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.     

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.     

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.     

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.     

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.     

Estimating sediment and caesium-137 fluxes in the Ribble Estuary through time-series airborne remote sensing

High spatial and temporal resolution airborne imagery were acquired for the Ribble Estuary, North West England in 1997 and 2003, to assess the application of time-series airborne remote sensing to quantify total suspended sediment and radionuclide fluxes during a flood and ebb tide sequence. Concomitant measurements of suspended particulate matter (SPM) and water column turbidity were obtained during the time-series image acquisition for the flood and ebb tide sequence on the 17th July 2003 to verify the assumption of a vertically well mixed estuary and thus justifying the vertical extrapolation of spatially integrated estimate of surface SPM. The ¹³⁷Cs activity concentrations were calculated from a relatively stable relationship between SPM and ¹³⁷Cs for the Ribble Estuary. Total estuary wide budgets of sediment and ¹³⁷Cs were obtained by combining the image-derived estimates of surface SPM and ¹³⁷Cs with estimates of water volume from a two-dimensional hydrodynamic model (VERSE) developed for the Ribble Estuary. These indicate that around 10,000 tonnes of sediment and 2.72 GBq of ¹³⁷Cs were deposited over the tidal sequence monitored in July 2003. This compared favourably with bed height elevation change estimated from field work. An uncertainty analysis on the total sediment and ¹³⁷Cs flux yielded a total budget of the order of 40% on the final estimate. The results represent a novel approach to providing a spatially integrated estimate of the total net sediment and radionuclide flux in an intertidal environment over a flood and ebb tide sequence.     

Correlations between potassium, rubidium and cesium ((133)Cs and (137)Cs) in sporocarps of Suillus variegatus in a Swedish boreal forest

An analysis of sporocarps of ectomycorrhizal fungi Suillus variegatus assessed whether cesium (¹³³Cs and ¹³⁷Cs) uptake was correlated with potassium (K) or rubidium (Rb) uptake. The question was whether intraspecific correlations of Rb, K and ¹³³Cs mass concentrations with ¹³⁷Cs activity concentrations in sporocarps were higher within, rather than among, different fungal species, and if genotypic origin of sporocarps within a population affected uptake and correlation. Sporocarps (n = 51) from a Swedish forest population affected by the fallout after the Chernobyl accident were studied. The concentrations were 31.9 ± 6.79 g kg⁻¹ for K (mean ± SD, dwt), 0.40 ± 0.09 g kg⁻¹ for Rb, 8.7 ± 4.36 mg kg⁻¹ for ¹³³Cs and 63.7 ± 24.2 kBq kg⁻¹ for ¹³⁷Cs. The mass concentrations of ¹³³Cs correlated with ¹³⁷Cs activity concentrations (r = 0.61). There was correlation between both ¹³³Cs concentrations (r = 0.75) and ¹³⁷Cs activity concentrations (r = 0.44) and Rb, but the ¹³⁷Cs/¹³³Cs isotopic ratio negatively correlated with Rb concentration. Concentrations of K and Rb were weakly correlated (r = 0.51). The ¹³³Cs mass concentrations, ¹³⁷Cs activity concentrations and ¹³⁷Cs/¹³³Cs isotopic ratios did not correlate with K concentrations. No differences between, within or, among genotypes in S. variegatus were found. This suggested the relationships between K, Rb, ¹³³Cs and ¹³⁷Cs in sporocarps of S. variegatus is similar to other fungal species.     

