Food chain enrichment of organochlorine compounds and mercury in clean and polluted lakes of Finland

Lakes polluted by pulp mill and urban wastes including chlorobleaching of pulp, semipolluted lakes and reference lakes in nearly natural condition in Central Finland were studied for contents of mercury, methyl mercury and organochlorine compounds in sediment, plankton, roach and pike. Chlorobleaching had caused a 30-fold concentration of Hg in bottom sediment related to that of the purest reference lake. This was not reflected to the mercury levels in fish which were highest at one natural condition (humic) lake and rather high also at semipolluted lake Päijänne. Mercury in fish was shown to be mostly methylated but not completely and its time trends could be estimated. Chloroform showed no but carbon tetrachloride, tetrachloroethylene and chlorinated cymenes significant bioaccumulation in fish. Levels of chlorophenols from bleaching had strongly decreased but pentachlorophenol and 2,3,4,6-tetrachlorphenol levels remained related to earlier results. Using fat basis attenuated the power of estimation of food chain enrichment by a three throphic level model for lipohilic biocides and a strong proof was obtained of the enrichment of hexachlorobenzene. The time trends at Päijänne were decreasing for mercury and DDE but increasing for PCB.     

Recent trends of biocides in pikes of the Lake Päijänne

Pikes were sampled in May 1980 from three areas of the Lake Päijänne, Finland and analyzed for their contents of total mercury, methyl mercury, hexachlorobenzene (HCB), DDE, PCB and chlorophenolic residues. An improved method for methyl mercury determination was applied and 82–84 % methylation of mercury in pikes regardless of area or biological variation was observed. Statistical analysis with previous results from the same areas gave a very significant decreasing trend of mercury levels at all three areas from 1970 to 1980. Future levels of mercury in fish to be consumed as food could be estimated from the trend regression. The very low levels of DDE and PCB showed some increasing trend when the influence of fat contents was eliminated by covariance analysis. General appearance of HCB at sub-ppb level was observed. Also pentachlorophenol occured at 10–70 ppb (fresh weight) levels at all areas, but the other chlorophenols were abundant only at Tiirinselkä which is most contaminated by pulp bleaching effluents.     

Suitability of passive sampling for the monitoring of pharmaceuticals in Finnish surface waters

The occurrence of five pharmaceuticals, consisting of four anti-inflammatory and one antiepileptic drug, was studied by passive sampling and grab sampling in northern Lake Päijänne and River Vantaa. The passive sampling was performed by using Chemcatcher® sampler with a SDB-RPS Empore disk as a receiving phase. In Lake Päijänne, the sampling was conducted during summer 2013 at four locations near the discharge point of a wastewater treatment plant and in the years 2013 and 2015 at four locations along River Vantaa. The samples were analyzed by liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS) in the multiple reaction monitoring mode. The concentrations of carbamazepine, diclofenac, ibuprofen, ketoprofen, and naproxen in Lake Päijänne determined by passive sampling ranged between 1.4–2.9 ng L^?1, 15–35 ng L^?1, 13–31 ng L^?1, 16–27 ng L^?1, and 3.3–32 ng L^?1, respectively. Similarly, the results in River Vantaa ranged between 1.2–40 ng L^?1, 15–65 ng L^?1, 13–33 ng L^?1, 16–31 ng L^?1, and 3.3–6.4 ng L^?1. The results suggest that the Chemcatcher passive samplers are suitable for detecting pharmaceuticals in lake and river waters.     

Chemical trends in Finnish wildlife: A study on time trends in starlings during 1967–1983

The OECD monitoring programmes 1966–1971 and 1972–1975 have been extended at national level in Finland to 1983 by analysing chlorinated hydrocarbons, mercury and chlorophenols in starlings (terrestrial environment). At the end of the study period levels in fresh muscles were for DDE 10, PCB 30, HCB 1, Lindan 8 and mercury 50 ppb. Of chlordane residues only traces of oxychlordane were found. Ten different chlorophenol compounds were detected at ppb levels, but most of them in only few samples. Pentachlorophenol was most frequently found. Statistical treatment of the analysis results gave some decreasing trends which were very significant for DDE, DDT and PCB 1967–1983, significant for mercury 1967–1983 and somewhat significant for lindane 1978–1983.     

