Atmospheric Mercury in Northern Wisconsin: Sources and Species

  • Carl H. Lamborg
  • William F. Fitzgerald
  • Grace M. Vandal
  • Kristofer R. Rolfhus

Abstract

The atmospheric chemistry, deposition and transport of mercury (Hg) in the Upper Great Lakes region is being investigated at a near-remote sampling location in northern Wisconsin. Intensive sampling over two years and various seasons has been completed. A multi-phase collection strategy (gas-, particle- and precipitation-phases) was employed to gain insight into the processes controlling concentrations and chemical/physical speciation of atmospheric Hg. Additional chemical and physical atmospheric determinations (e.g. ozone, particulate constituents, meteorology) were also made during these periods to aid in the interpretation of the Hg determinations. For example, correlations of Hg with ozone, sulfur dioxide and synoptic-scale meteorological features suggest a regionally discernible signal in Hg. Comparison to isosigma backward air parcel trajectories confirms this regionality and implicates the areas south, southeast and northwest of the site to be sources; for Hg. Particle-phase Hg (Hgp) was found to be approximately 40% in an oxidized form, or operationally defined as “reactive”. However, this was quite variable from year-to-year. Hgp and other particle constituents (esp. sulfate) show significant correlation and similarity in behavior (concentration ratios in precipitation and in particles). These observations are part of the growing evidence to support the hypothesis that precipitation-phase Hg arises in large part from the scavenging of atmospheric particulates bearing Hg. Observed concentrations of rain and particle-Hg fit broadly the theoretical expectations for nucleation and below-cloud scavenging. Significant increases in the Hg/aerosol mass ratio appear to take place during transport Enrichment of aerosols is taken as evidence of gas/particle conversion which could represent the step linking gas-phase Hg with rain. The refined budget indicates ca. 24% of total deposition is from summer particle dry deposition, and that this deposition also contributes ca. 24% of all reactive Hg deposition. Additionally, almost all (86%) deposition (wet and dry) occurs during the summer months.

Keywords

Great Lake Region Time Weight Washout Ratio Particle Scavenge Total Aerosol Mass 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.

