Sediment Contamination in Lake Erie: A 25-Year Retrospective Analysis

Lake Erie sediment surveys were conducted in 1997 and 1998 to characterize spatial and temporal trends in contamination and for comparison with historical levels to assess the degree of improvement in environmental quality since the advent of measures to reduce impacts from sources. These surveys were also designed to assist in identification of possible sources of contamination and areas where contamination exceeded Canadian sediment quality guidelines for protection of aquatic biota. Encouragingly, lakewide contaminant concentrations were found to have significantly decreased from levels observed in samples collected in 1971 in previous Environment Canada surveys. The lakewide average polychlorinated biphenyl (PCB) sediment concentrations decreased from 136 ng/g in 1971 to 43 ng/g in 1997. This decreasing temporal trend was also evidenced by contaminant profiles of core samples from all three major basins. There was a lakewide spatial trend in increasing sediment contamination from the eastern basin to the western basin, and from the north-central basin to the south-central basin. Sediments in many areas of Lake Erie still exceeded Canadian Federal and Provincial sediment quality guidelines. However, exceedences of sediment guidelines describing contaminated environments in 1997/98 were largely restricted to the western basin and the southern portion of the central basin. Exceedences of Canadian Sediment Quality probable effects guidelines were most numerous for dioxins and furans (40%) followed by mercury (6%). The Canadian threshold effects guideline for PCBs (34.1 ng/g) and the Provincial lowest effect guideline (70 ng/g) were exceeded at 52% and 22% of the sites, respectively. Mercury, PCBs and polychlorinated dibenzo-p-dioxins and dibenzofurans are responsible for fish consumption advisories in Lake Erie.     

Historical Changes in PCB Patterns in Lake Ontario and Green Bay,Lake Michigan, 1971 to 1982, from Herring Gull Egg Monitoring Data

Patterns of PCB congener bioaccumulation were examined in archived herring gull (Larus argentatus) eggs collected from Big Sister Island in Green Bay, Lake Michigan, and Scotch Bonnet Island in Lake Ontario from 1971 to 1982 as part of the Canadian Wildlife Service's Great Lakes Herring Gull Monitoring Program. Concentrations of 97 PCB congeners were measured. From 1971 to 1982, ecological half-lives of most congeners, particularly the tri- through hexachlorobiphenyls, were greater in eggs from Green Bay than Lake Ontario. Comparing sum PCB levels in eggs collected in 1971 and 1982, concentrations declined 80% at Scotch Bonnet Island and 74% at Big Sister Island. PCB congener patterns were different in eggs from the two colonies. Principal components analysis showed that inter-site differences in congener patterns became more apparent after 1976. This indicated that regional PCB sources were the most influential in determining patterns of biologically-available PCBs during the 1971 to 1982 period in these two lakes, via recycling of historical PCBs from sediments or gradually decreasing loading. Trend analysis of selected congeners specific to Aroclors 1242, 1254, and 1260 revealed that the rapid decline of less chlorinated congeners, observed from 1971 to 1976 in Lake Ontario, was explained by a decrease in loading of Aroclor 1242 to the lake. At both colonies, ecological half life of the congeners was significantly (p < 0.001) correlated with log K_ow and with –log HLC. Changes in PCB composition, after 1976 in Lake Ontario and from 1971 to 1982 in Green Bay, could be explained by differences in the physical behavior of individual congeners affecting removal by volatilization and sedimentation.     

