Microdistribution of Am in structures of submerged macrophyte Elodea canadensis growing in the Yenisei River

A submerged macrophyte of the Yenisei River, Elodea canadensis, was used to study the microdistribution of the artificial radionuclide ²⁴¹Am among different components of the plant. The total amount of ²⁴¹Am added to the experimental system was 1850 ± 31 Bq/L. The total amount of ²⁴¹Am accumulated by the plants was 182 Bq per sample, or 758,333 ± 385 Bq/kg dry mass. It has been found that the major portion of ²⁴¹Am accumulated by E. canadensis, up to 85%, was bound to solid components of the cells. It is observed that the microdistribution of ²⁴¹Am within different components of the submerged plant E. canadensis was not uniform. ²⁴¹Am distribution vary depending on the age of the leaf blades, the state of the cells and morphological features of the plant stem.     

Characterization of ²⁴¹ Am and ¹³⁴Cs bioaccumulation in the king scallop Pecten maximus: investigation via three exposure pathways

In order to understand the bioaccumulation of ²⁴¹Am and ¹³⁴Cs in scallops living in sediments, the uptake and depuration kinetics of these two elements were investigated in the king scallop Pecten maximus exposed via seawater, food, or sediment under laboratory conditions. Generally, ²⁴¹Am accumulation was higher and its retention was stronger than ¹³⁴Cs. This was especially obvious when considering whole animals exposed through seawater with whole-body concentration factors (CF_7d) of 62 vs. 1, absorption efficiencies (A_0l) of 78 vs. 45 for seawater and biological half-lives (T_b½l) of 892 d vs. 22 d for ²⁴¹Am and ¹³⁴Cs, respectively. In contrast, following a single feeding with radiolabelled phytoplankton, the assimilation efficiency (AE) and T_b½l of ¹³⁴Cs were higher than those of ²⁴¹Am (AE: 28% vs. 20%; T_b½l: 14 d vs. 9 d). Among scallop tissues, the shells always contained the higher proportion of the total body burden of ²⁴¹Am whatever the exposure pathway. In contrast, the whole soft parts presented the major fraction of whole-body burden of ¹³⁴Cs, which was generally associated with muscular tissues. Our results showed that the two radionuclides have contrasting behaviors in scallops, in relation to their physico-chemical properties.     

Accumulation of Am by suspended matter, diatoms and aquatic weeds of the Yenisei River

In this work we experimentally estimated the capacities of the key components of the Yenisei River (Russia): particulate suspended matter (seston), diatom microalgae, and submerged macrophytes for accumulating ²⁴¹Am from water. In our experiments large particles of seston (>8 μm), comparable in size with diatoms, took up most of americium from water. The accumulation of americium by isolated diatom algae (Asterionella formosa and Diatoma vulgare) was lower than by total seston. The concentration factors (CFs) of ²⁴¹Am for seston of the Yenisei River in our experiments were (2.8-6.9)·10⁵; for diatoms - (1.5-4.2)·10⁴. The CFs for aquatic plant Elodea canadensis were within the same order of magnitude as those for diatoms. Activity concentration and CFs of ²⁴¹Am were nearly the same in experiments under dark and light conditions. This is indicative of an energy independent mechanism of americium uptake from the water by diatoms and submerged macrophytes.     

Transport and distribution of artificial gamma-emitting radionuclides in the River Yenisei and its sediment

Discharges from the Krasnoyarsk Mining and Chemical Industrial Complex (KMCIC) near Krasnoyarsk resulted in radioactive contamination of sediments of the River Yenisei. Between 1999 and 2006, 16 sediment cores were collected at different positions 15-1500 km downstream from the discharge point. The concentration of artificial gamma-emitting radionuclides (¹³⁷Cs, ⁶⁰Co, ¹⁵²Eu, and ²⁴¹Am) was determined with the objective to analyze the migration processes leading to the transport of these radionuclides along the river and to their vertical distribution within the sediment. In cores taken in the vicinity of the reactors, the average activity concentration of ¹³⁷Cs, ¹⁵²Eu, and ⁶⁰Co was about 1000 Bq kg⁻¹, and the activity concentration of ²⁴¹Am was about 20 Bq kg⁻¹. Contamination levels of artificial radionuclides were decreasing with increasing distance downstream the KMCIC: The fastest decrease of average activity by a factor of 10 over a distance of 300 km was observed for ²⁴¹Am, whereas for ¹³⁷Cs this decrease occurred over a distance of 1100 km. Sequential extraction experiments revealed that in all depths and at all distances the studied radionuclides were tightly bound to the sediment.To investigate the mechanisms of transport of the ¹³⁷Cs and ⁶⁰Co contamination, mathematical models have been used to describe the contamination in the river water and within the sediments.     

