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Transmission of Atmospherically Derived Trace Elements Through an Undeveloped, Forested Maryland Watershed

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Abstract

The transmission of atmospherically derived trace elements (Al, As, Cd, Cr, Cu, Fe, Mn, Ni, Pb, Se, and Zn) was evaluated in a small, undeveloped, forested watershed located in north-central Maryland. Atmospheric input was determined for wet-only and vegetative throughfall components. Annual throughfall fluxes were significantly enriched over incident precipitation for most elements, although some elements exhibited evidence of canopy release (Mn) or preferential uptake (As, Cr, and Se). Stream export was gauged based on systematic sampling under varied flow regimes. Particle loading appears to contribute significantly to watershed export (> 10%) for only As, Pb, and Fe, and then only during large precipitation/runoff events. The degree of watershed transmission for each trace element was evaluated based on a comparison of total, net atmospheric input (throughfall) to stream export over an annual hydrologic cycle. This comparison indicates that the atmospheric input of some elements (Al, Cd, Ni, Zn) is effectively transmitted through the watershed, but other elements (Pb, As, Se, Fe, Cr, Cu) appear to be strongly sequestered, in the respective orders noted. Results suggest that precipitation and subsequent soil pH are the primary factors that determine the mobility of sequestered trace element phases.

To further resolve primary atmospheric and secondary weathering components, the geochemical model NETPATH was applied. Results indicate that minerals dissolved include chlorite, plagioclase feldspar, epidote, and potassium feldspar; phases formed were kaolinite, pyrite, and silica. The model also indicates that weathering processes contribute negligible amounts of trace elements to stream export, indicative of the unreactive orthoquartzite bedrock lithology underlying the watershed. Thus, the stream export of trace elements primarily reflects atmospheric deposition to the local watershed.

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References

  • Avila, A. and Rodrigo, A.: 2004, ‘Trace metal fluxes in bulk deposition, throughfall and stemflow at two evergreen oak stands in NE Spain subject to different exposure to the industrial environment’, Atmos. Environ. 38, 171.

    Article  CAS  Google Scholar 

  • Baker, J. E., Poster, D. L., Clark, C. A., Church, T. M., Scudlark, J. R., Ondov, J. M., Dickhut, R. M. and Cutter, G. A.: 1997, ‘Loadings of Atmospheric Trace Elements and Organic Contaminants to the Chesapeake Bay’, in J. E. Baker (ed.), Atmospheric Deposition of Contaminants to the Great Lakes and Coastal Waters, SETAC Press, Pensacola, FL, USA, Chap. 9, pp. 171–194.

    Google Scholar 

  • Bondeitti, E. A., Hoffman, F. O. and Larsen, I. L.: 1984, ‘Air-to-vegetation transfer rates of natural sub-micron aerosols’, J. Environ. Radioactivity 1, 5.

    Google Scholar 

  • Buchanan, T. J. and Somers, W. P.: 1968, Stage Measurements at Gauging Stations: U.S. Geological Survey Techniques of Water-Resources Investigations, Book 3, Chap. A7, pp. 28.

  • Buchanan, T. J. and Somers, W. P.: 1969, Discharge Measurements at Gauging Stations: U.S. Geological Survey Techniques of Water-Resources Investigations, Book 3, Chap. A8, pp. 65.

  • Castro, M. S. and Morgan, R. P. II: 2002, ‘Input-output budgets of major ions for a forested watershed in western Maryland’, Water Air Soil Pollut. 119, 121.

    Google Scholar 

  • Castro, M. S., Scudlark, J. R., Church, T. M. and Mason, R. P.: 2000, Input-Output Budgets of Major Ions, Trace Elements and Mercury in a Forested Maryland Watershed. Maryland Power Plant Research Program Report PPAD-AD-1, Annapolis, MD, pp. 72.

  • Church, T. M. and Scudlark, J. R.: 1992, ‘Trace elements in precipitation at the mid-Atlantic coast: A successful record since 1982’, in E. S. Verry and S. J. Vermette (eds.), The Deposition of Trace Metals in Our Environment, USDA Forest Service Report NC-150, Philadelphia, PA, USA, October 8, 1991, pp. 45–46.

