Modelling the spatio-temporal evolution of 3H in the waters of the River Tagus

Measurements of tritium specific activity levels and of temperatures in waters of the Torrejón-Tagus reservoir (Spain) showed that their radioactive characteristics were basically influenced by the radioactive liquid effluent from the Almaraz Nuclear Power Plant. This enters the Torrejón-Tagus reservoir via the Arrocampo cooling reservoir, which exchanges water with the first. We studied the temporal and spatial (in two dimensions) evolution of the mentioned parameters for years 1997 and 1998. The tritium levels were found to be significantly correlated with temperature. Two numerical models were constructed for a quantitative study of the tritium levels along Torrejón reservoir: a 1D model was used for the dispersion of tritium along the whole length of the reservoir, and a 2D depth-averaged model was used for a detailed study of the area where tritium is released into the reservoir. Both models solve the hydrodynamic equations, to obtain the currents induced by the exchanges of water between the reservoirs in the River Tagus and Arrocampo, and the advection/diffusion equation to calculate the dispersion of tritium. In general, the model results were in agreement with the experimental observations.     

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.     

Tritium in surface waters of the Yenisei River basin

This paper reports an investigation of the tritium content in the surface waters of the Yenisei River basin near the Mining and Chemical Combine (MCC). In 2001 the maximum tritium concentration in the Yenisei River did not exceed 4 +/- 1 Bq l(-1), which is consistent with the data of 1998-99. However, it has been found that there are surface waters containing enhanced tritium as compared with the background values for the Yenisei River. For instance, in the Ploskii Stream and the Shumikha River the maximum tritium concentrations amount to 168 and 81 Bq l(-1), respectively. The source of tritium in these surface waters is the last operating reactor at the MCC, which still uses the Yenisei water as coolant. In water and sediment samples of the Bolshaya Tel River (a tributary of the Yenisei River) the tritium content turned out to be at least 10 times higher than the background values for the Yenisei River. The measurements conducted at the RPA RADON (Moscow) revealed not only tritium but also the artificial radionuclide (14)C in the Bolshaya Tel samples. The data obtained suggest that the Bolshaya Tel River receives the major part of tritium from sediments rather than from the water catchment area. This allows the conclusion that there is water exchange between the surface waters and the radioactively contaminated underground horizons of the "Severny" testing site.     

Movement of a tritium plume in shallow groundwater at a legacy low-level radioactive waste disposal site in eastern Australia

Between 1960 and 1968 low-level radioactive waste was buried in a series of shallow trenches near the Lucas Heights facility, south of Sydney, Australia. Groundwater monitoring carried out since the mid 1970s indicates that with the exception of tritium, no radioactivity above typical background levels has been detected outside the immediate vicinity of the trenches. The maximum tritium level detected in groundwater was 390 kBq/L and the median value was 5400 Bq/L, decay corrected to the time of disposal. Since 1968, a plume of tritiated water has migrated from the disposal trenches and extends at least 100 m from the source area. Tritium in rainfall is negligible, however leachate from an adjacent landfill represents a significant additional tritium source. Study data indicate variation in concentration levels and plume distribution in response to wet and dry climatic periods and have been used to determine pathways for tritium migration through the subsurface.     

Simultaneous measurement of (226)Ra and (228)Ra in natural water by liquid scintillation counting

Several types of bottled drinking water originating from three different areas in Egypt are studied through measurement of radium activity, assessment of related annual dose for adults and finally to define the role of water quality on radium levels. The mean levels of (226)Ra activity range from 0.44 to 0.92 Bq/L and the mean levels of (228)Ra from 0.30 to 0.78 Bq/L, with related (226)Ra/(228)Ra ratios ranging from 2.61 to 0.56. Water types originating from the Eastern Nile Delta area are characterized by low (226)Ra levels and relatively high (228)Ra activity, presumably due to the muddy agricultural nature of this area, which is subject to water from several surface resources for irrigation. In general, the mean activity levels for both (226)Ra and (228)Ra are within those in drinking water in several other countries and the annual ingested dose is comparable with the typical range reported by UNSCEAR. Also, the effect of TDS, pH, calcium, bicarbonate, sulphate and chloride ion concentrations on radium levels is studied and discussed.     

