Conceptual and Numerical Modeling of Radionuclide Transport and Retention in Near-Surface Systems

Scenarios of barrier failure and radionuclide release to the near-surface environment are important to consider within performance and safety assessments of repositories for nuclear waste. A geological repository for spent nuclear fuel is planned at Forsmark, Sweden. Conceptual and numerical reactive transport models were developed in order to assess the retention capacity of the Quaternary till and clay deposits for selected radionuclides, in the event of an activity release from the repository. The elements considered were carbon (C), chlorine (Cl), cesium (Cs), iodine (I), molybdenum (Mo), niobium (Nb), nickel (Ni), radium (Ra), selenium (Se), strontium (Sr), technetium (Tc), thorium (Th), and uranium (U). According to the numerical predictions, the repository-derived nuclides that would be most significantly retained are Th, Ni, and Cs, mainly through sorption onto clays, followed by U, C, Sr, and Ra, trapped by sorption and/or incorporation into mineral phases.     

Experimental evidence of biomass burning as a source of atmospheric 137Cs,puy de Dôme (1465 m a.s.l.), France

The presence of cesium-137 (¹³⁷Cs) in the environment is mainly due to past nuclear tests and accidental reactor releases. Due to the half-life of ¹³⁷Cs (30.2 y), amounts of this radionuclide releases are in fact still detectable in soils, and at trace levels in the vegetation and the atmosphere. Since the middle of the 1990’s, the presence of ¹³⁷Cs in the atmosphere has long been attributed to the resuspension of terrestrial dust. Recently, modelling studies have demonstrated that an additional and possibly dominant source of this anthropogenic radionuclide is biomass burning. Here, we report the variations of atmospheric ¹³⁷Cs activity levels over a 2-year period at the puy de Dôme (1465 m a.s.l.), France in combination with measurements of the aerosol chemical composition, in particular with indicators for biomass burning (levoglucosan and potassium) and soil dust (calcium). Temporal co-variations of these chemical compounds in addition to back-trajectories are used to identify common source emissions. Significant correlation is found between these compounds. Hence, we experimentally confirm the modelling study highlighting the fact that the atmospheric ¹³⁷Cs is partly released by biomass burning. In addition, we observed that the correlations between the ¹³⁷Cs concentrations and levoglucosan and biomass burning K⁺ differ according to the season. This is in agreement with the temporal evolution of levoglucosan concentration, which has maxima in winter and minima in summer.     

A review of personal care products in the aquatic environment: environmental concentrations and toxicity

Considerable research has been conducted examining occurrence and effects of human use pharmaceuticals in the aquatic environment; however, relatively little research has been conducted examining personal care products although they are found more often and in higher concentrations than pharmaceuticals. Personal care products are continually released into the aquatic environment and are biologically active and persistent. This article examines the acute and chronic toxicity data available for personal care products and highlights areas of concern. Toxicity and environmental data were synergized to develop a preliminary hazard assessment in which only triclosan and triclocarban presented any hazard. However, numerous PCPs including triclosan, paraben preservatives, and UV filters have evidence suggesting endocrine effects in aquatic organisms and thus need to be investigated and incorporated in definitive risk assessments. Additional data pertaining to environmental concentrations of UV filters and parabens, in vivo toxicity data for parabens, and potential for bioaccumulation of PCPs needs to obtained to develop definitive aquatic risk assessments.     

Air pollution assessment based on elemental concentration of leaves tissue and foliage dust along an urbanization gradient in Vienna

Foliage dust contains heavy metal that may have harmful effects on human health. The elemental contents of tree leaves and foliage dust are especially useful to assess air environmental pollution. We studied the elemental concentrations in foliage dust and leaves of Acer pseudoplatanus along an urbanization gradient in Vienna, Austria. Samples were collected from urban, suburban and rural areas. We analysed 19 elements in both kind of samples: aluminium, barium, calcium, copper, iron, potassium, magnesium, sodium, phosphor, sulphur, strontium and zinc. We found that the elemental concentrations of foliage dust were significantly higher in the urban area than in the rural area for aluminium, barium, iron, lead, phosphor and selenium. Elemental concentrations of leaves were significantly higher in urban than in rural area for manganese and strontium. Urbanization changed significantly the elemental concentrations of foliage dust and leaves and the applied method can be useful for monitoring the environmental load.     