  • Church, T. M. and Scudlark, J. R.: 1998, ‘Trace metals in estuaries: A delaware bay synthesis’, in H. E. Allen, A. W. Garrison and G. W. Luther III (eds.), Metal Speciation and Contamination of Surface Water, Ann Arbor Press, Inc., Chelsea, MI, USA, Chap. 1, pp. 1–21.

    Google Scholar 

  • Church, T. M., Scudlark, J. R. and Conko, K. M.: 2002, ‘Atmospheric and fluvial sources of trace metals to the Delaware Inland Bays’, in R. L. Lipnick, R. P. Mason, M. L. Phillips and C. U. Pittman (eds.), Chemicals in the Environment: Fate, Impacts and Remediation, ACS Symposium Series No. 806, Washington, D.C., USA, Chapter 13, pp. 243–257.

  • Church, T. M., Scudlark, J. R., Conko, K. M., Bricker, O. P. and Rice, K. C.: 1998, Transmission of Atmospherically Deposited Trace Elements Through and Undeveloped, Forested Maryland Watershed, Maryland Department of Natural Resources Report CBWP-MANTA-AD-98-2, Annapolis, MD, pp. 87.

  • Correll, D. L., Goff, N. M. and Peterjohn, W. T.: 1984, ‘Ion balances between precipitation inputs and rhode river discharges’, in O. P. Bricker (ed.), Geological Aspects of Acid Deposition, Butterworths, Boston, MA, USA, Acid Precipitation Series Vol. 7, Chap. 5.

  • Cosby, B. J., Ryan, P. F., Webb, J. R., Hornberger, G. M. and Galloway, J. N.: 1991, ‘Mountains of Western Virginia’, in D. F. Charles (ed.), Acid Deposition and Aquatic Ecosystems: Regional Case Studies, Springer-Verlag, New York, pp. 297–318.

    Google Scholar 

  • Cutter, G. A.: 1986, ‘Speciation of Selenium and Arsenic in Natural Waters and Sediments Volume 1: Selenium Speciation’, EPRI Final Report EA-4641, Vol. 1. Research Project 2020-1.

  • Cutter, G. A. and Church, T. M.: 1986, ‘Selenium in Western Atlantic precipitation’, Nature 322, 720.

    CAS  Google Scholar 

  • Cutter, L. S., Cutter, G. A. and San Diego-McGlone, M. L. C.: 1991, ‘Simultaneous determination of inorganic arsenic and antimony species in natural waters using selective hydride generation with gas chromatograph-photoionization detection’, Anal. Chem. 36, 1138.

    Google Scholar 

  • Deer, W. A., Howie, R. A. and Zussman, J.: 1965, Rock Forming Minerals (5th edn.), Longsmans, Green and Company, Ltd., London, UK.

    Google Scholar 

  • Draaijers, G. P. J., Erisman, J. W., Spranger, T. and Wyers, G. P.: 1996, ‘The application of throughfall measurements for atmospheric deposition monitoring’, Atmos. Environ. 30, 3349.

    CAS  Google Scholar 

  • Drever, J. I.: 1988, The Geochemistry of Natural Waters (2nd edition), Prentice-Hall, Upper Saddle River, NJ, USA, pp. 438.

    Google Scholar 

  • Erel, Y., Morgan, J. J. and Patterson, C. C.: 1991, ‘Natural levels of lead and cadmium in a remote mountain stream’, Geochim. Cosmochim. Acta 55, 707.

    CAS  Google Scholar 

  • Erel, Y., Patterson, C. C., Scott, M. J. and Morgan, J. J.: 1990, ‘Transport of industrial lead in snow through soil to streamwater and groundwater’, Chem. Geol. 85, 383.

    CAS  Google Scholar 

  • Fauth, J. L.: 1977. Geologic Map of the Catoctin Furnace and Blue Ridge Summit quadrangles, Maryland: Maryland Geological Survey, 1 sheet, scale 1:24,000.

  • Friedland, A. J., Craig, B. W., Miller, E. K., Herrick, G. T., Siccama, T. G. and Johnson, A. H.: 1992, ‘Decreasing lead levels in the forest floor of the northeastern USA’, Ambio 21, 400.