Uptake of radionuclides and stable elements from paddy soil to rice: a review

The critical paths for radionuclides and the critical foods in Asian countries differ from those in Western countries because agricultural products and diets are different. Consequently, safety assessments for Asian countries must consider rice as a critical food. As most rice is produced under flooded conditions, the uptake of radionuclides by rice is affected by soil conditions. In this report, we summarize radionuclide and stable element soil-to-plant transfer factors (TFs) for rice. Field observation results for fallout ¹³⁷Cs and stable Cs TFs indicated that while fallout ¹³⁷Cs had higher TF than stable Cs over several decades, the GM (geometric mean) values were similar with the GM of TF value for ¹³⁷Cs being 3.6 × 10⁻³ and that for stable Cs being 2.5 × 10⁻³. Although there are some limitations to the use of TF for stable elements under some circumstances, these values can be used to evaluate long-term transfer of long-lived radionuclides in the environment. The compiled data showed that TF values were higher in brown rice than in white rice because distribution patterns for elements were different in the bran and white parts of rice grains.     

Natural and artificial radioactivity determination of some medicinal plants

Several medicinal plants used in Italy were analysed to determine natural and artificial radioactivity in those parts (leaves, fruits, seeds, roots, peduncles, flowers, barks, berries, thallus) used generally as remedies. The radionuclides were determined by alpha (²³⁸U, ²¹⁰Po) and gamma (²¹⁴Pb-Bi, ²¹⁰Pb, ⁴⁰K and ¹³⁷Cs) spectrometry. ²³⁸U ranged between <0.1 and 7.32 Bq kg_dry⁻¹; ²¹⁰Po between <0.1 and 30.3 Bq kg_dry⁻¹; ²¹⁴Pb-²¹⁴Bi between <0.3 and 16.6 Bq kg_dry⁻¹; ²¹⁰Pb between <3 and 58.3 Bq kg_dry⁻¹; ⁴⁰K between 66.2 and 3582.0 Bq kg_dry⁻¹; ¹³⁷Cs between <0.3 and 10.7 Bq kg_dry⁻¹. The percentage of ²¹⁰Po extraction in infusion and decoction was also determined; the arithmetical mean value of percentage of ²¹⁰Po extraction resulted 20.7 ± 7.5.     

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.     

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.     

Geochronology of anthropogenic radionuclides in Ribeira Bay sediments, Rio de Janeiro, Brazil

Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and ²⁰⁷Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of ²¹⁰Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y⁻¹ in the inner bay to 6.2 mm y⁻¹ close to its entrance.     

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.     

Distribution and ratios of Cs and K in control and K-treated coconut trees at Bikini Island where nuclear test fallout occurred: effects and implications

Coconut trees growing on atolls of the Bikini Islands are on the margin of K deficiency because the concentration of exchangeable K in coral soil is very low, ranging from only 20 to 80 mg kg⁻¹. When provided with additional K, coconut trees absorb large quantities of K and this uptake of K significantly alters the patterns of distribution of ¹³⁷Cs within the plant. Following a single K fertilization event, mean total K in trunks of K-treated trees is 5.6 times greater than in trunks of control trees. In contrast, ¹³⁷Cs concentration in trunks of K-treated and control trees is statistically the same while ¹³⁷Cs is significantly lower in edible fruits of K-treated trees. Within one year after fertilization (one rainy season), K concentration in soil is back to naturally low concentrations. However, the tissue concentrations of K in treated trees stays very high internally in the trees for years while ¹³⁷Cs concentration in treated trees remains very low in all tree compartments except for the trunk. Potassium fertilization did not change soil Cs availability.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides (⁹⁰Sr, ¹³⁷Cs and ^239+240Pu) in seabed sediment in the Japan Sea were collected during the period 1998–2002. Concentration of ⁹⁰Sr, ¹³⁷Cs and ^239+240Pu in seabed sediment was 0.07–1.6 Bq kg⁻¹, 0.4–9.1 Bq kg⁻¹ and 0.002–1.9 Bq kg⁻¹, respectively. In the northern basin of the sea (Japan Basin), ^239+240Pu/¹³⁷Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher ^239+240Pu/¹³⁷Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38°N), both inventories and ^239+240Pu/¹³⁷Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

The partitioning of sellafield-derived radiocaesium in scottish coastal sediments

