Are fish consumption advisories for the great lakes adequately protective against chemical mixtures?

Background: The North American Great Lakes are home to \u3e 140 types of fish and are famous for recreational and commercial fishing. However, the presence of toxic substances has resulted in the issuance of fish consumption advisories that are typically based on the most restrictive contaminant. Objectives: We investigated whether these advisories, which typically neglect the existence of a mixture of chemicals and their possible additive adverse effects, are adequately protective of the health of humans consuming fish from the Canadian waters of the Great Lakes. Methods: Using recent fish contaminant monitoring data collected by the government of Ontario, Canada, we simulated advisories using most-restrictive-contaminant (one-chem) and multi-contaminant additive effect (multi-chem) approaches. The advisories from the two simulations were compared to determine if there is any deficiency in the currently issued advisories. Results: Approximately half of the advisories currently issued are potentially not adequately protective. Of the four Great Lakes studied, the highest percentage of advisories affected are in Lake Ontario if an additive effect is considered. Many fish that are popular for consumption, such as walleye, salmon, bass and trout, would have noticeably more stringent advisories. Conclusions: Improvements in the advisories may be needed to ensure that the health of humans consuming fish from the Great Lakes is protected. In this region, total polychlorinated biphenyls (PCBs) and mercury are the major contaminants causing restrictions on consuming fish, whereas dioxins/furans, toxaphene, and mirex/photomirex are of minor concern. Regular monitoring of most organochlorine pesticides and metals in fish can be discontinued. © 2017, Public Health Services, US Dept of Health and Human Services. All rights reserved

Is it appropriate to composite fish samples for mercury trend monitoring and consumption advisories?

Monitoring mercury levels in fish can be costly because variation by space, time, and fish type/size needs to be captured. Here, we explored if compositing fish samples to decrease analytical costs would reduce the effectiveness of the monitoring objectives. Six compositing methods were evaluated by applying them to an existing extensive dataset and examining their performance in reproducing the fish consumption advisories and temporal trends. The methods resulted in varying amount (average 34-72%) of reductions in samples, but all (except one) reproduced advisories very well (96-97% of the advisories did not change or were one category more restrictive compared to analysis of individual samples). Similarly, the methods performed reasonably well in recreating temporal trends, especially when longer-term and frequent measurements were considered. The results indicate that compositing samples within 5 cm fish size bins or retaining the largest/smallest individuals and compositing in-between samples in batches of 5 with decreasing fish size would be the best approaches. Based on the literature, the findings from this study are applicable to fillet, muscle plug and whole fish mercury monitoring studies. Overall, compositing fish samples for mercury monitoring could result in a substantial savings (approximately 60% of the analytical cost) and should be considered in fish mercury monitoring, especially in long-term programs or when study cost is a concern

Levels, patterns, trends and significance of polychlorinated naphthalenes (PCNs) in Great Lakes fish

Polychlorinated naphthalenes (PCNs) were introduced to market about a century ago and their production is thought to have ceased by the early 1980s. However, relatively limited knowledge exists on their abundance in the edible portion of a variety of Great Lakes fish to aid in understanding their potential risk to human consumers. We studied levels, patterns, trends and significance of PCNs in a total 470 fillet samples of 18 fish species collected from the Canadian waters of the Great Lakes between 2006 and 2013. A limited comparison of fillet and wholebody concentrations in Carp and Bullhead was also conducted. The ∑ PCN ranged from 0.006–6.7 ng/g wet weight (ww) and 0.15–190 ng/g lipid weight (lw) with the dominant congeners being PCN-52/60 (34%), -42 (21%) and -66/67 (15%). The concentrations spatially varied in the order of the Detroit River \u3e Lakes Erie \u3e Ontario \u3e Huron \u3e Superior. PCN-66/67 was the dominating congener contributing on average 76–80% of toxic equivalent concentration (TEQPCN). Contribution of TEQPCN to TEQTotal (TEQDioxins + Furans + dioxin-likePCBs + PCNs) was mostly \u3c 15%, especially at higher TEQTotal, and PCB-126 remains the major congener contributing to TEQTotal. The congener pattern suggests that impurities in PCB formulations and thereby historical PCB contamination, instead of unintentional releases from industrial thermal processes, could be an important source of PCNs in Great Lakes fish. A limited temporal change analysis indicated declines in the levels of PCN-66/67 between 2006 and 2012, complemented by previously reported decrease in PCNs in Lake Ontario Lake Trout between 1979 and 2004. The whole body concentrations were 1.4–3.2 fold higher than the corresponding fillets of Carp and Bullhead. Overall, the study results suggest that only targeted monitoring of PCNs in Great Lakes fish, especially at the Detroit River, Lake Erie and Lake Ontario, is necessary to assess continued future improvements of this group of contaminants of concern

