Atmos. Chem. Phys. Discuss., 5, 10369-10408, 2005
www.atmos-chem-phys-discuss.net/5/10369/2005/
doi:10.5194/acpd-5-10369-2005
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
The heterogeneous chemical kinetics of N2O5 on CaCO3 and other atmospheric mineral dust surrogates
F. Karagulian, C. Santschi, and M. J. Rossi
Ecole Polytechnique Fédérale de Lausanne, Laboratoire de Pollution Atmosphérique et Sol (EPFL, LPAS), Bâtiment CH H5, Station 6, CH-1015 Lausanne, Switzerland

Abstract. Uptake experiments of N2O5 on several mineral dust powder samples were carried out under continuous molecular flow conditions at 298±2 K. At [N2O5]0=(4.0±1.0)×1011 cm−3 we have found γss values ranging from (3.5±1.1)×10−2 for CaCO3 to (0.20±0.05) for Saharan Dust with γss decreasing as [N2O5]0 increased. We have observed delayed production of HNO3 upon uptake of N2O5 for every investigated sample owing to hydrolysis of N2O5 with surface-adsorbed H2O. At high and low [N2O5] Arizona Test Dust and Kaolinite turned out to be the samples to produce the largest amount of gas phase HNO3 with respect to N2O5 taken up. In contrast, the yield of HNO3 for Saharan Dust and CaCO3 are lower. On CaCO3 the disappearance of N2O5 was also accompanied by the formation of CO2. For CaCO3 sample masses ranging from 0.33 to 2.0 g, the yield of CO2 was approximately 42–50% with respect to the total number of N2O5 molecules taken up. The reaction of N2O5 with mineral dust and the subsequent production of gas phase HNO3 leads to a decrease in [NOx] which may have a significant effect on global ozone.

Citation: Karagulian, F., Santschi, C., and Rossi, M. J.: The heterogeneous chemical kinetics of N2O5 on CaCO3 and other atmospheric mineral dust surrogates, Atmos. Chem. Phys. Discuss., 5, 10369-10408, doi:10.5194/acpd-5-10369-2005, 2005.
 
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