A Re-Evaluation of Sulfur Budgets, Lifetimes, and Scavenging Ratios for Eastern North America

Journal of Atmospheric Chemistry - 1997
GARY S. WOJCIK1, JULIUS S. CHANG1
1Atmospheric Sciences Research Center, University at Albany, State University of New York, Albany, U.S.A

Tóm tắt

Lifetimes, scavenging ratios, andbudgets describe the cycling of atmosphericconstituents and are often used in formulating airpollution control strategies. Most previous studiesof sulfur lifetimes, budgets, and scavenging ratioshave been based on limited observational data or datafrom highly simplified models. The Regional AcidDeposition Model (RADM2.61) shows some skill inpredicting atmospheric mixing ratios of acidicmaterials and other related trace constituents andacid deposition patterns in North America, and so,analysis of its established, theoretical, databaseserves as a counterpoint to previous studies of sulfurbudgets, lifetimes, and scavenging ratios. The annualbudget shows that the net transport (outflow minusinflow) of sulfur compounds out of eastern NorthAmerica is equal to the total deposition within thedomain. Of the total deposition, 63% is from wetdeposition and 37% is from dry deposition. Theannual average lifetime of sulfur dioxide (38 hours),estimated by the turnover time, is limited by aqueousconversion, while that for sulfate aerosols (54 hours)is limited by their removal in precipitation. Theannual average lifetime of sulfur in this domain isslightly more than three days. Episodic lifetimes andbudgets, based on particular synoptic situations, showlarge variations around the annual values. Episodicprecipitation scavenging ratios exhibit similarvariability and are used to offer explanations ofseveral potential biases found in the wet sulfurdeposition amounts as predicted by the EMEP sulfurtransport model and other published results.

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Tài liệu tham khảo

Alcamo, J., Shaw, R., and Hordijk, L. (eds.), 1990: The RAINS Model of Acidification: Science and Strategies in Europe, Kluwer Academic Publishers, Boston, 402 pp.

Alkezweeney, A. J. and Powell, D. C., 1977: Estimation of transformation rate of SO2 to SO4 from atmospheric concentration data, Atmos. Environ. 11, 179–182.

Anthes, R.A. and Warner, T. T., 1978: Development of hydrodynamic models suitable for air pollution and other mesometeorological studies, Mon. Weather Rev. 106, 1045–1078.

Anthes, R.A., Hsie, E.Y., and Kuo, Y. H., 1987: Description of the Penn State/NCAR Mesoscale model version 4 (MM4),NCAR Technical Note, NCAR/TN-282+STR, National Center for Atmospheric Research, Boulder, CO, 66 pp.

Balko, J. A. and Peters, L. K., 1983: A modeling study of SOx–NOx-hydrocarbon plumes and their transport to the background troposphere, Atmos. Environ. 17, 1965–1978.

Bamber, D. J., Clark, P. A., Glover, G.M., Healey, P. G. W, Kallend, A. S., Marsh, A. R. W., Tuck, A. F., and Vaughan, G., 1984: Air sampling flights round the British Isles at low altitudes: SO2 oxidation and removal rates, Atmos. Environ . 18, 1777–1790.

Barrie, L. A., 1981: The prediction of rain acidity and SO2 scavenging in eastern North America, Atmos. Environ. 15, 31–41.

Barrie, L. A., 1985: Scavenging ratios, wet deposition, and in-cloud oxidation: An application to the oxides of sulphur and nitrogen, J. Geophys. Res. 90, 5789–5799.

Barrie, L. A. and Hales, J. M., 1984: The spatial distributions of precipitation acidity and major ion wet deposition in North America during 1980, Tellus 36B, 333–355.

Barrie, L. A. and Hoff, R. M., 1984: The oxidation rate and residence time of sulphur dioxide in the Arctic atmosphere, Atmos. Environ. 18, 2711–2722.

Berge, E., 1993: Coupling of wet scavenging of sulfur to clouds in a numerical weather prediction model, Tellus 45B, 1–22.

