung |
| The effect of increased reaction rates of stabilized Criegee
intermediates (sCIs) with SO2 to produce sulfuric acid is
investigated using data from two different locations, SMEAR II,
Hyytiälä, Finland, and Hohenpeissenberg, Germany. Results
from MALTE, a zero-dimensional model, show that using previous
values for the rate coefficients of sCI + SO2, the model
underestimates gas phase H2SO4 by up to a factor of two
when compared to measurements. Using the rate coefficients recently
calculated by Mauldin et al. (2012) increases sulfuric acid by
30–40%. Increasing the rate coefficient for formaldehyde oxide
(CH2OO) with SO2 according to the values recommended by
Welz et al. (2012) increases the H2SO4 yield by 3–6%.
Taken together, these increases
lead to the conclusion that, depending on their concentrations, the
reaction of stabilized Criegee intermediates with SO2 could
contribute as much as 33–46% to atmospheric sulfuric acid gas
phase concentrations at ground level. Using the SMEAR II data,
results from SOSA, a one-dimensional model, show that the contribution
from sCI reactions to sulfuric acid production is most important in
the canopy, where the concentrations of organic compounds are the
highest, but can have significant effects on sulfuric acid
concentrations up to 100 m. The recent findings that the
reaction of sCI + SO2 is much faster than previously thought
together with these results show that the inclusion of this new
oxidation mechanism could be crucial in regional as well as global
models. |
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