    Google Scholar 

  • Godfrey, J. T., Foster, G. D. and Lippa, K. A.: 1995, ‘Estimated annual loads of selected organic contaminants to Chesapeake Bay via a major tributary’, Environ. Sci. Technol. 29, 2059.

    CAS  Google Scholar 

  • Greenburg, R. R., Zoller, W. H. and Gordon, G. E.: 1978, ‘Composition and size distribution of particles released in refuse incineration’, Environ. Sci. Technol. 19, 566.

    Google Scholar 

  • Gustaffson, J. P. and Jacks, G.: 1995, ‘Arsenic geochemistry in forested soil profiles as revealed by solid phase studies’, Appl. Geocehm. 10, 307.

    Google Scholar 

  • Han, M.: 1992, Receptor modeling of airborne pollutants in the State of Maryland. Ph.D. Dissertation, University of Maryland.

  • Hansen, K., Draaijers, G. P. J., Ivens, W. P. M., Gundersen, P. and vanLeeuwen, N. F. M.: 1994, ‘Concentration variations in rain and canopy throughfall collected sequentially during individual rain events’, Atmos. Environ. 28, 3195.

    CAS  Google Scholar 

  • Hanson, P. J. and Lindberg, S. E.: 1991, ‘Dry deposition of reactive nitrogen compounds: A review of leaf, canopy and non-foliar measurements’, Atmos. Environ. 25A, 1615.

    CAS  Google Scholar 

  • Heinrichs, H. and Mayer, R.: 1980, ‘The role of forest vegetation in the biogeochemical cycle of heavy metals’, J. Environ. Qual. 9, 111.

    CAS  Google Scholar 

  • Helz, G. R., Ferni, K. L., Nichols, M. and Sinex, A. S.: 1985, ‘Processes controlling Fe, Mn, and Zn in sediments of northern Chesapeake Bay’, Estuarine Coastal Shelf Sci. 21, 1–16.

    CAS  Google Scholar 

  • Hicks, B. B.: 1986, ‘Measuring dry deposition: A re-assessment of the state of the art’, Water Air Soil Pollut. 30, 75–90.

    Article  Google Scholar 

  • Johnson, D. W. and Lindberg, S. E.: 1992, Atmospheric Deposition and Forest Nutrient Cycling, Springer-Verlag, New York, pp. 707.

    Google Scholar 

  • Jordan, T. E., Correll, D. L., Weller, D. E. and Goff, N. M.: 1995, ‘Temporal variation in precipitation chemistry on the shore of the Chesapeake Bay’, Water Air Soil Pollut. 83, 263.

    CAS  Google Scholar 

  • Jouraeva, V. A., Johnson, D. L., Hassett, J. P. and Nowak, D. J.: 2002, ‘Differences in accumulation of PAHs and metals on the leaves of Tilia x euchlora and Pyrus calleryana’, Environ. Pollut. 120, 331.

    CAS  PubMed  Google Scholar 

  • Kabata-Pendias, A. and Pendias, H.: 1984, Trace Elements in Soils and Plants, CRC Press, Inc., Boca Raton, FL, pp. 315.

    Google Scholar 

  • Katz, B. G., Bricker, O. P. and Kennedy, M. M.: 1985, ‘Geochemical mass-balance relationships for selected ions in precipitation and streamwater, Catoctin Mountains, Maryland’, Amer. Journ. Sci. 285, 962.

    Google Scholar 

  • Kennedy, E. J.: 1983. Computation of Continuous Records of Streamflow: U.S. Geological Survey Techniques of Water-Resources Investigations, Book 3, Chap. A13, pp. 53.

  • Kennedy, E. J.: 1984. Discharge Ratings at Gauging Stations: U.S. Geological Survey Techniques of Water-Resources Investigations, Book 3, Chap. A10, pp. 59.

  • Kim, G., Scudlark, J. R. and Church, T. M.: 2000, ‘Atmospheric wet deposition of trace elements to Chesapeake and Delaware Bays’, Atmos. Environ. 34, 3437.

    CAS  Google Scholar 

  • Kolka, R. K., Nater, E. A., Gringal, D. F. and Verry, E. S.: 1999, ‘Atmospheric inputs of mercury and organic carbon into a forested upland/bog watershed’, Water Air Soil Pollut. 113, 273.