Berge, E., 1994: A comparison of results from the EMEP/MSC-W acid deposition model and the EMEP monitoring sites during the four seasons of 1989, EMEP/MSC-W/CCC, Note 1/94, The Norwegian Meteorological Institute, Oslo, Norway.

Bolin, B. and Rodhe, H., 1973: A note on the concepts of age distribution and transit time in natural reservoirs, Tellus XXV, 58–62.

Brook, J. R., Samson, P. J., and Sillman, S., 1995a: Aggregation of selected three-day periods to estimate annual and seasonal wet deposition totals for sulfate, nitrate and acidity: I. a synoptic and chemical climatology for eastern North America, J. Appl. Meteor. 3 4, 297–325.

Brook, J. R., Samson, P. J., and Sillman, S., 1995b: Aggregation of selected three-day periods to estimate annual and seasonal wet deposition totals for sulfate, nitrate and acidity: II. selection of events, deposition totals and source-receptor relationships, J. Appl. Meteor. 34, 326–339.

Brost, R. A., Chatfield, R. B., Greenberg, J. P., Haagenson, P. L., Heikes, B. G., Madronich, S., Ridley, B. A., and Zimmerman, P. R., 1988: Three-dimensional modeling of transport of chemical species from continents to the Atlantic Ocean, Tellus 40B, 358–379.

Cadle, S. H., VandeKopple, R. V., Mulawa, P. A., and Dasch, J. M., 1990: Ambient concentrations, scavenging ratios, and source regions of acid related compounds and trace metals during winter in northern Michigan, Atmos. Environ. 24A, 2981–2989.

Chan, W. H. and Chung, D. H. S., 1986: Regional-scale precipitation scavenging of SO2; SO4, NO3, and HNO3, Atmos. Environ. 20, 1397–1402.

Chang, J. S., Binkowski, F. S., Lansford, H. H., Madronich, S., Middleton, P. B., Pleim, J. E., Seamon, N. L., Stauffer, D. R., Stockwell, W. R., and Walcek, C. J., 1990: The regional acid deposition model and engineering model, NAPAP SOS/T report 4, in: National Acid Precipitation Assessment Program: State of Science and Technology, Vol.1, National Acid Precipitation Assessment Program, Washington, D.C.

Chang, J. S., Brost, R. A., Isaksen, I. S., Madronich, S., Middleton, P., Stockwell, W. R., and Walcek, C. J., 1987: A three dimensional Eulerian acid deposition model: physical concepts and formulation, J. Geophys. Res. 92, 14,681–14,700.

Chang, T. Y., 1979: Estimate of the conversion of SO2 to SO4 from the Da Vinci flight data, Atmos. Environ. 13, 1663–1664.

Dana, M. T., 1980: SO2 versus sulfate wet deposition in the eastern United States, J. Geophys Res. 85, 4475–4480.

Davis, D., Heaps, D. W., Philen, D., and McGee, T., 1979: Boundary layer measurements of the OH radical in the vicinity of an isolated power plant plume: SO2 and NO2 chemical conversion times, Atmos. Environ. 13, 1197–1203.

Deister, U., Neeb, R., Helas, G., and Warneck, P., 1986: Temperature dependence of the equilibrium CH2(OH)2 + HSO3 - = CH2(OH)SO3 - + H2O in aqueous solution, J. Phys. Chem. 90, 3213–3217.

Dennis, R. L., McHenry, J. N., Barchet, W. R., Binkowski, F. S., and Byun, D. W., 1993: Correcting RADM’s sulfate underprediction: Discovery and correction of model errors and testing the corrections through comparisons against field data, Atmos. Environ. 27A, 975–997.

Dennis, R. L., Barchet, W. R., Clark, T. L., and Seilkop, S. K., 1990: Evaluation of regional acidic deposition models (part I), NAPAP SOS/T report 5, in: National Acid Precipitation Assessment Program: State of Science and Technology , Vol. 1, National Acid Precipitation Assessment Program, Washington, D.C.