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References

  1. Arimoto, R., Ray, B.J., Duce, R.A., Hewitt, A.D., Boldi, R. and Hudson, A.: 1990, J. Geo. Res. 95, D13, 22389–22405.CrossRefGoogle Scholar
  2. Bloom, N.S. and Fitzgerald, W.F.: 1988, Anal Chim. Acta. 208, 151–161.CrossRefGoogle Scholar
  3. Bloom, N.S.: 1989, Can. J. Fish. Aq. Sci. 46, 7: 1131–1140.CrossRefGoogle Scholar
  4. Bloom, N.S. and Watras, C.J.: 1989, Sci. Tot. Environ. 87/88, 199–207.CrossRefGoogle Scholar
  5. Charlson, R.J., Vong, R. and Hegg, D.A.: 1983, J. Geo. Res. 88, C2, 1375–1377.CrossRefGoogle Scholar
  6. Draxler, R.R.: 1992, Hybrid Single-Particle Lagrangian Integrated Trajectories (HPUT): Version 3.0 – User’s Guide and Model Description. NO AA Technical Memorandum ERL ARL-195. U.S. BSpt. of Commerce.Google Scholar
  7. Ferrara, R., Maseiti, B., Petrosino, A. and Bargagli, R: 1986, Atmos. Environ. 20, 1, 125–128.CrossRefGoogle Scholar
  8. Finlayson-Pitts, B.J. and Pitts, J.N. Jr.: 1986, Atmospheric Chemistry: Fundamentals and Experimental Techniques, John Wiley & Sons, New York.Google Scholar
  9. Fitzgerald, W.F., Mason, R.P. and Vandal, G.M.: 1991, WA.S.P. 56, 745–767.Google Scholar
  10. Fitzgerald, W.F. and Watras, C.J.: 1982, Sci. Tot. Env. 87/88, 223–232.Google Scholar
  11. Fitzgerald, W.F. and Gill, G.A.: 1979, Anal. Chem. 51, 11, 1714–1720.CrossRefGoogle Scholar
  12. Fitzgerald, W.F., Gill, G.A and Kim, J.P.: 1984, Science 224, 597–599.PubMedCrossRefGoogle Scholar
  13. Fitzgerald, W.F., Gill, G.A. and Hewitt, A.D.: 1981, IAMAP 3rd Scientific Assembly, Hamburg, 17–28 August.Google Scholar
  14. Fitzgerald, W.F., Mason, R.P., Vandal, G.M. and Dulac, F.: 1994, Mercury as a Global Pollutant: Towards Integration and Synthesis. C.J. Watras and J.W. Huckabee, editors. Lewis Press, in press.Google Scholar
  15. Fitzgerald, W.F.: 1995, this volume.Google Scholar
  16. GESAMP Working Group 14: 1989, Duce, R. A, Liss, P.A, Merrill, J.T., Alias, E.A., Buat-Menard, P., Hicks, B.B., Miller, J.M., Prospero, J.M., Arimoto, R., Church, T.M., Ellis, W.G., Galloway, J.N., Hansen, LA., Jickells, T.D., Knap, A.H., Reinhardt, K.H., Schneider, B., Soudine, A, Tokos, J.J., Tsunogai, S., Wollast, R., and Zhou, M. World Meteorological Organization, p. 111.Google Scholar
  17. Horvat, M.: 1993, Anal. Chim. Acta 282, 153–168.CrossRefGoogle Scholar
  18. Hoyer, M., Burke, J., Cleckner, L., Mukheijee, K. and Keeler, G.: 1993, From: Proceedings of 9th. Intl. Conf. on Heavy Metals in the Environment. Allan, R.J. and Nriagu, J.O. eds. CEP Consultants Ltd Edinburgh.Google Scholar
  19. Iverfeldt, A: 1991, W.A.S.P. 56, 251–265.Google Scholar
  20. Keeler, G.J. and Samson, P.J.: 1989, ES&T 723, 1358–1364.CrossRefGoogle Scholar
  21. Koutrakis, P., Wolfson, J.M., Slater, J.L., Brauer, M., Spengler, J.D., Stevens, R.K. and Stone, C.L: 1988, ES&T 22, 1463–1468.CrossRefGoogle Scholar
  22. Lamborg, C.H., Hoyer, M.E., Keeler, G.J., Olmez, I. and Huang, X.: 1994, From: Mercury as a Global Pollutant-Toward Integration and Synthesis. Watras, C.J. and Huckabee, J. Eds. Lewis Publishers, in press.Google Scholar
  23. Lamborg, C.H., Fitzgerald, W.F., Vandal, G.M. and Rolfhus, K.R.: 1993, From:Proceedings of 9th. Intl Conf. on Heavy Metals in the Environment. Allan, R.J. and Nriagu, J.O. eds. CEP Consultants Ltd Edinburgh.Google Scholar
  24. Lindqvist, O., Johansson, K., Aastrup, M., Andersson, A., Bringmark, L, Hovsenius, G., Hakanson, L, Iverfeldt, A, Meili, M. and Timm, B.: 1991, WA.S.P. 55, 65–71.Google Scholar
  25. Mason, R.P., Fitzgerald, W.F. and Vandal, G.M.: 1992, J. Atmos. Chem. 14, 489–500.CrossRefGoogle Scholar
  26. Mason, R.P., Fitzgerald, W.F. and Morel, F.M.M.: 1994, Geochim. Cosmochim. Acta. 58, 15, 3191–3198.CrossRefGoogle Scholar
  27. Meij, R.: 1991, W.A.S.P. 56, 21–33.Google Scholar
  28. Miller, D.R. and Nikolaidis, N.P.: 1992, Quality Assurance Plan for Measurement of Atmospheric Dry Deposition to Long Island Sound. ERI Report No: 91–06. Environmental Research Institute, The University of ConnecticutGoogle Scholar
  29. Munthe, J.: 1992, Atmos. Environ. 26A, 8, 1461–1468.Google Scholar
  30. Nater, E.A and Grigal, D.F.: 1992, Nature 358, 139–141.CrossRefGoogle Scholar
  31. Nriagu, J.O. and Pacyna, J.M,: 1988,Nature 333, 134–139.PubMedCrossRefGoogle Scholar
  32. Prestbo, E.: 1995, this volume.Google Scholar
  33. Rasmussen, P.E., Mierle, G. and Nriagu, J.O.: 1991, WA.S.P. 56, 379–390.Google Scholar
  34. Samson, P.J.: 1980, J. App. Met. 19, 1382–1394.CrossRefGoogle Scholar
  35. Schroeder W.H and Markes, J.: 1994, J. Great Lakes Res. 20, 1, 240–259.CrossRefGoogle Scholar
  36. Seinfeld, J.H.: 1986, Atmospheric Chemistry and Physics of Air Pollution, John Wiley and Sons, New York.Google Scholar
  37. Slemr, F., Seiler, W. and Schuster, G.: 1981, J. Geo. Res. 86, 1159–1166.CrossRefGoogle Scholar
  38. Slemr, F. and Langer, E.: 1992, Nature 355, 434–437.CrossRefGoogle Scholar
  39. Stem, A.C., Boubel, R.W., Turner, D.B. and Fox, D.L.: 1984, Fundamentals of Air Pollution 2nd ed. Academic Press Inc., New York.Google Scholar
  40. Watras, C.J., Bloom, N.S., Hudson, R.J.M., Gherini, S.A, Munson, R., Claas, S.A., Morrison, K.A., Hurley, J., Wiener, J.G., Fitzgerald, W.F., Mason, R., Vandal, G.M., Powell, D., Rada, R., Rislow, L, Winfrey, M., Elder, J., Krabbenhoft, D., Andren, A., Babiarz, C., Porcella, D.B., Huckabee, J.W.: 1994, Mercury as a Global Pollutant: Towards Integration and Synthesis. C.J. Watras and J.W. Huckabee, editors. Lewis Press, in press.Google Scholar

Copyright information

© Springer Science+Business Media Dordrecht 1995

Authors and Affiliations

  • Carl H. Lamborg
    • 1
  • William F. Fitzgerald
    • 1
  • Grace M. Vandal
    • 1
  • Kristofer R. Rolfhus
    • 1
  1. 1.Dept. of Marine ScienceThe University of ConnecticutGrotonUSA

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