-
[show abstract]
[hide abstract]
ABSTRACT: Sediment quality thresholds (SQTs) are used by a variety of agencies to assess the potential for adverse impact of sediment-associated contaminants on aquatic biota, typically benthic invertebrates. However, sedimentary contaminants can also result in elevated fish contaminant levels, triggering consumption advisories that are protective of humans. As such, SQTs that would result in fish concentrations below consumption advisory levels should also be considered. To illustrate how this can be addressed, we first calculate biota sediment accumulation factors (BSAFs) for polychlorinated biphenyls (total PCB) and polychlorinated dioxins-furans (PCDD/Fs) in the Canadian Great Lakes using measured lake sediment and fish tissue concentrations in 4 fish species, namely, lake trout, whitefish, rainbow trout, and channel catfish. Using these BSAFs and tissue residue values for fish consumption advisories employed by the Ontario Ministry of the Environment (OMOE, Canada), we derive fish consumption advisory-based SQTs (fca-SQTs) that are likely to result in fish tissue residues that are safe to eat without restriction. The PCDD/Fs fca-SQTs ranged from 6 to 128 pg toxic equivalents (TEQ)/g dry weight (dw) and were above the Canadian Council of the Ministers of the Environment (CCME) threshold effect level (TEL) of 0.85 pg TEQ/g dw. In contrast, the total PCB fca-SQTs ranged from 1 to 60 ng/g dw and were generally below the CCME's TEL of 34.1 ng/g and OMOE's lowest effect level (LEL) of 70 ng/g; however, they were consistent with the OMOE's no effect level (NEL) of 10 ng/g. The fca-SQTs derived using the BSAF as well as food chain multiplier (FCM) approach for a smaller scale system (Hamilton Harbour in Lake Ontario) corresponded well with average lakewide Lake Ontario fca-SQTs. This analysis provides approximate sediment concentrations necessary for reducing fish consumption advisories for each of the Canadian Great Lakes and emphasizes the impacts of historical lake sediment contamination on fish advisories. We believe that this approach merits consideration in sediment guideline development.
Integrated Environmental Assessment and Management 10/2010; 6(4):641-52.
-
[show abstract]
[hide abstract]
ABSTRACT: Concentrations of the seventeen 2,3,7,8-substituted, most toxic congeners of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) were measured in lake trout (Salvelinus namaycush) or lake whitefish (Coregonus clupeaformis) collected between 1989 and 2003 from the Canadian Great Lakes as a part of the on-going Sport Fish Contaminant Monitoring Program of the Ontario Ministry of the Environment. These monitoring data were used to assess temporal trends and spatial variations of these compounds in the Canadian Great Lakes. Toxic equivalents (TEQs) were calculated using the measured congener concentrations and toxicity equivalency factors (TEFs) published by the World Health Organization in 1998. Five congeners, namely 2,3,7,8-TCDD, 2,3,7,8-TCDF, 1,2,3,7,8-PeCDD, 1,2,3,7,8-PeCDF, and 2,3,4,7,8-PeCDF, were the most dominant congeners among the 17 congeners analyzed. The highest TEQs were found for Lake Ontario lake trout (22-54 pg g(-1)) while the TEQs for the other Canadian Great Lakes were 60-95% lower. Non-parametric Mann-Kendall and Sen's tests performed on TEQs and PCDD/Fs standardized at a mean lake trout length of 60 cm suggest a linearly decreasing trend for PCDD/Fs in lake trout from Lakes Ontario and Huron. There was no monotonously increasing or decreasing trend found for Lake Superior lake trout. The ratios of 2,3,7,8-TCDD to 2,3,7,8-TCDF concentrations were generally constant during the 1989-2003 period with the values being in the order of Lakes Superior (0.05-0.3) <or= Huron (0.16-0.25)<Ontario (0.56-0.88). These spatial differences observed in the relative abundance of TCDD and TCDF suggest that the sources of dioxins and furans differ between the upper and lower Great Lakes.