Transfer of 241Am and 237Pu from euphausiid moults to a carbonate-rich marine sediment

Concentrations of ²⁴¹Am and ²³⁷Pu adsorbed onto moulted exoskeletons from the euphausiid Megancytiphanes norvegica decreased exponentially with 50% retention times of 3–7 d when moults were incubated in filtered seawater with small amounts of a carbonate-rich sediment. Over 95% of sediment weight was present as < 43 μm silt particles and 91 ± 4% of radioactivity lost from moults was recovered in this size fraction. Adsorption of both actinides (atoms μm⁻²) was greatest in the medium-fine sand fraction which had the highest carbonate content. These particles constituted <0·4% of total sediment dry weight but their reactivity (atoms μm⁻² surface: atoms μm⁻³ in solution) was 10³–10⁴ times higher than similar quotients for <43 μm particles. The enrichment shows that non-homogeneous distributions may arise between particle types when actinides such as ²⁴¹Am and ²³⁷Pu sorbed to surfaces of organic particles are transferred to sediments.     

Cs,Pu and Am in bottom sediments and surface water of Lake Päijänne,Finland

The concentrations and vertical distribution of ^239,240Pu, ²⁴¹Am and ¹³⁷Cs in the bottom sediments and water samples of Lake Päijänne were investigated. This lake is important, since the Päijänne area received a significant deposition from the Chernobyl fallout. Furthermore Lake Päijänne is the raw water source for the Helsinki metropolitan area. In addition no previous data on the distribution of plutonium and americium in the sediment profiles of Lake Päijänne exist. Only data covering the surface layer (0–1 cm) of the sediments are previously available. In the sediments the average total activities were 45 ± 15 Bq/m² and 20 ± 7 Bq/m² for ^239,240Pu and ²⁴¹Am, respectively. The average ²⁴¹Am/^239,240Pu ratio was 0.45 ± 0.14. The ²⁴¹Am/^239,240Pu ratio is lowest in the surface layer of the sediments and increases as a function of depth. The ²³⁸Pu/^239,240Pu ratio of the sediment samples varied between 0.012 ± 0.025 and 0.162 ± 0.079, decreasing as a function of depth. The average activity in water was 4.9 ± 0.9 mBq/m³ and 4.1 ± 0.2 mBq/m³ for ^239,240Pu and ²⁴¹Am, respectively. The ²⁴¹Am/^239,240Pu ratio of water samples was 0.82 ± 0.17. ^239,240Pu originating from the Chernobyl fallout calculated from the average total activities covers approximately 1.95 ± 0.01% of the total ^239,240Pu activity in the bottom sediments. The average total ¹³⁷Cs activity of sediment profiles was 100 ± 15 kBq/m² and 19.3 ± 1.4 Bq/m³ in water samples.     

A prognostic estimation of the area contaminated with alpha-emitting transuranium isotopes in Belarus following the Chernobyl accident

As a result of the Chernobyl accident, some regions of Belarus have been contaminated with the plutonium isotopes (238,239,240,241)Pu. Considering the importance of the environmental impact of the alpha-emitting radionuclides we have carried out a prognostic estimation of the area contaminated with (238,239,240)Pu and (241)Am (the latter being a decay product of (241)Pu) in Belarus. The calculations were made using measurements of (238,239,240)Pu activity concentrations in soil samples from about 600 settlements in the affected region, together with the estimated activity ratio A((241)Am)/A((238,239,240)Pu). The area contaminated with alpha-emitting transuranium isotopes predicted for the year 2006 has been compared with that estimated for 1986. The results show that by 2006, the area of inhabited districts where contamination with (238,239,240)Pu and (241)Am exceeds the threshold level of 740 Bq/m(2), will be 3.7 times larger, reaching approximately 3.5 x10(3)km(2). Of this, almost 20% will have a contamination level of 1850--3700 Bq/m(2).     

Similarity of 241Am and 59Fe specification in selected freshwaters and of their adsorption on crayfish exoskeleton

The particulate fraction (measured by filtration through 0·45 μm filters) and the organically complexed fraction (measured by gel filtration chromatography) of freshly added ²⁴¹Am and ⁵⁹Fe were determined in 21 prefiltered surface waters. The adsorptive behaviour of both radionuclides on a biological surface (isolated carapace segments of crayfish) was tested simultaneously. A striking similarity was observed in the chemical and adsorptive behaviours of both radionuclides. The stoichiometry of particulate formation revealed a 3/4, Am to Fe ratio. This same stoichiometric relationship was observed in organic complexation, while adsorptive behaviour was characterised by a 1/1, Am to Fe ratio. It is concluded that Am predictably follows the chemistry of freshly added Fe at least over a 15 day period. This observation may find interesting application in risk assessment where use can be made of the well-known geochemical cycling of iron to predict the behaviour of man-made Am.     

