A new generic sub-model for radionuclide fixation in large catchments from continuous and single-pulse fallouts, as used in a river model

This paper presents a new general sub-model for fixation in catchment areas to be used within the framework of a river model for substances such as radionuclides and metals from continuous and single-pulse fallouts. The model has been critically tested using data from 27 European river sites covering a very wide geographical area and contaminated by radiocesium and radiostrontium from the Chernobyl accident and from the nuclear weapons tests (NWT fallout). This modelling approach gives radionuclide concentrations in water (total, dissolved and particulate phases) at defined sites on a monthly basis. The overall river model is based on processes in the upstream river stretch and in the catchment area. The catchment area is differentiated into inflow (approximately dry land) areas and outflow (approximately wetland) areas. The model has a general structure, which can be used for all radionuclides or substances. It is simple to apply in practice since all driving variables may be readily accessed from maps and standard monitoring programs. The driving variables are: latitude, altitude, catchment area, mean annual precipitation and fallout. Note that for large catchments, this model does not require data on the characteristic soil type or the percentage of outflow areas (wet lands) in the catchment, as in most previous models, since in practice it is very difficult to obtain reliable data on characteristic soil type or percentage of outflow areas, especially in large and topographically complex catchments. Modelled values have been compared to empirical data from rivers sites covering a wide domain (catchment areas from 3000 to 3,000,000 km2, precipitation from 400 to 1700 mm/year; fallouts from 1600 to 280,000 Bq/m2; altitudes from 0 to 1000 m.a.s.l. and latitudes from 41 degrees to 72 degrees N). The river model with its sub-model for fixation predicts close to the uncertainty factors given by the empirical data, which have been shown to be about a factor of 1.6 for 137Cs and a factor of 2.2 for 90Sr in river water. The obtained characteristic uncertainty factors for 137Cs from the Chernobyl fallout is 2.4, for 137Cs from the NWT fallout it is 1.3 and for the 90Sr results from the NWT fallout it is 3 using the new model.     

A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Discharge of 137Cs and 90Sr by Finnish rivers to the Baltic Sea in 1986-1996

The total amounts of 137Cs and 90Sr transported from Finland by rivers into the Gulf of Finland, Gulf of Bothnia and Archipelago Sea since 1986 were estimated. The estimates were based on long-term monitoring of 137Cs and 90Sr in river and other surface waters and on the statistics of water discharges from Finnish rivers to the above sub-areas of the Baltic Sea. The total amounts of 137Cs and 90Sr removed from Finland into the Baltic Sea during 1986-1996 were estimated to be 65 and 10 TBq, respectively. The results show that, although the deposition of 137Cs was much higher than that of 90Sr after the Chernobyl accident, the amount of 137Cs removed from Finland is only six times as high as that of 90Sr. This emphasizes the importance of 90Sr while considering radiation doses from surface waters and 137Cs while estimating doses via pathways from catchment soil, lake sediments and biota after a fallout situation.     

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.     

Use of 129I and 137Cs in soils for the estimation of 131I deposition in Belarus as a result of the Chernobyl accident

Using radioactivity measurements for 131I and 137Cs and nuclear activation analysis (NAA) or accelerator mass spectrometry (AMS) for 129I, ratios of 131I/137Cs and 129I/137Cs have been determined in soils from Belarus. We find that the pre-Chernobyl ratio of 129I/137Cs in Belarus is significantly larger than expected from nuclear weapons fallout. For the Chernobyl accident, our results support the hypothesis that there was relatively little fractionation of iodine and caesium during migration and deposition of the radioactive cloud. For sites having 137Cs > 300 Bq/kg, 129I can potentially give more reliable retroactive estimates of Chernobyl 131I deposition. However, our results suggest that 137Cs can also give reasonably good (+/-50%) estimates for 131I in Belarus.     

Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples

Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu.     

