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Article Dans Une Revue Atmospheric Environment Année : 2000

A model for tropospheric multiphase chemistry: application to one cloudy event during the CIME experiment

Résumé

A multiphase box model for a remote environment of the troposphere has been developed with an explicit chemistry for both gas and aqueous phase. The model applied to a set of measurements performed by Voisin et al. (2000) during the European CIME experiment for a cloud event on 13th December 1997 at the top of the Puy de Dôme (France). The results of the simulation are compared to the measurements in order to follow the evolution of the ambient chemical composition as a function of the pH and of the varying water content. After verifying that the model retrieves the main features observed in the behavior of species in the cloud droplets, a detailed analysis of the simulated chemical regime is performed. It essentially discusses the sources and sinks of radical in aqueous phase, the relative importance of the oxidation pathways of volatile organic compounds by the main radicals and the conversion of S(IV) into S(VI) which seems to be influenced by the presence of peroxonitric acid, HNO4, in aqueous phase in the environmental conditions that are considered with low H2O2. These numerical results are then compared with the theoretical study from Herrmann et al. (2000), who proposed a slightly different mechanism, including C2 chemistry and transition metal chemistry whereas they neglect some reaction pathways, such as the one involving OHCH2O2 radical. This double confrontation between model results and both real experimental data and numerical results from Herrmann et al. (1999c) underlines limitations of such modeling approach that does not include any dynamical or microphysical coupling but also demonstrates its capability to identify the main oxidants or reactants in aqueous phase in real environmental conditions more realistic than a purely theoretical approach. The originality of this study resides in the explicit and exhaustive ways the chemical reactions are treated in aqueous phase and in a first attempt to compare such a detailed chemical scheme to real environmental conditions.
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Dates et versions

hal-01819409 , version 1 (01-09-2022)

Licence

Paternité - Pas d'utilisation commerciale - Pas de modification

Identifiants

Citer

Maud Leriche, Didier Voisin, Nadine Chaumerliac, Anne Monod, Bernard Aumont. A model for tropospheric multiphase chemistry: application to one cloudy event during the CIME experiment. Atmospheric Environment, 2000, 34 (29-30), pp.5015-5036. ⟨10.1016/S1352-2310(00)00329-0⟩. ⟨hal-01819409⟩
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