Particle and solution phase depth distributions of transuranics and 55Fe in the North Pacific

In situ large volume filtration and chemisorption techniques were used to collect samples from the North Pacific for radiochemical analyses of fallout transuranics and ⁵⁵Fe in filterable and filtered phases. The data cover several locations for surface collections and a detailed depth profile north of Hawaii at 30°N. The observed partition of these nuclides between suspended particulate and filtered phases is directly linked to the rates at which they are moved downward through the water column in association with sinking particles. Particulate phases in open ocean surface waters contain higher Pu (12–35%) than subsurface particulates (which average about 6%). ²⁴¹Am was found to exhibit much stronger particle association—typically close to 50% in both surface and subsurface waters—in accord with its known greater particle reactivity. In the high Pu deep water layer, particle associated Pu dropped to close to 1% of total Pu concentration. Together with a correlated increase in the proportion of oxidized Pu in this layer close to the sediment-water interface, this is taken as clear evidence of remobilization Pu from particles at, or near to, the interface. ⁵⁵Fe distributions on filtered particulates indicate a much deeper depth distribution relative to the transuranics. This may reflect both a higher particle association reactivity in respect to scavenging and a longer exposure history to scavenging (especially relative to ²⁴¹Am—produced by in situ decay).     

Microbial binding of trace metals and radionuclides in sediments: Results from an in situ dialysis technique

The microbial oxidation of Mn and the microbial binding of ²⁴¹Am to a lacustrine sediment were five times greater than the binding effects of abiotic adsorption. In contrast, the microbial enhancement of Cu and ¹³⁷Cs binding were far less pronounced, resulting in only a doubling of the effects of adsorption. The microbial binding of trace metals or radionuclides could not be adequately expressed in terms of adsorption coefficients. Instead, binding rates were determined as a more accurate index of short-term processes at work in the sediment.     

Polonium-210 in mussels and its implications for environmental alpha-autoradiography

Alpha-autoradiographic and radiochemical studies of the distributions of transuranic nuclides in the tissues and organs of mussels collected from the vicinity of the British Nuclear Fuels plc reprocessing plant at Sellafield, Cumbria, England, appeared to require assessment also of baseline alpha-activities of natural ²¹⁰ Po levels. Results for the latter were found to be in excess of the anthropogenic activities of Pu and Am isotopes. To ensure that the levels of ²¹⁰ Po in Cumbrian mussels were not artificially enhanced by local discharges and in the absence of published data, mussels from remote British and French coastal sites were also analyzed. General similarities in ²¹⁰Po concentrations (111 to 459 Bq kg⁻¹ dry) found in mussels soft parts suggest that the ²¹⁰Po levels in the Ravenglass mussels (279 Bq kg⁻¹) are natural and largely unsupported by ²¹⁰Pb; however these levels are as much as four times greater than the present day ^239+240Pu concentrations in the same samples. As the transuranic nuclide content of Cumbrian mussels produces a major component of the local critical group radiation exposure from the Sellafield discharges, this finding places in some perspective the significance of the baseline natural radionuclide concentrations in generating total exposure of the public. More specifically, these findings severely limit the usefulness of alpha-autoradiographic studies for transuranic nuclides performed on such samples. Because of the recently lower concentrations of alpha-emitting transuranic nuclides (mainly ²³⁸Pu, ^239+240Pu and ²⁴¹Am) in the Ravenglass environment, natural ²¹⁰Po is now a major contributor to alpha-track distributions in autoradiographic studies.     

The distribution of plutonium,Americium and curium isotopes in pond and stream sediments of the Savannah river plant,South Carolina,USA

The concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am and ²⁴⁴Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: ²³⁸Pu, 0·07–386 fCi g⁻¹; ^239,240Pu, 0·37–1410 fCi g⁻¹; ²⁴¹Am, 0·1–4360 fCi g⁻¹; ²⁴⁴Cm, <0·01–392 fCi g⁻¹. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of ²⁴⁰Pu/²³⁹Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.     

