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A computer modelling study of the chemistry occurring during cloud formation over hills
Institution:1. Schrodinger Inc., 120 W 45th Street, New York, NY 10036, USA;2. Department of Chemistry, Columbia University, 3000 Broadway, MC 3178, New York, NY 10027, USA;1. Research Group Electrochemical and Surface Engineering (SURF), Vrije Universiteit Brussel, Pleinlaan 2, Brussels 1050, Belgium;2. Applied Electrochemistry & Catalysis (ELCAT), University of Antwerp, Universiteitsplein 1, Wilrijk 2610, Belgium;3. Laboratory of Biophysics and Biomedical Physics (BIMEF), University of Antwerp, Universiteitsplein 1, Wilrijk 2610, Belgium;4. Chemistry of Surfaces, Interfaces and Nanomaterials (CHEMSIN), Université Libre de Bruxelles, Boulevard du Triomphe, Brussels 1050, Belgium
Abstract:A model has been developed which describes the chemical processes occurring during the formation of hill cloud. This model has been applied to the study of four cases which should be typical of the chemical conditions which can exist during the formation of such cloud over hills in the N of England.The results show that a wide range of chemical behaviour is possible in cloud droplets, depending on the history of the airmass. The composition of the water-soluble aerosol is of importance in determining the chemical composition of cloud droplets, with most of the sulphate and large proportions of the other ions being derived from this source. Gas-phase chemistry is also important, not only because it dictates the initial concentrations of oxidants such as H2O2 and O3 and of acidic gases such as HNO3 at the onset of condensation, but also because of the chemical processes which occur concurrently with those in clouds. These are important sources of radicals, as well as of nitric acid, which continue to dissolve in solution. Gasphase HCl, HNO3 and NH3 are all of primary importance in describing the acidity of cloud droplets. The various oxidation mechanisms for SO2 can all be important, with their relative contributions varying from case to case. H2O2 does not invariably dominate this process, especially in winter when its concentration may be low.The chemistry of hill clouds is far from trivial and oversimplification can result in a misunderstanding of the behaviour which occurs. There is a need, rather, to consider a wide range of reactions if the nature of the overall processes and the impact of manmade emissions on the environment via this route are to be understood.
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