Results from the U.S. Great Lakes Fish Monitoring Program and Effects of Lake Processes on Bioaccumulative Contaminant Concentrations

An analysis of composite samples of 820 lake trout, walleye, steelhead, Chinook, and coho from the Laurentian Great Lakes reveals differences in contaminant processing among and between lakes which results in differing concentrations of bioaccumulative contaminants. Generally, contaminants are most concentrated in fish from Lake Michigan and least concentrated in fish from Lake Superior, with the notable exceptions of toxaphene and alpha-HCH. Differences in contamination patterns, however, are apparent not only among the lakes but between sites within a lake or even fish within a site. Lake trout composites from Lake Superior show an increase in the degree of chlorination of PCBs with increasing total PCBs. The PCB congener profile of lake trout from the Sturgeon Bay site of Lake Michigan is substantially different from that of the Saugatuck site of Lake Michigan, possibly due to the influence of contamination from nearby Green Bay. Finally, the ratios of selected PBDE and PCB congeners are much different in Lake Superior fish compared to fishes from all the other lakes. We hypothesize that this is a result of the colder temperatures and associated lower plankton growth rates in Lake Superior allowing PCB and PBDE uptake by phytoplankton to reach near equilibrium, thus enhancing the relative concentrations, in phytoplankton and the food web in general, of congeners that may be kinetically limited in other lakes.     

Contaminant Trends in Lake Trout and Walleye From the Laurentian Great Lakes

Trends in PCBs, DDT, and other contaminants have been monitored in Great Lakes lake trout and walleye since the 1970s using composite samples of whole fish. Dramatic declines have been observed in concentrations of PCB, ΣDDT, dieldrin, and oxychlordane, with declines initially following first order loss kinetics. Mean PCB concentrations in Lake Michigan lake trout increased from 13 μg/g in 1972 to 23 μg/g in 1974, then declined to 2.6 μg/g by 1986. Between 1986 and 1992 there was little change in concentration, with 3.5 μg/g observed in 1992. ΣDDT in Lake Michigan trout followed a similar trend, decreasing from 19.2 μg/g in 1970 to 1.1 μg/g in 1986, and 1.2 μg/g in 1992. Similar trends were observed for PCBs and ΣDDT in lake trout from Lakes Superior, Huron and Ontario. Concentrations of both PCB and ΣDDT in Lake Erie walleye declined between 1977 and 1982, after which concentrations were relatively constant through 1990. When originally implemented it was assumed that trends in the mean contaminant concentrations in open-lake fish would serve as cost effective surrogates to trends in the water column. While water column data are still extremely limited it appears that for PCBs in lakes Michigan and Superior, trends in lake trout do reasonably mimic those in the water column over the long term. Hypotheses to explain the trends in contaminant concentrations are briefly reviewed. The original first order loss kinetics used to describe the initial decline do not explain the more recent leveling off of contaminant concentrations. Recent theories have examined the possibilities of multiple contaminant pools. We suggest another hypothesis, that changes in the food web may have resulted in increased bioaccumulation. However, a preliminary exploration of this hypothesis using a change point analysis was inconclusive.     

Spatiotemporal trends of polychlorinated biphenyls (PCBs) in surface and suspended sediments from the Lake Ontario Canadian nearshore 1994–2018: A fish consumption advisory perspective

Spatiotemporal trends for polychlorinated biphenyls (PCBs) were examined in surface and suspended sediments collected between 1994 and 2018 from over twenty nearshore stations on the Canadian side of Lake Ontario and the St. Lawrence River. In 2018, PCB concentrations ranged over an order-of-magnitude in surface (<10 ng/g?357 ng/g) and suspended sediments (<10 ng/g–330 ng/g), illustrating the presence of legacy hotspots as well as diffuse urban inputs. PCB concentrations in both surface and suspended sediments were consistently highest in Hamilton Harbour, but were also elevated at other stations around the perimeter of the Niagara basin as well as near Trenton and Kingston, Ontario. Generally, higher PCB concentrations were found in surface sediment relative to paired suspended sediment samples suggesting temporal improvements in nearshore sediment quality. However, many stations demonstrated temporal variability in PCB concentrations, a likely factor in the lack of an overall nearshore declining trend. Given that PCBs are listed as a consumption-limiting contaminant for all fish sampling blocks in the Canadian waters of Lake Ontario and are responsible for 78% of restricted advisories, sediment quality benchmarks that account for bioaccumulation potential should be considered over toxicologically-derived guidelines to gauge severity of PCB contamination of nearshore sediments. Relatively higher TOC-normalized PCB concentrations in the western end of Lake Ontario suggests additional research on PCB bioavailability from nearshore sediment would be beneficial in understanding basinwide trends of PCBs in fish, and that an adaptive approach to sediment management may be needed in the context of consumption advisories.     