Temporal changes of 7Be, 137Cs and 210Pb activity concentrations in surface air at Monaco and their correlation with meteorological parameters

Results of analysis of ⁷Be, ¹³⁷Cs and ²¹⁰Pb on aerosol filters carried out from 1998 to 2010 in Monaco show that a weak correlation between activity concentrations of these radionuclides in the atmosphere and meteorological parameters has been found for ⁷Be and temperature (r = 0.50), ²¹⁰Pb and temperature and humidity (r = 0.43 and 0.41, respectively), and ¹³⁷Cs and precipitation (r = 0.51). The minimum and maximum ⁷Be activity concentrations were observed during 2000 and 2009, corresponding with the maximum and minimum solar activity, respectively. The maximum ¹³⁷Cs activity concentration found in May-June 1998 was due to the accident at Algeciras in Spain. The deposition velocities of ⁷Be, ¹³⁷Cs and ²¹⁰Pb depended on the precipitation rate, and attained maximum values during dry seasons. The investigated radionuclides may be used as atmospheric tracers, especially in long-term periods.     

Adsorption of thorium from aqueous solutions by perlite

The use of expanded perlite for the adsorption of thorium from aqueous solution by batch technique is presented. The effects of particle size, pH of the solution, initial thorium concentration, shaking time, V/m ratio and temperature were determined. It was found that the adsorption capacity increases by the increase in the pH of the suspensions. The rate of thorium adsorption on expanded perlite was observed to be fast in the first hour of the reaction time. Adsorption isotherms were expressed by Langmuir and Freundlich adsorption models and the adsorption experiments conducted at 30 ± 1 °C showed that the adsorption isotherms correlated well with the Langmuir model. From the adsorption data, thermodynamic parameters such as ΔG^o, ΔH^o and ΔS^o were calculated as a function of temperature.     

Americium,plutonium and uranium contamination and speciation in well waters,streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site,Kazakhstan

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that ²⁴¹Am, ^239,240Pu and ²³⁸U concentrations in well waters within the study area are in the range 0.04–87 mBq dm⁻³, 0.7–99 mBq dm⁻³, and 74–213 mBq dm⁻³, respectively, and for ²⁴¹Am and ^239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm⁻³, 0.08 mBq dm⁻³ and 0.32 mBq dm⁻³ for ²⁴¹Am, ^239,240Pu and ²³⁸U, respectively. The ²³⁵U/²³⁸U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.     

Human exposure to environmental pollutants after a tire landfill fire in Spain: Health risks

In May 2016, a fire occurred in one of the largest landfills in Europe (Seseña, Toledo, Spain), where 70,000–90,000 tons of tires had been illegally accumulated for > 15 years. Because of the proximity of population nuclei and the duration of the episode (> 20 days), we conducted a preliminary human health risk assessment study just after the tire fire. Samples of air and soil were collected in 3 areas surrounding the landfill (El Quiñón, at only 500 m, and Seseña Nuevo and Seseña Viejo, both at 4 km), as well as in background sites. In addition, samples of crops (barley, wheat, cabbage and lettuce) were also obtained from local farmers. The concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs) and a number of trace elements (As, Cd, Co, Cr, Cu, Hg, Mn, Ni, Pb, Sb, Sn, Tl, and V) were analyzed in all the samples. The concentrations of all the target pollutants, excepting PAHs, were relatively similar at the different sampling zones, irrespective of the distance to the landfill. In turn, a significant increase of PAHs was noted near the tire landfill, with air levels up to 6-times higher than those found at 4 km (134 vs. 19.5–22.7 ng/m³). Similarly, PAH concentrations in lettuce were relatively higher than those typically found in monitoring programs of food safety. Because of the increase of airborne PAHs, cancer risks due to exposure to environmental pollutants for the population living at El Quiñón, near the landfill, were between 3- and 5-times higher than those estimated for the inhabitants of Seseña. After this preliminary study, further investigations, focused only on PAHs, but more extensive in terms of number of samples, should be conducted to assure that PAHs have been progressively degraded through time.     

Plutonium and americium in arctic waters,the North Sea and Scottish and Irish coastal zones

Plutonium and americium have been measured in surface waters of the Greenland and Barents Seas and in the northern North Sea from 1980 through 1984. Measurements in water and biota, Fucus, Mytilus and Patella, were carried out in North-English and Scottish waters in 1982 and Fucus samples were collected from the Irish coast in 1983. Fallout is found to dominate as a source of ^239+240Pu north of latitude 65°N, while for ²³⁸Pu a substantial fraction originates from European nuclear fuel reprocessing facilities. The ²³⁸Pu/^239+240Pu isotope ratio provides clear evidence of the transport of effluent plutonium from the latter to Spitsbergen waters. Fallout plutonium in Arctic waters has a residence time of the order of several years, while for Pu from Sellafield we estimate mean residence times of 11–15 months in Scottish waters and, tentatively, 1·5-3 y during transport from the North Channel (north of the Irish Sea) to Spitsbergen. ²⁴¹Am found in Arctic waters probably originates from the decay of fallout ²⁴¹Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters.     

