Assessment of atmospheric pollution in the vicinity of a tin and lead industry using lichen species Canoparmelia texana

This paper examines the viability of using Canoparmelia texana lichen species as a bioindicator of air pollution by radionuclides and rare earth elements (REEs) in the vicinity of a tin and lead industry. The lichen and soil samples were analyzed for uranium, thorium and REEs by instrumental neutron activation analysis. The radionuclides ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb were determined either by Gamma-ray spectrometry (GRS) (soils) or by radiochemical separation followed by gross alpha and beta counting using a gas flow proportional counter (lichens). The lichens samples concentrate radionuclides (on the average 25-fold higher than the background for this species) and REEs (on the average 10-fold higher), therefore they can be used as a fingerprint of contamination by the operation of the tin industry.     

Cs,Co and K uptake by lettuce plants in two distributions of soil contamination

¹³⁷Cs and ⁶⁰Co, two of the radionuclides more representative of discharges from nuclear facilities, are of interest for radiological protections because of their great mobility in biosphere and affinity with biological systems. The aim of the present work is the investigation of the possible influence of the vertical distribution of ¹³⁷Cs and ⁶⁰Co in soil upon their uptake by lettuce as function of plant's growth. An experiment ad hoc has been carried out in field conditions. The results show that (i) the transfer of ¹³⁷Cs and ⁶⁰Co from soil to lettuce is independent by their distribution in soil, (ii) the soil–plant transfer factors of ¹³⁷Cs and ⁶⁰Co show a similar trend vs. growth stage, (iii) the ⁴⁰K transfer factor trend is different from those of anthropogenic radionuclides, and (iv) ¹³⁷Cs and ⁶⁰Co specific activities are about 1 Bq/kg, in the mature vegetable with soil activity from 9 to 21 kBq/m².     

Bioavailability of sediment-associated and low-molecular-mass species of radionuclides/trace metals to the mussel Mytilus edulis

Sediments can act as a sink for contaminants in effluents from industrial and nuclear installations or when released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides and trace metals to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The marine mussel Mytilus edulis is a filter-feeding organism that via the gills is subjected to contaminants in dissolved form and from contaminants associated to suspended particles via the digestive system. In this paper the bioavailability of sediment-associated and seawater diluted Cs, Co, Cd and Zn radioactive tracers to the filtering bivalve M. edulis has been examined. The mussels were exposed to tracers diluted in ultrafiltered (<10 kDa) seawater (Low Molecular Mass form) or to tracers associated with sediment particles from the Stepovogo Fjord at Novaya Zemlya in short-term uptake experiments, followed by 1-month depuration experiments in flow-through tanks. A toxicokinetic model was fitted to the uptake and depuration data, and the obtained parameters were used to simulate the significance of the two uptake pathways at different suspended sediment loads and sediment-seawater distribution coefficients. The results of the model simulations, assuming steady state conditions, suggest that resuspended particles from contaminated sediments can be a highly significant pathway for mussels in the order ¹⁰⁹Cd ≌ ⁶⁵Zn < ¹³⁴Cs < ⁶⁰Co. The significance increases with higher suspended sediment load and with higher K_d. Furthermore, the experimental depuration data suggest that Cs is retained longer and Co, Cd and Zn shorter by the mussels when associated with ingested sediments, than if the metals are taken up from the low molecular mass (LMM) phase.     

Fate of Co at a sludge land application site

Vertical distributions of ⁶⁰Co are determined in soil cores obtained from a 10-ha grassland, where anaerobically digested sludge was applied by surface spraying from 1986 to 1995 on the U.S. Department of Energy's Oak Ridge Reservation. These results, along with historical application records, are used to estimate vertical-migration rates and perform a mass balance. The presence of ⁶⁰Co results solely from the sludge-application process. Soil, vegetation, and surface-water samples were collected. Eleven soil cores were sectioned into 3-cm increments and analyzed by gamma-ray spectrometry. No ⁶⁰Co was detected in the vegetation or water samples. The downward migration rate of ⁶⁰Co in the upper 15 cm of soil ranged from 0.50 to 0.73 cm/yr. About 98%, 0.020 ± 0.011 Bq/cm², of ⁶⁰Co remained in the upper 15 cm of soil, which compared favorably with the expected ⁶⁰Co activity based on historical records of 0.019 ± 0.010 Bq/cm².     

Occurrence and behaviour of radionuclides in the Moselle River—Part III: Dispersion of radionuclides along the river course

Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with ⁵⁸Co, ⁶⁰Co and ^110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.     

