Congener specific PCB and toxaphene (polychlorinated camphene, PCC) analyses were performed in seal blubber, collected in Svalbard, Norway. The concentration, body burden and metabolic index (PCB congener concentration in seal relative to their prey) were calculated. Multiple regression analyses were carried out to evaluate the influence of age, sex, blubber (as a percentage of total body weight) and cytochrome P450 activities on PCB and PCC levels. Levels of total PCBs found were five times higher than in ringed seals from the Canadian Arctic, corresponding with the relatively high contaminant levels in the European Arctic. The dominant PCB congeners (> 70% of the total PCBs measured) were 153, 138, 99, 180 and 101. The observed PCB and PCC accumulation patterns were very similar to patterns in seals from other studies, suggesting a large resemblance in contaminant metabolism. A decrease in the relative abundance of the lower chlorinated PCBs, was associated with higher concentrations of PCB 153. Since there was no indication for selective PCB excretion by lactating females, this suggests metabolism of these PCBs in ringed seals due to xenobiotic metabolising enzymes. The metabolic index confirmed the model of persistency of the different PCBs except for congener 128 and 138. These congeners, considered persistent in seals, could to some extent be metabolised in ringed seals. However, co-elution of PCB 138 with PCB 163 and of PCB 128 with TOX 50 possibly has resulted in an underestimation of the metabolic index for these congeners. Multiple regression analyses revealed a significant positive effect of age and a negative effect of the blubber content on the PCB concentrations. Since large fluctuations of body lipids occur between seasons in pinnipeds, PCB measurements should account for the total blubber content to avoid biased results. PCBs with vicinal H-atoms in the o, m or the m, p positions showed in addition a relation with cytochrome P450 enzyme activities. Surprisingly, no effect of sex on the PCB concentrations was observed, probably because female ringed seals, unlike other pinnipeds, continue feeding during lactation. This results in only small amounts of lipid and lipid-associated contaminants being mobilised from the blubber. Consequently, contaminant excretion with the milk will be low. Toxaphene concentrations found were low compared to levels found in the Canadian Arctic. Two congeners, TOX 26 and TOX 50 were predominant (15 and 18%, respectively of total toxaphene). There was no effect of sex, age, total blubber, or cytochrome P450 activities on the toxaphene levels. There was also no correlation between toxaphene and PCB levels, which may indicate differences in exposure and metabolism between these contaminants. Toxaphenes did not bioaccumulate to any substantial extent in ringed seals.
The potential health effects of environmental contaminants in traditional food has become a concern among northern communities because of the presence of environmental contaminants in the Arctic ecosystem. Exposure assessments are needed but they require comprehensive dietary information and contaminant data. Over the last 10 years, there has been considerable effort to monitor the level of contaminants in fish and wildlife collected from different regions in northern and Arctic Canada. The development of a database and its application for dietary contaminant exposure assessment are described. We conducted an extensive literature review on levels of environmental contaminants in northern and Arctic Canada. The ranges of levels of four contaminants of major concern (chlordane, mercury, polychlorinated biphenyls and toxaphene) in 81 species of marine mammals, terrestrial mammals, birds, fish and plants are summarized. These data represent 69% of the 117 species of fish, wildlife and plants mentioned in our dietary interviews conducted in the northern communities. A significant percentage of the foods had contaminant levels exceeding the guidelines used by Health Canada for market food consumed by the 'southern' populations. Mathematic modelling of the distributions of the data showed that contaminant levels in most food groups are log-normally distributed and have a typical coefficient of variation of about 100%. Examples are presented to demonstrate the use of the data for contaminant exposure assessment. Average contaminant exposure levels estimated using the database for two communities are comparable to those obtained previously using community specific data. With the current knowledge of environmental contaminant levels in the northern traditional food system, it may be feasible to conduct preliminary risk assessment of dietary exposure of environmental contaminants when some diet information for a community is available. Further sampling and analysis may be needed only for confirmation purposes.
Toxaphene production, in quantities similar to those of polychlorinated biphenyls, has resulted in high toxaphene levels in fish from the Great Lakes and in Arctic marine mammals (up to 10 and 16 microg g-1 lipid). Because of the large variabiliity in total toxaphene data, few reliable conclusions can be drawn about trends or geographic differences in toxaphene concentrations. New developments in mass spectrometric detection using either negative chemical ionization or electron impact modes as well as in multidimensional gas chromatography recently have led researchers to suggest congener-specific approaches. Recently, several nomenclature systems have been developed for toxaphene compounds. Although all systems have specific advantages and limitations, it is suggested that an international body such as the International Union of Pure and Applied Chemistry make an attempt to obtain uniformity in the literature. Toxicologic information on individual chlorobornanes is scarce, but some reports have recently appeared. Neurotoxic effects of toxaphene exposure such as those on behavior and learning have been reported. Technical toxaphene and some individual congeners were found to be weakly estrogenic in in vitro test systems; no evidence for endocrine effects in vivo has been reported. In vitro studies show technical toxaphene and toxaphene congeners to be mutagenic. However, in vivo studies have not shown genotoxicity; therefore, a nongenotoxic mechanism is proposed. Nevertheless, toxaphene is believed to present a potential carcinogenic risk to humans. Until now, only Germany has established a legal tolerance level for toxaphene--0.1 mg kg-1 wet weight for fish.
