Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

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.     

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.     

Transfer of Chernobyl-derived 134Cs, 137Cs, 131I and 103Ru from flowers to honey and pollen

The activity concentrations of ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were determined separately in honey and pollen samples collected from a single bee colony during several months after the deposition of Chernobyl fallout. The source of each honey and pollen sample was determined by pollen analysis. Although the activity concentrations in honey and pollen varied with time, the concentrations of ¹³⁷Cs and ¹³⁴Cs were, in general, higher in pollen than in honey. For ¹⁰³Ru and ¹³¹I, these differences were comparatively small. The mean ¹³¹ I/¹³⁷Cs and ¹⁰³Ru/¹³⁷Cs ratios were about one order of magnitude higher in honey than in pollen. The mean ¹³¹I/¹⁰³Ru ratio was about the same for honey and pollen. This observation, in the light of the corresponding nuclide ratios found in the deposition, suggests that ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and ¹⁰³Ru were taken up by the plant leaves and transported to nectar and pollen. The higher activity concentrations of ¹³⁷Cs and ¹³⁴Cs in pollen, relative to honey, indicate that these radionuclides behave analogously to potassium, which is also found in higher quantities in pollen.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.     

Accumulation of radionuclides from radioactive substrata by some micromycetes

Overgrowing (interaction) and dissolution of intact and milled hot particles by various micromycetes were studied under laboratory conditions. Hot particles used for the investigation originated from the Chernobyl accident release and atomic bomb testing sites. The micromycetes investigated were mitosporic fungi mainly isolated from the Chernobyl site and vicinity. Most of the fungal species and strains showed a tendency to grow towards the hot particle, overgrow it and dissolve it after prolonged contact. The accumulation (absorption and adsorption) of radionuclides from intact hot particles was generally more intensive for (152)Eu than for (137)Cs by a factor of about 2.6-134, while in experiments with milled samples the (152)Eu and (137)Cs accumulation was similar, except for some fungal species, which showed higher (152)Eu than (137)Cs sorption. It could be shown that the main factors influencing Cs and Eu accumulation in fungi are: fungal species and strains and the size and composition of the hot particle.     

Preliminary evaluation of (135)Cs/(137)Cs as a forensic tool for identifying source of radioactive contamination

Ratios of the fission products (135)Cs and (137)Cs were determined in soil and sediment samples contaminated from three different sources, to assess the use of (135)Cs/(137)Cs as an indicator of source of radioactive contamination. Soil samples from the Chernobyl exclusion zone were found to have to be heavily depleted in (135)Cs ((135)Cs/(137)Cs approximately 0.45), indicative of a high thermal neutron flux at the source. Sludge samples from a nuclear waste treatment pond were found to have a (135)Cs/(137)Cs ratio of approximately 1, whereas sediment collected downstream from a nuclear reactor was highly variable in both (137)Cs activity and (135)Cs/(137)Cs ratio. Comparison of these preliminary results of variability in radiocaesium isotope ratios with reports of Pu isotope ratios suggests (135)Cs/(137)Cs similarly varies with fuel and reactor conditions, and may be used to corroborate other methods of characterizing radioactive contamination.     

A comparison of 90Sr and 137Cs uptake in plants via three pathways at two Chernobyl-contaminated sites

Foliar absorption of resuspended 90Sr, root uptake and contamination adhering to leaf surfaces (i.e. soil loading) were compared at two Chernobyl-contaminated sites, Chistogalovka and Polesskoye. Although foliar absorption of resuspended 90Sr was quantifiable, its contribution amounted to less than 10% of the plants' total, above-ground contamination. Root uptake was 200 times greater than foliar absorption at the near-field site of Chistogalovka and eight times greater at Polesskoye, where the fallout consisted of the more soluble condensation-type, rather than fuel particles. Strontium's bioavailability exceeded that of 137Cs (analyzed in the same plants) by orders of magnitude when compared using concentration ratios. Simplistic, cumulative effective dose calculations for humans ingesting 90Sr- and 137Cs-contaminated plants revealed that the dose at Chistogalovka was greater from 90Sr (185 mSv vs. 3 mSv from 137Cs), while at Polesskoye the dose from 137Cs (66 mSv) was 30 times greater than from 90Sr (2 mSv).     

