Best practices for predictions of radionuclide activity concentrations and total absorbed dose rates to freshwater organisms exposed to uranium mining/milling.

Predictions of radionuclide dose rates to freshwater organisms can be used to evaluate the radiological environmental impacts of releases from uranium mining and milling projects. These predictions help inform decisions on the implementation of mitigation measures. The objective of this study was to identify how dose rate modelling could be improved to reduce uncertainty in predictions to non-human biota. For this purpose, we modelled the activity concentrations of 210Pb, 210Po, 226Ra, 230Th, and 238U downstream of uranium mines and mills in northern Saskatchewan, Canada, together with associated weighted absorbed dose rates for a freshwater food chain using measured activity concentrations in water and sediments. Differences in predictions of radionuclide activity concentrations occurred mainly from the different default partition coefficient and concentration ratio values from one model to another and including all or only some 238U decay daughters in the dose rate assessments. Consequently, we recommend a standardized best-practice approach to calculate weighted absorbed dose rates to freshwater biota whether a facility is at the planning, operating or decommissioned stage. At the initial planning stage, the best-practice approach recommend using conservative site-specific baseline activity concentrations in water, sediments and organisms and predict conservative incremental activity concentrations in these media by selecting concentration ratios based on species similarity and similar water quality conditions to reduce the uncertainty in dose rate calculations. At the operating and decommissioned stages, the best-practice approach recommends relying on measured activity concentrations in water, sediment, fish tissue and whole-body of small organisms to further reduce uncertainty in dose rate estimates. This approach would allow for more realistic but still conservative dose assessments when evaluating impacts from uranium mining projects and making decision on adequate controls of releases.

Quantifying historical releases and pre-operation levels of metals and radionuclides.

Assessing the recovery of aquatic ecosystems from metal and radionuclide contamination requires knowledge of the concentration of radionuclides and metals before anthropogenic releases. Pre-operational conditions, or baseline, are often unknown for many mining operations initiated decades ago. The objectives of this study were to quantify baseline levels of metals and radionuclides and describe historical releases of an industrialised watershed in Northern Ontario where mining operations were carried out from 1955 to 1996. For this purpose, water and surface sediment samples were collected from this watershed and in an adjacent non-industrialised watershed every 2 km. Using metal and radionuclide concentrations in the non-impacted watershed, we calculated water and sediment baseline concentrations as upper 95th percentile values. Baseline pH, 226Ra and uranium in water of lakes and rivers were similar at pH of 6.8, 10 mBq·l-1, and 2.5 µg·l-1, respectively. For sediments, baseline lake sediment exhibited concentrations of radionuclides that were higher than river sediments. We calculated baseline concentrations in lake sediment at 2,115 Bq·kg-1 210Pb, 535 Bq·kg-1 210Po, 218 Bq·kg-1 226Ra, 235 Bq· kg-1 228Th, 184 Bq·kg-1 230Th, and 223 Bq·kg-1 232Th. Baseline concentrations of metal levels in lakes were at 98 mg kg-1 Ni, 119 mg kg-1 Cu, 2300 mg kg-1 Zn, 112 mg kg-1 Pb and 19 mg kg-1 U. In Lake Huron, we collected two sediment core profiles along with surface sediment to estimate baseline radionuclide activities and metal concentrations and quantify historical releases from the industrialised watershed. The sediment core profiles reflected baseline conditions prior to releases from the uranium mining operation and contamination from its onset in 1955 to its closure in 1996. Concentration of metals in pre-industrial sediment layers were lower than in surface sediment of Lake Huron, suggesting atmospheric depositions. Our study indicates that collecting surface sediment in this non-impacted watershed may yield baseline concentrations for uranium and radionuclides. For metal, collecting surface sediment may yield ambient metal concentrations because of long-range atmospheric transport from remote sources. By comparison, sedimentary profiles can provide baseline concentrations of both metals and radionuclides. In the case of the Serpent River watershed, we report that water quality has recovered downstream of Quirke Lake as of 1993 and that additional sediment cores would better assess sediment recovery.

Microbial Degradation of Cellulosic Material and Gas Generation: Implications for the Management of Low- and Intermediate-Level Radioactive Waste.