Contamination of Austrian soil with caesium-137

Austria ranks among the countries that have been most strongly affected by the Chernobyl fallout. The mean contamination with 137Cs is 21.0 kBq/m2, of which 18.7 kBq/m2 is due to the Chernobyl accident, whereas global fallout contributes 2.3 kBq/m2. Maximum values of total 137Cs contamination are nearly 200 kBq/m2. Total deposition of Chernobyl 137Cs on Austrian territory is 1.6 PBq or a fraction of around 2% of the 137Cs released from the reactor. 2115 measurements were used to draw the Austrian "caesium map". The geographical pattern of fallout distribution shows regional differences of contamination as high as 1:100.     

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.     

Determining the Chernobyl impact on sediments of a pre-Alpine lake with a very comprehensive set of data

Man-made and natural radionuclides in Lake Wallersee were determined in the pre-Alpine environment at the northern slope of the Alps, which was heavily affected by the Chernobyl fallout in May 1986. The objective of this study was to get knowledge of location and quantity of man-made radionuclide input (especially (137)Cs) generated in the Chernobyl accident to lake sediments. Eleven sediment cores were sampled and activity depth profiles of (137)Cs and (210)Pb were determined with 5mm depth-resolution. The Chernobyl fallout produced an extreme (137)Cs peak in the sediment cores providing an excellent time marker. The chronological interpretation of deeper sediment layers was done by radiochemical analysis of (90)Sr and (239+240)Pu, which were released during atmospheric weapons' tests in the 1950s and 1960s. This allowed a complete chronological analysis of the sediment cores with a very compact set of data.     

The concentration of Cs in the surface of the Greek marine environment

The radiological status of the Greek marine environment, prior to the Chernobyl accident, was characterized mainly by the fallout from nuclear weapon tests. However, the release of radioactivity into the environment from the accident in the Chernobyl Nuclear Power Plant and its deposition in the Greek marine environment resulted in an increase of the ¹³⁷Cs activity concentration by approximately one order of magnitude. In addition, the direct transport of radiocaesium into the North Aegean Sea has been further influenced by the late impact of the Chernobyl accident on the Greek marine environment, related to the transfer of ¹³⁷Cs, mainly through the Dnieper but also the Danube rivers, to the Black Sea and further to the North Aegean Sea through the Straits of Dardanelles. The aim of this work is to provide a present day picture of the geographic variation of the concentration of ¹³⁷Cs in the surface layer of the Greek marine environment and hence, to evaluate the annual committed effective dose delivered to humans through the ingestion pathway from marine sources.     

90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans--WOMARS results

Under an IAEA's Co-ordinated Research Project "Worldwide Marine Radioactivity Studies (WOMARS)" 90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans have been investigated. The Pacific and Indian Oceans were divided into 17 latitudinal boxes according to ocean circulation, global fallout patterns and the location of nuclear weapons test sites. The present levels and time trends in radionuclide concentrations in surface water for each box were studied and the corresponding effective half-lives were estimated. For the year 2000, the estimated average 90Sr, 137Cs and (239,240)Pu concentrations in surface waters of the Pacific and Indian Oceans varied from 0.1 to 1.5 mBq/L, 0.1 to 2.8 mBq/L, and 0.1 to 5.2 microBq/L, respectively. The mean effective half-lives for 90Sr and 137Cs in surface water were 12+/-1 years for the North, 20+/-1 years for the South and 21+/-2 years for the Equatorial Pacific. For (239,240)Pu the corresponding mean effective half-lives were 7+/-1 years for the North, 12+/-4 years for the South and 10+/-2 years for the Equatorial Pacific. For the Indian Ocean the mean effective half-lives of 137Cs and (239,240)Pu were 21+/-2 years and 9+/-1 years, respectively. There is evidence that fallout removal rates before 1970 were faster than those observed during recent decades. The estimated surface water concentrations of 90Sr, 137Cs and (239,240)Pu in latitudinal belts of the Pacific and Indian Oceans for the year 2000 may be used as the average levels so that any new contribution from nuclear facilities, nuclear weapons test sites, radioactive waste dumping sites and from possible nuclear accidents can be identified.     