Uptake and loss of 134Cs and 60Co by the Baltic bivalve Macoma baltica in a laboratory microcosmos

Accumulation and clearance of ¹³⁴Cs and ⁶⁰Co by the Baltic bivalve Macoma baltica were experimentally investigated in a laboratory microcosmos. The nuclides were added to the water and the activities in bivalve flesh, shell, feces and sediment were determined at regular intervals. The uptake was quite rapid, 40% (Cs) and 55% (Co) of the final steady state values being attained after 24 h. The subsequent releases were also rapid, 50% (Cs) and 40% (Co), of the accumulated activity being lost within 6 days. The experiments demonstrated that the major intake route following short-term releases of activity will be from the water column and that the close relationship between activity in water and organism can thus be used for predictive purposes without the complication of radionuclide uptake from contaminated sediments. However, for longer periods, the subsequent intake of sediments will generate a significant exposure pathway for this deposit-feeding bivalve.     

Distributions of radionuclide sorption coefficients (Kd) in sub-surface sediments and the implications for transport calculations

The effect of the spatial variability of K_d on calculations of contaminant travel time in the vadose zone was determined. Depth discrete measurements of K_d were made for a suite of radionuclides (¹⁰⁹Cd, ⁵⁷Co, ⁶⁰Co, ⁸⁵Sr, ¹³⁷Cs, and ⁸⁸Y) utilizing a sediment core from the E-Area at the Savannah River Site. The K_d’s were ordered as ⁸⁵Sr²⁺ < ¹³⁷Cs⁺ < ¹⁰⁹Cd²⁺ < ⁵⁷Co²⁺ = ⁶⁰Co²⁺ << ⁸⁸Y³⁺ and the values generally fell below or near the lowest quartile of values reported in the literature. Correlations were generally weak between soil properties and K_d values. Most importantly, all of the K_d distributions could be reasonably approximated as log-normal. Deterministic and stochastic calculations of contaminant travel time to the water table were made. The deterministic calculations were based on each of three conceptual models of the vadose zone: complete stratification (17 strata, each with a different K_d), two strata (two sections of the vadose zone, each characterized by a single, average K_d), and unstratified (a single zone with an average K_d). Stochastic calculations were based on log-normal fits to the K_d data. The two strata model generally yielded travel times 2× greater than those in the completely stratified model. The unstratified model yielded travel times that were between 3 and 5 times greater than the completely stratified model. The stochastic mean travel times were comparable to those of the two strata model.     

Uptake of dry-deposited radionuclides in Fucus—A field study after the Chernobyl accident

The dry deposition of various radionuclides emanating from the plume from the Chernobyl reactor accident was measured at two locations in southern Sweden at the beginning of May, 1986. Samples of Fucus, taken at or near these locations, were also analysed. No precipitation had fallen during the time between the accident and the time of sampling. The ratios between activity concentrations in Fucus and dry depositions on the water surface have been calculated. For any specific radionuclide, this ratio was found to be the same at the two locations, after differences in salinity and in uptake between F. vesiculosus and F. serratus had been taken into account.     

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.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

Thermal neutron fluence from ultra low-level γ-ray spectrometry of spoons activated during the JCO criticality accident at Tokai-mura in 1999

During the JCO-accident in Tokai-mura in 1999, the surrounding village was irradiated by an uncontrolled neutron flux. At some locations in that village, the thermal neutron flux was determined retrospectively by measurement of the very low activity of ⁵¹Cr and ⁶⁰Co in stainless-steel spoons using γ-ray spectrometry in underground laboratories. Activities determined in the HADES underground facility are presented here, together with calibrations performed using a well-defined thermal neutron flux to directly estimate the fluence of thermal neutrons independent of most assumptions. The results show measurable ⁵¹Cr in three samples and ⁶⁰Co in four samples taken from locations at distances of up to 430 m from the accident location despite the elapse of 4 half-lives of ⁵¹Cr before measurement. Effects of air transport of the samples were considered and shown to be negligible.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Occurrence and behaviour of radionuclides in the Moselle River—Part I: Entry of natural and artificial radionuclides