Fixation of Cs to marine sediments estimated by a stochastic modelling approach

Dumping of nuclear waste in the Kara Sea represents a potential source of radioactive contamination to the Arctic Seas in the future. The mobility of 137Cs ions leached from the waste will depend on the interactions with sediment particles. Whether sediments will act as a continuous permanent sink for released 137Cs, or contaminated sediments will serve as a diffuse source of 137Cs in the future, depends on the interaction kinetics and binding mechanisms involved. The main purpose of this paper is to study the performance of different stochastic models using kinetic information to estimate the time needed for Cs ions to become irreversibly fixed within the sediments. The kinetic information was obtained from 134Cs tracer sorption and desorption (sequential extractions) experiments, conducted over time, using sediments from the Stepovogo Fjord waste dumping site, on the east coast of Novaya Zemlya. Results show that 134Cs ions interact rapidly with the surfaces of the Stepovogo sediment, with an estimated distribution coefficient Kd(eq) of 300 ml/g (or 13m2/g), and the 134Cs ions are increasingly irreversibly fixed to the sediment over time. For the first time, stochastic theory has been utilised for sediment-seawater systems to estimate the mean residence times (MRTs) of Cs ions in operationally defined sediment phases described by compartment models. In the present work, two different stochastic models (i) a Markov process model (MP) being analogous to deterministic compartment models, and (ii) a semi-Markov process model (SMP) which should be physically more relevant for inhomogeneous systems, have been compared. As similar results were obtained using the two models, the less complicated MP model was utilised to predict the time needed for an average Cs ion to become irreversibly fixed in the Stepovogo sediments. According the model, approximately 1100 days of contact time between Cs ions and sediments is needed before 50% of the 134Cs ion becomes fixed in the irreversible sediment phase. while about 12.5 years are needed before 99.7% of the Cs ions are fixed. Thus, according to the model estimates the contact time between 137Cs ions leached from dumped waste and the Stepovogo Fjord sediment should be about 3 years before the sediment will act as an efficient permanent sink. Until then a significant fraction of 137Cs should be considered mobile. The stochastic modelling approach provides useful tools when assessing sediment-seawater interactions over time, and should be easily applicable to all sediment-seawater systems including a sink term.     

Determination of low (137)Cs concentration in seawater using ammonium 12-molybdophosphate adsorption and chemical separation method

A new method has been developed for analyzing (137)Cs in a small volume of seawater. Ammonium 12-molybdophosphate (AMP) was used two times during pretreatment procedure. The first step was to adsorb (137)Cs in seawater samples into AMP in order to reduce sample volume, and the second was to remove (87)Rb, interference nuclide for beta counting. The AMP adsorbing (137)Cs was dissolved by sodium hydroxide solution, and then (137)Cs was finally formed to be cesium chloroplatinate precipitate by adding 10% hexachloroplatinic acid. The beta rays emitted from (137)Cs were measured with a low background gas-proportional alpha/beta counter. This method was applied to several seawater samples taken in the East Sea of Korea. Compared to the routinely used gamma-spectrometry method, this new AMP method was reliable and suitable for analyzing (137)Cs in deep seawater.     

Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples

In November 2000, surface and core soil samples were collected from different regions of Jordan. The samples were analyzed by direct gamma spectrometry and combined radiochemical separation procedure to quantify (40)K, (134)Cs, (137)Cs, (90)Sr, (241)Am, (238)Pu and (239+240)Pu radioactivity. Concentrations (Bq.kg(-1) dry weight) have been observed to vary in the range 1.5-2.6 for (134)Cs, 2.8-11.4 for (90)Sr, and 0.13-0.48 for (241)Am, 0.016-0.062 for (238)Pu, 0.28-1.01 for (239+240)Pu and 155-543 for (40)K. The typical concentration of (137)Cs found in topsoils (0-2 cm) ranged in 7.5-576 Bq.kg(-1), dry weight. These values were greater than those observed in samples taken at greater depths (up to 32 cm). Activity ratios of (134)Cs/(137)Cs, (90)Sr/(137)Cs, (239+240)Pu/(137)Cs, (238)Pu/(137)Cs, (241)Am/(137)Cs, (239+240)Pu/(238)Pu and (241)Am /(238)Pu have mean values of 0.0049 (R=1), 0.29 (R=0.76), 0.41 (R=0.90), 0.39 (R=0.85), 0.41 (R=0.88), 7.72 (R=0.97) and 16.66 (R=0.98), respectively. The underlying concentrations were correlated and relatively higher than those reported in neighboring countries. One moss sample, as a biomonitor indicator, was measured and evaluated along with the soil samples. Its data showed higher concentrations of all measured radionuclides due to accumulations over years. The depth distribution of the fission product (137)Cs and the total deposition (Bq.m(-2)) were also studied in selected samples. Estimations of the annual effective dose equivalent due to (137)Cs-soil contamination showed values up to more than 200 microSv.     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Changes in 137Cs concentrations in soil and vegetation on the floodplain of the Savannah River over a 30 year period

(137)Cs released during 1954-1974 from nuclear production reactors on the Savannah River Site, a US Department of Energy nuclear materials production site in South Carolina, contaminated a portion of the Savannah River floodplain known as Creek Plantation. (137)Cs activity concentrations have been measured in Creek Plantation since 1974 making it possible to calculate effective half-lives for (137)Cs in soil and vegetation and assess the spatial distribution of contaminants on the floodplain. Activity concentrations in soil and vegetation were higher near the center of the floodplain than near the edges as a result of frequent inundation coupled with the presence of low areas that trapped contaminated sediments. (137)Cs activity was highest near the soil surface, but depth related differences diminished with time as a likely result of downward diffusion or leaching. Activity concentrations in vegetation were significantly related to concentrations in soil. The plant to soil concentration ratio (dry weight) averaged 0.49 and exhibited a slight but significant tendency to decrease with time. The effective half-lives for (137)Cs in shallow (0-7.6 cm) soil and in vegetation were 14.9 (95% CI=12.5-17.3) years and 11.6 (95% CI=9.1-14.1) years, respectively, and rates of (137)Cs removal from shallow soil and vegetation did not differ significantly among sampling locations. Potential health risks on the Creek Plantation floodplain have declined more rapidly than expected on the basis of radioactive decay alone because of the relatively short effective half-life of (137)Cs.     

Evidence of the radioactive fallout in the center of Asia (Russia) following the Fukushima Nuclear Accident

It was recently reported that radioactive fallout due to the Fukushima Nuclear Accident was detected in environmental samples collected in the USA and Greece, which are very far away from Japan. In April-May 2011, fallout radionuclides (¹³⁴Cs, ¹³⁷Cs, ¹³¹I) released in the Fukushima Nuclear Accident were detected in environmental samples at the city of Krasnoyarsk (Russia), situated in the center of Asia. Similar maximum levels of ¹³¹I and ¹³⁷Cs/¹³⁴Cs and ¹³¹I/¹³⁷Cs ratios in water samples collected in Russia and Greece suggest the high-velocity movement of the radioactive contamination from the Fukushima Nuclear Accident and the global effects of this accident, similar to those caused by the Chernobyl accident.     

Distribution of pre- and post-Chernobyl radiocaesium with particle size fractions of soils

The association of radiocaesium with particle size fractions separated by sieving and settling from soils sampled eight years after the Chernobyl accident has been determined. The three size fractions were: <2 microm, 2-63 microm and >63 microm. 137Cs in the soil samples was associated essentially with the finer size fractions, which generally showed specific activities 3-5 times higher than the bulk samples. Activity ratios of 134Cs/137Cs in the clay-sized fractions appear to be lower with respect to the corresponding values in bulk soil samples. This result indicates that some differences still exists in the particle size distribution between 137Cs originating from nuclear weapons, which has been in the soil for decades after fallout, and 137Cs coming from the Chernobyl accident, eight years after the deposition event. This behaviour could be related to "ageing" processes of radiocaesium in soils.     