Monitoring and assessment of radionuclide discharges from Temelín Nuclear Power Plant into the Vltava River (Czech Republic)

The paper summarizes impacts of the Temelín Nuclear Power Plant (NPP) on the Vltava and Labe River basins. The study is based on the results of long-term monitoring carried out before the plant operation (1989–2000), and subsequently during the plant operation (2001–2005). In the first period, the main objective was to determine background radionuclide levels remaining in the environment after global fallout and due to the Chernobyl accident. A decrease in the concentrations of ⁹⁰Sr, ¹³⁴Cs and ¹³⁷Cs, which was observed before the plant operation, continued also during the subsequent period. Apart from tritium, the results of the observation did not indicate any impacts of the plant on the concentrations of activation and fission products in the hydrosphere. The annual average tritium concentrations in the Vltava River were in agreement with predicted values. The maximum annual average tritium concentration (13.5 Bq L⁻¹) was observed in 2004 downstream from the wastewater discharge in the Vltava River at Solenice. Estimated radiation doses for adults due to intakes of river water as drinking water contaminated by tritium are below 0.1 μSv y⁻¹.     

Radiocarbon behaviour in seawater and the brown algae Fucus serratus in the vicinity of the COGEMA La Hague spent fuel reprocessing plant (Goury)--France

Extensive studies of the radiocarbon (14C) distribution and transfer in the marine environment of the North-Cotentin peninsula and along the English Channel have been carried out. The main aims of these studies have been to estimate the spatial and temporal variation of the 14C concentration in seawater and to calculate 14C concentration factors for some biological species. Such information will be helpful in order to calculate precisely radiation doses to humans. First results obtained in the vicinity of the COGEMA La Hague nuclear plant (Goury) indicate a 14C labelling of the dissolved inorganic carbon (DIC) in seawater (8.0-26.2 Bq.m(-3)) and a tight relationship between the 14C in the liquid releases from the plant and the 14C concentrations in DIC. The particulate organic carbon (POC) is also labelled. The concentration factor calculations for the brown algae (Fucus serratus) sampled from Goury, and also along the English Channel, give 14C values around 3000 Bq.kg(-1) fresh weight / Bq.L(-1).     

Rodents as receptor species at a tritium disposal site

New methods are being employed on the Department of Energy's Savannah River Site to deal with the disposal of tritium, including the irrigation of a hardwood/pine forest with tritiated water from an intercepted contaminant plume to reduce concentrations of tritium outcropping into Fourmile Branch, a tributary of the Savannah River. The use of this system has proven to be an effective means of tritium disposal. To evaluate the impact of this activity on terrestrial biota, rodent species were captured on the tritium disposal site and a control site during two trapping seasons in order to assess tritium exposure resulting from the forest irrigation. Control site mice had background levels of tritium, 0.02 Bq/mL, with disposal site mice having significantly higher tritium concentrations, mean=34.86 Bq/mL. Whole body tritium concentrations of the mice captured at the disposal site were positively correlated with tritium application and negatively correlated with precipitation at the site.     

The distribution of tritium in the terrestrial and aquatic environments of the Creys-Malville nuclear power plant (2002-2005)

The Creys-Malville nuclear plant, located on the left bank of the Rh?ne, was shut down in 1998. The facilities are currently in their initial stage of dismantling. In order to establish a baseline for tritium in the vicinity of the site prior to the main dismantling phase, we carried out a monitoring program between 2002 and 2005 in the main terrestrial and aquatic compartments of the local environment. Tritium levels in the groundwaters and in the Rh?ne waters correspond to the regional tritium concentration in precipitation. The data obtained for the terrestrial environment are also in good agreement with the regional background and do not show any specific signature linked to the nuclear plant. The various aquatic compartments of the Rh?ne (fish, plant, sediment) are significantly enriched in tritium both upstream and downstream of the power plant: although Tissue-Free Water Tritium concentrations are in equilibrium with the river water, the non-exchangeable fraction of organic bound tritium in plants and fishes shows values which outpace the river water background by one to two orders of magnitude, and up to four to five orders of magnitude in the sediments. This tritium anomaly is not related to the nuclear plant, as it is already present at the Swiss border 100km upstream of the site. Although fine particles of tritiated polystyrene entering the composition of the luminous paints used by the clock industry have been suspected on several occasions, the exact nature and the origin of this tritium source remain unknown and require further investigations.     