Chlorinated hydrocarbons and shell thinning in eggs of (Accipiter) hawks in Ontario, 1986-1989

Eggs of sharp-shinned hawks (Accipiter striatus), Cooper's hawks (A. cooperii), and northern goshawks (A. gentilis) were collected from nests in south-central Ontario from 1986 to 1989. Detectable levels of the chlorinated hydrocarbons DDE, DDT, DDD, mirex, photomirex, cis-nonachlor, trans-nonachlor, oxychlordane, dieldrin, heptachlor expoxide, HCB and PCB were present in all the eggs analyzed. Mean contaminant levels were highest in sharp-shinned hawks, slightly lower in Cooper's hawks, and significantly lower in goshawks; for example, mean DDE values were 7.23, 4.48 and 0.90 mg kg(-1) (wet weight), respectively. Total PCB levels were generally less than 1.5 mg kg(-1), lower than those associated with reproductive effects in field and laboratory studies with other species. Mean shell thicknesses of sharp-shinned and Cooper's hawk eggs were significantly less than mean pre-DDT era thicknesses (-10 and -8%, respectively), reductions that were probably not relevant to reproductive success. Goshawk eggs exhibited no significant reduction in shell thickness. Contaminant levels among the three species probably reflect differing food habits and migratory patterns.     

Organochlorine and mercury contamination of little terns (Sterna albifrons) breeding at the western Baltic Sea, 1978-96

Between 1978 and 1996, egg and chick samples of little terns (Sterna albifrons) breeding at different colony sites along the eastern coast of Schleswig-Holstein, Germany, were annually gathered by chance in the framework of a long-term ringing programme. Analyses of polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethane (DDT), hexachlorobenzene (HCB), hexachlorocyclohexane (HCHs), and mercury were carried out on eggs, chicks, and down (only mercury). In all matrices, pollutant concentrations decreased over the 19-year period. The mixture compositions of Sigma PCB, Sigma DDT, and Sigma HCH changed during the previous decades indicating decreasing releases of PCB mixtures, DDT, and technical HCH mixtures. The pollutant concentrations currently found in the tern eggs are compared with those of other bird species from other Baltic Sea subregions, suggesting a relatively low pollution of the Belt Sea. The temporal trends in contamination are related to international measurements and conventions on bans of pollutants. Since individually known females were recaptured up to three times, inter-individual variation in pollutant burdens could be studied. Remarkable variation among individuals as well as between breeding seasons were found that were not explainable by general temporal trends. Influences of individually and seasonally varying feeding habits on this phenomenon are discussed. Compositions of individual PCB mixtures varied in relation to total PCB concentrations found in eggs suggesting a concentration-dependent metabolization of PCBs as with other species. Amounts of particular organochlorines varied between matrices possibly indicating metabolization of low chlorinated PCBs, beta-HCH, and HCB during embryogenesis. In mercury, body detoxification via down is assumed. As indicated by eggshell parameters (thickness and index) being not related to organochlorine concentrations and being similar to that found in historical studies, respectively, effects of recent organochlorine contamination on eggshell thickness seem to be improbable. In conclusion, influences of contamination on declining little tern stocks observed in Germany are discussed. Negative influences of contamination in the 1960s and 1970s are assumed to be probable.     

Environmental toxins in Finnish Wildlife. A study on time trends of residue contents in fish during 1973–1978

The O.E.C.D. monitoring Wildlife Sampling and Analysis Programme 1973–1975 has been extended at national level in Finland to 1978 by analysing chlorinated hydrocarbon residues in fish at two marine and two freshwater environments and mercury at the latter two freshwater environments. Statistical treatment of the analysis results gave significant decreasing trends in most cases of PCB and DDT residues but in mercury levels no significant change was detected.     

