Current practice in chemical hazard ranking and toxic impact assessments is to estimate fate and toxicity assuming the chemical exists in dissolved and particulate phases and, for metals, that all dissolved species are equally bioavailable. This introduces significant error since metal effects are related to the truly dissolved phase and free metal ion within it, not the total dissolved phase. We introduce a Bioavailability Factor (BF) to the calculation of hazard or Comparative Toxicity Potentials (CTPs) (also known as Characterization Factors; CFs) for use in Life Cycle Impact Assessment (LCIA). The method uses for calculation (1) USEtox for environmental fate, (2) WHAM 6.0 for metal partitioning and speciation in aquatic systems, and (3) Biotic Ligand Model (BLM) for average toxicity. For 12 EU water-types, we calculated medians (range) of CTPs of 1.5 x 10(4) (1.5 x 10(2) to 1.2 x 10(5)), 5.6 x 10(4) (9.4 x 10(3) to 4.1 x 10(5)), and 2.1 x 10(4) (7 x 10(3) to 5.8 x 10(4)) day*m(3)/kg for Cu, Ni, and Zn, respectively, which are up to approximately 1000 times lower than previous values. The greatest contributor to variability in CTPs was the BF, followed by toxicity Effect Factor (EF). The importance of the choice of water-type is shown by changes in the relative ranking of CTPs, which are equally influenced by water chemistry and inherent metal-specific differences.
Recent mercury levels and trends reported for North America suggest a mixed (positive/negative) outlook for the environmental mercury problem. Using one of the largest consistent monitoring data sets in the world, here we present long-term and recent mercury trends in Walleye, Northern Pike, and Lake Trout from the Province of Ontario, Canada, which contains about one-third of the world's fresh water and covers a wide geographical area (1.5 and 3 times larger than France and Germany, respectively). Overall, the results indicate that the fish mercury levels either declined (0.01-0.07 μg/g decade) or remained stable between the 1970s and 2012. The rates of mercury decline were substantially greater (mostly 0.05-0.31 μg/g decade) during the 1970s/80s possibly in response to reductions in mercury emissions. However, Walleye and Pike levels have generally increased (0.01-0.27 μg/g decade) in recent years (1995-2012), especially for northern Ontario (effect sizes for differences between the two periods ranged from 0.39 to 1.04). Proportions of Walleye and Pike locations showing a flat or increasing trend increased from 26-44% to 59-73% between the 1970s/80s and 1995-2012. Mercury emissions in North America have declined over the last few decades, and as such it is logical to expect recovery in fish mercury levels; however, other factors such as global emissions, climate change, invasive species, and local geochemistry are likely affecting the response time and magnitude.
A coupled metal transport and speciation model (TRANSPEC) has been developed for surface aquatic systems that explicitly considers the influence of metal speciation on fate. The TRANSPEC, which is general to most metal and surface aquatic systems, is constructed by sequentially coupling the speciation/complexation module (in this application MINEQL+) with the fugacity/aquivalence approach for the fate calculations. This model formulation increases the mechanistic detail, predictive power, and fidelity to reality of current fugacity-aquivalence fate models for metals by estimating aqueous speciation and complexation, rather than relying on empirically derived partition coefficients. A pseudo-steady state version of TRANSPEC was used to simulate Zn dynamics in Ross Lake (Flin Flon, MB, Canada) that received elevated metal and organic matter inputs for over 50 years. Field studies revealed that ZnS forms soluble ZnL, Zn2+, and ZnSO4(0) increasing pore water concentrations when surficial sediments turn oxic during fall. The model results for three seasonal scenarios suggest that Zn remobilization is driven by resuspension of insoluble ZnS and the contribution of diffusion is negligible, even during fall when ZnS dissolves to increase the concentration of soluble species under oxic conditions in the sediments. The low diffusive flux is due to the binding of Zn to colloidal dissolved organic matter (DOM) for which sediment-water diffusion is relatively slow, a result that was obtained as a result of considering metal speciation in the fate calculations.
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