Occurrence and behaviour of radionuclides in the Moselle River-Part II: Distribution of radionuclides between aqueous phase and suspended matter

Most of the radionuclides released from nuclear power plants ( NPPs) into rivers are primarily adsorbed onto suspended matter. To describe this nuclide transfer, a model was used which takes the total suspended matter load as solid phase into account. The necessary partition factors of various radionuclides were determined in river water/suspended matter of the Moselle in laboratory investigations. By use of this model, a conservative estimate of the radionuclide concentration of the solid phase could be obtained which proved to be more realistic than the results based on the distribution law.Furthermore, the influence of grain-size on the specific activity of single fractions of a Moselle sediment was demonstrated using ¹³⁷Cs, ¹⁰⁶Ru and ¹⁴⁴Ce from the Chernobyl nuclear accident as tracers. The grain-size pattern is considered to be a main factor which may seriously distort the determination of distribution coefficients and concentration factors that are needed in applying the model based on the distribution law.     

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.     

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.     

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.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

Vertical distribution of anthropogenic radionuclides in cores from contaminated floodplains of the Yenisey River

The Mining and Chemical Industrial Combine, Zheleznogorsk (MCIC, previously known as Krasnoyarsk-26) on the River Yenisey has contaminated the surrounding environment with anthropogenic radionuclides as a result of discharges of radioactive wastes. The purpose of this study was to investigate the vertical distribution of anthropogenic contamination (¹³⁷Cs and plutonium) within floodplain areas at different distances from the discharge point. Sites were chosen that display different characteristics with respect to periodic inundation with river water. Cs-137 activity concentrations were in the range 23–3770 Bq/kg (dry weight, d.w.); Pu-239,240 activity concentrations were in the range <0.01–14.2 Bq/kg (d.w.). Numerous sample cores exhibited sub-surface maxima which may be related to the historical discharges from the MCIC. Possible evidence indicating the deposition of earlier discharges at MCIC in deeper core layers was observed in the ²³⁸Pu:^239,240Pu activity ratio data: a Pu signal discernible from global fallout could be observed in numerous samples. Cs-137 and Pu-239,240 activity concentrations were correlated with the silt fraction (% by mass <63 μm) though no significant correlation was observed between (grain-size) normalised ¹³⁷Cs activity concentrations and distance downstream from the MCIC.     

Doses of external exposure in Jordan house due to gamma-emitting natural radionuclides in building materials

The use of building materials containing naturally occurring radionuclides as ⁴⁰K, ²³²Th, and ²³⁸U and their progeny results in external exposures of the residents of such buildings. In the present study, indoor dose rates for a typical Jordan concrete room are calculated using Monte Carlo method. Uniform chemical composition of the walls, floor and ceiling as well as uniform mass concentrations of the radionuclides in walls, floor and ceiling are assumed.Using activity concentrations of natural radionuclides typical for the Jordan houses and assuming them to be in secular equilibrium with their progeny, the maximum annual effective doses are estimated to be 0.16, 0.12 and 0.22 mSv a⁻¹ for ⁴⁰K, ²³²Th- and ²³⁸U-series, respectively. In a total, the maximum annual effective indoor dose due to external γ-radiation is 0.50 mSv a⁻¹. Additionally, organ dose coefficients are calculated for all organs considered in ICRP Publication 74. Breast, skin and eye lenses have the maximum equivalent dose rate values due to indoor exposures caused by the natural radionuclides, while equivalent dose rates for uterus, colon (LLI) and small intestine are found to be the smallest. More specifically, organ dose rates (nSv a⁻¹ per Bq kg⁻¹) vary from 0.044 to 0.060 for ⁴⁰K, from 0.44 to 0.60 for radionuclides from ²³⁸U-series and from 0.60 to 0.81 for radionuclides from ²³²Th-series.The obtained organ and effective dose conversion coefficients can be conveniently used in practical dose assessment tasks for the rooms of similar geometry and varying activity concentrations and local-specific occupancy factors.     

Modelling the reworking effects of bioturbation on the incorporation of radionuclides into the sediment column: implications for the fate of particle-reactive radionuclides in Irish Sea sediments

A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a ¹³⁷Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 ± 0.9 cm² y⁻¹, is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 ± 0.4 cm y⁻¹. The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured ⁹⁹Tc and ⁶⁰Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the ⁹⁹Tc and ⁶⁰Co cores were in the range 2-14 cm² y⁻¹, which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.     