Artificial radioactivity in environmental media (air, rainwater, soil, vegetation) in Austria after the Fukushima nuclear accident

Several environmental media in Austria were monitored for artificial radionuclides released during the Fukushima nuclear accident. Air (up to 1.2 mBq/m³ particulate ¹³¹I) and rainwater (up to 5.2 Bq/L ¹³¹I) proved to be the media best suited for the environmental monitoring, allowing also a temporal resolution of the activity levels. Significant regional differences in the wet deposition of ¹³¹I with rain could be observed within the city of Vienna during the arrival of the contaminated air masses. Forward-trajectory analysis supported the hypothesis that the contaminated air masses coming from the northwest changed direction to northeast over Northern Austria, leading to a strong activity concentration gradient over Vienna. In the course of the environmental monitoring of the Fukushima releases, this phenomenon—significant differences of ¹³¹I activity concentrations in rainwater on a narrow local scale (8.1 km)—appears to be unique. Vegetation (grass) was contaminated with ¹³¹I and/or ¹³⁷Cs at a low level. Soil (up to 22 Bq/kg ¹³⁷Cs) was only affected by previous releases (nuclear weapon tests, Chernobyl). Here, also significant local differences can be observed due to different deposition rates during the Chernobyl accident. The effective ecological half-lives of ¹³⁷Cs in soil were calculated for four locations in Austria. They range from 7 to 30 years. No Austrian sample investigated herein exceeded the detection limit for ¹³⁴Cs; hence, the Fukushima nuclear accident did not contribute significantly to the total radiocesium inventory in Austrian environmental media. The levels of detected radioactivity were of no concern for public health.     

Nitrate causes deleterious effects on the behaviour and reproduction of the aquatic snail Potamopyrgus antipodarum (Hydrobiidae, Mollusca)

Nitrate (NO₃ ^?) is present in aquatic ecosystems as a natural component of the nitrogen cycle. However, in the last decades, several human activities are the causes of the rising amounts of organic matter and inorganic nitrogen nutrients in aquatic ecosystems, causing notable increase of nitrate above background natural levels. In spite of the toxicity of nitrate to aquatic animals, there are relatively few studies on the chronic toxicity of this compound to invertebrates. The aim of our study is to assess the effect of chronic (35 days) exposure to nitrate on the behaviour (velocity of movement) and reproduction (number of newborns) of the aquatic snail Potamopyrgus antipodarum. Four actual concentrations of nitrate were used (21.4, 44.9, 81.8 and 156.1 mg?N-NO₃ ^?/L). In each treatment, 12 animals were individually monitored for velocity (weekly) and newborn production (every 3–4 days). Velocity was recorded using quantitative video monitoring. Our results showed that nitrate did not cause mortality, but it reduced the velocity of movement (at 44.9, 81.8 and 156.1 mg?N-NO₃ ^?/L) and number of live newborns (in all tested concentrations). Reproductive impairment was caused at realistic nitrate concentrations which is relevant to the risk assessment of this compound. Our study contributes to the knowledge of the chronic effects of nitrate on the behaviour and reproduction of an aquatic snail.     

Modelling PCB bioaccumulation in a Baltic food web

A steady state model is developed to describe the bioaccumulation of organic contaminants by 14 species in a Baltic food web including pelagic and benthic aquatic organisms. The model is used to study the bioaccumulation of five PCB congeners of different chlorination levels. The model predictions are evaluated against monitoring data for five of the species in the food web. Predicted concentrations are on average within a factor of two of measured concentrations. The model shows that all PCB congeners were biomagnified in the food web, which is consistent with observations. Sensitivity analysis reveals that the single most sensitive parameter is log K(OW). The most sensitive environmental parameter is the annual average temperature. Although not identified amongst the most sensitive input parameters, the dissolved concentration in water is believed to be important because of the uncertainty in its determination. The most sensitive organism-specific input parameters are the fractional respiration of species from the water column and sediment pore water, which are also difficult to determine. Parameters such as feeding rate, growth rate and lipid content of organism are only important at higher trophic levels.     

Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China

This study investigated the presence and distribution of 22 antibiotics, including eight quinolones, nine sulfonamides and five macrolides, in the water, sediments, and biota samples from Baiyangdian Lake, China. A total of 132 samples were collected in 2008 and 2010, and laboratory analyses revealed that antibiotics were widely distributed in the lake. Sulfonamides were the dominant antibiotics in the water (0.86-1563 ng L⁻¹), while quinolones were prominent in sediments (65.5-1166 μg kg⁻¹) and aquatic plants (8.37-6532 μg kg⁻¹). Quinolones (17.8-167 μg kg⁻¹) and macrolides [from below detection limit (BDL) to 182 μg kg⁻¹] were often found in aquatic animals and birds. Salvinia natans exhibited the highest bioaccumulation capability for quinolones among three species of aquatic plants. Geographical differences of antibiotic concentrations were greatly due to anthropogenic activities. Sewage discharged from Baoding City was likely the main source of antibiotics in the lake. Risk assessment of antibiotics on aquatic organisms suggested that algae and aquatic plants might be at risk in surface water, while animals were likely not at risk.     

The occurrence and bioavailability of radioactive 137Cs in small forest lakes in Southern Finland

Following the Chernobyl accident in late April 1986, central Finland was subjected to considerable radioactive fallout. The radioactive isotope of caesium, (137)Cs, was potentially the most harmful isotope in the fallout because of its long half-life (30 years). (137)Cs activities remained unexpectedly low within the biota (algae, zooplankton, aquatic moss, fish) of some humic forest lakes in southern Finland compared to the clear water lakes within the same district. This observation suggested that humic substances, by binding (137)Cs chemically, may reduce its bioavailability in lake water. Our laboratory experiments (throughflow systems; gel chromatography) demonstrated that binding of (137)Cs by humic substances was negligible in untreated lake waters; only when most of the alkali metals had been removed with an ion exchange resin was any binding of (137)Cs by low molecular humic fractions apparent. Instead, the concentrations of cations (especially potassium) were of overwhelming importance for the bioavailability of (137)Cs within the lacustrine ecosystems. The concentrations of (137)Cs within food chains are expected to stay at a high level for many years especially in lakes with long water renewal times.     

Fish pollution with anthropogenic 137Cs in the southern Baltic Sea

This paper presents the results of a study on changes in ¹³⁷Cs activity concentrations in three fish species from the southern Baltic Sea: cod (Gadus morhua), herring (Clupea harengus) and flounder (Platichtys flesus), in the period 2000–2010. During the study period a marked decline in cesium activity concentration in fish muscle tissue was observed, which reflected changes in radionuclide activity concentration in seawater. No statistically significant temporal trends were determined in changes of concentration factors (CF_{fish/seawater}) calculated for the examined fish species. The analysis of ¹³⁷Cs activity as a function of ichthyological parameters revealed the lack of a relationship between radionuclide activity concentrations in herring muscle tissue and the fish age in an narrow age range (2–4 years). However, a reverse proportionality of total fish mass, as well as body length, against ¹³⁷Cs activity concentrations in muscles was well documented. The latter observation can be the direct result of the dilution effect related to the increase of fish body weight. ¹³⁷Cs activity concentration in muscle tissue of the five fish species forms a declining sequence: Gadus morhua, Platichthys flesus, Clupea harengus, Perca fluviatilis and Neogobius melanostomus.     

