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Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds

Publication ,  Journal Article
Lin, X; Chameides, WL
Published in: Journal of Atmospheric Chemistry
August 1, 1991

A one-dimensional, time-dependent model of the physics and chemistry of a warm stratiform cloud is used to study the possible impact of chemical inhomogeneity among cloud and raindrops on the oxidation of SO2 in clouds. The effects of chemical inhomogeneity are examined using two contrasting models: In Model 1 a bulk-solution parameterization is adopted which effectively treats all cloud and raindrops as if they are chemically homogeneous; in Model 2 we allow the cloud and raindrops to have a dichotomous distribution. The dichotomous distribution in Model 2 is simulated by assuming that the two groups of cloud droplets nucleate from two chemically distinct populations of condensation nuclei; one being acidic and the other being alkaline. While the two models yield essentially identical results when the ambient levels of H2O2 are greater than the ambient levels of SO2, the rate of conversion of SO2 to sulfuric acid and the amount of sulfate removed in the precipitation can be significantly enhanced in Model 2 over that of Model 1 under conditions of oxidant limitation (i.e., H2O2 < SO2). This enhancement is critically dependent upon the fraction of alkaline nuclei assumed to be present in Model 2 and arises from the rapid increase in the aqueous-phase reaction between O3+SIV at high pH. Our results suggest that cloud models which adopt a bulk-solution parameterization for cloud droplet chemistry, may underestimate the amount of in-cloud SO2 oxidation under oxidant-limited conditions. © 1991 Kluwer Academic Publishers.

Duke Scholars

Published In

Journal of Atmospheric Chemistry

DOI

EISSN

1573-0662

ISSN

0167-7764

Publication Date

August 1, 1991

Volume

13

Issue

2

Start / End Page

109 / 129

Related Subject Headings

  • Meteorology & Atmospheric Sciences
  • 0401 Atmospheric Sciences
  • 0399 Other Chemical Sciences
  • 0306 Physical Chemistry (incl. Structural)
 

Citation

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MLA
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Lin, X., & Chameides, W. L. (1991). Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds. Journal of Atmospheric Chemistry, 13(2), 109–129. https://doi.org/10.1007/BF00115969
Lin, X., and W. L. Chameides. “Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds.” Journal of Atmospheric Chemistry 13, no. 2 (August 1, 1991): 109–29. https://doi.org/10.1007/BF00115969.
Lin X, Chameides WL. Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds. Journal of Atmospheric Chemistry. 1991 Aug 1;13(2):109–29.
Lin, X., and W. L. Chameides. “Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds.” Journal of Atmospheric Chemistry, vol. 13, no. 2, Aug. 1991, pp. 109–29. Scopus, doi:10.1007/BF00115969.
Lin X, Chameides WL. Model studies of the impact of chemical inhomogeneity on SO2 oxidation in warm stratiform clouds. Journal of Atmospheric Chemistry. 1991 Aug 1;13(2):109–129.
Journal cover image

Published In

Journal of Atmospheric Chemistry

DOI

EISSN

1573-0662

ISSN

0167-7764

Publication Date

August 1, 1991

Volume

13

Issue

2

Start / End Page

109 / 129

Related Subject Headings

  • Meteorology & Atmospheric Sciences
  • 0401 Atmospheric Sciences
  • 0399 Other Chemical Sciences
  • 0306 Physical Chemistry (incl. Structural)