Various sources contribute to the radioactive contamination of the Moselle River, among which the French NPP Cattenom with four units of 1300 M We represents the most important. Appropriate operational precautions were taken in order to monitor the nuclide transfer on different pathways under normal and accidental conditions and the effectiveness of these measures has been tested using natural (²¹⁴Pb/²¹⁴Bi, ⁷Be, ⁴⁰K) and artificial radionuclides. (³H, ⁵⁸Co, ⁶⁰Co, ¹³¹I, ¹³⁷Cs) as tracers. Measurements of suspended matter have revealed that the inputs of natural nuclides exceed the discharges of the NPP Cattenom. In 1992 the annual loads of ⁷Be and ⁴⁰K in suspended matter at Palzem amounted to 21 and 130 GBq year⁻¹, whereas the emission rates of ⁶⁰Co and ¹³⁷Cs were about 2.6 and 1.0 GBq year⁻¹. The total nuclide load of ¹³⁷Cs at Palzem reached 6.2 GBq year⁻¹, which is about six times the quantity emitted by the NPP Cattenom in the same year. This excess is due to the accident at Chernobyl and to a lesser extent to prior atmospheric weapons tests.     

The transfer of 60Co from feed into vitamin B12 in cow liver,milk and beef

The transfer of the radionuclide ⁶⁰Co from feed to milk, meat and the organs of a cow and its incorporation into vitamin B12 were studied in order to determine the transfer coefficient of ⁶⁰Co into vitamin B12 in cattle. Upper limits of transfer coefficients for ⁶⁰Co organically complexed into vitamin B12 were determined to be 6·0 × 10⁻⁵ days/litre in milk and 3·9 × 10⁻⁵ days/kg in meat, based on values measured after 140 days in bovine liver.     

A study of radium bioaccumulation in freshwater mussels, Velesunio angasi, in the Magela Creek catchment, Northern Territory, Australia

Freshwater mussels, Velesunio angasi, along Magela Creek in Australia’s Northern Territory were examined to study radionuclide activities in mussel flesh and to investigate whether the Ranger Uranium mine is contributing to the radium loads in mussels downstream of the mine. Radium loads in mussels of the same age were highest in Bowerbird Billabong, located 20 km upstream of the mine site. Variations in the ratio of [Ra]:[Ca] in filtered water at the sampling sites accounted for the variations found in mussel radium loads with natural increases in calcium (Ca) in surface waters in a downstream gradient along the Magela Creek catchment gradually reducing radium uptake in mussels. At Mudginberri Billabong, 12 km downstream of the mine, concentration factors for radium have not significantly changed over the past 25 years since the mine commenced operations and this, coupled with a gradual decrease of the ²²⁸Ra/²²⁶Ra activity ratios observed along the catchment, indicates that the ²²⁶Ra accumulated in mussels is of natural rather than mine origin. The ²²⁸Th/²²⁸Ra ratio has been used to model radium uptake and a radium biological half-life in mussels of approximately 13 years has been determined. The long biological half-life and the low Ca concentrations in the water account for the high radium concentration factor of 30,000-60,000 measured in mussels from the Magela Creek catchment.     

Sedimentation of cobalt-60 and caesium-137 released in Träven, a Baltic bay

The amounts of cobalt-60 and caesium-137 bound in the sediment in a bay off the Studsvik research station were determined. Of the cumulative released activity during 22 years, 19% of ⁶⁰Co and 1.8% of ¹³⁷Cs were found in the sediments within an area of 23 km². The rate of input through sedimentation and the loss rate through physical decay were of the same order in 1981 and were close to steady state for ⁶⁰Co while for ¹³⁷Cs they had only reached 30% of that level. The sedimentation coefficients calculated for the bay were 6·5 year⁻¹ for ⁶⁰Co and 0·49 year⁻¹ for ¹³⁷Cs, higher values than many published previously. Cobalt-60 seemed to precipitate close to the outlet and to migrate near the bottom as bed-load.     

Evaluation and assessment of 25 years of environmental radioactivity monitoring data at Tarapur (India) nuclear site

The evaluation and assessment of monitoring data generated over a period of 1983-2007 (25 years) of a nuclear facility is presented. Time trends of particulate radioactivity, correlation between ¹³⁷Cs in discharge canal seawater and station discharged activity and correlation of ¹³⁷Cs, ⁶⁰Co, and ¹³¹I in marine species such as sponge and Nerita (gastropod) and corresponding discharged activity are discussed. The concentration of ¹³⁷Cs and ¹³¹I in seawater versus biota are discussed. A good correlation between ¹³⁷Cs in seawater and ¹³⁷Cs in liquid waste discharged was observed (R² = 0.8, p < 0.001). Similarly, correlation was good for Nerita and discharged concentration of ¹³⁷Cs, ¹³¹I and ⁶⁰Co (R² = 0.55-0.73 and p < 0.001). The measurements over the years indicated that there is no accumulation of radionuclides in either the terrestrial or aquatic environments. The mean ¹³⁷Cs decreased from the pre-operational levels: 7.0-3.6 Bq kg⁻¹ in soil, 0.91-0.016 Bq L⁻¹ in milk and 0.28-0.036 Bq kg⁻¹ in vegetation. Similarly, the mean ⁹⁰Sr in these matrixes decreased from 3.9 to 0.26 Bq kg⁻¹; 0.37-0.011 Bq L⁻¹ and 0.34-0.022 Bq kg⁻¹ respectively. Cesium-137 of about 700 μBq m⁻³ was measured in the air filter disks during 1986 and there was a decrease of three orders of magnitude in concentration over the 25 years. The evaluation of environmental data indicated that the radionuclide concentrations and potential impacts, in terms of effective dose to the members of public, have significantly reduced since 1969.     