Methyl Tertiary Hexyl Ether and Methyl Tertiary Octyl Ether as Gasoline Oxygenates: Assessing Risks from Atmospheric Dispersion and Deposition

Abstract

Methyl tertiary hexyl ether (MtHxE) and methyl tertiary octyl ether (MtOcE) are currently being developed as replacement oxygenates for methyl tertiary butyl ether (MtBE) in gasoline. As was the case with MtBE, the introduction of these ethers into fuel supplies guarantees their introduction into the environment as well. In this study, a screening-level risk assessment was performed by comparing predicted environmental concentrations (PEC) of these ethers to concentrations that might cause adverse effects to humans or ecosystems. A simple box model that has successfully estimated urban air concentrations of MtBE was adapted to predict atmospheric concentrations of MtHxE and MtOcE. Expected atmospheric concentrations of these ethers were also estimated using the European Union System for the Evaluation of Substances (EUSES) multimedia fate model, which simultaneously calculates PECs in the various environmental compartments of air, water, soil, and sediment. Because little or no data are available on the physicochemical, environmental, and toxicological properties of MtHxE and MtOcE, estimation methods were used in conjunction with EUSES to predict both the PECs and the concentrations at which these ethers might pose a threat. The results suggest that these ethers would contaminate the air of a moderately sized U.S. city (Boston, MA) at levels similar to those found previously for MtBE. The risk assessment module in EUSES predicted risk characterization ratios of 10^?3 and 10^?2 for MtHxE and MtOcE, respectively, in Boston, and 10^?2 and 10^?1 in very large urban centers, suggesting that these ethers pose only a minimal threat to ecosystems at the anticipated environmental concentrations. The assessment also indicates that these compounds are possible human carcinogens and that they may be present in urban air at concentrations that pose an unacceptable cancer risk. Therefore, testing of the toxicological properties of these compounds is recommended before they replace MtBE in gasoline.     

Occurrence of antibiotics in water,sediments, aquatic plants,and animals from Baiyangdian Lake in North China

This study investigated the presence and distribution of 22 antibiotics, including eight quinolones, nine sulfonamides and five macrolides, in the water, sediments, and biota samples from Baiyangdian Lake, China. A total of 132 samples were collected in 2008 and 2010, and laboratory analyses revealed that antibiotics were widely distributed in the lake. Sulfonamides were the dominant antibiotics in the water (0.86–1563 ng L⁻¹), while quinolones were prominent in sediments (65.5–1166 μg kg⁻¹) and aquatic plants (8.37–6532 μg kg⁻¹). Quinolones (17.8–167 μg kg⁻¹) and macrolides [from below detection limit (BDL) to 182 μg kg⁻¹] were often found in aquatic animals and birds. Salvinia natans exhibited the highest bioaccumulation capability for quinolones among three species of aquatic plants. Geographical differences of antibiotic concentrations were greatly due to anthropogenic activities. Sewage discharged from Baoding City was likely the main source of antibiotics in the lake. Risk assessment of antibiotics on aquatic organisms suggested that algae and aquatic plants might be at risk in surface water, while animals were likely not at risk.     

Bioaccumulation and trophic transfer of mercury in a food web from a large, shallow, hypereutrophic lake (Lake Taihu) in China

Purpose

Due to the fast development of industry and the overuse of agrichemicals in past decades, Lake Taihu, an important source of aquatic products for Eastern China, has simultaneously suffered mercury (Hg) contamination and eutrophication. The objectives of this study are to understand Hg transfer in the food web in this eutrophic, shallow lake and to evaluate the exposure risk of Hg through fish consumption.

Methods

Biota samples including macrophytes, sestons, benthic animals, and fish were collected from Lake Taihu in the fall of 2009. The total mercury (THg), methyl mercury (MeHg), ??¹³C and ??¹⁵N in the samples were measured.

