Temporal trends of perfluoroalkyl compounds with isomer analysis in lake trout from Lake Ontario (1979-2004)

The temporal trends of perfluoroalkyl compounds (PFCs), including C7-C15 perfluorocarboxylates (PFCAs), perfluorosulfonates (PFSAs) and heptadecafluorooctane sulfonamide (PFOSA), were determined in lake trout collected between 1979 and 2004 from Lake Ontario. The average concentrations of total PFSAs (+/- standard error of the mean; range) increased from 20 ng g(-1) wet weight (+/- 4; 8-26) in 1979, peaked at 70 ng g(-1) (+/- 7; 58-91) in 1993, and were 46 ng g(-1) (+/- 10; 30-83) in 2004, with perfluorooctane sulfonate (PFOS) asthe most abundant PFC. The PFCAs exhibited similar temporal variation, with concentrations increasing from 1.4 ng g(-1) (+/- 0.1; 0.9-1.9) in 1979 to 9.4 ng g(1) (+/- 3.1; 3-17) in 1988, and were 6.8 ng g(-1) (+/- 1.0; 4.5-9.8) in 2004. Individual mean PFCA concentrations varied between 0.2 and 2 ng g(-1) (wet weight). Perfluorodecane sulfonate (PFDS) and PFOSA were the only compounds showing a declining trend in the past decade, after reaching a peak value in 1993. Branched C11 and C13 PFCA isomers were detected in the lake trout and confirmed in Niagara River suspended sediments, with trends in both matrices suggesting that declining emissions or use of products containing these isomers in part account for the observed PFCA trends in the mid-1990s. However, the most recent samples, comprised almost exclusively of linear isomers, indicate that current PFCA sources to Lake Ontario result from the telomerization process of linear telogens.