Plutonium contamination from accidental release or simply fallout: study of soils at Palomares (Spain)

The activity concentration of plutonium in an environmental sample does not usually constitute sufficient information to determine if it is due only to fallout. Alpha and gamma spectrometry are used here conjointly in the study of environmental soil samples to distinguish between samples showing plutonium contamination due to fallout exclusively, and samples contaminated with plutonium from another source. The method was applied to soil samples collected in Palomares (Spain), where an accidental release of aerosols contaminated with plutonium occurred. The two contributions (fallout and accidentally released plutonium) were separated by means of the activity ratios between various radionuclides present in the samples analyzed. The fallout level was estimated from the 239 + 240Pu/137Cs activity ratio. For samples showing contamination due to the accident, the 238Pu/239 + 240Pu and 239Pu/240Pu activity ratios were also calculated to determine the grade of plutonium of this contamination.     

Speciation of radionuclides - analytical challenges within environmental impact and risk assessments

The mobility, biological uptake and accumulation of radionuclides are essentially dependent on the physico-chemical form of the nuclides. As a major fraction of refractory radionuclides released during historical nuclear events is associated with particles, a key analytical challenge within environmental impact and risk assessments is to characterise radioactive particles with respect to properties influencing particle weathering, remobilisation and the subsequent ecosystem transfer of associated radionuclides. Preanalysis techniques are needed to fractionate, identify and localize individual particles in contaminated samples. To obtain information on particle characteristics such as particle size distributions, structures, elemental and radionuclide particle composition as well as oxidation state of matrix elements, solid-state speciation techniques are needed. Electron microscopy as well as X-ray microscopic techniques utilising synchrotron X-ray radiation have proved most useful in providing such information. The present paper summarises the present status on advanced techniques and presents historical sources that have contributed to radioactive particle contamination.     

Radionuclide speciation and its relevance in environmental impact assessments

To assess the long-term environmental impact of radioactive contamination of ecosystems, information on source terms including radionuclide speciation, mobility and biological uptake is needed. A major fraction of refractory radionuclides released from nuclear sources such as nuclear weapons tests and reactor accidents is present as radioactive particles, whilst radionuclides are also present as colloids or low molecular mass species in effluents from nuclear installations. Low molecular mass species are more mobile (lower apparent K(d)) and bioavailable (higher apparent BCF) than colloids and particles. Soils and sediments act as sinks for particles and colloids. Due to particle weathering, associated radionuclides can be remobilised over time. Thus, information on particle characteristics such as composition, particle size, crystalline structures and oxidation states influencing weathering rates and subsequent mobilisation is essential. The present article summarises current knowledge on radioactive particles released from different sources, and the relevance of radionuclide speciation for mobility and biological uptake.     

Multi-technique characterization of a nuclear bomb particle from the Palomares accident

A January 1966 accident dispersed Pu and other nuclear bomb materials in the vicinity of Palomares, a village in southeastern Spain. Radioactive particles were identified in a soil sample collected in 1998 and analytical results obtained from one of the isolated particles are presented here. Isolation of the particle was performed using gamma-ray spectrometry and imaging plates. Scanning electron microscopy with X-ray microanalysis revealed the presence of U and Pu as well as Pb and Fe in the particle of approximately 10microm diameter. Radioisotopes of U, Pu, and Am were quantified using radiometric methods, inductively coupled plasma mass spectrometry and secondary ion mass spectrometry. The elevated (235)U/(238)U atom ratio indicates enriched U, and the Pu atom ratios are consistent with weapons-grade material. This work demonstrates that the analysis of individual particles provides information not available through bulk sample analysis.     

Mesoscale modelling of radioactive contamination formation in Ukraine caused by the Chernobyl accident

This work is devoted to the reconstruction of time-dependent radioactive contamination fields in the territory of Ukraine in the initial period of the Chernobyl accident using the model of atmospheric transport LEDI (Lagrangian-Eulerian DIffusion model). The modelling results were compared with available 137Cs air and ground contamination measurement data. The 137Cs atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The detailed scenario of the release from the accidental unit of the Chernobyl nuclear plant has been built (including time-dependent radioactivity release intensity and time-varied height of the release). The calculations have enabled to explain the main features of spatial and temporal variations of radioactive contamination fields over the territory of Ukraine on the regional scale, including the formation of the major large-scale spots of radioactive contamination caused by dry and wet deposition.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Radioactive contamination of wild mushrooms: a cross-cultural risk perception study

The aim of the present work was to determine the public perception of radioactive contamination of wild mushrooms, to confront this perception with an expert opinion, and to determine those factors that are perceived differently by specialists and lay people. The Internet appeared to be a useful tool in attaining these goals by finding the appropriate people across the world. The statistically significant differences in the perception of various aspects of mushroom pollution were revealed between respondents from three world regions, which were differently affected by the Chernobyl accident. Moreover, the majority of people have demonstrated a considerable difference in the perception of the global contamination of the environment versus the pollution of their local counties. The socio-psychological explanations of data are given. In general, there is a steady consistency in the perception of factors, which may control the radioactive contamination of edible fungi, by the majority of respondents. However, experts (radioecologists) rank the factor of fungal species as an extremely important parameter, while other people perceive the factors of the distance from the source of the pollution and the time thereafter as the most important parameters. Such discrepancies between professional and unprofessional opinions are discussed and some recommendations for risk communications are presented.     

