Kinetics of dissolution of Chernobyl fuel particles in soil in natural conditions

Kinetic of fuel particles dissolution under natural environmental conditions has been investigated using the data on (90)Sr speciation in soils collected from 1995 to 1997 within the Chernobyl nuclear power plant 50 km zone. The dependency of fuel particles dissolution constants on the soil acidity (pH = 4-7) has been obtained on the basis of large and statistically reliable experimental data. Results show that between 2 and 21% of (90)Sr activity is associated with weathering resistant fuel particles. Therefore, these particles would not influence the radiological situation in the near future. The map of the main agrochemical characteristics and the map of the fuel particles dissolution constants have been created for the 30-km zone territory. According to the prognosis of dynamics of fuel particles dissolution in the investigated zone, a radiological situation along the fuel paths of radioactive fallout in present time reached a stable state. An increasing in absolute contents of (90)Sr mobile forms in neutral soils will be observed in the next 10-20 yr. However, the difference between the maximum level of mobile forms contents and their existing contents will not exceed 20%.     

Soil contamination with 90Sr in the near zone of the Chernobyl accident

Representative large-scale soil sampling on a regular grid of step width about 1 km was carried out for the first time in the near zone of the Chernobyl accident (radius 36 km). An integrated map of terrestrial 90Sr contamination density in the 30 km exclusion zone (scale 1:200,000) has been created from the analysed samples. Maps of the main agrochemical characteristics of the soils, which determine the fuel particle dissolution rates and the contamination of vegetation, were produced. The total contents of 90Sr on the ground surface of the 30 km zone in Ukraine (without the reactor site and the radioactive waste storages) was about 810 TBq (8.1 x 10(+14) Bq) in 1997, which corresponds to 0.4-0.5% of the Chernobyl reactor inventory at the time of the accident. This assessment is 3-4 times lower than previous estimates.     

An analysis of the environmental mobility of radiostrontium from weapons testing and Chernobyl in Finnish river catchments

The mobility of radiostrontium within the Arctic environment and surrounding area has been studied by analysing the mobility of 90Sr in river catchments that are within Finland. The environmental mobility of 90Sr deposited by both nuclear weapons testing and the Chernobyl accident has been investigated in five Finnish river catchments. Different models assessing the time-dependent mobility of 90Sr have been evaluated. No significant differences were found between the mobility of 90Sr from nuclear weapons tests and from the Chernobyl accident. Model parameters obtained by fitting to the measurements of the deposition and runoff rates of the nuclear weapons test fallout gave predictions which were consistent with the mid- and long-term contamination by the Chernobyl fallout. A comparison of 90Sr with 137Cs showed that they had similar mobility on deposition but, as time passed, the relative mobility of 90Sr increased with respect to 137Cs over a period of 5-8 years. Once the relative migration of 90Sr with respect to 137Cs reached equilibrium, its runoff rate was, on average, approximately an order of magnitude greater than 137Cs.     

Fuel particles in the Chernobyl cooling pond: current state and prediction for remediation options

During the coming years, a management and remediation strategy for the Chernobyl cooling pond (CP) will be implemented. Remediation options include a controlled reduction in surface water level of the cooling pond and stabilisation of exposed sediments. In terrestrial soils, fuel particles deposited during the Chernobyl accident have now almost completely disintegrated. However, in the CP sediments the majority of ⁹⁰Sr activity is still in the form of fuel particles. Due to the low dissolved oxygen concentration and high pH, dissolution of fuel particles in the CP sediments is significantly slower than in soils. After the planned cessation of water pumping from the Pripyat River to the Pond, significant areas of sediments will be drained and exposed to the air. This will significantly enhance the dissolution rate and, correspondingly, the mobility and bioavailability of radionuclides will increase with time. The rate of acidification of exposed bottom sediments was predicted on the basis of acidification of similar soils after liming. Using empirical equations relating the fuel particle dissolution rate to soil and sediment pH allowed prediction of fuel particle dissolution and ⁹⁰Sr mobilisation for different remediation scenarios. It is shown that in exposed sediments, fuel particles will be almost completely dissolved in 15–25 years, while in parts of the cooling pond which remain flooded, fuel particle dissolution will take about a century.     

