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Effects of humidity and fatty acid surfactants on the uptake of NO2 to NaCl : combined study of kinetics and surface analysis

Abstract : In this laboratory work we studied an important atmospheric process typical of polluted costal regions: the heterogeneous reaction of a gaseous pollutant of mainly anthropogenic origin, NO2, on NaCl(100), taken as a surrogate for marine aerosol. Evidence of the presence of a native organic coating on field-collected marine aerosol particles inspired us to investigate the effect of insoluble fatty acids on the heterogeneous removal reaction of NOx in the marine boundary layer. The originality of this work consists in coupling reactivity studies with high spatial resolution surface analysis. The surface is followed, before and after reaction, via Raman micro-spectrometry and AFM techniques. Significant modifications in the morphology and orientation of the formed NaNO3 crystals on the surface are found as a function of humidity during the reaction. A thin organic coating on the salt surface is prepared and characterized. The reactivity of the coated/uncoated salt is measured in a static reactor where the gaseous phase composition can be monitored by FTIR spectrometry in different humidities (RH=0-80%). From NO2 and ClNO kinetics we can independently estimate both the uptake (γ) and the reaction probability (φ) coefficients. The presence of a palmitic or oleic acid coating slightly hinders the reactivity, especially in some humidities. By coupling all experimental information to a simple reactivity model which fits the experimental data well, we can conclude that the NO2/NaCl reaction directly releases a precursor of active chlorine atoms (ClNO) into the atmosphere, even at high humidities.
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Submitted on : Tuesday, February 28, 2012 - 11:38:50 AM
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Sara Scolaro. Effects of humidity and fatty acid surfactants on the uptake of NO2 to NaCl : combined study of kinetics and surface analysis. Theoretical and/or physical chemistry. Université des Sciences et Technologie de Lille - Lille I, 2009. English. ⟨tel-00674517⟩

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