Results and discussion

The signature for ??¹⁵N increased with the trophic levels. Along with a diet composed of fish, the significant relationship between the ??¹³C and ??¹⁵N indicated that a pelagic foraging habitat is the dominant pathway for energy transfer in Lake Taihu. The concentrations of THg and MeHg in the organisms varied dramatically by ??3 orders of magnitude from primary producers (macrophytes and sestons) to piscivorous fish. The highest concentrations of both THg (100 ng g^?1) and MeHg (66 ng g^?1), however, were lower than the guideline of 200 ng g^?1 of MeHg for vulnerable populations that is recommended by the World Health Organization (WHO). The daily intake of THg and MeHg of 92 and 56 ng day^?1 kg^?1 body weight, respectively, was generally lower than the tolerable intake of 230 ng day^?1 kg^?1 body weight for children recommended by the Joint FAO/WHO Expert Committee on Food Additives. Significant relationships between the ??¹⁵N and the logarithm of THg and MeHg showed an obvious biomagnification of Hg along the food web. The logarithmic bioaccumulation factor of MeHg in the fish (up to 5.7) from Lake Taihu, however, was relatively low compared to that of other aquatic ecosystems.

Conclusion

Health risk of exposure to Hg by consumption of fish for local residents is relatively low in the Lake Taihu area. Dilution of Hg levels in the phytoplankton induced by eutrophication is a possible factor inhibiting accumulation of MeHg in fish in eutrophic Lake Taihu.     

Phytotoxicity of silver nanoparticles to Lemna minor L

The use of silver nanoparticles (AgNPs) in commercial products has increased significantly in recent years. Although there has been some attempt to determine the toxic effects of AgNPs, there is little information on aquatic plants which have a vital role in ecosystems. This study reports the use of Lemna minor L. clone St to investigate the phytotoxicity of AgNPs under modified OECD test conditions. AgNPs were synthesised, characterised and subsequently presented to the L. minor. Results showed that inhibition of plant growth was evident after exposure to small (∼20 nm) and larger (∼100 nm) AgNPs at low concentrations (5 μg L⁻¹) and this effect became more acute with a longer exposure time. There was a linear dose-response relationship after 14 d exposure. Using predicted environmental concentrations for wastewaters it was found that AgNPs may pose a significant potential risk to the environment.     

Effect of humic acids on physicochemical property and Cd(II) sorption of multiwalled carbon nanotubes

Zinc pyrithione is used as an antifouling agent. However, the environmental impacts of zinc pyrithione have recently been of concern. Zinc induces diverse actions during oxidative stress; therefore, we examined the effect of zinc pyrithione on rat thymocytes suffering from oxidative stress using appropriate fluorescent probes. The cytotoxicity of zinc pyrithione was not observed when the cells were incubated with 3 μM zinc pyrithione for 3 h. However, zinc pyrithione at nanomolar concentrations (10 nM or more) significantly increased the lethality of cells suffering from oxidative stress induced by 3 mM H₂O₂. The application of zinc pyrithione alone at nanomolar concentrations increased intracellular Zn²⁺ level and the cellular content of superoxide anions, and decreased the cellular content of nonprotein thiols. The simultaneous application of nanomolar zinc pyrithione and micromolar H₂O₂ synergistically increased the intracellular Zn²⁺ level. Therefore, zinc pyrithione at nanomolar concentrations may exert severe cytotoxic action on cells simultaneously exposed to chemicals that induce oxidative stress. If so, zinc pyrithione leaked from antifouling materials into surrounding environments would be a risk factor for aquatic ecosystems. Alternatively, zinc pyrithione under conditions of oxidative stress may become more potent antifouling ingredient.     

Selenium speciation and localization in chironomids from lakes receiving treated metal mine effluent

A lake system in northern Saskatchewan receiving treated metal mine and mill effluent contains elevated levels of selenium (Se). An important step in the trophic transfer of Se is the bioaccumulation of Se by benthic invertebrates, especially primary consumers serving as a food source for higher trophic level organisms. Chironomids, ubiquitous components of many northern aquatic ecosystems, were sampled at lakes downstream of the milling operation and were found to contain Se concentrations ranging from 7 to 80 mg kg⁻¹ dry weight. For comparison, laboratory-reared Chironomus dilutus were exposed to waterborne selenate, selenite, or seleno-DL-methionine under laboratory conditions at the average total Se concentrations found in lakes near the operation. Similarities in Se localization and speciation in laboratory and field chironomids were observed using synchrotron-based X-ray fluorescence (XRF) imaging and X-ray absorption spectroscopy (XAS). Selenium localized primarily in the head capsule, brain, salivary glands and gut lining, with organic Se species modeled as selenocystine and selenomethionine being the most abundant. Similarities between field chironomids and C. dilutus exposed in the laboratory to waterborne selenomethionine suggest that selenomethionine-like species are most readily accumulated, whether from diet or water.     