    CAS  Google Scholar 

  • Kowalczyk, G. S., Gordon, G. E. and Rheingrover, S. W.: 1982, ‘Identification of atmospheric particulate sources in Washington, D.C., using chemical element balances’, Environ. Sci. Technol. 16, 79–90.

    CAS  Google Scholar 

  • Lapham, D. M.: 1958, ‘Structural and chemical variations in chromium chlorite’, Am. Mineralogist 43, 921.

    CAS  Google Scholar 

  • Lawson, N. M. and Mason, R. P.: 2001, ‘Concentration of mercury, methylmercury, cadmium, lead, arsenic and selenium in the rain and stream water of two contrasting watersheds in western Maryland’, Water Res. 35, 4039.

    CAS  PubMed  Google Scholar 

  • Lindberg, S. E.: 1989, ‘Behavior of Cd, Mn, and Pb in Forest-Canopy Throughfall, in J.M. Pacyna and B. Ottar (eds.), Control and Fate of Atmospheric Trace Metals, Kluwer Academic Publishers, Dordrecht, the Netherlands, pp. 233–257.

    Google Scholar 

  • Lindberg, S. E., Harriss, R. C. and Turner, R. R.: 1982, ‘Atmospheric deposition of metals to forest vegetation’, Science 215, 1609.

    CAS  Google Scholar 

  • Lindberg, S. E. and Lovett, G. M.: 1985, ‘Field measurements of dry deposition rates of particles to inert and foliar surfaces in a forest’, Environ. Sci. Technol. 19, 228.

    Google Scholar 

  • Lindberg, S. E., Lovett, G. M., Richter, D. D. and Johnson, D. W.: 1986, ‘Atmospheric deposition and canopy interactions of major ions in a forest’, Science 231, 141.

    CAS  Google Scholar 

  • Lindberg, S. E., Owens, J. G. and Stratton, W. J.: 1994, ‘Application of throughfall methods to estimate dry deposition of mercury’, in C. J. Watras and J. W. Huckabee (eds.), Mercury Pollution: Integration and Synthesis, Lewis Publishers, Chelsea, MI, pp. 261–271.

    Google Scholar 

  • Lindberg, S. E. and Turner, R. R.: 1988, ‘Factors influencing atmospheric deposition, stream export, and landscape accumulation of trace metals in forested watersheds’, Water Air Soil Pollut. 39, 123.

    CAS  Google Scholar 

  • Lovett, G. M.: 1994, ‘Atmospheric deposition of nutrients and pollutants to North America: An ecological perspective’, Ecol. Appl. 4, 629.

    Google Scholar 

  • Lovett, G. M. and Lindberg, S. E.: 1984, ‘Dry deposition and canopy exchange in a mixed oak forest as determined by analysis of throughfall’, J. Appl. Ecol. 21, 1013.

    Google Scholar 

  • Lucey, D., Hadjiiski, L., Hopke, P. K., Scudlark, J. R. and Church, T.: 2001, ‘Identification of sources of pollutants in precipitation measured at the mid-Atlantic US coast using potential source contribution function (PSCF)’, Atmos. Environ. 35, 3979.

    CAS  Google Scholar 

  • Magill, A. H., Aber, J. D., Bernston, G. M., McDowell, W. H., Nadelhoffer, K. J., Melillo, J. M. and Steudler, P. A.: 2000, ‘Long-term nitrogen additions and nitrogen saturation in two temperate forests’, Ecosystems 3, 238.

    Article  Google Scholar 

  • Matthews, E. D.: 1960, ‘Soil Survey of Frederick County, Maryland’, U.S. Department of Agriculture, Soil Conservation Service, Series 1956, No. 15, 144 pp.

  • McKnight, D. M. and Bencala, K. E.: 1990, ‘The chemistry of iron, aluminum, and dissolved organic material in three acidic, metal-enriched, mountain streams, as controlled by watershed and in-stream processes’, Water Resour. 26, 3087.

