Pan-arctic river fluxes of polychlorinated biphenyls

Observations of polychlorinated biphenyls (PCB) concentrations in fluvial surface sediments near the mouths of the six Great Arctic Rivers (GARs; Ob, Yenisey, Lena, Indigirka, Kolyma, and Mackenzie) were combined with annual dissolved organic carbon (DOC) and particulate organic carbon (POC) loadings and hydraulic discharge to estimate the pan-Arctic river flux of PCBs. The highest total-phase fluxes of ∑(13)PCB were found for the Ob River, with 184 kg/yr and the smallest for the Indigirka River with 3.9 kg/yr. Consistent with a continent-scale trend among the Eurasian GARs of increasing POC concentrations eastward, which is extending to the North American Mackenzie River, a general shift in the estimated PCB partitioning from dissolved to particle-associated flux was found toward the east. Pentachlorinated and hexachlorinated PCBs constituted the majority (>70%) of the total PCB fluxes in the Eurasian Rivers. In contrast, trichlorinated and tetrachlorinated congeners were the most abundant in the Mackenzie (≈ 75%). The total ∑(13)PCB fluxes from the pan-Arctic rivers are here estimated to be ∼0.4 tonne/yr. This is geochemically consistent with the inventory of total PCBs in the Polar Mixed Layer of the entire Arctic Ocean (0.39 tonne) and about a factor 2 less than two new estimates of the PCB settling export to Arctic subsurface waters. Hence, the yearly Great Arctic River PCB fluxes only represent 0.001% of the historical PCB emission into the global environment. To our knowledge, this is the first estimate of circum-Arctic river flux of any organic pollutant based on a comprehensive investigation of the pollutants in several rivers and it contributes toward a more complete understanding of large-scale contaminant cycling in the Arctic.