Eliassen, A., 1978: The OECD study of long range transport of air pollutant: Long range transport modeling, Atmos. Environ. 12, 479–487.

Eliassen, A. and Saltbones, J., 1975: Decay and transformation rates of SO2, as estimated from emission data, trajectories and measured air concentrations, Atmos. Environ. 9, 425–429.

Eliassen, A. and Saltbones, J., 1983: Modeling of long-range transport of sulphur over Europe: A two-year model run and some model experiments, Atmos. Environ. 17, 1457–1473.

Eriksson, E., 1963: The yearly circulation of sulfur in nature, J. Geophys. Res. 68, 4001–4008.

Fay, J. A., Golomb, D., and Kumar, S., 1985: Source apportionment of wet sulfate deposition in eastern North America, Atmos. Environ. 19, 1773–1782.

Fay, J. A., Kumar, S., and Golomb, D., 1986: Annual and semi-annual anthropogenic sulfur budget for eastern North America, Atmos. Environ. 20, 1497–1500.

Fisher, B. E. A. and Callander, B. A., 1984: Mass balances of sulphur and nitrogen oxides over Great Britain, Atmos. Environ. 18, 1751–1757.

Galloway, J. N. and Whelpdale, D.M., 1980: An atmospheric sulfur budget for eastern North America, Atmos. Environ. 14, 409–417

Galloway, J. N. and Rodhe, H., 1991: Regional atmospheric budgets of S and N fluxes: How well can they be quantified?, Proc. R. Soc. Edinburgh 97B, 61–80.

Galloway, J. N., Whelpdale, D. M., and Wolff, G. T., 1984: The flux of S and N eastward from North America, Atmos. Environ. 18 ,2595–2607.

Galloway, J. N., Savoie, D. L., Keene, W. C., and Prospero, J. M., 1993: The temporal and spatial variability of scavenging ratios for nss sulfate, nitrate, methanesulfonate, sodiumin the atmosphere over the North Atlantic Ocean, Atmos. Environ. 27A, 235–250.

Garland, J. A., 1978: Dry and wet removal of sulphur from the atmosphere, Atmos. Environ. 12, 349–362.

Garland, J. A. and Branson, J. R., 1976: The mixing height and mass balance of SO2 in the atmosphere above Great Britain, Atmos. Environ. 10, 353–362.

Gotaas, Y., 1982: Vertical distribution of sulphur in the atmosphere in a case of long range transport and the rate of transformation to sulphate, Atmos. Environ. 16, 1043–1046.

Hansen, D. A., Barnes, M. H., Lusis, M., and Puckett, K. J., 1989: A North American field study to evaluate Eulerian models, in: H. van Dop (ed), Air Pollution Modeling and Its Application VII, Plenum Press, New York, pp. 297–306.

Harrison, R. M. and Allen, A. G., 1991: Scavenging ratios and deposition of sulphur, nitrogen and chlorine species in eastern England, Atmos. Environ. 25A, 1719–1723.

Hegg, D. A., 1985: The importance of liquid-phase oxidation of SO2 in the troposphere, J. Geophys. Res. 90, 3773–3779.

Hegg, D. A., Rutledge, S. A., and Hobbs, P. V., 1984: A numerical model for sulfur chemistry in warm-frontal rainbands, J. Geophys. Res. 89, 7133–7147.

Hegg, D. A., Rutledge, S. A., and Hobbs, P. V., 1986: A numerical model for sulfur and nitrogen scavenging in narrow cold-frontal rainbands 2. discussion of chemical fields, J. Geophys. Res. 91, 14,403–14,416.

Henmi, T. and Reiter, E. R., 1978: Regional residence times of sulfur dioxide over the eastern United States, Atmos. Environ. 12, 1489–1495.