Chemosphere 05/2008; 73(1 Suppl):S158-65. · 3.21 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: The toxic equivalent (TEQ) concept is widely used to assess toxicity potential of a dioxin-like chemical mixture. The TEQ approach converts concentrations of various dioxin-like compounds into a single concentration that is toxicologically equivalent to the most toxic dioxin compound, 2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD), using toxic equivalency factors (TEFs). It has been shown that in the absence of costly measurements of dioxin-like polychlorinated biphenyls (dl-PCBs) in fish, relatively inexpensive measurements of total PCB can be utilized to estimate dl-PCB-related TEQ (i.e., TEQ(dl-PCB)). The present study assesses the impacts of uncertainties in dl-PCB measurements and estimates, and mammalian TEFs on TEQ(dl-PCB) using the Monte Carlo technique. The analysis suggests that measurement errors for dl-PCBs translate into up to 1.3-fold uncertainty in TEQ(dl-PCB), while uncertainties in estimates of dl-PCBs generally produce up to a threefold uncertainty in TEQ(dl-PCB). In contrast, the uncertainty due to TEFs normally ranges 10- to 13-fold and spans over 30- to 40-fold under extreme cases. For 2005 TEFs, PCB-126 is the dominating contributor to uncertainty in TEQ(dl-PCB). When we considered uncertainties in the TEFs and estimated dl-PCB concentrations simultaneously, there was little increase in uncertainty in TEQ(dl-PCB) that was already produced by the TEFs only. These results indicate that the dl-PCB composition in fish and/or the relationship between total PCB and TEQ(dl-PCB) can be utilized to estimate TEQ(dl-PCB) with reasonable confidence.
Environmental Toxicology and Chemistry 05/2008; 27(4):997-1005. · 2.81 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: Toxic Equivalency Factors (TEFs) are an essential part of the Toxic Equivalent (TEQ) concept and have evolved for dioxins/dioxin-like compounds over the last two and half decades. Therefore, it is difficult to compare past and current TEQs that are reported using different TEFs without explicitly mentioning underlying congener concentrations. Using what likely is the largest known dioxin/furan (PCDD/F) and dioxin-like polychlorinated biphenyl (dl-PCB or DLP) fish database, here we present regression models that can facilitate conversion of a fish TEQ from an old to a newer TEF scheme. The results show that the mammalian PCDD/F-TEQ based on the latest TEF(WHO-05) is about 7.5% lower than that based on TEF(WHO-98). The mammalian DLP-TEQ(WHO-05) is on average 25-26% lower than almost identical DLP-TEQ(WHO-94) and DLP-TEQ(WHO-98). Total-TEQ(WHO-05) is on average 22% lower than Total-TEQ(WHO-98). According to the current toxicological standards for dioxins/furans, all previous major TEF schemes except TEF(Germany-85) and TEF(USEPA-87) were conservative (i.e., higher) in estimating TEQs. The major (> 75%) contribution to PCDD/F-TEQ(WHO-05) is from 2,3,7,8-TCDD (33%), 1,2,3,7,8-PCDD (26%), 2,3,7,8-TCDF (10%), and 2,3,4,7,8-PCDF (9%). The DLP-TEQ(WHO-05) is dominated by PCB-126 which on average contributes about 88%. The DLP-TEQ generally contribute > 70% of Total-TEQ. When reporting TEQs, we recommend that the underlying congener specific concentrations are presented, TEF scheme used is clearly stated, names of compounds included are explicitly expressed, and TEQs are identified accordingly (e.g., DLP-TEQ, PCDD/F-TEQ, Total-TEQ).
Environment International 03/2008; 34(7):915-21. · 5.30 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: The Toxic Equivalent (TEQ) concept is widely used to assess toxicity potential of a dioxin-like chemical mixture. The TEQ approach converts concentrations of various dioxin-like compounds into a single concentration, which is toxicologically equivalent to most toxic dioxin compound 2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD), using Toxic Equivalency Factors (TEFs). It has been shown that in the absence of costly measurements of dioxin-like PCBs (dl-PCBs) in fish, relatively inexpensive measurements of total PCB can be utilized to estimate dl-PCB related TEQ (i.e., TEQdl-PCB). This paper assesses impacts of uncertainties in dl-PCB measurements, dl-PCB estimates, and mammalian TEFs on TEQdl-PCB using the Monte Carlo technique. The analysis suggests that measurement errors for dl-PCBs translate into up to 1.3-fold uncertainty in TEQdl-PCB while uncertainties in estimates of dl-PCBs generally produce up to a 3-fold uncertainty in TEQdl-PCB. In contrast, the uncertainty due to TEFs normally ranges 10-13-fold and spans over 30-40-fold under extreme cases. For 2005 TEFs, PCB-126 is the dominating contributor to uncertainty in TEQdl-PCB. When we considered uncertainties in the TEFs and estimated dl-PCB concentrations simultaneously, there was little increase in uncertainty in TEQdl-PCB that was already produced by the TEFs only. These results indicate that the dl-PCB composition in fish and/or relationship between total PCB and TEQdl-PCB can be utilized to estimate TEQdl-PCB with reasonable confidence.
