Abstract
Polyethylene passive samplers (PEs) were used to measure concentrations of gaseous and dissolved polycyclic aromatic hydrocarbons (PAHs) in the air and water throughout the lower Great Lakes during summer and fall of 2011. Atmospheric Σ15PAH concentrations ranged from 2.1 ng/m3 in Cape Vincent (NY) to 76.4 ng/m3 in downtown Cleveland (OH). Aqueous Σ18PAH concentrations ranged from 2.4 ng/L at an offshore Lake Erie site to 30.4 ng/L in Sheffield Lake (OH). Gaseous PAH concentrations correlated strongly with population within 3-40 km of the sampling site depending on the compound considered, suggesting that urban centers are a primary source of gaseous PAHs (except retene) in the lower Great Lakes region. The significance of distant population (within 20 km) versus local population (within 3 km) increased with subcooled liquid vapor pressure. Most dissolved aqueous PAHs did not correlate significantly with population, nor were they consistently related to river discharge, wastewater effluents, or precipitation. Air-water exchange calculations implied that diffusive exchange was a source of phenanthrene to surface waters, while acenaphthylene volatilized out of the lakes. Comparison of air-water fluxes with temperature suggested that the significance of urban centers as sources of dissolved PAHs via diffusive exchange may decrease in warmer months.
Highlights
Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous pollutants that originate from oil spills as well as anthropogenic and natural combustion processes
passive samplers (PEs) were spiked with performance reference compounds (PRCs) via a method adapted from Booij et al.[27] and sent to trained volunteers throughout the Great Lakes region with the aim of completing three 8-week deployments at each site
Gaseous HMW PAHs are expected to have short atmospheric residence times due to reaction with hydroxyl radicals, which may contribute to the increased relevance of local versus long-range sources that was observed for these compounds.[7]
Summary
Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous pollutants that originate from oil spills as well as anthropogenic and natural combustion processes. Gaseous HMW PAHs are expected to have short atmospheric residence times due to reaction with hydroxyl radicals, which may contribute to the increased relevance of local versus long-range sources that was observed for these compounds.[7] These results suggest that reaction with hydroxyl radicals limited the importance of sources distant from sampling sites.
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