An interlaboratory comparison of nanosilver characterisation and hazard identification: Harmonising techniques for high quality data

Within the FP7 EU project NanoValid a consortium of six partners jointly investigated the hazard of silver nanoparticles (AgNPs) paying special attention to methodical aspects that are important for providing high-quality ecotoxicity data. Laboratories were supplied with the same original stock dispersion of AgNPs. All partners applied a harmonised procedure for storage and preparation of toxicity test suspensions. Altogether ten different toxicity assays with a range of environmentally relevant test species from different trophic levels were conducted in parallel to AgNP characterisation in the respective test media. The paper presents a comprehensive dataset of toxicity values and AgNP characteristics like hydrodynamic sizes of AgNP agglomerates and the share (%) of Ag⁺-species (the concentration of Ag⁺-species in relation to the total measured concentration of Ag). The studied AgNP preparation (20.4 ± 6.8 nm primary size, mean total Ag concentration 41.14 mg/L, 46–68% of soluble Ag⁺-species in stock, 123.8 ± 12.2 nm mean z-average value in dH₂O) showed extreme toxicity to crustaceans Daphnia magna, algae Pseudokirchneriella subcapitata and zebrafish Danio rerio embryos (EC50 < 0.01 mg total Ag/L), was very toxic in the in vitro assay with rainbow trout Oncorhynchus mykiss gut cells (EC50: 0.01–1 mg total Ag/L); toxic to bacteria Vibrio fischeri, protozoa Tetrahymena thermophila (EC50: 1–10 mg total Ag/L) and harmful to marine crustaceans Artemia franciscana (EC50: 10–100 mg total Ag/L). Along with AgNPs, also the toxicity of AgNO₃ was analyzed. The toxicity data revealed the same hazard ranking for AgNPs and AgNO₃ (i.e. the EC50 values were in the same order of magnitude) proving the importance of soluble Ag⁺-species analysis for predicting the hazard of AgNPs. The study clearly points to the need for harmonised procedures for the characterisation of NMs. Harmonised procedures should consider: (i) measuring the AgNP properties like hydrodynamic size and metal ions species in each toxicity test medium at a range of concentrations, and (ii) including soluble metal salt control both in toxicity testing as well as in Ag⁺-species measurements. The present study is among the first nanomaterial interlaboratory comparison studies with the aim to improve the hazard identification testing protocols.     

Am-241 remobilization in a calcareous soil under simplified rhizospheric conditions studied by column experiments

The effects of simplified rhizospheric conditions on the leaching of (241)Am from a calcareous soil, freshly contaminated, were investigated in batch and column experiments. Glucose and/or citrate were used as artificial exudate solutions at concentrations ranging from 10(-4) to 10(-2)moldm(-3). Am desorption, expressed in terms of distribution coefficients, varied from K(d)>10(4)dm(3)kg(-1) corresponding to a majority of experimental conditions, to K(d)/=10(-2)moldm(-3). Soil columns revealed successive steady states coupled with transitory episodes, the latter represented up to 90% of the total Am release. (241)Am fractions with different behaviours were thus highlighted in columns whereas batch only accounted for highest Am mobile fractions. The implications of the different processes are discussed in terms of modelling approach and risk assessment.     

Aspects of the uptake of radionuclides by sheep grazing on an estuarine saltmarsh. 2. Radionuclides in sheep tissues

The transfer ¹³⁷Cs, ²³⁸Pu, ^239/240Pu and ²⁴¹Am to sheep which graze a saltmarsh in the Esk estuary, 7 km south of the sellafield reprocessing plant in west Cumbria (UK), has been estimated.The concentrations of gamma-emitting radionuclides and of ²³⁸Pu, ^239/240Pu and ²⁴¹Am were measured in liver, lung, muscle, kidney and bone from saltmarsh ewes and lambs. ¹³⁷Cs concentrations in the soft tissues were similar in liver, lung and muscle but were consistently higher in kidney and much lower in bone. The highest concentration of the transuranics was found in liver.Transfer coefficients and concentration factors were calculated for both ewes and lambs. The concentration of ¹³⁷Cs in the tissues of 5-month old lambs was higher than in those of their mothers. Therefore, a higher transfer coefficient was obtained for lamb muscle (1·8 × 10^?1 d kg^?1) than for ewe muscle (6·4 × 10^?2 d kg^?1). Concentration factors were consistently higher for ¹³⁷Cs than for the transuranics.