Partitioning and bioaccumulation of metals from oil sands process affected water in indigenous Parachlorella kessleri

This paper studies the partitioning and bioaccumulation of ten target metals (⁵³Cr, Mn, Co, ⁶⁰Ni, ⁶⁵Cu, ⁶⁶Zn, As, ⁸⁸Sr, ⁹⁵Mo and Ba) from oil sands tailings pond water (TPW) by indigenous Parachlorella kessleri. To determine the role of extracellular and intracellular bioaccumulation in metal removal by P. kessleri, TPW samples taken from two oil sands operators (Syncrude Canada Ltd. and Albian Sands Energy Inc.) were enriched with nutrient supplements.Results indicate that intracellular bioaccumulation played the main role in metal removal from TPW; whereas extracellular bioaccumulation was only observed to some extent for Mn, Co, ⁶⁰Ni, ⁶⁵Cu, ⁸⁸Sr, ⁹⁵Mo and Ba. The FTIR scan and titration of functional groups on the cell surface indicated low metal binding capacity by indigenous P. kessleri. However, it is believed that the dissolved cations and organic ligand content in TPW (such as naphthenic acids) may interfere with metal binding on the cell surface and lower extracellular bioaccumulation. In addition, the total bioaccumulation and bioconcentration factor (BCF) varied during the cultivation period in different growth regimes.     

Atmospheric emissions from the Windscale accident of October 1957

Although it occurred nearly 50 years ago, the nuclear reactor fire of October 1957 at Windscale Works, Sellafield, England, continues to attract interest. Several attempts have been made to quantify the releases of radionuclides and their radiological consequences, but additional information and a re-analysis of meteorological data encourage a further examination of emissions. The limited instrumentation of the reactor provided little relevant information and, as in previous estimates, the discharges are deduced from environmental evidence, but here the recent meteorological analysis is used. The interpretation of the meteorological and environmental evidence requires both timing and quantity of the emitted radionuclides to be considered together.Significant fission product emission continued from about 15:00 or 16:00 on 10 October 1957 until noon the following day. There were two main peaks in discharge rate, during the evening and early hours and from roughly 06:00 until 10:30, and the amounts emitted during each of these periods were probably comparable.Iodine-131 (¹³¹I), caesium-137 (¹³⁷Cs) and polonium-210 (²¹⁰Po) activities dominated the radioactive emissions and there is sufficient environmental evidence for releases of these radionuclides to be estimated within a factor of about two. (Some additional ¹³¹I may have escaped in a chemical form that was not included in the estimate, but it appears likely that the fraction was small.) There is evidence that the plume extended further east than accepted in previous assessments and the estimates of quantities emitted have been increased to allow for this. For other radionuclides the environmental measurements were fewer and the uncertainties are greater.     

Mercury exposure in the freshwater tilapia Oreochromis niloticus

Mercury (Hg) can be strongly accumulated and biomagnified along aquatic food chain, but the exposure pathway remains little studied. In this study, we quantified the uptake and elimination of both inorganic mercury [as Hg(II)] and methylmercury (as MeHg) in an important farmed freshwater fish, the tilapia Oreochromis niloticus, using ²⁰³Hg radiotracer technique. The dissolved uptake rates of both mercury species increased linearly with Hg concentration (tested at ng/L levels), and the uptake rate constant of MeHg was 4 times higher than that of Hg(II). Dissolved uptake of mercury was highly dependent on the water pH and dissolved organic carbon concentration. The dietborne assimilation efficiency of MeHg was 3.7-7.2 times higher than that of Hg(II), while the efflux rate constant of MeHg was 7.1 times lower. The biokinetic modeling results showed that MeHg was the greater contributor to the overall mercury bioaccumulation and dietary exposure was the predominant pathway.