PCB Concentrations of Lake Michigan Invertebrates: Reconstruction Based on PCB Concentrations of Alewives (Alosa pseudoharengus) and their Bioenergetics

Invertebrate PCB concentrations are a poorly quantified but crucial step in the trophic transfer of organochlorine contaminants to fishes. In fact, current attempts to quantify PCB fluxes in the Lake Michigan pelagic food web are hampered by poor knowledge of invertebrate PCB concentrations. Models exist that estimate PCB concentrations in fish based upon PCB concentrations in their food. We have used a complementary approach and estimated invertebrate PCB concentrations based upon historical records of alewife PCB concentrations in Lake Michigan. We first developed a model of total PCB accumulation in alewife (Alosa pseudoharengus) using a bioenergetics-based approach to growth. The PCB assimilation efficiency between invertebrate prey and alewife predators was estimated to be about 0.40. We then used the model to hindcast PCB concentrations in the invertebrates that comprised alewife prey. We estimated that median PCB concentrations of Lake Michigan invertebrates have dropped roughly 10-fold from 1976 to 1990; for example, the estimated Diporeia hoyi PCB concentration has dropped from ca. 0.48 mgkg^-1 wet weight to 0.04 mgkg^-1 wet weight over this time period. The biomagnification ratio (alewife PCB/zooplankton PCB) is about 16-fold (Diporeia hoyi) to 40-fold (copepods/cladocerans). The PCB concentrations in Lake Michigan invertebrates and alewife that we have estimated for 1993 and 1994 should be viewed as predictions, testable as data become available. Because historic data on invertebrate PCB concentrations in Lake Michigan are exceedingly scarce, our estimates should be useful for studies that attempt to quantify the Lake Michigan PCB fluxes or future modeling efforts that attempt to incorporate multiple levels of the Lake Michigan food web.     

A River-wide Survey of Polychlorinated Biphenyls (PCBs), Polycylic Aromatic Hydrocarbons (PAHs), and Selected Organochlorine Pesticide Residues in Sediments of the Detroit River—1999

The spatial distribution of hydrophobic organic contaminants, including polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs), and octachlorostyrene (OCS) in sediments of the Detroit River was established using data from a 1999 river-wide survey. The survey employed a stratified random sampling design that divided the river into six geostatistical zones consisting of upper, middle, and lower U.S. and equivalent Canadian river reaches. Organic carbon normalized OCS sediment concentrations demonstrated no significant differences between U.S. or Canadian sediments or upstream/downstream gradients suggesting that OCS is derived primarily from sources upstream of the Detroit River. In contrast, sum PCBs and sum PAHs were significantly elevated at U.S. as compared to Canadian stations and demonstrated significant increasing upstream/downstream gradients in organic carbon normalized sediment contamination. The upper and middle U.S. river reaches contained a number of near-shore stations with high localized PCB and PAH sediment concentrations suggesting multiple inputs along the upper U.S. portion of the river. Consistent with past surveys, wide-spread sediment contamination of PCBs and PAHs continues to be observed in the highly industrialized Trenton Channel and downstream of Grosse Isle. Threshold effect level (TEL) sediment quality guidelines for PAHs and PCBs were exceeded in 92.6 and 77.8%, respectively, of stations in Trenton Channel and downstream of Grosse Isle. This large reservoir of degraded sediments in the lower U.S. river reach has the potential to enter Lake Erie during sediment disturbance events and likely contributes to gentoxic stress and increased bioaccumulation of PCBs in resident benthos, fish, and wildlife.     

