Polycyclic Aromatic Hydrocarbons in the Atmosphere near the Great Lakes: Why Do Their Concentrations Vary?

Polycyclic aromatic hydrocarbon (PAH) concentrations were measured in atmospheric samples collected at five sites near the shores of the North American Great Lakes once every 12 days from 1997 to 2018 (inclusive). These data were analyzed using multiple linear regression statistics to isolate the environmental variables controlling these PAH concentrations. About 74% of the variability is related to the number of people living and working within 25 km of the sampling site. Clearly, urban areas are major sources of PAH to the atmosphere. PAH concentrations at all sites lumped together are decreasing with halving times of about 25 years, and this factor represents about 1.5% of the variability. This is slower than the halving times for most banned compounds because PAH continue to be emitted directly into the atmosphere from many combustion sources. In the atmosphere, the concentrations of relatively volatile PAH maximize in July, but those of relatively nonvolatile PAH maximize in January. This seasonality factor represents about 2.5% of the variability. PAH concentrations at these Great Lakes sites tend to be elevated when the wind is coming out of the south-southeast, and this factor represents about 1.2% of the variability. PAH concentrations are lower when the wind speed is higher; this is a significant but small effect, representing only about 0.17% of the variability. The sum of these partial variabilities is about 80%, which suggests that the measurement and sampling errors are about 20%, which is a reasonable value. On the basis of two approaches, the range of atmospheric PAH transport from these sites is estimated to be on the order of 100-200 km. For these data, meteorology matters, but not by much.