Occurrence and biomagnification of polychlorinated naphthalenes and non- and mono-ortho PCBs in Lake Ontario sediment and biota

Biota and surface sediments collected from Lake Ontario were analyzed for polychlorinated naphthalenes (PCNs) and non- and mono-ortho-substituted polychlorinated biphenyls (n/m-o-PCBs) to compare bioaccumulation behavior of these classes of dioxin-like chemicals in a food web from the Great Lakes. Mean ΣPCN concentrations (tri-octaCN) ranged from 14 ± 9 pg/g in plankton to 3500 ± 3200 pg/g (wet weight) in lake trout, while sediments contained from 21 to 38 ng/g (dry weight). Principal components analysis of PCN congener patterns indicated that chlorine substitution determined which congeners favored accumulation (e.g., CN-42, -52, -60, -66, -67, and -73), while others may be subject to metabolism. The bioaccumulative congeners exhibited similar trophic magnification factors (TMFs; 1.23-1.42) and biomagnification factors (BMFs; 5.5-8.6) to the n/m-o-PCBs for the trout/weighted diet relation, although BMFs for a benthic feeding relationship (slimy sculpin/Diporeia) indicated that the n/m-o-PCBs were more bioavailable through the benthic pathway. PCNs contribute significantly to the burden of dioxin-like compounds in Lake Ontario biota, contributing between 12 and 22% of total PCN + PCB TEQ in lake trout and up to 69% in benthic organisms. © 2008 American Chemical Society

Perfluoroalkyl Acids in European Starling Eggs Indicate Landfill and Urban Influences in Canadian Terrestrial Environments

Perfluoroalkyl acids (PFAAs) were determined in European starling (<i>Sturnus vulgaris</i>) eggs collected between 2009 and 2014 from industrial, rural/agricultural, and landfill locations within five urban centers across Canada. Within each urban center, perfluoroalkyl sulfonic acid (PFSA) concentrations were generally greater in starling eggs collected from urban/industrial locations and PFSAs and perfluoroalkyl carboxylic acids (PFCAs) were generally greater at landfills compared to rural and remote locations. However, the relative importance of urban/industrial versus landfill locations as potential sources was chemical- and location-specific. PFSA concentrations in eggs collected from nonlandfills were positively correlated with human population. Despite the 2000 to 2002 phase-out of perfluorooctanesulfonic acid (PFOS) and its C₈ precursors, leaching from consumer products during use likely continues to be a major source to the environment. In comparison, the concentrations of most PFCAs in eggs were not related to population, which supports the hypothesis that atmospheric transport and degradation of precursor chemicals are influencing their spatial trends. PFAA concentrations in eggs from landfills were not correlated with the quantity of waste received by a given landfill. The variability in PFAAs between landfills may be due to the specific composition of waste items

Perfluoroalkyl Contaminants in Lake Ontario Lake Trout: Detailed Examination of Current Status and Long-Term Trends

Perfluoroalkyl contaminants (PFCs) were determined in Lake Ontario Lake Trout sampled annually between 1997 and 2008 in order to assess how current trends are responding to recent regulatory bans and voluntary phase-outs. We also combined our measurements with those of a previous study to provide an updated assessment of long-term trends. Concentrations of PFCs generally increased from the late 1970s until the mid-1980s to mid-1990s, after which concentrations either remained unchanged (perfluorooctane sulfonate (PFOS) and perfluorocarboxylates) or declined (perfluorodecanesulfonate (PFDS)). The temporal trends were assessed using three models, quadratic, exponential rise to maximum, and two-segment linear piecewise function, and then evaluated for best fit using Akaike Information Criteria. For PFOS and perfluorocarboxylates, the exponential rise to maximum function had the best fit. This is particularly interesting for PFOS as it suggests that although concentrations in Lake Ontario Lake Trout may have stopped increasing in response to voluntary phase-outs in 2000–2002, declines have yet to be observed. This may be due to continuing input of PFOS from products still in use and/or slow degradation of larger precursor molecules. A power analysis of PFOS suggested that 15 years of data with a within-year sample size of 10 is required to obtain sufficient power (80%) to detect a 5% decreasing trend. However, the length of the monitoring program had a greater influence on the ability to detect a trend compared to within-year sample size. This provides evidence that additional sampling years are required to detect a response to bans and phase-outs, given the variability in the fish data. The lack of observed declines of perfluorocarboxylate residues in fish may be expected as regulations for these compounds were only recently enacted. In contrast to the other compounds, the quadratic model had the best fit for PFDS. The results of this study emphasize the importance of long-term monitoring for assessing the effectiveness of bans and phase-outs on PFCs in the environment