Contribution of PAHs from coal-tar pavement sealcoat and other sources to 40 U.S. lakes

Contamination of urban lakes and streams by polycyclic aromatic hydrocarbons (PAHs) has increased in the United States during the past 40 years. We evaluated sources of PAHs in post-1990 sediments in cores from 40 lakes in urban areas across the United States using a contaminant mass-balance receptor model and including as a potential source coal-tar-based (CT) sealcoat, a recently recognized source of urban PAH. Other PAH sources considered included several coal- and vehicle-related sources, wood combustion, and fuel-oil combustion. The four best modeling scenarios all indicate CT sealcoat is the largest PAH source when averaged across all 40 lakes, contributing about one-half of PAH in sediment, followed by vehicle-related sources and coal combustion. PAH concentrations in the lakes were highly correlated with PAH loading from CT sealcoat (Spearman's rho=0.98), and the mean proportional PAH profile for the 40 lakes was highly correlated with the PAH profile for dust from CT-sealed pavement (r=0.95). PAH concentrations and mass and fractional loading from CT sealcoat were significantly greater in the central and eastern United States than in the western United States, reflecting regional differences in use of different sealcoat product types. The model was used to calculate temporal trends in PAH source contributions during the last 40 to 100 years to eight of the 40 lakes. In seven of the lakes, CT sealcoat has been the largest source of PAHs since the 1960s, and in six of those lakes PAH trends are upward. Traffic is the largest source to the eighth lake, located in southern California where use of CT sealcoat is rare.