Temporal and spatial variability of PCB concentrations in lake trout (Salvelinus namaycush) in Lake Superior from 1995 to 2016

Production of polychlorinated biphenyl compounds (PCBs) was banned over 40 years ago in the United States and Canada, but they remain a dominant contaminant in Great Lakes fish. Although PCB concentrations in Great Lakes fish have declined since the 1980s, there is concern that the rate of decline has slowed in recent years. Canadian and U.S. national agencies monitor trends in fish contaminants at only a few sites in each lake, while states and provinces monitor fish at more locations. In this study, we compare fish PCB measurements made by five agencies at multiple locations in order to evaluate spatial as well as temporal patterns in Lake Superior. For several monitoring locations, rapid increases and decreases in concentrations were observed. The wide range of concentrations (up to 1000 ng/g) reported among all stations in any single year is unlikely to result solely from differences in fish preparation or analytical techniques. Recent measurements indicate that spatial variation in fish PCB concentrations exists with peak concentrations 30-fold higher than lowest concentrations. After 1995, statistically significant changes, all declines, in PCB concentrations were observed at only three of seven locations; half-lives in these locations ranged from 9 to 14 years. Differences in diet and food web structure likely contribute both to the spatial variability of concentrations within the lake as well as to the rapid, short-term changes in concentrations at single sites that make long-term trends difficult to discern and to predict.     

Spatial Patterns in PCB Concentrations of Lake Michigan Lake Trout

Most of the PCB body burden in lake trout (Salvelinus namaycush) of the Great Lakes is from their food. PCB concentrations were determined in lake trout from three different locations in Lake Michigan during 1994–1995, and lake trout diets were analyzed at all three locations. The PCB concentrations were also determined in alewife (Alosa pseudoharengus), rainbow smelt (Osmerus mordax), bloater (Coregonus hoyi), slimy sculpin (Cottus cognatus), and deepwater sculpin (Myoxocephalus thompsoni), five species of prey fish eaten by lake trout in Lake Michigan, at three nearshore sites in the lake. Despite the lack of significant differences in the PCB concentrations of alewife, rainbow smelt, bloater, slimy sculpin, and deepwater sculpin from the southeastern nearshore site near Saugatuck (Michigan) compared with the corresponding PCB concentrations from the northwestern nearshore site near Sturgeon Bay (Wisconsin), PCB concentrations in lake trout at Saugatuck were significantly higher than those at Sturgeon Bay. The difference in the lake trout PCB concentrations between Saugatuck and Sturgeon Bay could be explained by diet differences. The diet of lake trout at Saugatuck was more concentrated in PCBs than the diet of Sturgeon Bay lake trout, and therefore lake trout at Saugatuck were more contaminated in PCBs than Sturgeon Bay lake trout. These findings were useful in interpreting the long-term monitoring series for contaminants in lake trout at both Saugatuck and the Wisconsin side of the lake.     

Are PCB Levels in Fish from the Canadian Great Lakes Still Declining?

Long- and short-term levels and trends of polychlorinated biphenyls (PCBs) in lake trout (Salvelinus namaycush) and walleye (Sander vitreus) from the Canadian waters of the Great Lakes are examined using the bootstrap resampling method in light of the Great Lakes Strategy 2002 (GLS-2002) objective of decrease in concentrations by 25% during 2000–2007. This objective has been set as an indicator of progress toward the long-term goal of all Great Lakes fish being safe to eat without restriction. Lake Superior lake trout and walleye PCB concentrations were almost unchanged between 1990-2006, and the bootstrap analysis suggests that the probability of achieving the GLS-2002 objective is negligible (< 2%). The PCB levels in Lake Huron lake trout and walleye are decreasing; the declines between 2000–2007 are estimated to be 25–35% and 5–30%, respectively. In contrast, Lake Erie walleye concentrations will likely increase by 25–50% between 2000–2007. For Lake Ontario lake trout, achieving the 25% reduction target seems highly probable with a likely decrease of 45–55%; for Lake Ontario walleye, the probability of achieving such a reduction is only 8% with an expected change of −13 to +15%. Although the targeted reduction may not be achieved for walleye from Lakes Superior, Huron, and Ontario, their best projected 2007 PCB levels are below the unlimited fish consumption guideline of 105 ng/g wet weight used by the Ontario Ministry of the Environment. In contrast, although there are high probabilities of achieving the goal for lake trout from Lakes Huron and Ontario, their best projected 2007 PCB levels (160 and 370 ng/g ww, respectively) will continue to result in consumption restrictions. Lake Superior lake trout concentrations may remain unchanged at the current elevated level of 160 ng/g ww. For Lake Erie fish, the projected 2007 concentrations and the increasing trends are both worrisome. Additional measurements beyond 2007 are necessary to confirm these estimates because of the observed periodic oscillations in the concentrations.     

