Chlorinated Polycyclic Aromatic Hydrocarbons in Sediments from Industrial Areas in Japan and the United States

Abstract

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) are widespread environmental pollutants in the urban environment. Nevertheless, there is little information available regarding the occurrence and profiles of ClPAHs in environmental matrices. In this study, residual concentrations and profiles of 20 individual ClPAHs and 16 US EPA-priority PAHs were determined using high- resolution gas chromatography-high-resolution mass spectrometry in sediments from water bodies near industrialized areas: Tokyo Bay, Japan; the Saginaw River watershed, Michigan, USA; a former chlor-alkali plant, Georgia, USA; and the New Bedford Harbor Superfund site, Massachusetts, USA. A sediment core from Tokyo Bay showed temporal patterns in the distribution of ClPAHs from the 1950s through 2004. The fluxes of ClPAHs and 16 priority PAHs in Tokyo Bay sediment core were 0.029-0.57 ng/cm(2)/year and 85-609 ng/cm(2)/year, respectively; fluxes were lowest in the 1950s and highest in 1989-1990. In the United States, a high mean concentration of ClPAHs was found in sediment collected near a former chlor-alkali plant [8820 pg/g dry weight (dry wt)], and lower mean concentrations were found for New Bedford Harbor (1880 pg/g dry wt) and the Saginaw River watershed (1140 pg/g dry wt). Among individual ClPAHs, 6-ClBaP and 1-ClPyr were the dominant compounds in sediments; this pattern is similar to the pattern reported in the literature for waste incineration and ambient urban air samples. Significant correlation between SigmaClPAH concentrations and Sigmaparent-PAH concentrations in Tokyo Bay sediment implies that the sources and distribution of ClPAHs are directly related to those of parent PAHs. We also analyzed ClPAHs and parent PAHs in blue mussels from New Bedford Harbor. The mean concentration of ClPAHs in mussels from New Bedford Harbor was 21 ng/g lipid weight, a concentration three orders of magnitude lower than the mean concentration of parent PAHs. Low-molecular-weight ClPAHs predominated in mussel tissues. Toxic equivalents (TEQs) of ClPAHs analyzed in sediment ranged between 1.1 fg TEQ/g dry wt (Tokyo Bay) and 2.4 fg TEQ/g dry wt (Saginaw River watershed). The dioxinlike toxicity contributed by ClPAHs in sediment from contaminated areas was five orders of magnitude lower than that previously reported for dioxins.