Abstract
For detailed modeling of atmospheric chemistry it is necessary to consider aqueous-phase reactions in cloud droplets and deliquesced aerosol particles. Often, the gas-phase concentration is in equilibrium with the aqueous phase. Then Henry′s law can be used to describe the distribution between the phases provided that the Henry′s law coefficient is known. In some cases, thermodynamic equilibrium will not be reached and it is necessary to use kinetic expressions of the rates involved. These rates depend on diffusion constants, accommodation coefficients, Henry′s law coefficients, particle size distributions, and several other parameters. This review describes how these processes can be treated in computer modeling and how the necessary data can be obtained. Even though it is written primarily for use in modeling atmospheric chemistry, some parts will also be useful for waste water and pesticide control and in other areas where the distribution of chemicals between the aqueous and the gas phase is important.
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Atkins, P.W.: 1986, Physical Chemistry, Oxford University Press.
Battino, R., Clever, H.L., Fogg, P.G.T., and Young, C.L.: 1995, 'Introduction to the solubility data series. Solubility of gases in liquids', http://www.unileoben.ac.at/~eschedor/gl-intro.html.
Betterton, E.A.: 1992, 'Henry's law constants of soluble and moderately soluble organic gases: Effects on aqueous phase chemistry', Adv. Environ. Sci. Technol. 24, 1-50.
Bower, K.N., Hill, T.A., Coe, H., and Choularton, T.W.: 1991, 'SO2 oxidation in an entraining cloud model with explicit microphysics', Atmos. Environ. 25A, 2401-2418.
Brimblecombe, P. and Clegg, S.L.: 1988, 'The solubility and behaviour of acid gases in the marine aerosol', J. Atmos. Chem. 7, 1-18.
Chameides, W.L. and Davis, D.D.: 1982, 'The free radical chemistry of cloud droplets and its impact upon the composition of rain', J. Geophys. Res. 87C, 4863-4877.
Chameides, W.L. and Stelson, A.W.: 1992, 'Aqueous phase chemical processes in deliquescent seasalt aerosols: A mechanism that couples the atmospheric cycles of S and sea salt', J. Geophys. Res. 97D, 20565-20580.
De Bruyn, W.J., Swartz, E., Hu, J.H., Shorter, J.A., Davidovits, P., Worsnop, D.R., Zahniser, M.S., and Kolb, C.E.: 1995, 'Henry's law solubilities and Śetchenow coefficients for biogenic reduced sulfur species obtained from gas-liquid uptake measurements', J. Geophys. Res. 100D, 7245-7251.
DeMore, W.B., Sander, S.P., Golden, D.M., Hampson, R.F., Kurylo, M.J., Howard, C.J., Ravishankara, A.R., Kolb, C.E., and Molina, M.J.: 1997, 'Chemical kinetics and photochemical data for use in stratospheric modeling', JPL Publication 97-4, Jet Propulsion Laboratory, Pasadena, CA.
Dubik, N.A., Titova, G.M., and Loshakova, E.I.: 1987, 'Partition coefficients of bromine and bromine chloride between air and natural brines', Issled. v Obl. Poluch. Magniya, Ioda, Broma i ikh Soed., M. pp. 53-57. (in Russian, see also Chem. Abstr., 109, 213154j).
Frenzel, A., Scheer, V., Sikorski, R., George, C., Behnke, W., and Zetzsch, C.: 1998, 'Heterogeneous interconversion reactions of BrNO2, ClNO2, Br2, and Cl2', J. Phys. Chem. A 102, 1329-1337.
Fuchs, N.A. and Sutugin, A.G.: 1971, Highly Dispersed Aerosols, Ann Arbor Science, Ann Arbor, Mich.
Graedel, T.E. and Weschler, C.J.: 1981, 'Chemistry within aqueous atmospheric aerosols and raindrops', Rev. Geophys. Space Phys. 19, 505-539.
Jacob, D.J.: 1986, 'Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate', J. Geophys. Res. 91D, 9807-9826.
Jaenicke, R.: 1987, 'Aerosol physics and chemistry', In: Landolt-Börnstein New Series V/4b.
Keene, W.C., Sander, R., Pszenny, A.A.P., Vogt, R., Crutzen, P.J., and Galloway, J.N.: 1998, 'Aerosol pH in the marine boundary layer: A review and model evaluation', J. Aerosol Sci. 29, 339-356.
Kojima, K., Zhang, S., and Hiaki, T.: 1997, 'Measuring methods of infinite dilution coefficients and a database for systems including water', Fluid Phase Equilib. 131, 145-179.
Lelieveld, J. and Crutzen, P.J.: 1991, 'The role of clouds in tropospheric photochemistry', J. Atmos. Chem. 12, 229-267.
Lide, D.R. and Frederikse, H.P.R. (eds.): 1995, CRC Handbook of Chemistry and Physics, 76th Edition. CRC Press, Inc., Boca Raton, FL.
