Abstract
Polycyclic aromatic hydrocarbons (PAHs) are among the most widespread and potentially toxic contaminants in Great Lakes (USA/Canada) tributaries. The sources of PAHs are numerous and diverse, and identifying the primary source(s) can be difficult. The present study used multiple lines of evidence to determine the likely sources of PAHs to surficial streambed sediments at 71 locations across 26 Great Lakes Basin watersheds. Profile correlations, principal component analysis, positive matrix factorization source‐receptor modeling, and mass fractions analysis were used to identify potential PAH sources, and land‐use analysis was used to relate streambed sediment PAH concentrations to different land uses. Based on the common conclusion of these analyses, coal‐tar–sealed pavement was the most likely source of PAHs to the majority of the locations sampled. The potential PAH‐related toxicity of streambed sediments to aquatic organisms was assessed by comparison of concentrations with sediment quality guidelines. The sum concentration of 16 US Environmental Protection Agency priority pollutant PAHs was 7.4–196 000 µg/kg, and the median was 2600 µg/kg. The threshold effect concentration was exceeded at 62% of sampling locations, and the probable effect concentration or the equilibrium partitioning sediment benchmark was exceeded at 41% of sampling locations. These results have important implications for watershed managers tasked with protecting and remediating aquatic habitats in the Great Lakes Basin. Environ Toxicol Chem 2020;39:1392–1408. © 2020 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
Highlights
Representing 84% of the fresh surface water in North America (US Environmental Protection Agency 2015), the Great Lakes are an invaluable natural resource to the United States and Canada
Within 48 h of collection, samples were shipped to the Battelle Memorial Institute (Norwell, MA, USA) for analysis of 18 parent and 18 alkylated Polycyclic aromatic hydrocarbons (PAHs) (Supplemental Data, Table S2) via gas chromatography mass– spectrometry operated in selected ion monitoring mode
All PAH and total organic carbon (TOC) results are provided in the Supplemental Data, Table S6
Summary
Representing 84% of the fresh surface water in North America (US Environmental Protection Agency 2015), the Great Lakes are an invaluable natural resource to the United States and Canada. A history of industrial, agricultural, and household pollution has left a legacy of contaminated sediments in many areas of the Great Lakes and their tributaries. The PAHs are a class of >100 organic compounds composed of 2 or more fused aromatic rings. They are widespread contaminants with sources both historical and modern, and both natural and anthropogenic. Anthropogenic sources of pyrogenic PAHs include residential wood burning, exhausts from diesel and gasoline engines, and emissions from coal‐fired power plants and coke‐ovens, creosote, and coal tar from pavement sealants and former manufactured gas plants (Mahler et al 2005; Neff et al 2005; Pietara et al 2010)
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