Bioaccumulation and Spatiotemporal Trends of Polyhalogenated Carbazoles in Great Lakes Fish from 2004 to 2016

Polyhalogenated carbazoles (PHCZs) were recently discovered in Great Lakes sediment and other aquatic systems. However, knowledge about their bioaccumulation and potential risks to fish and wildlife remains very limited. The present study investigated PHCZs in Great Lakes lake trout (Salvelinus namaycush) and walleye (Sander vitreus; Lake Erie only) composites collected between 2004 and 2016. Median concentrations of Sigma PHCZs by lake ranged from 54.7 to 154 ng/g lipid weight or lw (6.8-28.0 ng/g wet weight). Dominant congeners included 3,6-dichlorocarbazole, 1,3,6-tribromocarbazole, and 1,3,6,8-tetrachlorocarbazole. The highest Sigma PHCZs concentrations were found in Lakes Michigan and Ontario fish, followed by Lake Huron, whereas Lakes Erie and Superior fish contained the lowest concentrations. Congener profiles of PHCZs also exhibited spatial variations. After age normalization to minimize fish age influence on bioaccumulation rates, fish Sigma PHCZs' concentrations declined significantly over time in all lakes except Lake Erie, with slopes ranging from -10.24% to -3.8S% per year. The median toxic equivalent (TEQ) of PHCZs due to their dioxin-like activity was determined to range from 8.7 to 25.7 pg/g lw in Great Lakes fish. This study provides the first insight into the bioaccumulation and spatiotemporal trends of PHCZs in Great Lakes and suggests the need for further research on this group of chemicals.