    CAS  Google Scholar 

  • National Oceanic & Atmospheric Administration (NOAA): 1981, ‘Division Normals and Standard Deviation of Temperature and Precipitation (1931-80)’, U.S. Department of Commerce, Climatography of the United States, No. 85, 176 pp.

  • Nieminen, T. M., Derome, J. and Helmisaari, H.-S.: 1999, ‘Interactions between precipitation and Scots pine canopies along a heavy metal pollution gradient’, Environ. Pollut. 106, 129.

    CAS  PubMed  Google Scholar 

  • Nriagu, J. O.: 1989, ‘A global assessment of natural sources of atmospheric trace metals’, Nature 338, 47.

    Article  CAS  Google Scholar 

  • Parker, G. G.: 1983, ‘Throughfall and stemflow in the forest nutrient cycle’, Adv. Ecol. Res. 13, 58.

    Google Scholar 

  • Patterson, C. C.: 1965, ‘Contaminated and natural lead environments of man’, Arch. Env. Health 11, 344.

    CAS  Google Scholar 

  • Patterson, C. C. and Settle, D. M.: 1987, ‘Review of data on eolian fluxes of industrial and natural lead to the lands and seas in remote regions on a global scale’, Marine Chem. 22, 137.

    CAS  Google Scholar 

  • Petty, W. H. and Lindberg, S. E.: 1990, ‘An intensive 1-month investigation of trace metal deposition and throughfall at a mountain spruce forest’, Water Air Soil Pollut. 53, 213.

    CAS  Google Scholar 

  • Pierce, M. L. and Moore, C. B.: 1982, ‘Adsorption of arsenite and arsenate on amorphous iron hydroxide’, Water Res. 16, 1247.

    CAS  Google Scholar 

  • Plummer, L. N., Prestemon, E. C. and Parkhurst, D. L.: 1994, ‘An Interactive Code (netpath) for Modeling Net Geochemical Reactions Along a Flow Path Version 2.0’, U.S. Geological Survey Water-Resources Investigations Report 94-4169, 130 pp.

  • Rea, A. W., Keeler, G. J. and Scherbatskoy, T.: 1996, ‘The deposition of mercury in throughfall and litterfall in the Lake Champlain watershed: A short-term study’, Atmos. Environ. 30, 3257.

    CAS  Google Scholar 

  • Rice, K. C. and Bricker, O. P.: 1995, ‘Seasonal cycles of dissolved constituents in streamwater in two forested catchments in the Mid-Atlantic region of the Eastern USA’, J. Hydrol. 170, 137.

    CAS  Google Scholar 

  • Rice, K. C. and Bricker, O. P.: 1996, ‘Hydrologic and Geochemical Factors Affecting the Chemistry of Small Headwater Streams in Response to Acidic Deposition on Catoctin Mountain, North-Central Maryland’, U.S. Geological Survey Water-Resources Investigations Report 95-4155, pp. 63.

  • Rice, K. C., Kennedy, M. M., Bricker, O. P. and Donnelly, C. A.: 1993, ‘Data On the Quantity and Chemical Quality of Precipitation, Catoctin Mountain, North-Central Maryland, 1982–91, U.S. Geological Survey Open-File Report 93–169, pp. 46.

  • Ruhling, A. and Tyler, G.: 1973, ‘Heavy metal pollution and decomposition in spruce needle litter’, Oikos 24, 264.

    Google Scholar 

  • Ryan, P. F., Hornberger, G. M., Cosby, B. J., Galloway, J. N., Webb, J. R. and Rastetter, E. B.: 1989, ‘Changes in the chemical composition of streamwater in two catchments in the Shenandoah National Park, Virginia, in response to atmospheric deposition of sulfur’, Water Resour. Res. 25, 2091.

    CAS  Google Scholar 

  • Salomons, W. and Forstner, U.: 1984, Metals in the Hydrocycle, Springer-Verlag, New York, pp. 349.

    Google Scholar 

  • Scudlark, J. R. and Church, T. M.: 1988, ‘The atmospheric deposition of arsenic and association with acid precipitation’, Atmos. Environ. 22, 937.

    CAS  Google Scholar 

  • Scudlark, J. R. and Church, T. M.: 1997, ‘Atmospheric deposition of trace elements to the Mid-Atlantic Bight’, in J. E. Baker (ed.), Atmospheric Deposition of Contaminants to the Great Lakes and Coastal Waters, SETAC Press, Pensacola, FL, USA, Chap. 10, pp. 195–208.