14C and 210Pb in NE atlantic sediments: Evidence of biological reworking in the context of radioactive waste disposal

Scavenging by the seabed and by sedimentary particles in the deep ocean may have a significant effect on the removal of artificial radionuclides released to the water column as a result of radioactive waste disposal operations. Biological activity in the upper layers of the sediment column will enhance the rate of removal for those particle-reactive radionuclides with a short half-life relative to the turnover time of the upper mixed layer. For longer-lived radionuclides the rate of sediment accumulation will determine the ultimate rate of removal.The rate of sediment accumulation and extent of biological mixing of deep-sea sediment from three areas of the NE Atlantic Ocean have been investigated using ¹⁴C and ²¹⁰Pb data. Treatment of the radiocarbon with a simple box model provided estimates of sedimentation rate (ω), mixed layer depth (L), mixed layer age (T_ML) and the age of material arriving at the surface (T₀), which were broadly similar to previously published values from other ocean basins. Box cores from the Iberia Abyssal Plain, Madeira Abyssal Plain and from the NEA low-level radioactive waste dumpsite yielded sedimentation rates in the range 0.8 to 2.2 cm ky^?1 over the upper 16–25 cm. Continuous particle mixing appears to be taking place to a depth of 4 to 6 cm below the present sediment-water interface. Closely spaced vertical sampling of core 161-2 for ²¹⁰Pb allowed a biodiffusion coefficient (D_B) to be calculated (4 × 10^?9cm²s^?1), treating bioturbations as a diffusive term and sedimentations as an advective term in a simple mathematical model. In general, values of D_B in deep ocean sediments fall within the range 1–10 × 10^?9cm²s^?1, two orders of magnitude lower than nearshore values. From a review of published data it is concluded that biological mixing takes place extensively in the deep ocean; it appears to be fairly constant on a basin-wide scale and amenable to incorporation in mathematical models of radionuclide behaviour in the water column.     

Concentrations of (137)Cs in summer pasture plants that reindeer feed on in the reindeer management area of Finland

Samples of summer pasture plants that reindeer feed on were collected in order to study ¹³⁷Cs concentrations in different plant species and in species nested in certain site types, and to study the regional distribution of ¹³⁷Cs in the Finnish reindeer management area. Plant species were categorized by the site types of mineral soil forest (xeric heath forest and mesic heath forest) and peatland. A third category called ’other plant species’ included plants with various site types, poorly determined species and species with poor statistics. The ¹³⁷Cs concentrations in different site types differed significantly. The mean ¹³⁷Cs concentrations of the whole reindeer management area in the xeric heath forest plant species was 44 ± 27 Bq/kg dw, in the mesic heath forest plant species 75 ± 59 Bq/kg dw and in the peatland plant species 219 ± 150 Bq/kg dw. The peatland species uptake ¹³⁷Cs more efficiently than plant species of mineral soil forests. A particularly efficient collector of ¹³⁷Cs was Trichophorum sp. It is suggested that Trichophorum sp. could be used as an indicator species for reindeer summer fodder plants. The highest concentrations of ¹³⁷Cs were found in Southern Lapland and the lowest in Northern Lapland. Today, the concentrations of ¹³⁷Cs in summer pasture plants that reindeer feed on in Finland are at such a level that there is no need to avoid any plant species. In the case of future nuclear fallout, reindeer grazing in peatlands would increase concentrations of ¹³⁷Cs in reindeer meat.     

Germination and growth effects of hexavalent chromium in Orocol TL (a corrosion inhibitor) on Phaseolus vulgaris

This research was designed to address the potential for germination and growth effects in bush beans (Phaseolus vulgaris L. var. Bush Blue Lake) from hexavalent chromium in Orocol TL, a proprietary chromated, zinc-phosphate compound added to DOE cooling water systems for corrosion inhibition. Studies were conducted at low and high Orocol TL concentrations in the soil by adjusting soil pH and the percent of organic matter. Germination effects were determined for seeds germinated in soils adjusted to differing pH ranges (4–4.5, 5–5.5, and 6.5–7), levels of organic matter (1.8%, 3%, and 5%), and Orocol TL amendments (control of 0, 10, and 500 μg/g chromium). Growth responses (effects) were determined from plants cultured in the same soil treatment combinations as described for the germination study. High levels (500 μg/g) of hexavalent chromium in soil (as Orocol TL) affected germination and growth, while a high level of organic matter significantly reduced chromium toxicity on germination. At lower chromium concentrations there was significant uptake by all plant parts, with a corresponding reduction in biomass of leaves. Consequently, adjustments of soil pH from 4.0 to 7.0 appear to have no significant effect on chromium uptake in plants. Increasing the organic matter level to 5%, while decreasing the toxicity of high chromium levels to germinating seed, did not affect chromium uptake.     