Organochlorines and heavy metals have bioaccumulated in Arctic wildlife, which is an important food source for the Inuit. In this study, we have developed a statistical model to describe the population distribution of contaminant exposure and the usual intake of the high-end contaminant consumers. Monte Carlo methods are used to account for variations due to seasonal dietary pattern and contaminant concentrations. Distribution of the dietary intake of the contaminants of most concern-mercury, polychlorinated biphenyls (PCBs), chlordane, and toxaphenes-are described. Over 50% of the residents had dietary exposure levels exceeding the tolerable daily intake or provisional tolerable daily intake for Hg, toxaphene, and chlordane (83, 91, and 71% for men and 73, 85, and 56% for women, respectively). The high-end consumers (i.e. the 95th centile) have intake levels 6 times higher than the provisional tolerable weekly intake of Hg, and over 20 times the tolerable daily intake of chlordane and toxaphene. Assessment of health risks of the relative high contaminant exposure in this community must also consider the nutritional, economical, cultural, and social importance of these traditional foods. A comprehensive risk management scheme has yet to be developed.
The concentrations of HCB, alpha-, beta- and gamma-HCH, 3 chlordanes (CHLs), p,p'-DDE, p,p'-DDD, p,p'-DDT, and 30 PCBs (polychlorinated biphenyls) were determined in 140 human milk samples from Kargopol (n=19), Severodvinsk (n=50), Arkhangelsk (n=51) and Naryan-Mar (n=20). Pooled samples were used for determination of three toxaphenes (chlorobornanes, CHBs). The concentrations of HCB, beta-HCH and p,p'-DDE in Russian human milk were 2, 10 and 3 times higher than corresponding levels in Norway, respectively, while concentrations of sum-PCBs and sum-TEQs (toxic equivalent quantities) of the mono-ortho substituted PCBs were in the same range as corresponding levels in Norway. The PCB-156 contributed most to the sum-TEQs. Highest mean concentrations of HCB (129 microg/kg milk fat) and sum-PCBs (458 microg/kg milk fat) were detected in Naryan-Mar, while highest mean concentrations of sum-HCHs (408 microg/kg milk fat), sum-CHLs (48 microg/kg milk fat), sum-DDTs (1392 microg/kg milk fat) and sum-toxaphenes (13 microg/kg milk fat) were detected in Arkhangelsk. An eastward geographic trend of increasing ratios of alpha/beta-HCH, gamma/beta-HCH, p,p'-DDT/p,p'-DDE and PCB-180/28 was observed. In all areas the levels of sum-HCHs decreased with parity (number of children born). Considerable variation in levels of the analysed organochlorines (OCs) was found in all the studied areas. Breast milk from mothers nursing their second or third child (multiparas) in Naryan-Mar showed a significant different PCB profile compared to mothers giving birth to their first child (primiparas) from the same area and to primi- and multiparas in the other areas. Both p,p'-DDE and p,p'-DDT showed a significant, but weak, negative correlation with the infants birth weight.
One hundred and five human adipose tissue samples were recovered during surgical operations or postmorten examinations of patients experiencing death due to traumatic injury. The sample donors were between the ages of 2 mo and 91 yr. Samples were analyzed by GLC-MS techniques for polychlorobiophenyl (PCB) and dichlorodiphenyl trichloroethane (DDT) compounds, chlordanes, hexachlorobenzene, and chlorinated phenols. Special attention was paid to the concentration of hepatchlor epoxide, a metabolite of heptachlor, commonly used as an insecticide in the Finnish plywood industry. The mean concentrations of PCB, DTTs, HCB, and chlordanes were 0.26, 0.33, 0.02, and 0.007 mg/kg fresh weight, respectively, while the mean concentration of heptachlor epoxide was 2.3 micrograms/kg. The geometric means were 0.20, 0.28, 0.018, 0.0055, and 0.002 mg/kg, respectively. The concentrations of PCB and DDT compounds in Finnish human adipose tissue has rapidly decreased during the last 10 yr. The average concentrations were higher in south Finland than those in north Finland, and the results clearly indicate the prominent influence of fish meals and the age of sample donors on the pollutant concentrations in adipose tissue. The results were further analyzed and discussed with respect to sex, smoking habits, and number of childbirths of the sample donors.