Husain, L., Dutkiewicz, V. A., Hussain, M. M., Khwaja, H. A., Burkhard, E. G., Mehmood, G., Parekh, P. P., and Canelli, E., 1991: A study of heterogeneous oxidation of SO2 in summer clouds, J. Geophys. Res. 96, 18,789–18,805.

Husain, L. and Dutkiewicz, V. A., 1992: Elemental tracers for the study of homogeneous gas phase oxidation of SO2 in the atmosphere, J. Geophys. Res. 97, 14,635–14,643.

Husar, R. B., Patterson, D. E., Husar, J. D., and Gillani, N. V., 1978: Sulfur budget of a power plant plume, Atmos. Environ. 12, 549–568.

Ito, T., Okita, T., Ikegami, M., Kanazawa, I., 1986: The characterization and distribution of aerosol and gaseous species in the winter monsoon over the Western Pacific Ocean, J. Atmos. Chem. 4, 401–411.

Jakobsen, H. A., Jonson, J. E., and Berge, E., 1996: Transport and deposition calculations of sulphur and nitrogen compounds in Europe for 1992 in the 50 km grid by use of the multi-layer Eulerian model, EMEP/MSC-W Note 2/96, The Norwegian Meteorological Institute, Oslo.

Jaffrezo, J., Colin, J., and Gros, J., 1990: Some physical factors influencing scavenging ratios, Atmos. Environ. 24A, 3073–3083.

Kleinman, L. I., 1983: A regional scale modeling study of the sulfur oxides with a comparison to ambient and wet deposition monitoring data, Atmos. Environ. 17, 1107–1121.

Langner, J. and Rodhe, H., 1991: A global three-dimensional model of the troposphere sulfur cycle, J. Atmos. Chem. 13, 225–263.

Leaitch, W. R., Strapp, J. W., Schemenauer, R. S., and Isaac, G. A., 1984: Observations of Cloud Droplets, Aerosol Particles, and Cloud Condensation Nuclei in Continental Air Masses, Paper presented at the 11th Conference on Atmospheric Aerosols, Condensation, and Ice Nucleii, Hungary.

Liebsch, E. J. and de Pena, R. G., 1982: Sulfate aerosol production in coal-fired power plant plumes, Atmos. Environ. 16, 1323–1331.

McHenry, J. N. and Dennis, R. L., 1994: The relative importance of oxidation pathways and clouds to atmospheric ambient sulfate production as predicted by the Regional Acid Deposition Model, J. Appl. Meteor. 33, 890–905.

Meetham, A. R., 1950: Natural removal of pollution from the atmosphere, Q. J. R. Meteorol. Soc. 76, 359–371.

Mészáros, E., Varhelyi, G., and Haszpra, L., 1978: On the atmospheric sulfur budget over Europe, Atmos. Environ. 12, 2273–2277.

Middleton, P. and Chang, J. S., 1990: Analysis of RADM gas concentration predictions using OSCAR and NEROS monitoring data, Atmos. Environ. 24A, 2113–2125.

Middleton, P., Chang, J. S., del Corral, J. C., Geiss, H., and Rosinski, J. M., 1988: Comparison of RADM and OSCAR chemistry data, Atmos. Environ. 22, 1195–1208.

Misra, P. K., Chan, W. H., Chung, D., and Tang, AL. J. S., 1985: Scavenging ratios of acidic pollutants and their use in long-range transport models, Atmos. Environ. 19, 1471–1475.

Möller, D., 1984: Estimation of the global man-made sulphur emission, Atmos. Environ. 18, 19–27.

Nordlund, G., 1983: Seasonal averages of net decay rate of SO2over northern Europe, Atmos. Environ. 17, 1199–1201.

Omstedt, G. and Rodhe, H., 1978: Transformation and removal processes for sulfur compounds in the atmosphere as described by a one-dimensional time-dependent diffusion model, Atmos. Environ. 12, 503–509.

Oppenheimer, M., 1983: The relationship of sulfur emissions to sulfate in precipitation, Atmos. Environ. 17, 451–460.