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.     

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.     

The influence of hot particle contamination on Sr and Cs transfers to milk and on time-integrated ingestion doses

Most models for transfers of radionuclides through the food chain typically assume that the radioactivity is initially deposited in chemically available forms. It is known, however, that releases of radionuclides in the form of hot particles may significantly influence their environmental transfers and uptake to the food chain. This study presents models for time changes in ⁹⁰Sr and ¹³⁷Cs in milk which incorporate hot particle contamination using observed rates of hot particle dissolution following the Chernobyl accident. A general equation is presented for the influence of hot particles on overall ingestion doses. As expected from previous work, fallout of hot particles significantly influences time changes in radionuclide activity concentrations in foodstuffs. It is also shown that incorporation of radionuclides in hot particles influences time-integrated ingestion doses. For a situation in which a large proportion (90–100%) of fallout is in slowly dissolving hot particles, time-integrated ingestion doses from ⁹⁰Sr and ¹³⁷Cs are reduced by a factor of approximately two compared to the case where all radioactivity is deposited in bioavailable forms. However, the influence of rapidly dissolving hot particles on time-integrated ingestion doses is relatively minor. Remaining significant uncertainties in dose estimates are discussed.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: "mobile" species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides ((3)H, (14)C, (36)Cl, (99)Tc and (129)I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and (36)Cl showed little evidence of retardation, while the transport of (14)C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially (99)Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of (129)I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some "mobile" radionuclides (especially (99)Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

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).     

Soil-to-plant halogens transfer studies 2. Root uptake of radiochlorine by plants

Long-term field experiments have been carried out in the Chernobyl exclusion zone in order to determine the parameters governing radiochlorine (36Cl) transfer to plants from four types of soil, namely, podzoluvisol, greyzem, and typical and meadow chernozem. Radiochlorine concentration ratios (CR) in radish roots (15+/-10), lettuce leaves (30+/-15), bean pods (15+/-11) and wheat seed (23+/-11) and straw (210+/-110) for fresh weight of plants were obtained. These values correlate well with stable chlorine values for the same plants. One year after injection, 36Cl reached a quasi-equilibrium with stable chlorine in the agricultural soils and its behavior in the soil-plant system mimicked the behavior of stable chlorine (this behavior was determined by soil moisture transport in the investigated soils). In the absence of intensive vertical migration, more than half of 36Cl activity in arable layer of soil passes into the radish, lettuce and the aboveground parts of wheat during a single vegetation period.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

The radiological impact of the Chernobyl debris compared with that from nuclear weapons fallout

Our basic knowledge of the radiological impact of fallout from nuclear accidents is based on the experience gained from the study of nuclear weapons fallout. Radioecologically, the most important radionuclides generated by the Chernobyl accident were ¹³⁷Cs, ¹³⁴Cs, ¹³¹I and, to a lesser degree, ⁹⁰Sr. These nuclides are well known from global fallout, although in different relative amounts to those observed in the Chernobyl debris. Another important difference between the fallout from Chernobyl and that from nuclear weapon tests is that their seasonal and geographical distributions were quite dissimilar. A number of examples show how these differences influenced transfer factors and thus population doses. Special emphasis is paid to the contamination of milk and cereal products.Furthermore, it is shown how the composition of the Chernobyl debris changed with distance from Chernobyl, due to the differences in volatility of the various radionuclides involved. Finally, the paper compares the dose equivalents received from unit releases (1 P Bq ¹³⁷Cs) of global fallout and of Chernobyl accident debris.     

