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Long-Range Atmospheric Transport of Polycyclic Aromatic Hydrocarbons: A Global 3-D Model Analysis Including Evaluation of Arctic Sources

Author(s)
Friedman, Carey; Selin, Noelle E
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Abstract
We use the global 3-D chemical transport model GEOS-Chem to simulate long-range atmospheric transport of polycyclic aromatic hydrocarbons (PAHs). To evaluate the model’s ability to simulate PAHs with different volatilities, we conduct analyses for phenanthrene (PHE), pyrene (PYR), and benzo[a]pyrene (BaP). GEOS-Chem captures observed seasonal trends with no statistically significant difference between simulated and measured mean annual concentrations. GEOS-Chem also captures variability in observed concentrations at nonurban sites (r = 0.64, 0.72, and 0.74, for PHE, PYR, and BaP). Sensitivity simulations suggest snow/ice scavenging is important for gas-phase PAHs, and on-particle oxidation and temperature-dependency of gas-particle partitioning have greater effects on transport than irreversible partitioning or increased particle concentrations. GEOS-Chem estimates mean atmospheric lifetimes of <1 day for all three PAHs. Though corresponding half-lives are lower than the 2-day screening criterion for international policy action, we simulate concentrations at the high-Arctic station of Spitsbergen within four times observed concentrations with strong correlation (r = 0.70, 0.68, and 0.70 for PHE, PYR, and BaP). European and Russian emissions combined account for 80% of episodic high-concentration events at Spitsbergen.
Date issued
2012-08
URI
http://hdl.handle.net/1721.1/82191
Department
Massachusetts Institute of Technology. Center for Global Change Science; Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences; Massachusetts Institute of Technology. Engineering Systems Division
Journal
Environmental Science & Technology
Publisher
American Chemical Society (ACS)
Citation
Friedman, Carey L., and Noelle E. Selin. “Long-Range Atmospheric Transport of Polycyclic Aromatic Hydrocarbons: A Global 3-D Model Analysis Including Evaluation of Arctic Sources.” Environmental Science & Technology 46, no. 17 (September 4, 2012): 9501-9510.
Version: Author's final manuscript
ISSN
0013-936X
1520-5851

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