Biota–sediment accumulation factor (BSAF), bioaccumulation factor (BAF), and contaminant levels in prey fish to indicate the extent of PAHs and OCPs contamination in eggs of waterbirds

Samples of pond sediment, fish, and shrimp were collected from the Ramsar site at Mai Po marshes, Hong Kong (south China), and samples of pond sediment, fish, and shrimp, as well as eggs of water birds (Chinese Pond Herons (Ardeola bacchus) and Little Egrets (Egretta garzetta)), were collected from two smaller wetland sites at Jiangsu Province (mid-China), between 2004 and 2007. Accumulation levels of polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs) in the biota were used to calculate biota–sediment accumulation factor (BSAF) and bioaccumulation factor (BAF). For fish and shrimp, BSAFs of OCPs (3.8–56) were greater than those of PAHs (0.12–6.3). BSAFs and BAFs of 11–79 and 4–34, respectively, were registered for OCPs in eggs of the birds and were greater than those for PAHs (0.11–1.5 and 0.02–1.3, respectively). Assuming that fish were the main prey of the birds, greater bioaccumulation of OCPs was detected for both bird species (BAFs?=?4.5–34), while accumulation of PAHs was only detected in Little Egret (BAF?=?1.3). A significant linear relationship (p?<?0.01) was observed between concentrations of OCPs in bird eggs and in the prey fish. The present study provides a new possibility of using OCP levels detected in prey fish to predict the extent of OCPs contamination in eggs of waterbirds including the endangered species, as a noninvasive method.     

Levels of polychlorinated biphenyls, organochlorine pesticides, mercury, cadmium, copper, selenium, arsenic, and zinc in the harbour seal, Phoca vitulina, in Norwegian waters

Residue levels of the chlorinated hydrocarbons polychlorinated biphenyls (PCBs), total DDT, alpha-, beta- and gamma-hexachlorocyclohexane (HCH), hexachlorobenzene (HCB), and oxychlordane in blubber, and the elements mercury, cadmium, copper, selenium, arsenic, and zinc in liver, of 82 harbour seals, Phoca vitulina, were determined. The seals were found dead or dying in Norwegian waters during the disease outbreak caused by a morbilli virus in 1988. Of the chlorinated hydrocarbons, the highest concentrations were found of PCBs, which were 2-4 times higher than the total DDT concentrations. P,p'-DDE was the main contributor to the total DDT, and constituted about 80%. The PCB and total DDT concentrations ranged from 0.4-38 and 0.1-8.8 mg kg(-1), respectively. The mercury concentrations ranged from 0.1-89 mg kg(-1). Significantly higher mean levels of PCBs (13 mg kg(-1) and mercury (16 mg kg(-1)) were found in blubber and liver, respectively, of seals from the Southern coast of Norway, as compared to the corresponding mean levels in seals from the Oslofjord (8.8 and 4.1 mg kg(-1)), and at the Northwestern coast (5.8 and 7.9 mg kg(-1)), respectively. A significant positive correlation was found between the concentrations of selenium and mercury. When the seals were grouped according to sex and age, females of ageclass > 1 and pups of both sexes had significantly lower PCB and total DDT levels than males ageclass > 1. Significantly higher hepatic mercury levels were found in seals ageclass > 1 as compared to pups. Only low levels of the other organochlorines, cadmium and arsenic, were found. Copper and zinc were considered to be present at normal physiological levels. The present organochlorine and heavy metal concentrations gave no support to suggestions that organochlorines and heavy metal pollution may be directly involved in the observed seal deaths.     

Large-scale spatial pollution patterns around the North Sea indicated by coastal bird eggs within an EcoQO programme

To categorize the marine environmental health status, the Oslo and Paris commissions have recently formulated Ecological Quality Objectives (EcoQOs) for many ecological features including the contamination of coastal bird eggs with mercury and organochlorines. In this study, we describe spatial and temporal patterns of egg contamination around the North Sea and compared them to the EcoQOs. Concentrations of mercury, polychlorinated biphenyl (??PCB) congeners, dichlorodiphenyltrichloroethane (??DDT) and derivatives, hexachlorobenzene (HCB) and hexachlorocyclohexane (??HCH) isomers were analysed in two tern species (Sterna hirundo and Sterna paradisaea) and Oystercatcher (Haematopus ostralegus) eggs collected between 2008 and 2010 in a total of 21 sites in seven countries surrounding the North Sea. Hg, ??PCB and HCB were highest in the southern sites, while ??DDT and ??HCH concentrations were greatest in eggs from the western North Sea and the Elbe estuary. There were rarely any consistent decreases over time for any compounds. In the terns, Hg, HCB and ??HCH increased at most sites, ??PCB and ??DDT in Sweden and Norway. In the Oystercatcher, HCB and ??HCH increased at more than the half of the sites, ??PCB, ??DDT and Hg at several German sites. In the terns, Hg, ??PCB and ??DDT exceeded the EcoQO in all, HCB in most years and sites. At most sites, ??HCH fulfilled the EcoQO in some study years. In the Oystercatcher, Hg, ??PCB and ??DDT exceeded the EcoQO in all or most years and sites. HCB and ??HCH fulfilled the EcoQO in some or all years at most sites. The EcoQO was exceeded most frequently in estuaries. We conclude that EcoQOs are suitable for drawing contamination patterns of the coastal North Sea in an easily understandable manner, offering the opportunity to harmonize the EcoQOs with coordinated environmental monitoring programmes.     