On-site gamma dose rates at the Andreeva Bay shore technical base, northwest Russia

The spent nuclear fuel (SNF) and radioactive waste (RAW) storage facility at Andreeva Bay shore technical base (STB) is one of the largest and most hazardous nuclear legacy sites in northwest Russia. Originally commissioned in the 1960s the facility now stores large amounts of SNF and RAW associated with the Russian Northern Fleet of nuclear powered submarines. The objective of the present study was to map ambient gamma dose rates throughout the facility, in particular at a number of specific sites where SNF and RAW are stored. The data presented here are taken from a Norwegian-Russian collaboration enabling the first publication in the scientific literature of the complete survey of on-site dose rates. Results indicate that elevated gamma dose rates are found primarily at discrete sites within the facility; maximum dose rates of up to 1000 microSv/h close to the ground (0.1m) and up to 3000 microSv/h at 1m above ground were recorded, higher doses at the 1m height being indicative primarily of the presence of contaminated equipment as opposed to ground contamination. Highest dose rates were measured at sites located in the immediate vicinity of buildings used for storing SNF and sites associated with storage of solid and liquid radioactive wastes. Elevated dose rates were also observed near the former channel of a small brook that became heavily contaminated as a result of radioactive leaks from the SNF storage at Building 5 starting in 1982. Isolated patches of elevated dose rates were also observed throughout the STB. A second paper detailing the radioactive soil contamination at the site is published in this issue of Journal of Environmental Radioactivity.     

Anomalous concentrations of atmospheric plutonium-238 over Paris

Analysis of monthly rain samples collected in Paris reveals that ²³⁸Pu/ ^239,240Pu activity ratios, usually about 0·04, the fallout value, rose suddenly to 25 in October 1982. Abnormal ratios continued to be observed during the following months. Excess ²³⁸Pu from atmospheric nuclear tests can be eliminated as a possible cause. No correlation was found either with identified satellite re-entries or with atmospheric radioactive anomalies already detected in Northern Europe prior to the Chernobyl accident. Different potential industrial sources are discussed here, but the authors remain unable to identify the origin of the abnormally high ratio. This study shows that a careful investigation of ²³⁸Pu fallout is needed if environmental processes are to be traced via plutonium activity ratios.     

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia)

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.     

Assessment of state-of-the-art models for predicting the remobilisation of radionuclides following the flooding of heavily contaminated areas: the case of Pripyat River floodplain

The performances of models are assessed to predict the wash-off of radionuclides from contaminated flooded areas. This process should be accounted for in the proper management of the aftermath of a nuclear accident. The contamination of the Pripyat River water following the inundation of a floodplain heavily contaminated by (90)Sr and (137)Cs of Chernobyl origin is used as the basis for modelling. The available experimental evidence demonstrated that remobilisation of radiostrontium is an important process implying a significant secondary radioactive load of water flowing over the contaminated floodplain. On the contrary, there is no empirical evidence of a similar behaviour for radiocaesium. In general, state-of-the-art models properly predicted the remobilisation of strontium, whereas they significantly overestimated radiocaesium concentrations in water. The necessary model improvements for a more accurate prediction of radiocaesium contamination levels include a reassessment of the values of the model parameters controlling the remobilisation process.     

Reconstruction of radioactive plume characteristics along Chernobyl's Western Trace

Using data obtained from 435 radiation sampling stations in the Red Forest, 1.5 km W if the Chernobyl Nuclear Complex, we reconstructed the deposition pathway of the first plume released by the accident, Chernobyl's Western Trace. The dimensions and deposition rates of the plume remain sharply defined 15 years after the accident. Assuming a uniform particle distribution within the original cloud, we derived estimates of plume dimensions by applying geometric transformations to the coordinates at each sample point. Our derived estimates for the radioactive cloud accounted for 87% of the variation of radioactivity in this region. Results show a highly integrated bell-shaped cross-section of the cloud of radiation, approximately 660 m wide and 290 m high, traveling at a bearing of 264 degrees from reactor IV. Particle sizes within Chernobyl's Western Trace were within the most dangerous range for inhaled aerosols (2-5 microm). Therefore, reconstruction of the dispersion of such particles is critical for understanding the aftermath of nuclear and biological aerosol releases.     

