Abstract

The atmospheric concentrations of PCDDs and PCDFs were measured in four sites near the shores of the North American Great Lakes. The sites included an urban site (Chicago, Illinois) and three rural/remote sites (Eagle Harbor, Michigan; Sleeping Bear Dunes, Michigan; and Sturgeon Point, New York). Sampling occurred every 24 days between November 2004 and December 2007. The concentration of PCDD/Fs averaged 2.3 +/- 0.2 fg WHO TEQ/m3 at Eagle Harbor, 35 +/- 3 fg WHO TEO/ m3 at Chicago, 7.4 +/- 1.4 fg WHO TEO/m3 at Sleeping Bear Dunes, and 13 +/- 2 fg WHO TED/m3 at Sturgeon Point. The total concentration of the 17 toxic PCDD/F congeners showed a significant seasonal trend at all sites, except Chicago. The date of maximum concentration averaged Dec 6 +/- 35 days, which is consistent with residential heating being an important source of PCDD/Fs to the atmosphere. A significant positive relationship between the logarithm of the total concentration of the 17 toxic PCDD/F congeners and the logarithm of the number of people within a 25 km radius around the sampling site was found. We suggest that urban and industrial areas, which are heavily populated, act as sources of PCDDs and PCDFs to the atmosphere.

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