Sequential leaching of Clyde Sea Area and Loch Etive sediments suggests that partitioning of Sellafield (formerly Windscale)-derived ¹³⁷Cs is related, to a larger than expected extent, to the concentration of sedimentary oxides, organics and, less importantly, carbonates. These components act to prevent ¹³⁷Cs release from clay mineral exchange sites. Leaching of wet sediments appears to provide quite different and presumably more realistic information on nuclide associations relative to that produced by leaching dry ground sediments. The latter ¹³⁷Cs partitioning data appear to overestimate the degree of ¹³⁷Cs fixation in these coastal deposits. Because of the observed partial association of ¹³⁷Cs with nonclay constituents, diagenetic remobilisation of the nuclide is in theory feasible and a preliminary study suggests its occurrence to a minor degree.     

Vertical distribution of radionuclides in soil of a grassland site in Chernobyl exclusion zone

Five soil profiles from a site about 8 km SE of the Chernobyl NPP were investigated for the vertical distribution of radionuclides. The average (137)Cs-inventory at the site is about 2.6 MBq/m(2) (reference date 1 May 1986). Apart from (137)Cs, the following radionuclides have been identified (their activity ratios to (137)Cs in brackets): (134)Cs (0.537), (125)Sb (0.068), (60)Co (0.0022), (154)Eu (0.016), (155)Eu (0.020), (94g)Nb (9.5E-5), (239/240)Pu (0.0088), (238)Pu (0.040), (90)Sr (0.30) and (241)Am (0.011). Apparent vertical migration velocities are between 0.14 and 0.26 cm/a, apparent dispersion coefficients range from 0.02 to 0.13 cm(2)/a. The rankings of the velocities v for different radionuclides are (Sr, Cs, Sb, Co, Pu)< Am < Eu and Sr < (Cs, Nb), for D, the following rankings have been found: (Nb, Sr, Cs) < Am < Eu, Cs相似文献   

Ecological half-life of Cs in mosses and lichens in the Ordu province,Turkey by Cevik and Celik

Twenty-one years after the Chernobyl accident, lichen and moss samples were collected from the Ordu province, which was already chosen for a related study some years ago. It was observed that ¹³⁷Cs activity concentration ranged from 31 to 469 Bq kg⁻¹ in the moss and from 132 to 1508 Bq kg⁻¹ in the lichen samples. The decrease of the activity concentrations in the present measurements (2007) relative to those in 1997 (over a period of 10 y) indicated ecological half-lives between 1.8 and 10.4 y for the moss and between 2.1 and 13.7 y for the lichen samples. It was observed that ¹³⁷Cs was still eminent in the area studied. Moreover, ⁴⁰K activity concentrations and K element concentrations were measured and their relationships were discussed.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

Long-term effects of single potassium fertilization on 137Cs levels in plants and fungi in a boreal forest ecosystem

We examined the long-term effects of a single application of potassium (K) fertilizer (100 kg K ha⁻¹) in 1992 on ¹³⁷Cs uptake in a forest ecosystem in central Sweden. ¹³⁷Cs activity concentrations were determined in three low-growing perennial shrubs, heather (Calluna vulgaris), lingonberry (Vaccinium vitis-idaea) and bilberry (Vaccinium myrtillus), and in four wild fungal species (Cortinarius semisanguineus, Lactarius rufus, Rozites caperata and Suillus variegatus). Uptake of ¹³⁷Cs by plants and fungi growing on K-fertilized plots 17 years after application of the K fertilizer was significantly lower than in corresponding species growing in a non-fertilized control area. The ¹³⁷Cs activity concentration was 21-58% lower in fungal sporocarps and 40-61% lower in plants in the K-fertilized area compared with the control. Over the study period, this decrease in ¹³⁷Cs activity concentration was more consistent in plants than in fungi, although the effect was statistically significant and strongly pronounced in all species. The effect of K fertilization in reducing ¹³⁷Cs activity concentration in fungi and plants decreased over time but was still significant in 2009, 17 years after fertilization. This suggests that application of K fertilizer to forests is an appropriate and effective long-term measure to decrease radiocaesium accumulation in plants and fungi.