Mackay, D. and Shiu, W.Y.: 1981, 'A critical review of Henry's law constants for chemicals of environmental interest', J. Phys. Chem. Ref. Data 10, 1175-1199.
Mackay, D., Shiu, W.Y., and Sutherland, R.P.: 1979, 'Determination of air-water Henry's law constants for hydrophobic pollutants', Environ. Sci. Technol. 13, 333-337.
Mills, I., Cvitaš, T., Homann, K., Kallay, N., and Kuchitsu, K.: 1993, International Union of Pure and Applied Chemistry: Quantities, Units and Symbols in Physical Chemistry, Blackwell Science, Boca Raton.
Müller, F.: 1998, 'Compilation of accommodation coefficients', http://www.mi.uni-hamburg.de/technische_meteorologie/Meso/homepages/fmueller.html.
Nathanson, G.M., Davidovits, P., Worsnop, D.R., and Kolb, C.E.: 1996, 'Dynamics and kinetics at the gas-liquid interface', J. Phys. Chem. 100, 13007-13020.
Nielsen, F., Olsen, E., and Fredenslund, A.: 1994, 'Henry's law constants and infinite dilution activity coefficients for volatile organic compounds in water by a validated batch air stripping method', Environ. Sci. Technol. 28, 2133-2138.
Pandis, S.N. and Seinfeld, J.H.: 1989, 'Sensitivity analysis of a chemical mechanism for aqueousphase atmospheric chemistry', J. Geophys. Res. 94D, 1105-1126.
Pitzer, K.S. (ed.): 1991, Activity Coefficients in Electrolyte Solutions, 2nd Edition, CRC Press, Inc., Boca Raton, FL.
Régimbal, J.-M. and Mozurkewich, M.: 1997, 'Peroxynitric acid decay mechanisms and kinetics at low pH', J. Phys. Chem. A 101, 8822-8829.
Sahni, D.C.: 1966, 'The effect of a black sphere on the flux distribution in an infinite moderator', J. Nucl. Energy 20, 915-920.
Sander, R.: 1996, 'Compilation of Henry's law constants for inorganic and organic species of potential importance in environmental chemistry (version 2)', http://www.mpch-mainz.mpg.de/~sander/res/henry.html.
Sander, R. and Crutzen, P.J.: 1996, 'Model study indicating halogen activation and ozone destruction in polluted air masses transported to the sea', J. Geophys. Res. 101D, 9121-9138.
Schwartz, S.E.: 1986, 'Mass-transport considerations pertinent to aqueous phase reactions of gases in liquid-water clouds', In: W. Jaeschke (ed.): Chemistry of Multiphase Atmospheric Systems, NATO ASI Series, Vol. G6. pp. 415-471.
Schwartz, S.E. and Freiberg, J.E.: 1981, 'Mass-transport limitation to the rate of reaction of gases in liquid droplets: Application to oxidation of SO2 in aqueous solutions', Atmos. Environ. 15, 1129-1144.
Seinfeld, J.H. and Pandis, S.N.: 1998, Atmospheric Chemistry and Physics, John Wiley & Sons, Inc.
Sievering, H., Boatman, J., Galloway, J., Keene, W., Kim, Y., Luria, M., and Ray, J.: 1991, 'Heterogeneous sulfur conversion in sea-salt aerosol particles: The role of aerosol water content and size distribution', Atmos. Environ. 25A, 1479-1487.
Staudinger, J. and Roberts, P.V.: 1996, 'A critical review of Henry's law constants for environmental applications', Crit. Rev. Environ. Sci. Technol. 26, 205-297.
Stephen, H. and Stephen, T.: 1963, Solubilities of inorganic and organic compounds, Vol. 1. Pergamon Press, Oxford.
Vogt, R., Crutzen, P.J., and Sander, R.: 1996, 'A mechanism for halogen release from sea-salt aerosol in the remote marine boundary layer', Nature 383, 327-330.
Wagman, D.D., Evans, W.H., Parker, V.B., Schumm, R.H., Halow, I., Bailey, S.M., Churney, K.L., and Nuttall, R.L.: 1982, 'The NBS tables of chemical thermodynamic properties; Selected values for inorganic and C1 and C2 organic substances in SI units', J. Phys. Chem. Ref. Data 11, suppl. 2.
Wilhelm, E., Battino, R., and Wilcock, R.J.: 1977, 'Low-pressure solubility of gases in liquid water', Chem. Rev. 77, 219-262.
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Sander, R. Modeling Atmospheric Chemistry: Interactions between Gas-Phase Species and Liquid Cloud/Aerosol Particles. Surveys in Geophysics 20, 1–31 (1999). https://doi.org/10.1023/A:1006501706704
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DOI: https://doi.org/10.1023/A:1006501706704