Long-term investigations of radiocaesium activity concentrations in carp in North Croatia after the Chernobyl accident

Long-term investigations of radiocaesium activity concentrations in carp in the Republic of Croatia are presented. The radiocaesium levels in carp decreased exponentially and the effective ecological half-life of (137)Cs was estimated to be about 1 year during 1987-2002 and 5 years during 1993-2005. The observed (134)Cs:(137)Cs activity ratio in carp was found to be similar to the ratio observed in other environmental samples. The concentration factor for carp (wet weight) was estimated to be 128+/-74 Lkg(-1), which is in reasonable agreement with model prediction based on K(+) concentrations in water. Estimated annual effective dose received by adult members of the Croatian population due to consumption of carp contaminated with (134)Cs and (137)Cs are small: per capita dose from this source during 1987-2005 was estimated to be 0.5+/-0.2 microSv. Due to minor freshwater fish consumption in Croatia and low radiocaesium activity concentrations in carp, it can be concluded that carp consumption was not a critical pathway for the transfer of radiocaesium from fallout to humans after the Chernobyl accident.     

Resuspension of coarse fuel hot particles in the Chernobyl area

Measurements of resuspended aerosol in the Chernobyl 30-km exclusion zone have shown coarse fuel hot particles in the activity range 1-12 Bq 137Cs per particle. The particles were sampled with newly designed rotating arm impactors which simultaneously collect during the same experiment three samples with fuel particles in the size ranges larger than 3 microns, larger than 6 microns and larger than 9 microns in geometric diameter. The radionuclide ratios, determined after gamma-spectrometry, were in good agreement with the theoretical calculations for the radionuclide-composition of the Chernobyl Nuclear Power Plant at the moment of the accident and the measured hot particles in soil in the early years after the accident. The number concentrations of airborne hot particles were derived from digital autoradiography. For wind resuspension, maximal concentrations of 2.6 coarse hot particles per 1000 m3 and during agricultural activities 36 coarse hot particles per 1000 m3 were measured. The geometric diameter of single hot particles was estimated to be between 6 and 12 microns.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

137Cs and 40K in the terrestrial vegetation of the Yenisey Estuary: landscape, soil and plant relationships

Plant species, forming important components of Arctic food chains and of interest from a monitoring perspective, were studied at 36 plots representing flood plain and terrace landscapes of the Yenisey River and Estuary from its upper delta to the gulf. (137)Cs contamination densities at the plots varied from 0.35kBq/m(2) (central delta, sandy riverside plot) to 88kBq/m(2) (the upper delta plot) indicating both global and regional sources of anthropogenic pollution. Cs-137 levels in plants were within the range expected from global fallout inputs and varied from 31 to 140Bq/kg d.w. increasing in dominant groups in the order: grasses相似文献   

Deposition of 137Cs in Rokkasho, Japan and its relation to Asian dust

Biweekly atmospheric depositions of (137)Cs were measured in Rokkasho, Aomori, Japan from March 2000 to March 2006 to study recent (137)Cs deposition. Although the deposition level was generally lower than the detectable limit, deposition samples collected in spring occasionally had measurable levels of (137)Cs. The annual (137)Cs deposition from 2001 to 2005 was 0.04-0.69 Bq m(-2) with a mean value of 0.27 Bq m(-2). Depositions of insoluble Al, Fe and Ti were strongly correlated with the (137)Cs deposition, suggesting that suspension of soil particles was the main source of the recent (137)Cs deposition. Asian dust events were coincident with some of the significant (137)Cs depositions in spring. It was found that the ratios of (137)Cs/Al and Fe/Al could be used as indices for discriminating Asian dust from suspension of the local surface soil. Backward trajectory analysis suggested southern Mongolian and northeastern China regions as sources of the significant (137)Cs depositions.