Is it safe to eat fish from the Great Lakes? An adaptive modelling-monitoring framework to assess compliance with consumption advisories

In this study, we conducted a retrospective analysis of the spatio-temporal trends of fish contamination in the Canadian Great Lakes. We subsequently formulated consumption advisories that explicitly account for all sources of uncertainty, such as model error, sampling bias, and natural variability of fish assemblages. Our analysis generated exceedance frequency maps of the tolerable daily intakes (TDIs), which showed that mercury (Hg) concentrations are generally at a safer level for consumption, whilst polychlorinated biphenyls (PCBs) continue to result in restrictive advisories. Specifically, the initial decline in PCBs has transitioned into a steady state, possibly due to the combined effects of external contamination sources and internal abiotic and biotic factors. Our assessment of the PCB decline rates required to comply with TDI thresholds over the next twenty years suggest that a small degree of reduction is needed for Walleye (Sander vitreus) across all sampled sites, whereas much faster decay rates are needed for Lake Trout (Salvelinus namaycush), especially in lower Lake Huron, Lake Erie, and Lake Ontario. We also detected a distinct Hg gradient whereby the southernmost waterbody, Lake Erie, had the lowest average concentrations, whereas the highest levels amongst the fish species sampled were registered in St. Lawrence River. Finally, we show the ability of our Bayesian approach to fish consumption advisories to produce time-specific, highly customizable, risk-assessment statements that account for the inherent variability in natural fish communities and the variant degree of empirical evidence about the contamination history in different locations around the Great Lakes.     

Polychlorinated biphenyls and organochlorine pesticides concentration patterns and trends in top predator fish of Laurentian Great Lakes from 1999 to 2014

Concentration patterns and temporal trends of legacy persistent, bioaccumulative and toxic (PBT) contaminants were determined using the Great Lake Fish Monitoring and Surveillance Program (GLFMSP) top predator fish data from 1999 to 2014 and applying Kendall-Theil robust regression after cluster-based age normalization. For most Great Lakes sites, significant decreasing concentration trends ranging from ?4.1% to ?21.6% per year (with the only exception being mirex in Lake Erie walleye) were found for PBTs including polychlorinated biphenyls (PCBs), dichloro-diphenyl-trichlorethane (DDTs), dieldrin, endrin, chlordane, oxychlordane, nonachlor, mirex, and hexachlorobenzene (HCB) reflecting the successful historical and ongoing reduction of fugitive releases and remediation efforts in the U.S. and Canada including physical removal (dredging) coupled with sediment sequestration. Generally, lower concentrations and faster decreasing trends are observed in western/northern sampling sites compared to eastern/southern sites as the former sites are generally more remote from population centers and industrial activities. PCBs, which can be released from ongoing sources, have the highest concentration, the second slowest decreasing trend, and increasing mass fractions of the contaminants studied suggesting that they will continue to be the legacy contaminant of greatest concern into the future.     

Concentrations of Polychlorinated Biphenyls in the Water Column of the Laurentian Great Lakes: Spring 1993

PCB concentrations were measured in the Laurentian Great Lakes of North America in the Spring of 1993. Quality control criteria were met for 97% of the dissolved phase samples and 90% of the particulate phase samples. Data are reported as total PCBs and as homolog groups for both of the operationally-defined phases at a 0.7 μM cutoff. Detection limit estimates were 21 pg/L for dissolved phase and 23 pg/L for particulate phase total PCBs, based on a sample volume of 190 L. Total PCB concentrations ranged from 100 pg/L in Lake Superior to 1.6 ng/L in the western basin of Lake Erie. Lakes Michigan and Ontario had the highest lakewide average total PCB concentrations, followed by Lake Huron, and then Lake Superior. Lakewide averaging across the three basins of Lake Erie was too variable to be useful.     

