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.     

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.     

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.     

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.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

Ecological half-life of 137Cs in plants associated with a contaminated stream

Ecological half-life (Te) is a useful measure for studying the long-term decline of contaminants, such as radionuclides, in natural systems. The current investigation determined levels of radiocesium (137Cs) in two aquatic (Polygonum punctatum, Sagittaria latifolia) and three terrestrial (Alnus serrulata, Myrica cerifera, Salix nigra) plant species from a contaminated stream and floodplain on the U.S. Department of Energy's Savannah River Site. Current 137Cs levels in plants were used in conjunction with historical data to determine Te of 137Cs in each species. Median concentrations of 137Cs were highest in S. latifolia (0.84 Bq g(-1)) and lowest in M. cerifera (0.10 Bq g(-1)). Te's ranged from 4.85 yr in M. cerifera to 8.35 yr in S. nigra, both terrestrial species. Te's for all aquatic (6.30 yr) and all terrestrial (5.87) species combined were very similar. The Te's of the two aquatic primary producers (P. punctatum and S. latifolia) in the Steel Creek ecosystem were somewhat longer than Te values previously reported for some consumers from this ecosystem.     

Detection of tritium sorption on four soil materials

In order to measure groundwater age and design nuclear waste disposal sites, it is important to understand the sorption behavior of tritium on soils. In this study, batch tests were carried out using four soils from China: silty clays from An County and Jiangyou County in Sichuan Province, both of which could be considered candidate sites for Very Low Level Waste disposal; silty sand from Beijing; and loess from Yuci County in Shanxi Province, a typical Chinese loess region. The experimental results indicated that in these soil media, the distribution coefficient of tritium is slightly influenced by adsorption time, water/solid ratio, initial tritium specific activity, pH, and the content of humic and fulvic acids. The average distribution coefficient from all of these influencing factors was about 0.1-0.2 mL/g for the four types of soil samples. This relatively modest sorption of tritium in soils needs to be considered in fate and transport studies of tritium in the environment.     

Variation in transfer factor of radiocaesium in bank voles (Clethrionomys glareolus) in clear cut and mature forest sites after the Chernobyl accident

Bank voles that were collected between 1986 and 2004 at sites in Chernobyl fallout areas of northern Sweden showed higher (137)Cs activity concentrations at the mature forest sites compared to clear cuts. This difference was not attributed to differences in ground deposition between sites but to differences in aggregated transfer rates to voles. Differences in transfer between forest types were evident for all years 1986-2004 but the change occurred at different rates in the two habitats. The apparent transfer factor between bilberry (Vaccinium myrtillus) and voles was positively related and indicated that a biomagnification was about 1.5 from vegetation to these small mammalian herbivores. The aggregated transfer factor to bank voles measured in the forest habitat, although starting at higher levels declined faster with time than clear cut sites and the differences between the forest habitat and the clear cut areas diminished with time. After the Chernobyl accident in 1986 the mean level in bank vole was 514Bq/kg fresh mass (SD=505) that increased to 1485Bq/kg (SD=881) in 1988. The activity concentration declined thereafter. The bank voles collected in similar habitats in 2004 contained on average 1022Bq/kg (SD=723). Still 18 years after the radionuclide fallout over Sweden high activity concentrations in voles could be found.     

Distribution of 137Cs in soil along Ta-han River Valley in Tau-Yuan County in Taiwan

Environmental 137Cs contamination was suspected from accidents at spent fuel storage pits of a research reactor site in the Ta-han River valley in Taiwan. In order to further characterize this contamination, soil samples were collected and measured by a gamma-spectroscopy system in 1999. It was found that 137Cs contamination is distributed up to 4 km from the reactor in an area covered mostly by rice and plant fields. 137Cs concentration in the topsoil ranged up to about 1000 Bq kg-1, as compared with soil beyond the contaminated area, which does not exceed 15 Bq kg-1. Spatial distribution of 137Cs was characterized by strong non-uniformity, which complicated our understanding of the distribution pathway of the radionuclides. The highest concentrations of 137Cs, up to more than 1000 Bq kg-1, were found within a few rice fields. The relative location of these rice fields and the water supplies from local streams suggested that the 137Cs was distributed along water pathways in the valley.     

HTO and OBT activity concentrations in soil at the historical atmospheric HT release site (Chalk River Laboratories)

Tritium is routinely released by the Chalk River Laboratories (CRL) nuclear facilities. Three International HT release experiments have been conducted at the CRL site in the past. The site has not been disturbed since the last historical atmospheric testing in 1994 and presents an opportunity to assess the retention of tritium in soil. This study is devoted to the measurement of HTO and OBT activity concentration profiles in the subsurface 25 cm of soil.In terms of soil HTO, there is no evidence from the past HT release experiments that HTO was retained. The HTO activity concentration in the soil pore water appears similar to concentrations found in background areas in Ontario. In contrast, OBT activity concentrations in soil at the same site were significantly higher than HTO activity concentrations in soil. Elevated OBT appears to reside in the top layer of the soil (0-5 cm). In addition, OBT activity concentrations in the top soil layer did not fluctuate much with season, again, quite in contrast with soil HTO. This result suggests that OBT activity concentrations retained the signature of the historical tritium releases.     