Deep geologic repositories (DGR) in Canada are designed to contain and isolate low- and intermediate-level radioactive waste. Microbial degradation of the waste potentially produces methane, carbon dioxide and hydrogen gas. The generation of these gases increase rock cavity pressure and limit water ingress which delays the mobility of water soluble radionuclides. The objective of this study was to measure gas pressure and composition over 7 years in experiments containing cellulosic material with various starting conditions relevant to a DGR and to identify micro-organisms generating gas. For this purpose, we conducted experiments in glass bottles containing (1) wet cellulosic material, (2) wet cellulosic material with compost Maker, and (3) wet cellulosic material with compost Accelerator. Results demonstrated that compost accelerated the pressure build-up in the containers and that methane gas was produced in one experiment with compost and one experiment without compost because the pH remained neutral for the duration of the 464 days experiment. Methane was not formed in the other experiment because the pH became acidic. Once the pressure became similar in all containers after 464 days, we then monitored gas pressure and composition in glass bottle containing wet cellulosic material in (1) acidic conditions, (2) neutral conditions, and (3) with an enzyme that accelerated degradation of cellulose over 1965 days. In these experiments, acetogenic bacteria degraded cellulose and produced acetic acid, which acidity suppressed methane production. Microbial community analyses suggested a diverse community of archaea, bacteria and fungi actively degrading cellulose. DNA analyses also confirmed the presence of methanogens and acetogens in our experiments. This study suggests that methane gas will be generated in DGRs if pH remains neutral. However, our results showed that microbial degradation of cellulose not only generated gas, but also generated acidity. This finding is important as acids can limit bentonite swelling and potentially degrade cement and rock barriers, thus this requires consideration in the safety case as appropriate.

Bioaccumulation and toxicity of uranium, arsenic, and nickel to juvenile and adult Hyalella azteca in spiked sediment bioassays.

Uranium (U) mining and milling release arsenic (As), nickel (Ni) and U to receiving waters, which accumulate in sediments. The objective of the present study was to investigate if As, Ni, and U concentrations in tissue residue of Hyalella azteca, overlying water, sediment porewater, and solids could predict juvenile and adult survival and growth in conditions similar to lake sediments downstream of U mines and mills. We conducted 14-d static sediment toxicity tests spiked with U, As, and Ni salts. For U, we spiked uranyl nitrate with sodium bicarbonate to limit U precipitation once in contact with circumneutral sediment. The median lethal concentrations for As, Ni, and U of juveniles and adults based on measured concentrations in sediments were 134 and 165 µg/g, 370 and 787 µg/g, and 48 and 214 µg/g, respectively. Adult survival and growth linearly decreased with increasing bioaccumulation. For juveniles, metal accumulation linearly predicted survival. We calculated median lethal body concentrations for juveniles and adults of 5 and 36 µg As/g, 14 and 49 µg Ni/g, and 0.4 and 1.0 µg U/g. The concentrations of As, Ni, and U in tissue residue leading to a 20% decrease in adult growth were 32 µg As/g, 44 µg Ni/g, and 1 µg U/g. Overall, the present study showed that U was the most toxic element, followed by As and Ni; that juveniles were more sensitive to the 3 metals tested than adults; and that threshold body concentrations can support assessment of benthic invertebrate community impairment. Environ Toxicol Chem 2018;37:2340-2349. © 2018 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals, Inc. on behalf of SETAC.

Impact of environmentally based chemical hardness on uranium speciation and toxicity in six aquatic species.

Treated effluent discharge from uranium (U) mines and mills elevates the concentrations of U, calcium (Ca), magnesium (Mg), and sulfate (SO4 (2-) ) above natural levels in receiving waters. Many investigations on the effect of hardness on U toxicity have been experiments on the combined effects of changes in hardness, pH, and alkalinity, which do not represent water chemistry downstream of U mines and mills. Therefore, more toxicity studies with water chemistry encountered downstream of U mines and mills are necessary to support predictive assessments of impacts of U discharge to the environment. Acute and chronic U toxicity laboratory bioassays were realized with 6 freshwater species in waters of low alkalinity, circumneutral pH, and a range of chemical hardness as found in field samples collected downstream of U mines and mills. In laboratory-tested waters, speciation calculations suggested that free uranyl ion concentrations remained constant despite increasing chemical hardness. When hardness increased while pH remained circumneutral and alkalinity low, U toxicity decreased only to Hyalella azteca and Pseudokirchneriella subcapitata. Also, Ca and Mg did not compete with U for the same uptake sites. The present study confirms that the majority of studies concluding that hardness affected U toxicity were in fact studies in which alkalinity and pH were the stronger influence. The results thus confirm that studies predicting impacts of U downstream of mines and mills should not consider chemical hardness. Environ Toxicol Chem 2015;34:562-574. © 2014 The Authors. Published by Wiley Periodicals, Inc. on behalf of SETAC.

Temporal trends and spatial variability of mercury in four fish species in the Ontario segment of the St. Lawrence River, Canada.

The Massena (New York) and Cornwall (Ontario) region has a long history of Hg discharge into the St. Lawrence River. The objectives of this study were to evaluate if Hg levels have declined in this portion of the river since 1975 and to compare Hg level in fish species upstream and downstream of this area in order to evaluate the anthropogenic contribution to Hg levels in fish. Mercury levels in four fish species were monitored over a 20-year period (1975-1995). A general linear model and an analysis of covariance were used to extract temporal trends and spatial variability, respectively, while correcting the data for fish length. Over time, Hg levels declined in most fish species. In the four regions studied, Hg levels in fish were similar, which suggests that other sources like atmospheric deposition and Hg loading from the Great Lakes may also contribute to the Hg burden in fish in the St. Lawrence River. This indicates that fish, with large home range, are good biomonitors of temporal Hg releases but their ability to avoid point sources makes them less appealing as biomonitors to address spatial variability in Hg releases.