Watershed wash-off of atmospherically deposited radionuclides: a review of normalized entrainment coefficients

Radionuclide wash-off is the transport of activity by flowing water over the soil surface (runoff). To complete existing reviews on long-term removal rates, this paper focuses on short-term wash-off fluxes, quantified in the literature by soil-runoff transfer factors called normalized liquid and solid entrainment coefficients (noted K(l)(*), K(s)(*)). Compiled data concerned essentially (137)Cs and (90)Sr wash-off measured under simulated rainfalls on small experimental plots after Chernobyl fallout in the exclusion zone. K(l)(*) and K(s)(*) values span approximately one order of magnitude. Their validity is limited to a season, and their representativeness is limited by restricted studied situations, notably dominant unsoluble forms in fallout, light soils and intense rainfalls. Formulas based on a simplified representation of the soil-runoff system were proposed to generalize the existing values for other conditions. However, their implementation requires a more systematic compilation of the available information, including decisive influence factors such as the fraction of exchangeable form, distribution coefficient, suspended matter enrichment ratio. Entrainment coefficients K(l)(*) and K(s)(*) were mathematically related to the transfer function approach. The proposed relationships proved their complementarity in terms of time support and captured fluctuations. Both approaches should be used in assessments to estimate average fluxes and their variability.     

Overview of strontium-89,90 deposition measurements in Finland 1963-2005

In Finland the deposition of strontium-89 (⁹⁰Sr) and strontium-90 (⁹⁰Sr) has been monitored since the early 1960s. The measured cumulative ⁹⁰Sr deposition in 1963-2005 is on average 1200 Bq m⁻², of which 150 Bq m⁻² originates from the Chernobyl accident. Adding to this the deposition in 1945-1962 produces a value of 2040 Bq m⁻² for the cumulative deposition in Finland. The nuclear explosion-derived deposition up to 1985 obtained in this study, 1850 Bq m⁻², is in good agreement with the zonal ⁹⁰Sr deposition of 1740 Bq m⁻² in the 60°N-70°N latitude band estimated by UNSCEAR. The regional deposition patterns of ⁸⁹Sr and ⁹⁰Sr following the Chernobyl accident resemble those of the refractory nuclides such as ^239,240Pu and ⁹⁵Zr. The total deposition of Chernobyl-derived ⁹⁰Sr in Finland was about 5.3 × 10¹³ Bq. This activity corresponds to 0.027% of the reactor core inventory and 0.66% of the atmospheric emissions from the accident. The corresponding figures for ⁸⁹Sr are 4.5 × 10¹⁴ Bq, 0.023% and 0.56%, respectively.     

238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague

Forty-four soil samples were taken around the nuclear research centre Rez, near Prague. The mean activity concentrations of 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in uncultivated soil were 0.010, 0.26, 0.12, 2.7 and 23 Bq.kg(-1), respectively. Contents of radionuclides in cultivated soil were lower and in forest soil higher than in uncultivated soil. The mean activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu, 90Sr/239,240Pu and 239,240Pu/137Cs in uncultivated soil were 0.041, 0.47, 10.9 and 0.013, respectively. The mean activity ratios in cultivated and forest soils were close to the values given above. It follows from the results that the source of 239,240Pu, 90Sr and 137Cs in the studied area is deposition from atmospheric nuclear tests, in the case of 137Cs also deposition from Chernobyl accident. The contribution of the research centre effluents was not proved for these radionuclides. Increased activity ratio of 241Am/239,240Pu indicates the presence of 241Am in the soils studied emanating from sources other than nuclear tests. Uniform distribution of the 241Am/239,240Pu activity ratio around the nuclear research centre and the absence of an area with evidently higher activity ratio, including at sites lying in the main wind direction, suggest that the additional activity of 241Am does not originate from the nuclear research centre. The additional source might be the deposition following the Chernobyl accident.     

Uptake and distribution of 137Cs and 90Sr in salix viminalis plants

Agricultural areas in middle and northern parts of Sweden were contaminated with radionuclides after the Chernobyl accident in 1986. Alternative crops in these areas are biomass plantations with fast-growing Salix clones for energy purposes. The uptake and internal distribution of 137Cs and 90Sr in Salix viminalis were studied. Plants were grown in microplots under field conditions. The soils in the experimental site had been contaminated in 1961 with 35.7 and 13.4 MBq m(-2) of 137Cs and 90Sr, respectively. The experiment was carried out during three years. The plots were fertilised with 60 kg N ha(-1) and three treatments of K, consisting of 0, 80 and 240 kg K ha(-1) during the first two years. The activity concentration of 137Cs in the different plant parts varied between 140 and 20,000 Bq kg(-1) and was ranked in the following order: lowest in stems < cuttings < leaves < roots. The fine roots (0-1 mm) had the highest 137Cs activity concentration. One-year-old stems had higher 137Cs activity concentrations than two-year-old stems. The activity concentration of 137Cs in the plants was significantly affected by K-supply and was higher in the 0 kg K treatment than in the 80 or 240kg K treatment. Leaves contained more 90Sr than stems and cuttings.     