Environmental Toxicology and Chemistry 01/2008; · 2.81 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: Polychlorinated biphenyls (PCBs) are 209 related compounds, a dozen of which are known as dioxin-like PCBs (dl-PCBs) and are among the most toxic PCBs. Polychlorinated biphenyls contribute to many adverse effects to human health, including cancer, and are a major cause of fish advisories in North America. It is a common perception that individual PCB compounds, especially dl-PCBs, rather than total PCB need to be quantified to predict the environmental hazard because of differences in their toxicity potential and distribution among various environmental matrices, including aquatic food webs. Because the current analytical methods for quantifying dl-PCBs are complex and four- to fivefold more expensive, limited fish samples are analyzed for dl-PCBs. Using what likely is the largest dl-PCB fish data set (n = 912) with a wide distribution of fish species (n = 22), size (19-112 cm), weight (100-14,300 g), sex (male:female, 51:49), and PCB contamination level (20-7,300 ng/g wet wt), we show that the comparatively less expensive and rapid measurements of total PCB in fish can be utilized to assess dl-PCB-related toxicological hazard, measured as 2,3,7,8-tetrachlorodibenzo-p-dioxin toxic equivalents (TEQ). A regression equation of dl-PCB-related TEQ (i.e., TEQdl-PCB) to total PCB in fish is presented (TEQdi-PCB = [2.56 x 10(-5)]CtotalPCB, r = 0.89, p < 0.001). The regression was evaluated by applying it to three independent data sets of substantial sizes (n = 55, 141, and 176). The TEQdl-PCB estimated using the regression and total PCB measurements were within a reasonable factor of two to three of the TEQdl-PCB calculated from the dl-PCB measurements. The successful evaluation indicates versatility of the regression.
Environmental Toxicology and Chemistry 08/2007; 26(8):1622-8. · 2.81 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: It is widely accepted that a congener-specific analysis of polychlorinated biphenyls (PCBs), rather than traditional Aroclor equivalent total PCB analysis, is required for risk assessment. This is based on the fact that environmental processes alter the original distribution of PCB congeners in Aroclors and that toxicity varies considerably among the congeners with dioxin-like PCBs (dl-PCBs) generally being among the most toxic. Using the largest known dl-PCB fish dataset, here we present a likely composition of dl-PCBs in fish. In contrast to common perception, we found that the dl-PCB composition is relatively constant (within approximately a factor of 2) regardless of fish species and total PCB level. The abundance of dl-PCBs expressed as a percentage of total PCB (25-75 quartile range) in fish is generally in the order of PCB-118 (3.0-6.2%) > PCB-105 (1.1-2.4%) > PCB-156 (0.39-0.75%) > PCB-167 (0.20-0.43%) > PCB-123 (0.11-0.26%) > PCB-157 (0.09-0.19%) = PCB-114 (0.08-0.18%) > PCB-189 (0.045-0.094%) > PCB-77 (0.018-0.093%) > PCB-126 (0.015-0.036%) > PCB-81 (0.002-0.007%) = PCB-169 (0.001-0.006%). The most toxic dl-PCB congeners PCB-126 and -169 contribute on average only 0.027 and 0.004% of total PCB, respectively. The statistically significant relationships presented between individual di-PCB and total-PCB concentrations can be used as a practical tool to estimate dl-PCBs for risk assessment purposes. A comparison of the dl-PCB pattern presented here with other studies suggests that this dl-PCB composition is applicable to fish from North America and perhaps from other geographical regions throughout the world.
Environmental Science and Technology 06/2007; 41(9):3096-102. · 5.23 Impact Factor
-
[show abstract]
[hide abstract]
ABSTRACT: 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.
Journal of Great Lakes Research 12/2006; · 1.52 Impact Factor