Harbor porpoises from the German North and Baltic Seas exhibit a higher incidence of bacterial infections compared to whales from less polluted arctic waters. The potential adverse effect of environmental contaminants such as polychlorinated biphenyls (PCBs) and heavy metals on the immune system and the health status of marine mammals is still discussed controversially. The aim of the present study was to investigate the possible influence of PCB, polybrominated diphenyl ether (PBDE), toxaphene, (p,p'-dichlorodiphenyl)trichlorethane (DDT), and (p,p'-dichlorodiphenyl)dichlorethene (DDE) on the immune system of harbor porpoises. Lymphoid organs are influenced by a variety of factors, and therefore special emphasis was given to separating the confounding effect of age, health status, nutritional state, geographical location, and sex from the effect of contaminant levels upon thymus and spleen. Contaminant analysis and detailed pathological examinations were conducted on 61 by-caught and stranded whales from the North and Baltic Seas and Icelandic and Norwegian waters. Stranded harbor porpoises were more severely diseased than by-caught animals. Thymic atrophy and splenic depletion were significantly correlated to increased PCB and PBDE levels. However, lymphoid depletion was also associated with emaciation and an impaired health status. The present report supports the hypothesis of a contaminant-induced immunosuppression, possibly contributing to disease susceptibility in harbor porpoises. However, further studies are needed to determine if lymphoid depletion is primarily contaminant-induced or secondary to disease and emaciation in this cetacean species.
Arctic fox (Alopex lagopus) is a circumpolar species distributed across northern Canada and Alaska. Arctic fox muscle and liver were collected at Barrow, AK, USA (n=18), Holman, NT, Canada (n=20), and Arviat, NU, Canada (n=20) to elucidate the feeding ecology of this species and relate these findings to body residue patterns of organochlorine contaminants (OCs). Stable carbon (delta 13C) and nitrogen (delta 15N) isotope analyses of Arctic fox muscle indicated that trophic position (estimated by delta 15N) is positively correlated with increasing delta 13C values, suggesting that Arctic fox with a predominantly marine-based foraging strategy occupy a higher trophic level than individuals mostly feeding from a terrestrial-based carbon source. At all sites, the rank order for OC groups in muscle was polychlorinated biphenyls (Sigma PCB) > chlordane-related compounds (Sigma CHLOR) > hexachlorocyclohexane (Sigma HCH) > total toxaphene (TOX) > or = chlorobenzenes (Sigma ClBz) > DDT-related isomers (Sigma DDT). In liver, Sigma CHLOR was the most abundant OC group, followed by Sigma PCB > TOX > Sigma HCH > Sigma ClBz > Sigma DDT. The most abundant OC analytes detected from Arctic fox muscle and liver were oxychlordane, PCB-153, and PCB-180. The comparison of delta 15N with OC concentrations indicated that relative trophic position might not accurately predict OC bioaccumulation in Arctic fox. The bioaccumulation pattern of OCs in the Arctic fox is similar to the polar bear. While Sigma PCB concentrations were highly variable, concentrations in the Arctic fox were generally below those associated with the toxicological endpoints for adverse effects on mammalian reproduction. Further research is required to properly elucidate the potential health impacts to this species from exposure to OCs.
Levels of organochlorines (PCBs, sigma DDT, lindane and its isomers, HCB, chlordane, and toxaphene) were determined in blubber of marine mammals from the northern hemisphere. Differences in both levels and ratios of organochlorine compounds were detected in different species of marine mammals living in the same region, e.g. blubber of harbour seals (Phoca vitulina) accumulated significantly lower levels of lindane, HCB, toxaphene, and DDT and its metabolites than harbour porpoises (Phocoena phocoena). Compared to such elementary differences in the organochlorine pattern in different marine mammals, the influence of age and sex on the results was only minimal. Varying ratios of contaminants in individual harbour porpoises were explained by migration. Constant PCB/DDT ratios were measured in harbour seals. Due to the sedentariness of harbour seals, even local sources of contaminants could be recognized. Careful evaluation of the organochlorine levels and ratios in marine mammals made it possible to monitor the transport of PCBs from the European continent to European Arctic regions.
Beluga whales bioaccumulate organochlorines from their environment. Blubber samples of Beluga Whales from Alaska's north coast contain organochlorines, including Toxaphene (polychlorinated camphenes) PCBs, DDTs and chlordane. Toxaphene was the organochlorine pesticide found in the highest concentration in all samples with the exception of the 6 year old male where PCBs were highest. The source of these organochlorines is likely global distillation from lower latitudes. Males had higher concentrations than females and the oldest male had higher concentration than the younger male. Females exhibit a decrease in concentrations with age. The fetus had about 10% higher concentrations for all organochlorines compared to the mother. Transplacental transfer of organochlorines and lactation lower the contaminant concentration in females. Older females have lower contaminate concentrations likely due to continual reproductive success. Consumption of older males will expose humans to higher levels of organochlorines.