Organochlorine compounds in Baltic salmon and trout. I. Chlorinated hydrocarbons and chlorophenols 1982

Polychlorinated hydrocarbons and chlorophenol compounds were analyzed in three populations of Baltic salmon (Salmo salar) and one population of Bothnian Bay trout (Salmo trutta). Muscles, livers and unfertilized eggs were studied and the analysis results treated by standard statistical methods. PCB, DDT residues, HCB and lindan were detected in most, 2,3,6-t-richlorocymene in some samples at levels which are near to the global baseline. Ten chlorophenol compounds were detected, 34DCC at 0–1000 ug/kg the others 0–100 ug/kg (fresh weight) levels. Chlorohydrocarbons showed some significant positive correlations with weight, and fat contents of the fish. Significances of the differences between populations and tissues were low or neglible except that the chlorophenols in liver were at clearly higher level than in muscle or eggs.     

Contaminant residues in seabird eggs from the Canadian Arctic. Part I. Temporal trends 1975-1998.

Concentrations of total mercury, selenium and a suite of organochlorine compounds were measured in eggs of thick-billed murres (Uria lomvia), northern fulmars (Fulmarus glacialis) and black-legged kittiwakes (Rissa tridactyla) collected on Prince Leopold Island in Lancaster Sound, Nunavut, Canada, between 1975 and 1998. Mercury levels in thick-billed murre and northern fulmar eggs increased significantly during this period while selenium concentrations decreased significantly in northern fulmar eggs. Mercury and selenium concentrations in black-legged kittiwake eggs exhibited no significant temporal trends. Concentrations of sigma PCB, sigma DDT and total chlorobenzenes decreased over time for all three species and there was a shift in the PCB congener pattern as the hexachlorobiphenyl fraction of sigma PCB increased and the lower chlorinated biphenyl fraction decreased. Total chlordane, dieldrin and mirex concentrations decreased in kittiwake eggs while no significant trends were observed for the other two species. Increases in sigma HCH levels were detected in thick-billed murre eggs but not in northern fulmar and black-legged kittiwake eggs. Levels of the beta-HCH isomer, however, increased significantly in murres and fulmars. Stable-nitrogen isotope analyses (delta 15N) indicate that the temporal trends observed for contaminant concentrations in eggs were not the result of shifts in trophic level. Changing deposition patterns of xenobiotic compounds over the summer and winter ranges of these birds provide a likely explanation for differing exposures through time.     

Organochlorine contaminant assessment in great blue herons using traditional and nonlethal monitoring techniques

A nonlethal method is discussed for the evaluation of contaminant concentrations in whole eggs. Concentrations of pentachlorobenzene, hexachlorobenzene, DDE, and the PCB congeners, BZ-60, BZ-118, BZ-138, BZ-180, and BZ-170 were quantified in tissue samples from great blue herons (Ardea herodias). All tissues within whole eggs from two colonies were homogenized together and analysed for these chlorinated contaminants. Contents and chorio-allantoic membranes (CAMs) of additional whole eggs were separated and analysed. Contaminant distributions were determined for the CAM and contents of whole eggs from the same colonies. CAM tissues remaining in hatched eggs were also analysed for comparative purposes. Utilizing the distributions derived for contaminants between CAM and egg contents and the chemical concentrations determined in CAMs from hatched eggs, contaminant burdens in whole eggs were calculated. This process produced concentration estimates that described actual, whole egg burdens of chlorinated contaminants within a factor of 2 (1.03-3.7). Contaminant burdens in eggs from the two colonies were also statistically different for DDE and total PCB concentrations.     