Changes in plankton abundance, biomass, and chemical composition under the influence of the cooling system of the Beloyarsk Nuclear Power Plant

The abundance and biomass of phytoplankton and zooplankton proved to noticeably decrease after the water passed through the cooling system of the Beloyarsk Nuclear Power Plant: the phytoplankton perished by 38% (65 metric tons per day), and the zooplankton, by 55% (6 t/day). In the period between 1985 and 1991, the concentration of⁶⁰Co in the plankton of water intake and discharge canals varied from 120 to 1400 Bq/kg dry weight, and that of¹³⁷Cs, from 150 to 1040 Bq/kg dry weight, which is commensurable with the content of radionuclides in the plants and grounds of the Beloyarsk reservoir. In 1985, it was noted that the plankton passing through the cooling system of the nuclear power plant became enriched with Ca, Fe, Mg, Mn, Co, Cs, Cu, Mo, Ni, Pb, Si, Sn, Ti, V, and W.     

Short- and long-term patterns of ¹³⁷Cs in fish and other aquatic organisms of small forest lakes in southern Finland since the Chernobyl accident

We summarize the patterns of ¹³⁷Cs activity concentrations and transfer into fish and other biota in four small forest lakes in southern Finland during a twenty-year period following the Chernobyl accident in April 1986. The results from summer 1986 showed fastest accumulation of ¹³⁷Cs into planktivorous fishes, i.e. along the shortest food chains. Since 1987, the highest annual mean values of ¹³⁷Cs have been recorded in fish occupying the highest trophic levels, for perch (Perca fluviatilis) 13,600 Bq/kg (ww) and for pike (Esox lucius) 20,700 Bq/kg (ww). At the same time, activity concentrations of ¹³⁷Cs in crustacean zooplankton and Asellus aquaticus have ranged between 1000 and 19,500 Bq/kg (dw). In 2006, 5-28% of the 1987 ¹³⁷Cs activity concentration levels were still present in perch and pike. Since 1989 their ¹³⁷Cs activity concentrations in oligohumic seepage lakes have remained significantly higher than in polyhumic drainage lakes due to the increased transfer of ¹³⁷Cs into fish in the seepage lakes with lower electrolyte concentrations, longer water retention times and lower sedimentation rate.     

Measured and modelled tritium concentrations in freshwater Barnes mussels (Elliptio complanata) exposed to an abrupt increase in ambient tritium levels

To improve understanding of environmental tritium behaviour, the International Atomic Energy Agency (IAEA) included a Tritium and C-14 Working Group (WG) in its EMRAS (Environmental Modelling for Radiation Safety) program. One scenario considered by the WG involved the prediction of time-dependent tritium concentrations in freshwater mussels that were subjected to an abrupt increase in ambient tritium levels. The experimental data used in the scenario were obtained from a study in which freshwater Barnes mussels (Elliptio complanata) were transplanted from an area with background tritium concentrations to a small Canadian Shield lake that contains elevated tritium. The mussels were then sampled over 88 days, and concentrations of free-water tritium (HTO) and organically-bound tritium (OBT) were measured in the soft tissues to follow the build-up of tritium in the mussels over time.The HTO concentration in the mussels reached steady state with the concentration in lake water within one or two hours. Most models predicted a longer time (up to a few days) to equilibrium. All models under-predicted the OBT concentration in the mussels one hour after transplantation, but over-predicted the rate of OBT formation over the next 24 h. Subsequent dynamics were not well modelled, although all participants predicted OBT concentrations that were within a factor of three of the observation at the end of the study period. The concentration at the final time point was over-predicted by all but one of the models. The relatively low observed concentration at this time was likely due to the loss of OBT by mussels during reproduction.     