Vertical migration studies of 137Cs from nuclear weapons fallout and the Chernobyl accident

The vertical migration of (137)Cs originating from nuclear weapons fallout (NWF) and the Chernobyl accident has been studied at 33 sampling sites in western Sweden. An attempt to describe the present depth distribution with a solution to the convection-diffusion equation (CDE) with a pulse-like fallout event as the initial condition was made. A sum of two CDEs describing the NWF and Chernobyl debris was fitted to the actual depth profiles measured by soil sampling. The fitted depth profiles were used to correct in situ measurements for the actual depth distribution, showing good agreement with the accumulated activities in soil samples. As expected, the vertical migration was very slow and most caesium was still present in the upper soil layers. The ranges of the apparent convection velocity, v, and apparent diffusion coefficient, D, were between 0 and 0.35 cm/year and 0.06 and 2.63 cm(2)/year, respectively.     

Migration of Cs in tributaries,lake water and sediment of Lago Maggiore (Italy,Switzerland) – analysis and comparison with Lago di Lugano and other lakes

This paper describes the behaviour of ¹³⁷Cs in Lago Maggiore and other pre-alpine lakes as a consequence of atmospheric nuclear weapons testing fallout and the fallout from the nuclear accident in Chernobyl. It presents data on the ¹³⁷Cs distribution in tributaries, lake water, bottom sediments and reveals the role of ¹³⁷Cs as a marker of the sedimentation processes. The run-off of ¹³⁷Cs from the watershed to the lake is described with a simple compartment model. Measurements of the activity concentration of ¹³⁷Cs in sediments are compared with the output of a model (diffusion–convection type) which describes the input of ¹³⁷Cs into and its vertical distribution within the sediment. Varying sedimentation rates (0.05–0.90 g (cm² y)⁻¹) in Lago Maggiore are compared with data of other authors. Sedimentation rates and total distribution coefficients (of about 10⁵ L kg⁻¹) in Lago Maggiore are discussed and compared with those of Lago di Lugano, Lake Constance, and Lake Vorsee.     

Determination of Cs in the water system of a pre-Alpine lake

The aim of this study was to measure the ¹³⁷Cs activity derived from the Chernobyl accident in the water system of Lake Wallersee, a pre-Alpine lake in Austria within an area highly contaminated by the Chernobyl fallout.     

Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (240)Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(239)Pu atomic ratio ranging between 0.16 +/- 0.01 and 0.44 +/- 0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The (237)Np/(239)Pu atomic ratios ranged between 0.06 +/- 0.01 and 0.42 +/- 0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 degrees N, 12.38 degrees E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.     

A blind test of the MOIRA lake model for radiocesium for Lake Uruskul, Russia, contaminated by fallout from the Kyshtym accident in 1957

This paper presents results of a model-test carried out within the framework of the COMETES project (EU). The tested model is a new lake model for radiocesium to be used within the MOIRA decision support system (DSS; MOIRA and COMETES are acronyms for EU-projects). This model has previously been validated against independent data from many lakes covering a wide domain of lake characteristics and been demonstrated to yield excellent predictive power (see H?kanson, Modelling Radiocesium in Lakes and Coastal Areas. Kluwer, Dordrecht, 2000, 215 pp). However, the model has not been tested before for cases other than those related to the Chernobyl fallout in 1986, nor for lakes from this part of the world (Southern Urals) and nor for situations with such heavy fallout as this. The aims of this work were: (1) to carry out a blind test of the model for the case of continental Lake Uruskul, heavily contaminated with 90Sr and 137Cs as a result of the Kyshtym radiation accident (29 September 1957) in the Southern Urals, Russia, and (2) if these tests gave satisfactory results to reconstruct the radiocesium dynamics for fish, water and sediments in the lake. Can the model provide meaningful predictions in a situation such as this? The answer is yes, although there are reservations due to the scarcity of reliable empirical data. From the modelling calculations, it may be noted that the maximum levels of 137Cs in fish (here 400 g ww goldfish), water and sediments were about 100,000 Bq/kg ww, 600 Bq/l and 30,000 Bq/kg dw, respectively. The values in fish are comparable to or higher than the levels in fish in the cooling pond of the Chernobyl NPP. The model also predicts an interesting seasonal pattern in 137Cs levels in sediments. There is also a characteristic "three phase" development for the 137Cs levels in fish: first an initial stage when the 137Cs concentrations in fish approach a maximum value, then a phase with relatively short ecological half-lives followed by a final phase with long ecological half-lives more or less corresponding to the physical decay of radiocesium.     

