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A study of PCB concentrations and fluxes in lake sediments was conducted to test the “global fractionation” hypothesis that deposition of semivolatile organics will decline while more volatile congeners will be enriched in polar regions. Sediment cores were collected from 11 remote lakes in Canada ranging from 49° N to 82° N and were dated using excess 210Pb and 137Cs. Sediment extracts were analyzed for up to 90 PCB congeners by capillary GC-ECD with confirmation by GC/high-resolution MS. Total PCB (∑PCB) concentrations in surface slices ranged from 2.4 to 39 ng g-1 (dry wt) and showed no latitudinal trend. Fluxes (ng m-2 yr-1) and inventories of ∑PCB as well as total tetra- to octachlorobiphenyls declined with increasing north latitude while those for di/trichlorobiphenyls showed no latitudinal trend. The proportion of di/trichloro congeners of ∑PCB also increased significantly with latitude, while total octachlorobiphenyls declined. Maximum ∑PCB concentrations were observed in subsurface slices dating to the 1960−1970s in most lakes except those in the high Arctic, where maxima were generally in surface slices. The onset of elevated ∑PCB deposition was delayed in the high Arctic (1950−1960s) relative to the midlatitude and sub-Arctic lakes (1930−1940s). The high proportions of lower chlorinated congeners and the delayed appearance of PCBs are consistent with predictions of the global fractionation model.

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Sediment cores from six lakes in Canada ranging from 49°N to 81°N were analyzed for C10−C13 polychlorinated n-alkanes (PCAs) with the intent of (i) examining the depositional trends with increasing latitude, (ii) studying the historical profiles and fluxes of PCAs in dated sediment slices, and (iii) investigating possible in situ degradation. Sediment slices were dated using 210Pb and 137Cs, and extracts were analyzed for PCA concentrations by high resolution gas chromatography electron capture negative ion high resolution mass spectrometry (HRGC-ECNI/HRMS) in the selected ion monitoring (SIM) mode. Concentrations of total PCAs in surface sediments declined significantly from 135 ng/g (dry weight (dw)) in sediments from the southern basin of Lake Winnipeg (50°N/96°W, Manitoba) to 4.52 ng/g in Hazen Lake (81°N/71°W, high Arctic); corresponding surficial fluxes were 147 and 0.9 μg/m2 yr, respectively. The high flux of PCAs to the south Lake Winnipeg basin suggests local contamination. This was confirmed by analyzing water collected from the Red River, a river that discharges into the southern basin of Lake Winnipeg, in which elevated levels of PCAs were detected (0.02−0.05 μg/L). The surficial flux of PCAs to Fox Lake (61°N/135°W), a subarctic lake in the Yukon, was also high, 34 μg/m2 yr. Much lower fluxes were found in Lake Nipigon (49°N/89°W, N. Ontario), 3 μg/m2 yr, the northern basin of Lake Winnipeg (52°N/98°W, Manitoba), 4 μg/m2 yr, and to Ya Ya Lake (69°N/134°W, Arctic) 0.45 μg/m2 yr. The remote locations of Hazen and Ya Ya Lakes and the low levels of PCAs observed in their corresponding sediment slices are consistent with long-range atmospheric transport. The profiles of PCAs in the midcontinental lakes showed maxima in slices dated from the early 1980s to the 1990s while that of ΣDDT showed a maxima in the 1960s. The presence of PCAs in surface sediments over a wide geographic area, including the Canadian Arctic, suggests that these compounds, which are components of commercial short chain chlorinated paraffins, are regionally and globally distributed by long-range atmospheric transport.

Concentrations of toxaphene and other organochlorine compounds are high in fishes from subarctic Lake Laberge, Yukon Territory, Canada. Nitrogen isotope analyses of food chains and contaminant analyses of biota, water, and dated lake sediments show that the high concentrations of toxaphene in fishes from Laberge resulted entirely from the biomagnification of atmospheric inputs. A combination of low inputs of toxaphene from the atmosphere and transfer through an exceptionally long food chain has resulted in concentrations of toxaphene in fishes that are considered hazardous to human health.

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