Radionuclide transfer to freshwater biota species: review of Russian language studies

Around 130 publications reporting studies on radionuclide transfer to freshwater biota species conducted in the former USSR were reviewed to provide the concentration ratio values. None of these studies were available up to now in the English language reviews or publications. The values derived have been compared with the CR values used for freshwater systems in the International reviews. For some radionuclides reviewed in this paper, the data are in good agreement with the mean CR values presented earlier, however for some of them, in particular, for ²⁴¹Am (bivalve molluscs, gastropods and pelagic fish), ⁶⁰Co (gastropods, benthic fish and insect larvae), ⁹⁰Sr and ¹³⁷Cs (benthic fish and zooplankton), the mean values given here are substantially different from those presented earlier. The data reported in this paper for thirty five radionuclides and eleven groups of freshwater species markedly improve the extent of available data for evaluation of radiation impact on freshwater species.     

Dividivi tannins: an ecological product for water-based drilling fluids

Modified tannins are used as deflocculant additives in the formulation of water-based drilling fluids (WBDF) for drilling operations in any scenario. Due to their high heavy metals content, these additives are toxic and hazardous for any environmental scenario. Deflocculant efficiency of unmodified tannins (UDT) extracted from fruit pods of “dividivi” (Caesalpinia coriaria) as an additive for WBDF was assessed. Raw materials for UDT elaboration come from the rural and sustainable exploitation of natural occurring dividivi trees, growing in dry tropical forests in Anzoátegui state (Orinoco Oil Belt, eastern Venezuela). The tannins extract, in the form of dividivi fruit powder, contains 47.0 % of total tannins (hydrolyzable tannins plus condensed tannins), of which 67.4 % corresponds to hydrolyzable tannins. Dividivi tannins in WBDF showed nine (9) times deflocculant efficiency than heavy metals commercial modified tannins. Moreover, commercial modified tannins do not improve their deflocculant efficiency with increased tannin content. Ecotoxicological studies were carried out for WBDF formulations with UDT, using freshwater microalgae Scenedesmus dimorphus as chronic toxicity bioindicator. Toxicity bioassays performed with these microalgae did not show significant effects on its population growth. The EC₅₀ values resulted in over 100,000 mg L^?1, and these formulations were therefore considered non-toxic. Values of LC₅₀ obtained this time with Poecilia reticulata, as acute toxicity bioindicator are around 100,000 mg L^?1, with no significant effects on population mortality. Thus, WBDF formulated with UDT can be considered non-toxic formulations for populations of this freshwater fish. From the social perspective, the use of UDT in WBDF fosters organized communities economical activities based on the maintenance of a sustainable supply chain for processing fruits in a quantity enough to obtain three thousand seven hundred fifty kilograms (3750 Kg). The UDT so obtained was used as deflocculant in four (4) oil wells producing excellent performance and relevant savings compared with commercial modified tannin.     

Uptake and loss of Cs and Co by the Baltic bivalve Macoma baltica in a laboratory microcosmos

Accumulation and clearance of ¹³⁴Cs and ⁶⁰Co by the Baltic bivalve Macoma baltica were experimentally investigated in a laboratory microcosmos. The nuclides were added to the water and the activities in bivalve flesh, shell, feces and sediment were determined at regular intervals. The uptake was quite rapid, 40% (Cs) and 55% (Co) of the final steady state values being attained after 24 h. The subsequent releases were also rapid, 50% (Cs) and 40% (Co), of the accumulated activity being lost within 6 days. The experiments demonstrated that the major intake route following short-term releases of activity will be from the water column and that the close relationship between activity in water and organism can thus be used for predictive purposes without the complication of radionuclide uptake from contaminated sediments. However, for longer periods, the subsequent intake of sediments will generate a significant exposure pathway for this deposit-feeding bivalve.