    Google Scholar 

  • Scudlark, J. R., Church, T. M., Conko, K. M. and Moore, S. M.: 1992, ‘A method for the automated collection, proper handling and accurate analysis of trace metals in precipitation’, in E. S. Verry and S. J. Vermette (eds.), The Deposition of Trace Metals in Our Environment, USDA Forest Service Report NC-150, Philadelphia, PA, USA, October 8, 1991, pp. 57–71.

  • Scudlark, J. R., Conko, K. M. and Church, T. M., 1993, ‘The Wet Deposition of Trace Elements on Delmarva and Their Utility as Emission Source Indicators’, Chesapeake Bay Research and Monitoring Division, Report CBRM-AD-94-3, Annapolis, MD, 80 pp.

  • Scudlark, J. R., Conko, K. M. and Church, T. M.: 1994, ‘Atmospheric wet deposition of trace elements to Chesapeake Bay: CBAD Study year 1 results’, Atmos. Environ. 28, 1487.

    CAS  Google Scholar 

  • Smith, W. H. and Siccama, T. G.: 1981, ‘The Hubbard Brook ecosystem study: Biogeochemistry of lead in the northern hardwood forest’, J. Environ. Qual. 10, 323.

    CAS  Google Scholar 

  • Stumm, W. and Morgan, J. J.: 1981, Aquatic Chemistry, an Introduction Emphasizing Chemical Equilibria in Natural Waters, Wiley-Interscience, New York, 780 pp.

    Google Scholar 

  • Sverdrup, H. U.: 1990, The Kinetics of Base Cation Release Due to Chemical Weathering, Lund University Press, Lund, pp. 246.

    Google Scholar 

  • Tramontano, J. M., Scudlark, J. R. and Church, T. M.: 1987, ‘A method for the collection, handling and analysis of trace metals in precipitation’, Environ. Sci. and Tech. 21, 749.

    CAS  Google Scholar 

  • Turekian, K. K. and Wedepohl, K. H.: 1961, ‘Distribution of the elements in some major units of the earth’s crust’, Geolog. Soc. Am. Bull. 72, 175.

    CAS  Google Scholar 

  • Ukonmaanaho, L., Starr, M., Mannio, J. and Ruoho-Airola, T.: 2001, ‘Heavy metal budgets for two headwater forested catchments in background areas of Finland’, Environ. Pollut. 114, 63.

    CAS  PubMed  Google Scholar 

  • Vossler, T. L., Lewis, C. W., Stevens, R. K., Dzubay, T. G., Gordon, G. E., Tuncel, S. G., Russwurm, G. M. and Keeler, G. J.: 1989, ‘Composition and origin of summertime air pollutants at Deep Creek Lake, Maryland’, Atmos. Environ. 23, 1535.

    CAS  Google Scholar 

  • Wollast, R. and Chou, L.: 1985, ‘Kinetic study of the dissolution of albite with a continuous flow-through fluidized bed reactor’, in J. I. Drever (ed.), The Chemistry of Weathering, D. Reidel Publishing Company, Dordrecht, The Netherlands, pp. 75–76.

    Google Scholar 

  • Wu, Z. Y., Han, M., Lin, Z. C. and Ondov, J. M.: 1994, ‘Chesapeake Bay Atmospheric Deposition Study, Year 1: Sources and dry deposition of selected elements in aerosol particles’, Atmos. Environ. 28, 1471.

    CAS  Google Scholar 

  • Yang, J.-K., Barnett, M. O., Jardine, P. M., Basta, N. T. and Castrell, S. W.: 2002, ‘Adsorption, sequestration and bioaccessibility of As(V) in soils’, Environ. Sci. & Tech. 36, 4562.

    Google Scholar 

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Scudlark, J.R., Rice, K.C., Conko, K.M. et al. Transmission of Atmospherically Derived Trace Elements Through an Undeveloped, Forested Maryland Watershed. Water Air Soil Pollut 163, 53–79 (2005). https://doi.org/10.1007/s11270-005-8135-5

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