Derek C. G. Muir

Science and policy on endocrine disrupters must not be mixed: a reply to a “common sense” intervention by toxicology journal editors

The “common sense” intervention by toxicology journal editors regarding proposed European Union endocrine disrupter regulations ignores scientific evidence and well-established principles of chemical risk assessment. In this commentary, endocrine disrupter experts express their concerns about a recently published, and is in our considered opinion inaccurate and factually incorrect, editorial that has appeared in several journals in toxicology. Some of the shortcomings of the editorial are discussed in detail. We call for a better founded scientific debate which may help to overcome a polarisation of views detrimental to reaching a consensus about scientific foundations for endocrine disrupter regulation in the EU.

Organochlorine contaminants in arctic marine food chains: accumulation of specific polychlorinated biphenyls and chlordane-related compounds

Polychlorinated biphenyl congeners (S-PCB) and chlordane-related compounds (S-CHLOR) as well as DDT, hexachlorocyclohexane, toxaphene, and chlorobenzenes were determined in pooled arctic cod (Boreogadus saida) muscle and polar bear (Ursus maritimus) fat and in the blubber and liver of 59 ringed seals (Phoca hispida) from the east-central Canadian Arctic. S-PCB concentrations ranged from 0.0037 mg/kg (wet wt) in cod muscle to 0.68 mg/kg in male seal blubber and 4.50 mg/kg in bear fat. Tri- and tetrachloro PCB homologues were the dominant PCBs in fish, while pentachloro/hexachloro and hexachloro/heptachloro congeners predominated in ringed seal blubber and polar bear fat, respectively. Chlordane compounds detected in seal blubber were oxychlordane, cis- and trans-nonachlor, and cis-chlordane as well as nine minor components of technical chlordane, including nonachlor-III (a nonachlor isomer). Toxaphene and HCH isomers were the major organochlorines in cod muscle with mean concentrations of 0.018 and 0.010 mg/kg, respectively. S-CHLOR/S-PCB ratios ranged from 0.6 in fish muscle and bear fat to 0.7-0.9 in seal blubber, much higher than observed in more southerly marine environments, suggesting a proportionally greater input of chlordane into the Arctic.

Monitoring of perfluorinated compounds in aquatic biota: an updated review.

The goal of this article is to summarize new biological monitoring information on perfluorinated compounds (PFCs) in aquatic ecosystems (post-2005) as a followup to our critical review published in 2006. A wider range of geographical locations (e.g., South America, Russia, Antarctica) and habitats (e.g., high-mountain lakes, deep-ocean, and offshore waters) have been investigated in recent years enabling a better understanding of the global distribution of PFCs in aquatic organisms. High concentrations of PFCs continue to be detected in invertebrates, fish, reptiles, and marine mammals worldwide. Perfluorooctane sulfonate (PFOS) is still the predominant PFC detected (mean concentrations up to 1900 ng/g ww) in addition to important concentrations of long-chain perfluoroalkyl carboxylates (PFCAs; sum PFCAs up to 400 ng/g ww). More studies have evaluated the bioaccumulation and biomagnification of these compounds in both freshwater and marine food webs. Several reports have indicated a decrease in PFOS levels over time in contrast to PFCA concentrations that have tended to increase in tissues of aquatic organisms at many locations. The detection of precursor metabolites and isomers has become more frequently reported in environmental assessments yielding important information on the sources and distribution of these contaminants. The integration of environmental/ecological characteristics (e.g., latitude/longitude, salinity, and/or trophic status at sampling locations) and biological variables (e.g., age, gender, life cycle, migration, diet composition, growth rate, food chain length, metabolism, and elimination) are essential elements in order to adequately study the environmental fate and distribution of PFCs and should be more frequently considered in study design.

Organochlorine contaminants in arctic marine food chains: identification, geographical distribution and temporal trends in polar bears.

Contamination of Canadian arctic and subarctic marine ecosystems by organochlorine (OC) compounds was measured by analysis of polar bear (Ursus maritimus) tissues collected from 12 zones between 1982 and 1984. PCB congeners (S-PCB), chlordanes, DDT and metabolites, chlorobenzenes (S-CBz), hexachlorocyclohexane isomers (S-HC-H), and dieldrin were identified by high-resolution gas chromatography-mass spectrometry. Nonachlor-III, a nonachlor isomer in technical chlordane, was positively identified for the first time as an environmental contaminant. S-PCB and S-CHLOR accounted for >80% of the total organochlorines in adipose tissue. Six PCB congeners constituted approximately 93% of S-PCB in polar bears. Levels of most OCs were lowest in the high Arctic, intermediate in Baffin Bay, and highest in Hudson Bay. Levels of ..cap alpha..-HCH were evaluated in zones influenced by surface runoff. Levels of S-CHLOR were four times higher and levels of the other OCs were two times higher in adipose tissue of bears from Hudson Bay and Baffin Bay in 1984 than in adipose tissue archived since 1969 from these areas; levels of S-DDT did not change.