Evidence for bioamplification of nine polychlorinated biphenyl (PCB) congeners in yellow perch (Perca flavascens) eggs during incubation

This study investigated bioamplification of polychlorinated biphenyls (PCBs) in yellow perch (Perca flavescens) eggs resulting from nutrient utilization by developing embryos during incubation. Newly fertilized eggs containing trace levels of PCBs via maternal deposition were collected from an aquaculture pond in which adult broodstock had been reared over their natural lives. The eggs were incubated using a flow through system that received the same pond water at in-situ temperatures from which they were spawned. Replicate samples of eggs were collected at six time points throughout incubation, ranging from day 0 (newly fertilized eggs) to post-hatch larvae (2-d old). Congener specific PCB fugacities in pooled egg samples showed increases over the incubation period. Just prior to hatching, incubated eggs averaged 2.7-fold higher PCB fugacities compared to fresh eggs. The increase in PCB fugacity with egg incubation time was independent of chemical K_OW. After hatching, PCB residues were lost from the larvae, attenuating the maximum chemical fugacity achieved in late-incubated eggs. However, the rate of PCB elimination in the early larvae stages was K_OW dependent such that a significant larvae/egg fugacity ratio was still evident for intermediate and highly hydrophobic compounds 2 d post-hatching. This study provides the first evidence of in-ovo PCB bioamplification in eggs of an aquatic species and suggests that incubating fish embryos are exposed to higher chemical fugacities in-ovo than would be predicted by maternal deposition alone.     

Organochlorine contamination in bird's eggs from the Danube Delta

In this study we report the levels of organochlorine compounds in eggs of aquatic birds from the Danube Delta, a major European wetland. The eggs were collected in 1997 and belonged to the following species: the mallard (Anas platyrhynchos), the greylag goose (Anser anser), the mute swan (Cygnus olor), the coot (Fulica atra), the glossy ibis (Plegadis falcinellus), the spoonbill (Platalea leucorodia), the little egret (Egretta garzetta), the night heron (Nycticorax nycticorax), the grey heron (Ardea cinerea), the great white egret (Egretta alba), the red-necked grebe (Podiceps griseus), the Dalmatian pelican (Pelecanus crispus), the Pygmy cormorant (Phalacrocorax pygmaeus) and the common cormorant (Phalacrocorax carbo). Dichlorodiphenyltrichloroethane (DDT) levels were higher in eggs of the little egret, the great white egret, the cormorant and the Pygmy cormorant with respect to the other species (48,399, 13,613, 12,400 and 10,417 ng/g dry wt., respectively). Hexachlorobenzene (HCB) levels were lower than 1393 ng/g dry wt. in all species while polychlorinated biphenyl (PCB) concentrations in the Pygmy cormorant (2565 ng/g dry wt.) were higher than in the other species. The toxicity evaluation was based on 2,3,7,8-TCDD toxic equivalent factors (TEF) and non-ortho PCB congeners contributed much more than mono-ortho PCBs in most of species. A further aim of this study was to evaluate the possible differences of organochlorine levels in bird eggs collected in the same area in 1982 and in 1997; generally speaking the levels detected in the latter period were lower than those detected in the earlier one.     

Environmental contaminants and reproductive success of great blue herons Ardea herodias in British Columbia, 1986-1987

In 1986, eggs were collected and productivity estimated at four great blue heron (Ardea herodias) colonies on the coast of British Columbia. Polychlorinated dibenzodioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) were present in all eggs in a qualitatively similar pattern among colonies. PCDD levels were significantly elevated at a colony near a kraft pulp mill at Crofton on Vancouver Island, although there was no correlation between the number of young raised in a nest and levels of either PCDDs, PCDFs, PCBs, organochlorine pesticides or mercury. In 1987, heron productivity was normal at three colonies, while the colony at Crofton failed to raise any young. A normal complement of eggs were apparently laid in about 57 nests, but during incubation they were destroyed and the broken eggshells were found in and beneath the nests. Analysis of eggs salvaged from nests showed that 2378-TCDD levels were about three times higher in 1987 than in 1986. At a colony in Vancouver, 2378-TCDF levels were significantly higher in 1987 than 1986 eggs. Levels of organochlorine pesticides and total mercury in eggs were generally low; highest residue levels were found in two mainland colonies, particularly at one adjacent to an agricultural area. Total PCB levels were low and did not differ significantly among locations. Analysis of PCB congener ratios indicated different sources of PCBs. Regurgitated prey samples collected in 1986 from four locations had generally low levels of PCDD, PCDF, mercury, lead and cadmium contamination.     