Dynamic multipathway modeling of Cd bioaccumulation in Daphnia magna using waterborne and dietborne exposures.

We tested the predictive ability of the dynamic multipathway bioaccumulation model (DYMBAM) to characterize Cd accumulation in Daphnia magna, a species commonly used in toxicity tests and because of its sensitivity, particularly to metals, a species that is relied upon in ecological risk assessments. We conducted chronic exposure experiments in which D. magna were exposed to either dietborne Cd alone or to both dietborne and waterborne Cd. In the food-only treatments, the algae Chlamydomonas reinhardtii or Pseudokirchneriella subcapitata were pre-exposed to free Cd ion concentrations, [Cd(2+)], from 0.001 to 100nM (0.001-11microgL(-1)) then, on a daily feeding renewal basis, fed to D. magna over 21 days. In the water plus food treatment, D. magna were exposed for 21 days to the same range of [Cd(2+)] and fed with the same algal species that had been exposed to Cd at various concentrations. In the algal exposure media, Cd concentrations in algae were directly related to those in water and were characterized by a linear regression model using the log transformed concentration of the WHAM predicted Cd(2+) concentration. The DYMBAM was used with estimated values of the model constants for ingestion rate (0.08-0.34gg(-1)day(-1)) and growth rate (0.085-0.131day(-1)) based on our experimental data and with literature values for rate constants of Cd influx and efflux as well as Cd assimilation efficiency. Measured Cd concentrations in D. magna agreed with model predictions within a factor of 3. Using the model, we predict that food is an important contributor of Cd burden to D. magna, particularly at lower Cd exposure concentrations over an environmentally realistic gradient of free Cd in water. However, this cladoceran also takes up Cd from water and this exposure route becomes increasingly important at very high concentrations of free Cd (>10nM or 1.1microgL(-1)). Nevertheless, Cd produced lethal effects in D. magna that were exposed to this metal in water and diet, but exposure to Cd in food only did not result in toxic effects (as measured by survival and reproduction).

Phytoremediation of effluents from aluminum smelters: a study of Al retention in mesocosms containing aquatic plants.

Four mesocosms were exposed to circumneutral and aluminum (Al)-rich wastewater during two successive summers (2000, 2001). The goals of the study were to measure the bioaccumulation of dissolved Al by the aquatic plants Typha latifolia, Lemna minor, Nuphar variegatum and Potamogeton epihydrus, and to evaluate their importance in the retention of Al by the mesocosms. In 2000, inlet concentrations of total monomeric Al were reduced by 56% and 29% at the Arvida and Laterrière mesocosms, respectively, whereas in 2001 inlet dissolved Al concentrations in the inlet decreased by 40% and 33%. L. minor had the highest Al uptake rate (0.8--17 mg Al g(-1)d(-1)). However, because T. latifolia (cattails) yielded the highest biomass, it was responsible for 99% of the Al uptake, largely in its root tissue. In 2001, Al uptake by macrophytes accounted for 2--4% and 15--54% of the total Al retained by the Laterrière and Arvida mesocosms, respectively. In the Laterrière mesocosms, Al uptake by cattails could account for 12% and 18% of the dissolved Al retained by both mesocosms. In contrast, dissolved Al was not significantly reduced in the Arvida enclosures, yet cattails did accumulate Al in their roots. Further research is needed to identify the species community composition that would optimize dissolved Al retention.

Testing sediment biological effects with the freshwater amphipod Hyalella azteca: the gap between laboratory and nature.

The freshwater amphipod, Hyalella azteca, is widely used in laboratory sediment toxicity and bioaccumulation tests. However, its responses in the laboratory are probably very different from those in the field. A review of the literature indicates that in its natural habitat this species complex is primarily epibenthic, derives little nutrition from the sediments, and responds primarily to contaminants in the overlying water column (including water and food), not sediment or porewater. In laboratory sediment toxicity tests H. azteca is deprived of natural food sources such as algal communities on or above the sediments, and is subjected to constant light without any cover except that afforded by burial into the sediments. Under these constraining laboratory conditions, H. azteca has been reported to respond to sediment or porewater contamination. In nature, contamination of overlying water from sediment is less likely than in the laboratory because of the large, generally non-static sink of natural surface water. H. azteca does not appear to be the most appropriate test species for direct assessments of the bioavailability and toxicity of sediment contaminants, though it is probably appropriate for testing the toxicity of surface waters. Toxic and non-toxic responses will be highly conservative, though the latter are probably the most persuasive given the exposure constraints. Thus H. azteca is probably a suitable surrogate species for determining sediments that are likely not toxic to field populations; however, it is not suitable for determining sediments that are likely toxic to field populations.