Classification of hot particles from the Chernobyl accident and nuclear weapons detonations by non-destructive methods.

Both after the Chernobyl accident and nuclear weapon detonations, agglomerates of radioactive material, so-called hot particles, were released or formed which show a behaviour in the environment quite different from the activity released in gaseous or aerosol form. The differences in their characteristic properties, in the radionuclide composition and the uranium and actinide contents are described in detail for these particles. While nuclear bomb hot particles (both from fission and fusion bombs) incorporate well detectable trace amounts of 60Co and 152Eu, these radionuclides are absent in Chernobyl hot particles. In contrast, Chernobyl hot particles contain 125Sb and 144Ce which are absent in atomic bomb HPs. Obvious differences are also observable between fusion and fission bombs' hot particles (significant differences in 152Eu/l55Eu, 154Eu/155Eu and 238Pu/239Pu ratios) which facilitate the identification of HPs of unknown provensence. The ratio of 239Pu/240Pu in Chernobyl hot particles could be determined by a non-destructive method at 1:1.5. A non-destructive method to determine the content of non-radioactive elements by Kalpha-emission measurements was developed by which inactive Zr, Nb, Fe and Ni could be verified in the particles.     

The effective and environmental half-life of 137Cs at Coral Islands at the former US nuclear test site

The United States (US) conducted nuclear weapons testing from 1946 to 1958 at Bikini and Enewetak Atolls in the northern Marshall Islands. Based on previous detailed dose assessments for Bikini, Enewetak, Rongelap, and Utirik Atolls over a period of 28 years, cesium-137 (137Cs) at Bikini Atoll contributes about 85-89% of the total estimated dose through the terrestrial food chain as a result of uptake of 137Cs by food crops. The estimated integral 30, 50, and 70-year doses were based on the radiological decay of 137Cs (30-year half-life) and other radionuclides. However, there is a continuing inventory of 137Cs and 90Sr in the fresh water portion of the groundwater at all contaminated atolls even though the turnover rate of the fresh groundwater is about 5 years. This is evidence that a portion of the soluble fraction of 137Cs and 90Sr inventory in the soil is lost by transport to groundwater when rainfall is heavy enough to cause recharge of the lens, resulting in loss of 137Cs from the soil column and root zone of the plants. This loss is in addition to that caused by radioactive decay. The effective rate of loss was determined by two methods: (1) indirectly, from time-dependent studies of the 137Cs concentration in leaves of Pisonia grandis, Guettarda specosia, Tournefortia argentea (also called Messerschmidia), Scaevola taccada, and fruit from Pandanus and coconut trees (Cocos nucifera L.), and (2) more directly, by evaluating the 137Cs/90Sr ratios at Bikini Atoll. The mean (and its lower and upper 95% confidence limits) for effective half-life and for environmental-loss half-life (ELH) based on all the trees studied on Rongelap, Bikini, and Enewetak Atolls are 8.5 years (8.0 years, 9.8 years), and 12 years (11 years, 15 years), respectively. The ELH based on the 137Cs/90Sr ratios in soil in 1987 relative to the 137Cs/90Sr ratios at the time of deposition in 1954 is less than 17 years. The magnitude of the decrease below 17 years depends on the ELH for 90Sr that is currently unknown, but some loss of 90Sr does occur along with 137Cs. If the 15-year upper 95% confidence limit on ELH (corresponding to an effective half-life of 9.8 years) is incorporated into dose calculations projected over periods of 30, 50, or 70 years, then corresponding integral doses are 58, 46 and 41%, respectively, of those previously calculated based solely on radiological decay of 137Cs.