Contaminant Residues in Tissues of Adult and Prefledged Herring Gulls from the Great Lakes in Relation to Diet in the Early 1990s

In the early 1990s, herring gulls (Larus argentatus) were collected in 15 breeding colonies throughout the Great Lakes basin and in two reference colonies on Lake Winnipeg and the Bay of Fundy. Organochlorine and metal concentrations, and stable isotope ratios (¹⁵N/¹⁴N and ¹³C/¹²C) were measured in their tissues, and we qualitatively assessed their diet. Breast muscle δ¹⁵N suggested that adults fed on planctivorous or insectivorous fish at six colonies, on piscivorous fish at four, and at a lower trophic level at the remaining three. The concentrations of Co, Ni, Al, Cr, Sn, Fe, and Pb in kidneys of adults suggested anthropogenic enrichment in the Great Lakes basin. Concentrations of contaminants were highest most often in tissues of gulls from Lake Ontario and northern Lake Michigan colonies. Concentrations of Pb in adults from Hamilton Harbour and the Detroit River, and of Se in adults from the southern Lake Huron colony, were similar to published toxicity thresholds. Tissue levels of Cd have increased, while those of Pb have decreased markedly since 1983. DDE, dieldrin, mirex, and ΣPCB concentrations in livers collected from nine of these colonies revealed declines of 16 to 87% at most locations since the early 1980s. 2,3,7,8-tetrachlorodibenzo-p-dioxin equivalents were highest in adults from the offshore colonies in western Lake Erie and northern Lake Michigan, where gulls feed on piscivorous fish, and were driven by non-ortho PCBs. There was evidence of an unusually high bioavailablity of organochlorines, especially dieldrin, near the northern Lake Michigan colony during the period of chick growth, and of an ongoing loading of mercury to eastern Lake Ontario. Tissues of adult gulls from colonies on Lakes Ontario, Erie, and Michigan best reflect local conditions whereas those from Lake Superior and northern Lake Huron reflect contaminants accumulated from time spent on the lower lakes.     

Total and methyl mercury accumulation in 1994–1995 Lake Michigan lake trout and forage fish

As part of the Lake Michigan Mass Balance Project, total and methyl mercury were determined for lake trout (Salvelinus namaycush) and five forage fish species collected from Lake Michigan near Saugatuck, Michigan, and Port Washington, Sheboygan Reef, and Sturgeon Bay, Wisconsin, between 1994 and 1995. With a mean concentration of 179 ng/g wet wt., whole lake trout total mercury (Hg_T) concentrations ranged between 27.6 and 348 ng/g wet wt. For combined sites, 1–4 yrs, 5–6 yrs, 7–11 yrs, and 12–15 yrs lake trout mean Hg_T concentrations were 73.7, 130, 212, and 280 ng/g, respectively. Forage fish species alewife (Alosa pseudoharengus), bloater (Coregonus hoyi), slimy sculpin (Cottus cognatus), deepwater sculpin (Myoxocephalus thompsoni), and rainbow smelt (Osmerus mordax) had mean Hg_T concentrations of 63.8, 55.3, 36.7, 51.4, and 35.2 ng/g wet wt., respectively. With the exception of alewife, bloater, and slimy sculpin, all fish species contained approximately 100% methyl mercury (MeHg). Field bioaccumulation factors (BAF) were consistent with a Lake Michigan food chain that is more efficient at transferring MeHg to higher trophic levels than some inland lakes. This and other studies of lake trout from Lake Michigan document decreasing Hg_T concentrations in lake trout from 1971 to 1985 and constant or increasing concentrations between 1985 and 2000. These observations were supported by a similar trend in Lake Michigan Hg sediment fluxes. To our knowledge, this is the most intense two year study of mercury in fish for any Great Lake or other large fresh water system and is one of the most complete studies of mercury cycling in the Lake Michigan food chain.     