Dynamics of dietary bioaccumulation and faecal elimination of hydrophobic organic chemicals in fish

A compilation of available literature data on uptake efficiencies of hydrophobic, organic chemicals from food by fish is presented. It is shown that the uptake efficiency of chemical from food (EO) follows a relationship with the 1-octanol-water partition coefficient (KOW), i.e., 1EO = 5.3.10−8.KOW + 2.3. A model is derived for chemical uptake from food, which is shown to be consistent with the observed food-uptake data. The equations provide an explanation for the phenomenon of food chain accumulation, which is observed in natural ecosystems for several hydrophobic halogenated aromatic hydrocarbons.

Spatial and temporal trends of contaminants in Canadian Arctic freshwater and terrestrial ecosystems: a review

The state of knowledge of contaminants in Canadian Arctic biota of the freshwater and terrestrial ecosystems has advanced enormously since the publication of the first major reviews by Lockhart et al. and Thomas et al. in The Science of the Total Environment in 1992. The most significant gains are new knowledge of spatial trends of organochlorines and heavy metal contaminants in terrestrial animals, such as caribou and mink, and in waterfowl, where no information was previously available. Spatial trends in freshwater fish have been broadened, especially in the Yukon, where contaminant measurements of, for example, organochlorines were previously non-existent. A review of contaminants data for fish from the Northwest Territories, Yukon and northern Quebec showed mercury as the one contaminant which consistently exceeds guideline limits for subsistence consumption or commercial sale. Lake trout and northern pike in the Canadian Shield lakes of the Northwest Territories and northern Quebec generally had the most elevated levels. Levels of other heavy metals were generally not elevated in fish. Toxaphene was the major organochlorine contaminant in all fish analyzed. The concentrations of organochlorine contaminants in fish appear to be a function not only of trophic level but of other aspects of the lake ecosystem. Among Arctic terrestrial mammals, PCBs and cadmium were the most prominent contaminants in the species analyzed. Relatively high levels (10-60 micrograms g-1) of cadmium were observed in kidney and liver of caribou from the Yukon, the Northwest Territories and northern Quebec, with concentrations in western herds being higher than in those from the east. For the organochlorine contaminants, a west to east increase in zigma PCBs, HCB and zigma HCH was found in caribou, probably as a result of the predominant west to east/north-east atmospheric circulation pattern which delivers these contaminants from industrialized regions of central and eastern North America to the Arctic via long-range atmospheric transport. Radiocesium contamination of lichens and caribou has continued to decrease. Significant contamination by PCBs and lead of soils and vascular plants was observed in the immediate vicinity and within a 20-km radius of DEW line sites in the Canadian Arctic. There was also evidence for transfer of PCBs from plants to lemmings. There was no evidence, however, that large mammals such as caribou living in the general area of the DEW line sites had elevated levels of PCBs. There is very limited temporal trend information for most contaminants in biota of Arctic terrestrial and freshwater environments.

Chlorinated hydrocarbon contaminants in arctic marine mammals

By 1976, the presence of chlorinated hydrocarbon contaminants (CHCs) had been demonstrated in fur seal (Callorhinus ursinus), ringed seal (Phoca hispida), hooded seal (Cystophora cristata), bearded seal (Erignathus barbatus), walrus (Obdobenus rosmarus divergens), beluga (Delphinapterus leucas), porpoise (Phocoena phocoena) and polar bear (Ursus maritimus) in various parts of the Arctic. In spite of this early interest, very little subsequent research on contaminants in Arctic marine mammals was undertaken until the mid-1980s. Since that time, there has been an explosion of interest, resulting in a much expanded data base on contaminants in Arctic marine mammals. Except in the Russian Arctic, data have now been obtained on the temporospatial distribution of PCBs and other contaminants in ringed seal, beluga and polar bear. Contaminants in narwhal (Monodon monoceros) have also now been measured. On a fat weight basis, the sum of DDT-related compounds (S-DDT) and PCB levels are lowest in walrus (< 0.1 microgram/g), followed by ringed seal, (0.1-1 microgram/g range). Levels are an order of magnitude higher in beluga and narwhal (1-10 micrograms/g range). It appears that metabolism and excretion of S-DDT and PCBs may be less efficient in cetaceans, leading to greater biomagnification. Polar bears have similar levels of PCBs as cetaceans (1-10 micrograms/g), but with a much simpler congener pattern. DDE levels are lowest in polar bear, indicating rapid metabolism. Effects of age and sex on residue levels are found for all species where this was measured. Among cetaceans and ringed seal, sexually mature females have lower levels than males due to lactation. Although PCB levels in adult male polar bears are about twice as high as females, there is only a trivial age effect in either sex apart from an initial decrease from birth to sexual maturity (age 0-5). Comparison of levels of S-DDT and PCBs in Arctic beluga and ringed seal with those in beluga in the Gulf of St. Lawrence and ringed seal in the Baltic Sea, indicate that overall contamination of the Arctic marine ecosystem is 10-50 times less than the most highly contaminated areas in the northern hemisphere temperate latitude marine environment. Geographic distribution of residue levels in polar bears indicates a gradual increase from Alaska east to Svalbard, except PCB levels are significantly higher in eastern Greenland and Svalbard. Information on temporal trends is somewhat contradictory.(ABSTRACT TRUNCATED AT 400 WORDS)

