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Sources and Deposition of Polycyclic Aromatic Hydrocarbons to Western U.S. National Parks

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Department of Chemistry and Department of Environmental & Molecular Toxicology, Oregon State University, Corvallis, Oregon 97331, Department of Chemistry, University of Otago, Dunedin 9014 New Zealand, United States Department of Agriculture - Forest Service, Pacific Northwest Region Air Program, Corvallis, Oregon 97330, US Geological Survey - Water Resources Division, Denver Federal Center, Lakewood, Colorado, Environmental Radioactivity Research Centre, University of Liverpool, Liverpool L69 3BX, U.K., United States Environmental Protection Agency - Western Ecology Division, Corvallis, Oregon 97333
* Corresponding author phone: +541-737-9194; fax: +541-737-0497; e-mail: [email protected]
†Department of Chemistry, Oregon State University.
‡Department of Environmental & Molecular Toxicology, Oregon State University.
§University of Otago.
∥United States Department of Agriculture - Forest Service.
⊥US Geological Survey - Water Resources Division.
#University of Liverpool.
∇United States Environmental Protection Agency - Western Ecology Division.
¶Current affiliation: Department of Environmental Science, Baylor University, One Bear Place #97266, Waco, Texas 76798.
Cite this: Environ. Sci. Technol. 2010, 44, 12, 4512–4518
Publication Date (Web):May 14, 2010
https://doi.org/10.1021/es903844n
Copyright © 2010 American Chemical Society

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    Abstract

    Seasonal snowpack, lichens, and lake sediment cores were collected from fourteen lake catchments in eight western U.S. National Parks and analyzed for sixteen polycyclic aromatic hydrocarbons (PAHs) to determine their current and historical deposition, as well as to identify their potential sources. Seasonal snowpack was measured to determine the current wintertime atmospheric PAH deposition; lichens were measured to determine the long-term, year around deposition; and the temporal PAH deposition trends were reconstructed using lake sediment cores dated using 210Pb and 137Cs. The fourteen remote lake catchments ranged from low-latitude catchments (36.6° N) at high elevation (2900 masl) in Sequoia National Park, CA to high-latitude catchments (68.4° N) at low elevation (427 masl) in the Alaskan Arctic. Over 75% of the catchments demonstrated statistically significant temporal trends in ΣPAH sediment flux, depending on catchment proximity to source regions and topographic barriers. The ΣPAH concentrations and fluxes in seasonal snowpack, lichens, and surficial sediment were 3.6 to 60,000 times greater in the Snyder Lake catchment of Glacier National Park than the other 13 lake catchments. The PAH ratios measured in snow, lichen, and sediment were used to identify a local aluminum smelter as a major source of PAHs to the Snyder Lake catchment. These results suggest that topographic barriers influence the atmospheric transport and deposition of PAHs in high-elevation ecosystems and that PAH sources to these national park ecosystems range from local point sources to diffuse regional and global sources.

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    Detailed information about the sample sites, radionuclide activity, PAH composition for each site, doubling times, half-lives, ratios of select PAHs, PCA scores and loadings, and the physical and chemical limnological characteristics of each lake site. This material is available free of charge via the Internet at http://pubs.acs.org.

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