137Cs and (239+240)Pu levels in the Asia-Pacific regional seas

137Cs and (239+240)Pu data in seawater, sediment and biota from the regional seas of Asia-Pacific extending from 50 degrees N to 60 degrees S latitude and 60 degrees E to 180 degrees E longitude based on the Asia-Pacific Marine Radioactivity Database (ASPAMARD) are presented and discussed. 137Cs levels in surface seawater have been declining to its present median value of about 3 Bq/m3 due mainly to radioactive decay, transport processes, and the absence of new significant inputs. (239+240)Pu levels in surface seawater are much lower, with a median of about 6 mBq/m3. (239+240)Pu appears to be partly scavenged by particles and is therefore more readily transported down the water column. As with seawater, (239+240)Pu concentrations are lower than 137Cs in surface sediment. The median 137Cs concentration in surface sediment is 1.4 Bq/kg dry, while that of (239+240)Pu is only 0.2 Bq/kg dry. The vertical profiles of both 137Cs and (239+240)Pu in the sediment column of coastal areas are different from deep seas which can be attributed to the higher sedimentation rates and additional contribution of run-offs from terrestrial catchment areas in the coastal zone. Comparable data for biota are far less extensive than those for seawater and sediment. The median 137Cs concentration in fish (0.2 Bq/kg wet) is higher than in crustaceans (0.1 Bq/kg wet) or mollusks (0.1 Bq/kg wet). Benchmark values (as of 2001) for 137Cs and (239+240)Pu concentrations in seawater, sediment and biota are established to serve as reference values against which the impact of future anthropogenic inputs can be assessed. ASPAMARD represents one of the most comprehensive compilations of available data on 137Cs and (239+240)Pu in particular, and other anthropogenic as well as natural radionuclides in seawater, sediment and biota from the Asia-Pacific regional seas.     

Radioactivity measurements in moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis) samples collected from Marmara region of Turkey

The present study was conducted to compare the ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U activity concentrations in epigeic moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis). The activity levels in 37 moss and 38 lichen samples collected from the Marmara region of Turkey were measured using a gamma spectrometer equipped with a high purity germanium (HPGe) detector. The activity concentrations of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U in the moss samples were found to be in the range of 0.36-8.13, 17.1-181.1, 1.51-6.17, and 0.87-6.70 Bq kg⁻¹ respectively, while these values were below detection limit (BDL)-4.32, 16.6-240.0, 1.32-6.47, and BDL-3.57 Bq kg⁻¹ respectively in lichen. The average moss/lichen activity ratios of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U were found to be 1.32 ± 0.57, 2.79 ± 1.67, 2.11 ± 0.82, and 2.19 ± 1.02, respectively. Very low ¹³⁷Cs concentrations were observed in moss and lichen samples compared to soil samples collected from the same locations in a previous study. Seasonal variations of the measured radionuclide activities were also examined in the three sampling stations.     

Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate ³He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.     

A simple bubbling system for measuring radon (222Rn) gas concentrations in water samples based on the high solubility of radon in olive oil

Based on the different levels of solubility of radon gas in organic solvents and water, a bubbling system has been developed to transfer radon gas, dissolving naturally in water samples, to an organic solvent, i.e. olive oil, which is known to be a good solvent of radon gas. The system features the application of a fixed volume of bubbling air by introducing a fixed volume of water into a flask mounted above the system, to displace an identical volume of air from an air cylinder. Thus a gravitational flow of water is provided without the need for pumping. Then, the flushing air (radon-enriched air) is directed through a vial containing olive oil, to achieve deposition of the radon gas by another bubbling process. Following this, the vial (containing olive oil) is measured by direct use of gamma ray spectrometry, without the need of any chemical or physical processing of the samples. Using a standard solution of 226Ra/222Rn, a lowest measurable concentration (LMC) of radon in water samples of 9.4 Bq L(-1) has been achieved (below the maximum contaminant level of 11 Bq L(-1)).     

Determination of organically bound tritium background level in biological samples from a wide area in the south-west of France

In this paper, the authors describe a sensitive method for low-level non-exchangeable OBT determination. This methodology combines suitable sample treatment, a combustion apparatus for large-sized samples and low-background liquid scintillation spectrometry, along with precautions that substantially reduce the risks of sample contamination. Great care must be taken in the measurement of non-exchangeable OBT at environmental levels. Many authors have discussed the opportunities for cross-contamination between samples and contamination by exchange with the laboratory atmosphere. The authors also describe an application of the methodology to a large-scale sampling and measurement campaign, aimed at the determination of the environmental non-exchangeable OBT background level in tree leaves and ferns collected on the site and in the vicinity of a research centre located in the south-west of France, not far from Bordeaux. This study constitutes a "zero level" for the non-exchangeable OBT activity, as, to our knowledge, there is no tritium source within or in the surroundings of the sampled area capable of producing non-exchangeable OBT activities above the natural levels. Our analyses showed that non-exchangeable OBT activities in the collected samples were very low, ranging from below the detection limit (ca 0.7 Bq kg(-1) of dry material) to ca 2 Bq kg(-1) of dry material. These values are similar to the natural tritium background measured in water samples. No discrepancies can be shown between fern samples and oak tree leaf samples or between samples collected inside and outside the research site.