Organochlorine pesticides, PCBs and mercury in antarctic and subantarctic seabirds

Between 1978 and 1983, eggs from 15 species of Antarctic and Subantarctic seabirds were collected and analysed for organochlorine pesticides, PCBs, and mercury residues. The lowest levels of these chemicals were detected in the eggs of Adélie Penguins from Prydz Bay. Antarctica. On a wet weight basis, the mean concentrations in eggs of these penguins were 0.01 μg/g HCB, 0.005 μg/g DDE, less than 0.1 μg/g PCBs (1260) and 0.02 μg/g mercury. Such values indicate that the environmental levels of these contaminants in the biotypes of these species are extremely low, and present no significant threat.

The highest levels of contaminants were found in the eggs of species which breed in Antarctica and migrate to regions well north of the Antarctic Convergence in the non-breeding season. On a wet weight basis, Northern Giant-Petrel eggs contained 0.11 μg/g HCB, 0.95 μg/g DDE and 1.8 μg/g PCB (1260), and 1.8 μg/g mercury. There are indications that DDE levels are increasing for both Southern and Northern Giant-Petrels, and it is possible that reports of a decreasing number of breeding pairs of these species at several colonies are due to one or more of these contaminants reaching toxic levels.

Analysis of penguin tissues show that preen gland lipid is suitable for monitoring the body burden of organochlorine insecticides and PCBs in seabirds.

Variation in DDE and mercury residue levels for some of these species suggest that the biotypes in which they live are quite different, and that the Antarctic Convergence may have a major influence in protecting the Antarctic ecosystem from these pollutants.     

Pesticide and PCB levels in fish from Alberta (Canada)

Pesticide and PCB analyses were completed on fat and muscle samples of 750 fish collected from 11 major lakes and rivers in Alberta. Although phenoxy and organophosphate residues were always below detectable limits, traces of chlorinated pesticides and their derivatives, particularly DDE, DDD and chlordane, were detected in most fat samples. Methoxychlor was frequently found in goldeye from the North Saskatchewan River but not recorded in fish from any other lake or river. Its presence in goldeye, a highly migratory species, was probably a result of biting-fly control programs in the Saskatchewan part of the river. PCB levels exceeded 25 mg/kg in the fat of several species from the North Saskatchewan River but were generally lower in the other systems. Analysis of 160 sediment samples from the North Saskatchewan River revealed no point source of PCB contamination, with residues always <0.01 mg/kg dry weight.     

Polychlorinated phenols,guaiacols and catechols in environment

Emissions, bioaccumulation and possible food chain enrichment of polychlorinated phenols, guaiacols and catechols have been studied by analyses of water, snow, ash, benthic animal, fish and bird samples in Finland. Seventeen individual compounds were analyzed using authentic reference model compounds and internal standard by GC/ECD. Although the enrichment potential of the studied compounds appeared to be lower than that of the chlorinated hydrocarbons, they proved to be very general pollutants and some of them showed specific bioaccumulation to certain species and high persistency thus forming environmental hazards.     

Long-term trends in organochlorine and mercury residues in some predatory birds in Britain

Residue levels of organochlorine pesticides (HEOD, DDE), polychlorinated biphenyls (PCBs) and mercury (Hg) in the livers of five predatory bird species were monitored in Britain over a 28-year (1963-1990) period. Of two raptor species, sparrowhawks contained higher levels of most chemicals than did kestrels. Among three fish-eaters, herons and kingfishers contained the highest levels of DDE and HEOD, while herons and great-crested grebes contained the highest levels of PCBs and mercury. Species differences were related partly to diet and habitat. In sparrowhawks and kestrels, residues of HEOD and DDE were higher in eastern, arable districts than elsewhere, especially in the 1960s and 1970s. In the fish-eaters, similar regional differences in residue levels were apparent in herons, especially in the 1970s, but not in the other species, for which samples were smaller. Over the 28 years, most species showed significant downward trends in HEOD, DDE and Hg levels, but only two fish-eaters showed significant declines in PCB levels. The downward trends in DDE and HEOD followed successive restrictions in the use of organochlorine pesticides, and were accompanied by recoveries in the populations and breeding success of affected species. Downward trends in mercury were associated with reductions in both agricultural use and industrial emissions.