On-site radioactive soil contamination at the Andreeva Bay shore technical base, Northwest Russia

The radioactive waste (RAW) storage site at Andreeva Bay in the Russian Northwest has experienced radioactive contamination both as a result of activities carried out at the site and due to incidents that have occurred there in the past such as accidental releases of radioactive materials. The site is an interesting case study for decommissioning due to the extremely large amounts of radioactivity present at the site and the conditions under which it is stored; very little has been previously published in the scientific literature about this site. This paper complements the paper describing dose rates at Andreeva Bay which is published in this issue of Journal of Environmental Radioactivity by the same authors. This study presents new data related to the activity concentrations of (137)Cs and (90)Sr in surface soils and measurements of alpha- and beta-particle fluxes taken at different areas around the site. Limited data on 60Co is also presented. The results of the study indicate that the main areas of site contamination are associated with the former spent nuclear fuel storage facility at Building 5, due to accidental discharges which began in 1982. Substantial contamination is also observed at the solid radioactive waste storage facilities, probably due to the ingress of water into these facilities. More than 240 samples were measured: maximum contamination levels were 1 x 10(6)Bq/kg (137)Cs (mean value 4.1 x 10(5)Bq/kg) and 4 x 10(6)Bq/kg (90)Sr (mean value 1.2 x1 0(5)Bq/kg). Localised patches of alpha and beta contamination were also observed throughout the site.     

Study of the comparative dynamics of the incorporation of tissue free-water tritium (TFWT) in bulrushes (Typha latifolia) and carp (Cyprinus carpio) in the Almaraz nuclear power plant cooling reservoir

The Almaraz nuclear power plant (Spain) uses the water of Arrocampo reservoir for cooling, and consequently raises the radioactive levels of the aquatic ecosystem of this reservoir. From July 2002 to June 2005, monthly samples of surface water, bulrushes (Typha latifolia) and carp (Cyprinus carpio) were collected from this reservoir. They were analyzed to determine the temporal evolution of the levels of ³H in surface water and of its transfer from the surface water to free-water in the tissues (TFWT) of the aforementioned two organisms. The tritium levels in the surface water oscillate with a biannual period, with their values in the study period ranging between 53 and 433 Bq/L. The incorporation of tritium to bulrushes and carp was fairly similar, the respective mean concentration factors being 0.74 and 0.8 (unitless, as Bq/L tissue water per Bq/L reservoir water). The temporal evolution of the levels fairly closely followed that observed for the surface water tritium, although detailed analysis showed the dominant periodicity for the bulrushes to be annual. This difference reflects the influence on the incorporation of tritium to bulrushes of diverse environmental and metabolic factors, especially evapotranspiration and the seasonal growth of this plant.     

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.     

Radiobiological monitoring of striped field mouse populations in the Moscow recreation forest "Kuzminki"

The results of radiometric and haematological studies of striped field mice (Apodemus agrarius) sampled over the years 1995-2003 from the territory of the preserved radioactive waste burial (RWB), which is located in the Moscow recreation forest "Kuzminki", are presented and discussed in the paper. It was shown that the level of 90Sr-90Y content in mice sampled from the RWB area varies within the range of 0-1200 Bq/kg with an average of 98.7+/-21.5 Bq/kg. The content of 90Sr-90Y in the body of 80% of the mice sampled from the RWB area was below 100 Bq/kg. Only in 4% of the sampled mice, the 90Sr-90Y specific radioactivity was above 300 Bq/kg. Haematological indications of the animals sampled from the RWB area were within the range of normal physiological fluctuations. Nevertheless, a slight but statistically significant increase in the average amount of erythrocytes and the average percentage of banded neutrophils was registered in peripheral blood of the mice.     

He mass spectrometry for very low-level measurement of organic tritium in environmental samples

The design, setup and performance of a mass spectrometric system for the analysis of low to very low-level tritium in environmental samples are described. The tritium concentration is measured indirectly by the ³He ingrowth from radioactive decay after complete initial degassing of the sample. The analytical system is fully computer-controlled and consists in a commercial helium isotope mass spectrometer coupled with a high vacuum inlet system. A detection limit of 0.15 Bq/kg is routinely obtainable for sample sizes of 20 g of water equivalent and an accumulation time of three months. Larger samples (and/or longer accumulation time) can be used to obtain lower detection limits. In addition to the benefit of a lower detection limit, another advantage of this non-destructive method lies in the simplicity of the analytical procedure which strongly limits the risk of contamination. An inter-comparison was successfully performed with the conventional beta counting technique on lyophilized grass samples, in a range of tritium concentrations of environmental interest. It shows that the ³He mass spectrometry method yields results that are fully consistent with the conventional liquid scintillation technique over a wide range of tritium concentrations.     