Placet, M., Battye, R. E., Fehsenfeld, F. C., and Bassett, G. W., 1990: Emissions involved in acidic deposition processes, NAPAP SOS/T report 1, in: National Acid Precipitation Assessment Program: State of Science and Technology, Vol. 1, National Acid Precipitation Assessment Program, Washington, D.C.

Prahm, L. P., Torp, U., and Stern, R.M., 1976: Deposition and transformation rates of sulphur oxides during atmospheric transport over the Atlantic, Tellus 27, 355–372.

Research and Monitoring Coordinating Committee (RMCC), 1990: The 1990 Canadian Long-Range Transport of Air Pollutants and Acid Deposition Assessment Report, 3, Atmospheric Sciences, Atmos. Environ. Serv., Environ. Can., Downsview, Ont.

Renner, E., Ratzlaff, U., and Rolle, W., 1985: A Lagrangian multi-level model of transport, transformation and deposition of atmospheric sulfur dioxide and sulfate, Atmos. Environ. 19, 1351–1359.

Rodhe, H., 1972: A study of the sulfur budget for the atmosphere over Northern Europe, Tellus 24, 128–138.

Rodhe, H., 1976: An atmospheric sulfur budget for NW Europe, in: Nitrogen, Phosphorus, and Sulfur-Global Cycles, SCOPE Report 7, Berglingska Boktryckeriet, Sweden.

Rodhe, H., 1978: Budgets and turn-over times of atmospheric sulfur compounds, Atmos. Environ. 12, 671–680.

Rodhe, H. and Grandell, J., 1972: On the removal time of aerosol particles from the atmosphere by precipitation scavenging, Tellus XXIV, 442–454.

Rodhe, H. and Isaksen, I., 1980: Global distribution of sulfur compounds in the troposphere estimated in a height/latitude transport model, J. Geophys. Res. 85, 7401–7409.

Schwartz, S. E., 1979: Residence times in reservoirs under non-steady-state conditions: Applications to atmospheric SO2 and aerosol sulfate, Tellus 31, 530–547.

Seland, O., van Pul, A., Sorteberg, A., and Tuovinen, J-P., 1995: Implementation of a resistance dry deposition module and a variable local correction factor in the Lagrangian EMEP model, EMEP/MSC-W Report 3/95, The Norwegian Meteorological Institute, Oslo.

Shannon, J. D., 1981: A model of regional long-term average sulfur atmospheric pollution, surface removal, and net horizontal flux, Atmos. Environ. 15, 689–701.

Sheih, C. M., Wesley, M. L., and Hicks, B. B., 1979: Estimated dry deposition velocities of sulfur over the eastern United States and surrounding regions, Atmos. Environ. 13, 1361–1368.

Sisterson, D. L., Bowersox, V. C., Meyers, T. P., Olsen, A. R., and Vong, R. J., 1990: Deposition monitoring: Methods and results, NAPAP SOS/T report 6, in: National Acid Precipitation Assessment Program: State of Science and Technology, Vol. 1, National Acid Precipitation Assessment Program, Washington, D.C.

Smith, F. B. and Jeffrey, G. H., 1975: Airborne transport of sulphur dioxide from the U.K., Atmos. Environ. 9, 643–659.

Summers, P.W. and Fricke, W., 1989: Atmospheric decay distances and times for sulphur and nitrogen oxides from air and precipitation monitoring in eastern Canada, Tellus 41B, 286–295.

Taylor, G. R., 1989: Sulfate production in midlatitude continental cumulus clouds. Part II: Chemistry model formulation and sensitivity analysis, J. Atmos. Sci. 46, 1991–2007.

Venkatram, A., Karamchandani, P.K., and Misra, P.K., 1988: Testing a comprehensive acid deposition model, Atmos. Environ. 22, 737–747.

Warneck, P., 1988: Chemistry of the Natural Atmosphere, Academic Press, San Diego, pp. 757.

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