Temporal and spatial trends of organochlorines and mercury in fishes from the St. Clair River/Lake St. Clair corridor,Canada

The temporal and spatial relationships of a suite of organochlorine contaminants and mercury were examined in various fish species of the St. Clair River/Lake St. Clair corridor, Canada, in order to evaluate the effectiveness of remediation efforts and to assess the risk to human and wildlife fish consumers. In Lake St. Clair, fish tissue concentrations of mercury, polychlorinated biphenyls (PCBs), octachlorostyrene (OCS), hexachlorobenzene (HCB), and dichlorodiphenyltrichloroethane (DDT) decreased consistently from the 1970s until the 1980s and 1990s, after which the rate of contaminant decline slowed or concentrations stabilized. This trend was consistent in up to 13 species (both young-of-the-year and adult fishes) comprising different trophic positions and dietary habits, suggesting that the changes were reflective of ambient conditions rather than food web processes. Elevated concentrations of mercury, PCBs, OCS, HCB, and DDT were detected in St. Clair River young-of-the-year spottail shiner compared with fish from Lake Huron, indicating that non-atmospheric inputs of these chemicals, likely originating from sediment, remain in the St. Clair River. Current concentrations of mercury and PCBs, and mercury, PCBs, and DDT remain of concern to human and wildlife fish consumers, respectively. Given that contaminant decreases have generally stabilized in fish, we suggest that further natural recovery of contaminants in St. Clair corridor fishes will be slow since contaminants will likely continue to be influenced by sediment levels.     

Organochlorine and Heavy Metal Residues in Standard Fillets of Coho and Chinook Salmon of the Great Lakes - 1980

Coho (Oncorhynchus kisutch) and chinook (O. tshawytscha) salmon were collected from seven Michigan tributaries to the Great Lakes and analyzed for chlorinated hydrocarbon pesticides, polychlorinated biphenyls (PCB), and metals. Analyses of standard skin-on fillets of these salmon revealed the presence of PCBs, DDT, dieldrin, zinc (found in one chinook), and mercury, but no detectable residues of aldrin, chlordane, heptachlor, heptachlor epoxide, toxaphene, arsenic, cadmium, chromium, copper, or lead. Chlorinated hydrocarbon contaminants were present at significantly lower levels than were found in salmon samples collected in 1971. No sample of either species exceeded FDA action levels for DDT, dieldrin, or mercury; however, 6 of 63 coho and 29 of 50 chinook salmon exceeded the FDA action level for PCBs. In general, chinook salmon had higher contaminant levels than did coho salmon collected at the same time and location. Salmon collected from the southernmost Lake Michigan tributary had highest contaminant levels (especially PCBs) while salmon from the Lake Erie tributaries had lowest contaminant levels. Samples analyzed as skinless fillets showed dramatically reduced levels of PCBs and DDT analogs compared to standard, skin-fillets from the same fish. A strong linear correlation was observed between residues of DDT and PCBs in samples analyzed     

Chlorinated Contaminants in Surficial Sediments of Lakes Huron,St. Clair,and Erie: Implications Regarding Sources Along the St. Clair and Detroit Rivers

Surficial sediments from southern Lake Huron, Lake St. Clair, and Lake Erie have been analyzed for a broad spectrum of chlorinated organics including PCBs, chlorobenzenes, and several pesticides. The differences between sediment contaminant concentrations in Lake Huron and Lake St. Clair indicated sources of hexachlorobenzene, hexachlorobutadiene, octachlorostyrene, and several other chlorinated benzenes along the St. Clair River. Similar differences between sediment PCB concentrations in Lakes Huron/St. Clair and Lake Erie indicated major PCB sources along the Detroit River. Specific PCB congener analysis revealed that PCBs discharged to the Detroit River contained especially high concentrations of highly chlorinated hexa-, hepta-, and octachloro-biphenyls which are major constituents of the industrial mixture Aroclor 1260. The analysis of individual PCB congeners made it possible to trace PCBs of Detroit River origin to the central and eastern basins of Lake Erie, and to estimate the contribution of the Detroit River to the PCB burden in sediments of these basins.     