Formation of radioactivity enriched soils in mountain areas

A field study was carried out in the Mercantour Mountains at 2200 m altitude to investigate the processes of soil enrichment in atmospheric Chernobyl (137)Cs. Soils with high (137)Cs activities have been collected in the pasture areas with frequently measured (137)Cs activity values of the order of 7000 Bq m(-2). At some single spots (about 6% of the studied area), activity in soils reached 300000 Bq m(-2), which represents 44% of the (137)Cs of the total area. Data further showed that spatial distribution of Cs depends widely on its origin: Chernobyl Cs is mainly concentrated in "enriched" soils, whereas older Cs and (241)Am fallout from nuclear weapons tests (NWTs) and natural atmospheric (210)Pb in soils is less heterogeneously distributed.In order to elucidate the processes which have led to the enrichment in Chernobyl (137)Cs in the Alps in May of 1986, we have studied the repartition of atmospheric (7)Be isotope (half-life=53.3 d) in the pasture compartments (soil, litter, grass, and snow). Snow (7)Be data give evidence that fallout enrichment is related to snow accumulation (snow drift). The transfer of beryllium occurs rapidly to the grass and litter, where the strongest pollutant accumulations were measured. However, (7)Be transport to the soil required more than 8 months.     

Migration of Cs and Sr in undisturbed soil profiles under controlled and close-to-real conditions

Migration of ¹³⁷Cs and ⁹⁰Sr in undisturbed soil was studied in large lysimeters three and four years after contamination, as part of a larger European project studying radionuclide soil–plant interactions. The lysimeters were installed in greenhouses with climate control and contaminated with radionuclides in an aerosol mixture, simulating fallout from a nuclear accident. The soil types studied were loam, silt loam, sandy loam and loamy sand. The soils were sampled to 30–40 cm depth in 1997 and 1998. The total deposition of ¹³⁷Cs ranged from 24 to 45 MBq/m², and of ⁹⁰Sr from 23 to 52 MBq/m². It was shown that migration of ¹³⁷Cs was fastest in sandy loam, and of ⁹⁰Sr fastest in sandy loam and loam. The slowest migration of both nuclides was found in loamy sand. Retention within the upper 5 cm was 60% for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, while in loamy sand it was 97 and 96%, respectively. In 1998, migration rates, calculated as radionuclide weighted median depth (migration centre) divided by time since deposition were 1.1 cm/year for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, 0.8 and 1.0 cm/year, respectively, in loam, 0.6 and 0.8 cm/year in silt loam, and 0.4 and 0.6 cm/year for ¹³⁷Cs and ⁹⁰Sr, respectively, in loamy sand. A distinction is made between short-term migration, caused by events soon after deposition and less affected by soil type, and long-term migration, more affected by e.g. soil texture. Three to four years after deposition, effects of short-term migration is still dominant in the studied soils.     

137Cs and 90Sr behavioural regularities in the southeastern part of the Baltic Sea

Variations in 137Cs concentrations were investigated over the period 1986-1997 in the southeastern part of the Baltic Sea, following the Chernobyl power plant accident. The rate of "self-cleaning" was demonstrated to be very slow, the average concentration of 137Cs in 1996 being almost the same as that measured directly after the accident, in 1986. Measurements of both 137Cs and 90Sr concentrations generally revealed homogeneous distributions in this region of the Baltic Sea, though patchy distributions did develop under some hydrometeorological conditions. Specifically, the 137Cs concentration distribution became heterogeneous with values varying in the range 60-92 Bq/m3 under south-southwesterly wind conditions whilst the 90Sr concentration distribution developed similar characteristics with values ranging from 15 to 64 Bq/m3 under east-southeasterly wind conditions. In addition, in coastal waters, over extensive periods of north-northwesterly winds in 1995, 137Cs concentrations increased to values 1.5-2 times the overall average concentration, which was registered in 1986 and 1996. These data therefore reveal a continuing significant pollution of the waters of the Baltic Sea resulting from the Chernobyl power plant accident, a pollution compounded by the slow rate of radionuclide self-cleaning and significant probability of sudden regional concentration increase.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.