A complimentary tool in the determination of activity concentrations of naturally occurring radionuclides

The determination of activity concentrations of radionuclides requires a reliable gamma spectrometry system, which also depends on the compulsory attainment of secular equilibrium amongst the progenies of the radionuclide of interest. This is often difficult to attain and hence a helium particle induced x-ray emission technique, not requiring the compulsory attainment of secular equilibrium, was used to determine the actual concentrations of the elemental content of tailings from the high background radiation tin mining area, Jos, Nigeria. The activity concentrations of the radionuclides of ⁴⁰K, ²³²Th and ²³⁸U were also calculated based on their elemental analyses, providing reliable information about the heads of uranium (²³⁸U) and thorium (²³²Th) series on the study area.     

Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.     

Chernobyl radionuclides in shellfish

Radionuclides from the Chernobyl accident arrived at Monaco on 30 April, 1986. A sample of Mytilus galloprovincialis collected six days later showed near-maximum levels of most radionuclides. Monitoring continued for seven months thereafter, peak concentrations being transiently as high as 480 Bq kg⁻¹ (all soft parts, wet weight) for ¹⁰³Ru. Other radionuclides detected included ¹³²Te, ^129mTe, ¹³¹I, ¹⁰⁶Ru, ¹³⁴Cs, ¹³⁷Cs, ^110mAg, ¹⁴⁰Ba, ¹²⁵Sb, ⁹⁵Nb and ¹⁴¹Ce. Biological half-lives for elimination in this environment were generally around 10 days or longer and most elimination curves contained a number of components. Radionuclide contents of the mussels were predicted quite accurately from concentrations observed on air filters collected simultaneously, but were not satisfactorily explained relative to total radionuclide concentrations in the seawater even three days after peak air filter activities. The use of concentration factors from the literature did not improve the latter predictions. This suggests that the radionuclides were absorbed very rapidly from the fallout particles, rather than from radionuclides first solubilised from particles. Patella lusitanica specimens contained activities about 20–50 times higher than those in the mussels.     

Accumulation of anthropogenic radionuclides in cryoconites on Alpine glaciers

Cryoconites are airborne sediments which accumulate on the surface of glaciers. In samples of cryoconites a temperate Austrian glacier high activity concentrations of anthropogenic radionuclides were found, which stem from global and Chernobyl fallouts. Radionuclides identified were ¹³⁷Cs, ¹³⁴Cs, ²³⁸Pu, ^239+240Pu, ⁹⁰Sr, ²⁴¹Am, ⁶⁰Co, ¹⁵⁴Eu, ²⁰⁷Bi, and ¹²⁵Sb.     

Long-term investigation of anthropogenic and naturally occurring radionuclides at reference sites in western Sweden

In case of an accidental release of radioactive substances into the environment, it is important to quickly and reliably estimate the radiation dose received by people in the affected area, and to determine the extent of the contamination. Measurements of the extent of the release and the subsequent contamination can be facilitated if there are predetermined reference sampling sites with known background radiation and inventory of radionuclides. Since 1996, 34 reference sites for soil sampling, field gamma, and intensimeter measurements have been established in western Sweden. Time series data for dose rates and radioisotope inventory have been collected at these sites, allowing for the investigation of changes in these parameters over time. The mass activity densities for the uranium and thorium series elements varied approximately between 10 and 50 Bq/kg and between 10 and 40 Bq/kg, respectively. The mass activity density of ⁴⁰K was approximately in the range 300–800 Bq/kg. The radiation exposure due to ¹³⁷Cs was rather small in this area. The dose rates calculated from in situ measurement data showed that the contribution to the total dose rate was almost entirely due to naturally occurring radionuclides. The measured dose rate was about twice as high as the calculated rate, even after subtracting the contribution from cosmic radiation. This may be explained by the fact that intensimeters generally are calibrated to measure the quantity ambient dose equivalent, which should not underestimate the effective dose.     

Preliminary assessment of current radiation doses to the population of Brodokalmak from contamination of the Techa River

Significant quantities of liquid radioactive waste were discharged to the Techa River in the southern Urals region of Russia in the early years of operation of the Mayak PA plant (1948–1951). A collaborative project is underway under contract to the European Commission to consider the radiological impact of radioactive contamination in the Southern Urals. Part of this project involves the calculation of radiation doses currently received by the population of Brodokalmak on the Techa river. The assessment made use of local data on the habits of the population and measurements of radionuclide activity concentrations in food and water. Exposure pathways included in the assessment were ingestion of foods and external exposure to gamma radiation from radionuclides deposited on the banks of the river. A range of doses was calculated for different age groups, firstly, assuming that the restrictions in place are retained and, secondly, assuming that there are no restrictions. These restrictions include bans on drinking river water, fishing and bathing in the river and the prohibition of use of the river and surrounding flood plains by humans and cattle. With restrictions the highest dose estimated was 0.56 mSv y⁻¹ for the most exposed adults and without restrictions this increased to 3.4 mSv y⁻¹.     

