Polychlorinated biphenyls and organochlorine pesticides concentration patterns and trends in top predator fish of Laurentian Great Lakes from 1999 to 2014

Concentration patterns and temporal trends of legacy persistent, bioaccumulative and toxic (PBT) contaminants were determined using the Great Lake Fish Monitoring and Surveillance Program (GLFMSP) top predator fish data from 1999 to 2014 and applying Kendall-Theil robust regression after cluster-based age normalization. For most Great Lakes sites, significant decreasing concentration trends ranging from −4.1% to −21.6% per year (with the only exception being mirex in Lake Erie walleye) were found for PBTs including polychlorinated biphenyls (PCBs), dichloro-diphenyl-trichlorethane (DDTs), dieldrin, endrin, chlordane, oxychlordane, nonachlor, mirex, and hexachlorobenzene (HCB) reflecting the successful historical and ongoing reduction of fugitive releases and remediation efforts in the U.S. and Canada including physical removal (dredging) coupled with sediment sequestration. Generally, lower concentrations and faster decreasing trends are observed in western/northern sampling sites compared to eastern/southern sites as the former sites are generally more remote from population centers and industrial activities. PCBs, which can be released from ongoing sources, have the highest concentration, the second slowest decreasing trend, and increasing mass fractions of the contaminants studied suggesting that they will continue to be the legacy contaminant of greatest concern into the future.