Radioactive contamination of tropical rainforest soils in Southern Costa Rica

Radionuclide content in soils from four locations in a tropical rainforest near Golfito in Southern Costa Rica was investigated. For comparison, two nearby locations in open grassland were also studied. From each site 5 soil cores down to a depth of 15 cm were taken. The median contamination with 137Cs was 584 Bq m-2 (reference date 1 January 1996) and the coefficient of variation (CV) was 50%. This contamination can be attributed to global fallout from atmospheric nuclear weapon tests between 1945 and 1980. The mean contamination is slightly lower than the value expected for the latitude (8 degrees 42': 700 Bq m-2), which may be explained by migration of radiocaesium to subsoil below 15 cm or by uptake into the living biomass. Out of the total variability of 50%, around 20% can be attributed to the sampling and measuring process uncertainties, thus leaving a 45% contribution of spatial variability. A significant difference between forest and meadow sites could be detected: the meadow sites showed lower radiocaesium soil inventories (median: 291 Bq m-2) than the forest sites (643 Bq m-2). This may be explained by the agricultural activities carried out on meadow sites which lead to an increased redistribution of caesium in the soil profile and therefore a larger fraction of the total 137Cs lying below 15 cm. Another reason for higher contamination levels under forest can be attributed to the high interception potential of dense tree canopies for dry deposition. Extrapolating the 137Cs concentration below the sampling horizon, i.e. accounting for the cut-off of the profiles by the sampling technique, results in an estimated mean of 710 Bq m-2 for the forest sites, which is very close to the expected figure. The mainly mineral part of the forest soil profiles was analysed for the 137Cs transport parameters, apparent convection velocity (v = 0.14 +/- 0.09 cm a-1) and apparent diffusion constant (D = 0.79 +/- 0.49 cm2 a-1). The maximum concentration can be found at 5.3 +/- 2.9 cm depth, the half-value depth being 7.4 +/- 1.3 cm. The mean 40K activity concentration was 175 Bq kg-1 dry matter (CV = 69%) and 226Ra and 228Ra concentrations of 9.90 Bq kg-1 (CV = 23%) and 7.93 Bq kg-1 (CV = 20%) have been found, respectively.     

Potential of largemouth bass as vectors of 137Cs dispersal

We conducted a radio telemetry study on the movements of potentially contaminated largemouth bass between Steel Creek, a restricted access (137)Cs contaminated stream on the Savannah River Site (located in South Carolina, USA), and the publicly accessible Savannah River. Largemouth bass were relatively mobile in lower Steel Creek and the portion of the Savannah River near Steel Creek, and there was considerable movement between these two habitats. Largemouth bass had home ranges of about 500 linear meters of shoreline in the Savannah River but sometimes moved long distances. Such movements occurred primarily during the spawning season, largely upstream, and increased when water levels were changing or elevated. However, approximately 90% of the largemouth bass observations were within 10 km of Steel Creek. The total quantity of (137)Cs transported into the Savannah River by largemouth bass was much less than transported by water and suspended sediments discharged from Steel Creek. We conclude that largemouth bass from the Savannah River Site are unlikely to be responsible for long distance dispersal of substantial radiological contamination in the Savannah River.     

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.     

Spatial variability of fallout-90Sr in soil and vegetation of an alpine pasture

According to the soil-to-plant transfer concept generally used in dose assessment modeling, the plant uptake of a radionuclide should depend linearly on its concentration in the soil. In order to validate this concept for (90)Sr in a semi-natural ecosystem, plant and soil samples were taken at 100 plots of a 100 x 100 m(2) area within an alpine pasture near Berchtesgaden, Germany. At three plots, the vertical distribution of (90)Sr in the soil was determined in addition. A statistically significant correlation between the soil and plant concentration of (90)Sr was not detectable (Spearman correlation coefficient R=-0.116, p>0.05) within the range of the Sr-concentration covered (15-548 Bq kg(-1) dry soil and 17-253 Bq kg(-1) dry plant material). Thus, the prerequisite of the soil-to-plant transfer concept was not fulfilled for (90)Sr at this site. Organic carbon and total nitrogen were also determined in the soil samples. Both elements were highly correlated (R=0.912, p<0.001), their ratio being C/N=10.9+/-0.7. While C was positively correlated with the (90)Sr concentrations in the soil (R=0.342, p<0.001), negative correlations were observed for the plant concentrations (R=-0.286, p<0.01) and the concentration ratios (R=-0.444, p<0.001) of (90)Sr. These results are compared with those recently obtained for (137)Cs by Bunzl et al. (J Environ Radioactiv 48 (2000) 145).     

A dynamic model for assessing radiological consequences of tritium routinely released in rivers. Application to the Loire River

A dynamic model for assessing the transfer of tritium in a food chain was applied to the Loire River, where 14 nuclear power plants situated on five different sites operate. The model considers several potential exposure pathways in the aquatic and terrestrial ecosystems: transfer of tritium through the aquatic food chain (especially fish); use of river water for agricultural purposes (irrigation) and transfer of radionuclides through the terrestrial food chain (vegetables, meat, milk); subsequent internal exposure of humans due to ingestion of contaminated foodstuffs. For biological environmental compartments, the transfer of tritium to organic matter (i.e. OBT) was simulated. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analyses, was proposed. Uncertainty/sensitivity analyses were performed to determine a confidence interval for the mean annual dose to critical groups and to identify the parameters responsible for the uncertainty and subsequent research priorities.