Concentration of radionuclides in hydrosphere affected by Temelín Nuclear Power Plant in Czech Republic

The paper presents results of a long-term field study of the possible impact of Temelín NPP on the Vltava and Elbe Rivers. The study was divided into 2 stages: before and after the operation of the NPP. The main goal of the investigation before the operation (1989–2000) was to determine the background levels of radionuclides resulting from the tests of nuclear weapons and the Chernobyl accident for different components of the environment. The paper discusses also the risk of a river radioactive contamination due to the tritium discharges in wastewater from Temelín NPP. During the operation period of 2001–2006, the results of the monitoring did not detect any impact of Temelín NPP on the concentrations of activation and fission products in the hydrosphere, apart from tritium. The annual average tritium concentrations in the Vltava River correspond with the previously calculated predictions for the conditions of the average and minimum guaranteed flows. The maximum concentration of tritium of 26.6 Bq/l in Vltava River at Prague was observed after dry period in 2003.     

The importance of physico-chemical parameters on the speciation of natural radionuclides in riverine ecosystems

External gamma radiation levels were measured in the catchment areas of the Sharavathi River and the dose rates in air were found to be in the range 26.0-61.0 nGy h⁻¹. Soil and sediment samples of the riverine environment were analysed for natural radionuclides such as ²²⁶Ra, ²³²Th and ⁴⁰K using a NaI(Tl) gamma spectrometer. The activity concentration of ²¹⁰Pb and ²¹⁰Po in soil and sediment samples was determined by radiochemical separation techniques. Evaluation of the activity concentration of radionuclides with grain size revealed an increase in the activity of ²²⁶Ra, ²³²Th and ⁴⁰K towards fine grain size. The activity concentrations for all isotopes in all samples were not significantly correlated with pH. However, the activity of ²¹⁰Po and ²¹⁰Pb in sediment showed a moderate positive correlation with organic matter content and a good correlation with clay content of sediment.     

Natural and anthropogenic radionuclides in airborne particulate samples collected in Barcelona (Spain)

Results for naturally occurring ⁷Be, ²¹⁰Pb, ⁴⁰K, ²¹⁴Bi, ²¹⁴Pb, ²¹²Pb, ²²⁸Ac and ²⁰⁸Tl and anthropogenic ¹³⁷Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The ²¹²Pb and ²⁰⁸Tl, ²¹⁴Bi and ²¹⁴Pb, ⁷Be and ²¹⁰Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The ⁷Be and ²¹⁰Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the ⁷Be, ²¹⁰Pb, ⁴⁰K and ¹³⁷Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.     

Concentrations of long-lived artificial radionuclides in the moss-lichen cover of mountain plant communities

Specific features of⁹⁰Sr and¹³⁷Cs accumulation in individual lichen species and in the moss-lichen cover of plant communities were studied in some mountain ranges of the Polar and Northern Urals. The results showed that the amounts of radionuclides in lichens and mosses of mountain plant communities are at the level characteristic of the moss-lichen cover of flat ecosystems, and their accumulation depends on⁹⁰Sr and¹³⁷Cs input with the global radioactive fallout. The radionuclide contents in lichens and mosses sampled from different mountain rocks, slopes, and elevations fluctuate around this level. The differences depend both on the structural and functional properties of plants and on the climatic and ecological features of their environment.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Deposition of gamma emitters from Chernobyl accident and their transfer in lichen–soil columns

Lichen–soil column samples were taken from several locations in the Southern Finland between 1986 and 2006. Columns were divided into three parts, upper lichen, lower lichen and underlying soil, and their gamma emitting radionuclides, ¹³⁴Cs, ¹³⁷Cs, ¹⁰³Ru, ⁹⁵Zr, ¹⁰⁶Ru, ^110mAg, ¹²⁵Sb and ¹⁴⁴Ce, were measured with gamma spectrometry. Deposition values were calculated as Bq/m² for each sampling site. Distribution of various radionuclides in the three compartments as a function of time was determined. Both effective and ecological half-lives of all radionuclides were calculated for upper lichen, whole lichen and whole lichen–soil column. A linear relation was derived between the physical half-lives and effective half-lives for whole lichen and for whole lichen–soil column. Reindeer meat activity concentrations of various radionuclides and ensuing radiation doses to reindeer-herding people were also estimated for a hypothetical case where a similar high radioactive pollution, as was taken place in the Southern Finland, would have occurred in the reindeer-herding areas in the Finnish Lapland.