核电与核废物管理

核能是一种能量密度大、稳定性好、燃料运输量小、综合经济效益好的能源。世界各国核电在总发电量中的比例逐年上升,1992年达17％,而我国仅占0.1％。在目前我国电力短缺的条件下,发展核电、提高核电在总电量中的比例,不失为我国发展能源工业的一个战略目标。在发展核电过程中,要重视核废物的处理和处置,以保证人类健康和环境免遭放射性的污染。     

Estimation of critical loads for radiocaesium in Fennoscandia and Northwest Russia

The application of the critical loads methodology for radioactive contamination of Arctic and sub-arctic ecosystems, where natural and semi-natural food products are important components of the diet of many people, is proposed and discussed. The critical load is herein defined as the amount of radionuclide deposition necessary to produce radionuclide activity concentrations in food products exceeding intervention limits. The high transfer of radiocaesium to reindeer meat gives this product the lowest critical load, even though the intervention limit is relatively high compared with other products. Ecological half-lives of radiocaesium in natural and semi-natural products are often very long, and it is therefore important to take account of contamination already present in the event of an accident affecting areas where such products are important. In particular, the long ecological half-life for radiocaesium in moose meat means that the critical load is highly sensitive to prior deposition. An example of the potential application of the method for emergency preparedness is given for the Chernobyl accident.     

Lake fish as the main contributor of internal dose to lakeshore residents in the Chernobyl contaminated area

Two field expeditions in 1996 studied 137Cs intake patterns and its content in the bodies of adult residents from the village Kozhany in the Bryansk region, Russia, located on the shore of a drainless peat lake in an area subjected to significant radioactive contamination after the 1986 Chernobyl accident. The 137Cs contents in lake water and fish were two orders of magnitude greater than in local rivers and flow-through lakes, 10 years after Chernobyl radioactive contamination, and remain stable. The 137Cs content in lake fish and a mixture of forest mushrooms was between approximately 10-20 kBq/kg, which exceeded the temporary Russian permissible levels for these products by a factor of 20-40. Consumption of lake fish gave the main contribution to internal doses (40-50%) for Kozhany village inhabitants Simple countermeasures, such as Prussian blue doses for dairy cows and pre-boiling mushrooms and fish before cooking, halved the 137Cs internal dose to inhabitants, even 10 years after the radioactive fallout.     

Model testing using data on 137Cs from Chernobyl fallout in the Iput River catchment area of Russia

Data collected for 10 years following the Chernobyl accident in 1986 have provided a unique opportunity to test the reliability of computer models for contamination of terrestrial and aquatic environments. The Iput River scenario was used by the Dose Reconstruction Working Group of the BIOMASS (Biosphere Modelling and Assessment Methods) programme. The test area was one of the most highly contaminated areas in Russia following the accident, with an average contamination density of 137Cs of 800,000 Bq m-2 and localized contamination up to 1,500,000 Bq m-2, and a variety of countermeasures that were implemented in the test area had to be considered in the modelling exercise. Difficulties encountered during the exercise included averaging of data to account for uneven contamination of the test area, simulating the downward migration and changes in bioavailability of 137Cs in soil, and modelling the effectiveness of countermeasures. The accuracy of model predictions is dependent at least in part on the experience and judgment of the participant in interpretation of input information, selection of parameter values, and treatment of uncertainties.     

A prognostic estimation of the area contaminated with alpha-emitting transuranium isotopes in Belarus following the Chernobyl accident

As a result of the Chernobyl accident, some regions of Belarus have been contaminated with the plutonium isotopes (238,239,240,241)Pu. Considering the importance of the environmental impact of the alpha-emitting radionuclides we have carried out a prognostic estimation of the area contaminated with (238,239,240)Pu and (241)Am (the latter being a decay product of (241)Pu) in Belarus. The calculations were made using measurements of (238,239,240)Pu activity concentrations in soil samples from about 600 settlements in the affected region, together with the estimated activity ratio A((241)Am)/A((238,239,240)Pu). The area contaminated with alpha-emitting transuranium isotopes predicted for the year 2006 has been compared with that estimated for 1986. The results show that by 2006, the area of inhabited districts where contamination with (238,239,240)Pu and (241)Am exceeds the threshold level of 740 Bq/m(2), will be 3.7 times larger, reaching approximately 3.5 x10(3)km(2). Of this, almost 20% will have a contamination level of 1850--3700 Bq/m(2).     

Long-term environmental problems of radioactively contaminated land

This paper examines the various sources of radiological land contamination; its extent; its impacts on man, agriculture, and the environment; countermeasures for mitigating exposures; radiological standards; alternatives for achieving land decontamination and cleanup; and possible alternatives for utilizing the land. The major potential sources of extensive long-term land contamination with radionuclides, in order of decreasing extent, are nuclear war, detonation of a single nuclear weapon (e.g. terrorist act), serious reactor accidents, and nonfission nuclear weapons accidents that disperse the nuclear fuels (termed) “broken arrows”). Over the long term, external radiation doses are dominated primarily by ¹³⁷Cs and internal radiation doses primarily by ⁹⁰Sr. Plutonium and the transuranic elements are also important, primarily because of their long half-lives and relatively high inhalation doses. Costs for cleanup of contaminated land are very high. For example, cleanup of the broken arrow in Palomares, Spain, was approximately $33,600 per hectare. If cleanup of agricultural land is impractical, alternative land uses might include production of fiber crops, seed-stock crops, or plant biomass for alcohol fuels, or diversion of the land from crop production. Conversion of cropland to pasture or rangeland takes benefit from the generally lower accumulation of radionuclides into animals products compared with plant products. Another alternative is to fence off the land and use it for production of timber. This alternative would allow for 25–100 y or more of radiological decay before recovery of the timber.     

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.