The transport of beta-hexachlorocyclohexane to the western Arctic Ocean: a contrast to alpha-HCH.

A large database for alpha-hexachlorocyclohexane (alpha-HCH), together with multimedia models, shows this chemical to have exhibited classical 'cold condensation' behavior. The surface water of the Arctic Ocean became loaded between 1950 and 1990 because atmospheric transport of alpha-HCH from source regions to the Arctic was rapid and because alpha-HCH partitioned strongly into cold water there. Following emission reductions during the 1980s, alpha-HCH remained trapped under the permanent ice pack, with the result that the highest oceanic concentrations in the early 1990s were to be found in surface waters of the Canada Basin. Despite a much stronger partitioning into water than for alpha-HCH, beta-HCH did not accumulate under the pack ice of the Arctic Ocean, as might be expected from the similar emission histories for the two chemicals. Beta-HCH appears to have loaded only weakly into the high Arctic through the atmosphere because it was rained out or partitioned into North Pacific surface water. However, beta-HCH has subsequently entered the western Arctic in ocean currents passing through Bering Strait. Beta-HCH provides an important lesson that environmental pathways must be comprehensively understood before attempting to predict the behavior of one chemical by extrapolation from a seemingly similar chemical.

Contaminants in the Canadian Arctic: 5 years of progress in understanding sources, occurrence and pathways.

Recent studies of contaminants under the Canadian Northern Contaminants Program (NCP) have substantially enhanced our understanding of the pathways by which contaminants enter Canada's Arctic and move through terrestrial and marine ecosystems there. Building on a previous review (Barrie et al., Arctic contaminants: sources, occurrence and pathways. Sci Total Environ 1992:1-74), we highlight new knowledge developed under the NCP on the sources, occurrence and pathways of contaminants (organochlorines, Hg, Pb and Cd, PAHs, artificial radionuclides). Starting from the global scale, we examine emission histories and sources for selected contaminants focussing especially on the organochlorines. Physical and chemical properties, transport processes in the environment (e.g. winds, currents, partitioning), and models are then used to identify, understand and illustrate the connection between the contaminant sources in industrial and agricultural regions to the south and the eventual arrival of contaminants in remote regions of the Arctic. Within the Arctic, we examine how contaminants impinge on marine and terrestrial pathways and how they are subsequently either removed to sinks or remain where they can enter the biosphere. As a way to focus this synthesis on key concerns of northern residents, a number of special topics are examined including: a mass balance for HCH and toxaphene (CHBs) in the Arctic Ocean; a comparison of PCB sources within Canada's Arctic (Dew Line Sites) with PCBs imported through long-range transport; an evaluation of concerns posed by three priority metals--Hg, Pb and Cd; an evaluation of the risks from artificial radionuclides in the ocean; a review of what is known about new-generation pesticides that are replacing the organochlorines; and a comparison of natural vs. anthropogenic sources of PAH in the Arctic. The research and syntheses provide compelling evidence for close connectivity between the global emission of contaminants from industrial and agricultural activities and the Arctic. For semi-volatile compounds that partition strongly into cold water (e.g. HCH) we have seen an inevitable loading of Arctic aquatic reservoirs. Drastic HCH emission reductions have been rapidly followed by reduced atmospheric burdens with the result that the major reservoir and transport agent has become the ocean. In the Arctic, it will take decades for the upper ocean to clear itself of HCH. For compounds that partition strongly onto particles, and for which the soil reservoir is most important (e.g. PCBs), we have seen a delay in their arrival in the Arctic and some fractionation toward more volatile compounds (e.g. lower-chlorinated PCBs). Despite banning the production of PCB in the 1970s, and despite decreases of PCBs in environmental compartments in temperate regions, the Arctic presently shows little evidence of reduced PCB loadings. We anticipate a delay in PCB reductions in the Arctic and environmental lifetimes measured in decades. Although artificial radionuclides have caused great concern due to their direct disposal on Russian Shelves, they are found to pose little threat to Canadian waters and, indeed, much of the radionuclide inventory can be explained as remnant global fallout, which was sharply curtailed in the 1960s, and waste emissions released under license by the European reprocessing plants. Although Cd poses a human dietary concern both for terrestrial and marine mammals, we find little evidence that Cd in marine systems has been impacted by human activities. There is evidence of contaminant Pb in the Arctic, but loadings appear presently to be decreasing due to source controls (e.g. removal of Pb from gasoline) in Europe and North America. Of the metals, Hg provokes the greatest concern; loadings appear to be increasing in the Arctic due to global human activities, but such loadings are not evenly distributed nor are the pathways by which they enter and move within the Arctic well understood.

Melting glaciers: a major source of persistent organochlorines to subalpine Bow Lake in Banff National Park, Canada.

Organochlorine pesticides and polychlorinated biphenyls (PCBs) are ubiquitous and persistent in the environment. They are known to concentrate in cold environments as a result of progressive evaporation from warm regions, and condensation in colder regions. In this study we show that melting glaciers supply 50 to 97% of the organochlorine inputs to a subalpine lake in Alberta, Canada, while contributing 73% of input water. Tritium analyses indicated that during the mid- to late summer warm period, at least 10% of the glacial melt originated from ice that was deposited in 1950-1970, when it was more contaminated with organochlorines. This finding suggests that climate warming may cause melting glaciers to become increasing sources of contaminants to freshwaters. Organochlorines from glacial streams were largely in dissolved form because the organic-poor glacial clays had a limited sorption capacity for the more hydrophobic chemicals.

