Oxidation of SO2 by stabilized Criegee intermediate (sCI) radicals as a crucial source for atmospheric sulfuric acid concentrations

10314 11 33080 2 70811 document 33080 acp-13-3865-2013.pdf application/pdf 9991004be9ddaac5579c0c398eeb3c7e MD5 2283216 2016-02-19 12:38:04 https://pure.iiasa.ac.at/id/eprint/10314/1/acp-13-3865-2013.pdf 10314 1 1 application/pdf text en public

acp-13-3865-2013.pdf

published 33086 2 70821 document 33086 lightbox.jpg image/png 97414c77356df8982e20343a847b1ac8 MD5 57389 2016-02-19 12:38:38 https://pure.iiasa.ac.at/id/eprint/10314/2/lightbox.jpg 10314 2 2 image/png other Thumbnails conversion from text to thumbnail_lightbox en public

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http://eprints.org/relation/isVersionOf https://pure.iiasa.ac.at/id/document/33080 http://eprints.org/relation/isVolatileVersionOf https://pure.iiasa.ac.at/id/document/33080 http://eprints.org/relation/isIndexCodesVersionOf https://pure.iiasa.ac.at/id/document/33080 archive 351 disk0/00/01/03/14 2016-01-15 08:48:29 2021-08-27 17:23:07 2016-01-15 08:48:29 article show 1 Boy M. Mogensen D. Smolander S. Zhou L. AL1410 Nieminen T. Paasonen P. 8716 Oxidation of SO2 by stabilized Criegee intermediate (sCI) radicals as a crucial source for atmospheric sulfuric acid concentrations pub iis_env prog_mag prog_air 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, Hyytiaelae, 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 100m. 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. 2013-04 published European Geosciences Union (EGU) 10.5194/acp-13-3865-2013 XJ-13-233 Atmospheric Chemistry and Physics; 13(7):3865-3879 (April 2013) [doi:10.5194/acp-13-3865-2013] 2547 1493 public Atmospheric Chemistry and Physics 13 7 3865-3879 TRUE 1680-7324 FALSE info:eu-repo/semantics/article