Maternal Transfer of Organochlorines to Eggs of Walleye (Stizostedion vitreum) in Lake Manitoba and Western Lake Superior

Gravid walleye were sampled from Lake Manitoba and western Lake Superior (St. Louis River) to measure the concentrations of organochlorine contaminants (OCs) in eggs and muscle and to assess the influence of maternal age and size on the transfer of OCs from mother to egg. Concentrations of most OCs in Lake Superior walleye eggs were 1 to 3 orders of magnitude greater than in Lake Manitoba eggs. Toxaphene (mean concentration (wet weight) ± 1 SE, 1580 ± 462 ng/g) and polychlorinated biphenyls (PCBs) (240 ± 24 ng/g) were the predominant OCs in Lake Superior walleye eggs, whereas DDT and metabolites (eggs 16 ± 1.5 ng/g, muscle 2.1 ± 0.36 ng/g) and PCBs (eggs 9.2 ± 0.83 ng/g, muscle 2.0 ± 2.4 ng/g) were the most common OCs in Lake Manitoba walleye eggs and female muscle. Egg size (dry mass) and the concentration of most OCs in Lake Manitoba walleye eggs were positively correlated with female length and age. This relationship was strongest for more hydrophobic OCs (e.g., PCBs) but was not significant for less hydrophobic OCs (e.g., hexachlorocyclohexanes (HCHs)). Neither egg size nor egg OC concentration of Lake Superior walleye were significantly correlated with female length or age. There was no relationship between OC concentrations in muscle tissue and female length or age of Lake Manitoba walleye. OC concentrations in Lake Manitoba walleye eggs were not correlated with concentrations in the muscle tissue of the mothers, suggesting that OCs in walleye eggs are derived from various tissues. A positive relationship between the egg:muscle ratio of PCB concentrations and the egg:muscle ratio oflipid in freshwater fish suggests that the maternal transfer of PCBs in freshwater fish is related to the relative amounts of lipid in the eggs and mother. The transfer of hydrophobic OCs from mother to eggs in freshwater fish appears to vary within and among fish species and with the hydrophobicity of the OC.     

Trends of PCB concentrations in Lake Michigan coho and chinook salmon, 1975–2010

The manufacture and use of polychlorinated biphenyls (PCBs) was banned in the United States in 1977 after it was determined that these compounds adversely affect animals and humans. The Wisconsin Department of Natural Resources has quantified total PCB concentrations in Lake Michigan chinook (n = 765) and coho (n = 393) salmon (Oncorhynchus tshawytscha and Oncorhynchus kisutch, respectively) filets since 1975. We analyzed these data to estimate trends in PCB concentrations in these fish (1975–2010). We used generalized linear models with a gamma error distribution and log link fit to the untransformed concentrations. Trend patterns were examined using graphical smoothing and generalized additive models. We identified a candidate set of models that included time trend and other predictor variables. Using the Akaike Information Criterion to select among models we found the best models for both species included piecewise linear time trends, total body length, % lipid, and collection season as predictor variables. The intersection of the two trends was 1985 for chinook salmon and 1984 for coho salmon. PCB concentrations in both species increased with body length and % lipid, and were higher for individuals caught in the fall. Our data reveals a dramatic decline in PCB concentrations of − 16.7% and − 23.9% per year for chinook and coho, respectively, up until the intersection year likely reflecting implementation of restrictions on Aroclor-based PCBs. After the intersection year to 2010, PCB concentrations declined at an annual rate of − 4.0% (95% CI: − 4.4% to − 3.6%) and − 2.6% (95% CI: − 3.3% to − 1.9%) for chinook and coho, respectively.