Trophic magnification factors: Considerations of ecology, ecosystems, and study design

Recent reviews by researchers from academia, industry, and government have revealed that the criteria used by the Stockholm Convention on persistent organic pollutants under the United Nations Environment Programme are not always able to identify the actual bioaccumulative capacity of some substances, by use of chemical properties such as the octanol-water partitioning coefficient. Trophic magnification factors (TMFs) were suggested as a more reliable tool for bioaccumulation assessment of chemicals that have been in commerce long enough to be quantitatively measured in environmental samples. TMFs are increasingly used to quantify biomagnification and represent the average diet-to-consumer transfer of a chemical through food webs. They differ from biomagnification factors, which apply to individual species and can be highly variable between predator-prey combinations. The TMF is calculated from the slope of a regression between the chemical concentration and trophic level of organisms in the food web. The trophic level can be determined from stable N isotope ratios (δ(15) N). In this article, we give the background for the development of TMFs, identify and discuss impacts of ecosystem and ecological variables on their values, and discuss challenges and uncertainties associated with contaminant measurements and the use of δ(15) N for trophic level estimations. Recommendations are provided for experimental design, data treatment, and statistical analyses, including advice for users on reporting and interpreting TMF data. Interspecies intrinsic ecological and organismal properties such as thermoregulation, reproductive status, migration, and age, particularly among species at higher trophic levels with high contaminant concentrations, can influence the TMF (i.e., regression slope). Following recommendations herein for study design, empirical TMFs are likely to be useful for understanding the food web biomagnification potential of chemicals, where the target is to definitively identify if chemicals biomagnify (i.e., TMF > or < 1). TMFs may be less useful in species- and site-specific risk assessments, where the goal is to predict absolute contaminant concentrations in organisms in relation to threshold levels.

Legacy of a half century of Athabasca oil sands development recorded by lake ecosystems

The absence of well-executed environmental monitoring in the Athabasca oil sands (Alberta, Canada) has necessitated the use of indirect approaches to determine background conditions of freshwater ecosystems before development of one of the Earth’s largest energy deposits. Here, we use highly resolved lake sediment records to provide ecological context to ∼50 y of oil sands development and other environmental changes affecting lake ecosystems in the region. We show that polycyclic aromatic hydrocarbons (PAHs) within lake sediments, particularly C1-C4–alkylated PAHs, increased significantly after development of the bitumen resource began, followed by significant increases in dibenzothiophenes. Total PAH fluxes in the modern sediments of our six study lakes, including one site ∼90 km northwest of the major development area, are now ∼2.5–23 times greater than ∼1960 levels. PAH ratios indicate temporal shifts from primarily wood combustion to petrogenic sources that coincide with greater oil sands development. Canadian interim sediment quality guidelines for PAHs have been exceeded since the mid-1980s at the most impacted site. A paleoecological assessment of Daphnia shows that this sentinel zooplankter has not yet been negatively impacted by decades of high atmospheric PAH deposition. Rather, coincident with increases in PAHs, climate-induced shifts in aquatic primary production related to warmer and drier conditions are the primary environmental drivers producing marked daphniid shifts after ∼1960 to 1970. Because of the striking increase in PAHs, elevated primary production, and zooplankton changes, these oil sands lake ecosystems have entered new ecological states completely distinct from those of previous centuries.

Melting Glaciers: A Major Source of Persistent Organochlorines to Subalpine Bow Lake in Banff National Park, Canada

Abstract 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.