Spatial differences in persistent organochlorine pollutant concentrations between the Bering and Chukchi Seas (1993).

During August-September 1993, a joint Russian-United States expedition to the Bering and Chukchi Seas took place. Surface water samples were collected from 21 sites and separated into dissolved (duplicates) and suspended solids; 19 sediment and 6 air samples were also collected. These samples were analysed for 19 organochlorine pesticides, 11 chlorobenzenes and 113 PCB congeners. The report provides data on selected compounds which occured in > or = 75% of the water samples. Highest water concentrations were observed for HCH in open waters north and south of the Bering Strait, both regions being similar (alpha-HCH; 2.2 ng/L and lindane: 0.35 ng/L). Air levels observed were also constant (alpha-HCH; 0.041 ng/m3, lindane: 0.0093 ng/m3). Suspended solids and air particulares contributed little to the concentrations in their respective media, an observation common to all analytes except for the PCBs and the DDT residues. The sum of PCB concentrations in water were higher in the Bering Sea area compared to the Chukchi Sea (1.0 vrs 0.67 ng/L) and lower for air (0.46 vrs 0.23 ng/m3). Sum of DDT in water was higher in the Bering Sea than in the Chukchi Sea (0.23 vrs 0.15 ng/L) while in sediments and air, the Bering Sea concentrations were lower (0.95 vrs 1.6 ng/g and 36 vrs 56 pg/m3, respectively). Other organochlorine compounds for which data are presented include: pp'-DDE, pp'-DDT, dieldrin, HCB, 3 chlorobenzenes and 3 PCB congeners. Fluxes of all these chemicals through the Berin Strait are estimated; they ranged from 57 t/a (alpha-HCH) through 26 t/a (for sum of PCBs) to 0.2 t/a (pp'-DDE, dieldrin and 1,2,3-trichlorobenzene). Fugacity ratios for the HCHs and PCBs indicate the alpha-HCH is degassing in both the Bering and Chukchi Seas and that the gamma-isomer is degassing in the Bering Sea and is close to equilibrium (weakly absorbing) in the Chuchi Sea; the sum of PCBs are strongly absorbing in both areas.

Organochlorine pesticide and trace metal monitoring of Russian rivers flowing to the Arctic Ocean: 1990-1996.

Information is presented on the concentrations of organochlorine pesticides (HCHs and DDT residues) and trace metals (Fe, Cu, Zn and Ni) in waters of 15 large Russian rivers flowing to the Arctic Ocean during 1990-1996. Estimates of the corresponding annual fluxes are made. Other contaminants (Hg, Pb, Cr, Mn, beta-HCH and dihydroheptachlor) were examined briefly. Concentration data are presented as averaged annual means for each of the seven years with the ranges, standard deviations and numbers of samples. Also given are data on locations, the methods of analysis and limited quality assurance data. Data on discharges to the Northern Seas for the more frequently monitored contaminants are given for rivers accounting for >70% of the total northerly flows. Scaled-up fluxes to account for unmonitored rivers as well are given for each sea; totals over the period were: Fe, 1452; Cu, 15; Zn, 59 (x 10(3) t yr(-1)); alpha-HCH, 25; gamma-HCH, 44 (t yr(-1)). Ni was monitored at too few rivers to estimate its total Russian flux. The fluxes for the HCHs considerably exceed previous estimates and indicate that the Arctic Ocean is not in balance as much as was previously believed.

Distribution of pesticides and polychlorinated biphenyls in water, sediments, and seston of the upper Great Lakes--1974.

Samples of water, seston, and sediment from the upper Great Lakes were collected during the summer of 1974 for analyses of polychlorinated biphenyls (PCS's), 15 organochlorine pesticides, and 17 organophosphorus pesticides. Samples were taken from 9 sites in Lake Huron, 2 in the North Channel, 5 in Georgian Bay, and 17 in Lake Superior. In the water samples all compounds analyzed were below quantification limits and traces of lindane were found in each sample. In seston samples, PCB's were above quantification limits at nearly every station and some traces of dieldrin and DDE were measured. Sediments contained PCB compounds at all stations. Dieldrin was occasionally observed, and DDT and/or its derivatives DDE and TDE were found in over one-third of all samples. No clear correlation was found between quantities of these compounds in sediments and either the percentage of clay or organic matter in the samples. Nor were any definite geographic trends present in terms of distributions observed, although concentrations were higher in areas of higher sedimentary deposition such as deeper basins. No organophosphorus compounds were detected in any sample. The highest level of DDT residues detected, 20 ppb, was lower than levels found in other studies in the lower Great Lakes and some tributary river sediments of Georgian Bay. In general, DDT residues were higher in Lake Huron and Georgean Bay sediments than in Lake Superior although PCB's were higher in some Lake Superior sediments.