Review and assessment of models used to predict the fate of radionuclides in lakes

A variety of models for predicting the behaviour of radionuclides in fresh water ecosystems have been developed and tested during recent decades within the framework of many international research projects. These models have been implemented in Computerised Decision Support Systems (CDSS) for assisting the appropriate management of fresh water bodies contaminated by radionuclides. The assessment of the state-of-the-art and the consolidation of these CDSSs has been envisaged, by the scientific community, as a primary necessity for the rationalisation of the sector. The classification of the approaches of the various models, the determination of their essential features, the identification of similarities and differences among them and the definition of their application domains are all essential for the harmonisation of the existing CDSSs and for the possible development and improvement of reference models that can be widely applied in different environmental conditions. The present paper summarises the results of the assessment and evaluation of models for predicting the behaviour of radionuclides in lacustrine ecosystems. Such models were developed and tested within major projects financed by the European Commission during its 4th Framework Programme (1994-1998). The work done during the recent decades by many modellers at an international level has produced some consolidated results that are widely accepted by most experts. Nevertheless, some new results have arisen from recent studies and certain model improvements are still necessary.     

Assessment of natural radiation exposure and radon exhalation from building materials in Greece

In controlling the natural radiation exposure for the residents of dwellings, it is necessary to determine the levels of natural radioactivity (external exposure) and radon exhalation rate (internal exposure) from building materials. Using a high-resolution gamma ray spectrometry system, the activity concentration of natural radionuclides was measured. The radon exhalation rate was measured by hermetically closing the sample in a container and following the radon activity growth as a function of time. Three different methods were applied in order to find the most appropriate, i.e. that with the less uncertainty for the less exposure time. Typical building materials were analyzed in order to examine the external and internal exposures. In addition, the total annual effective dose was evaluated for the residents of a typical Greek dwelling.     

Present background levels of surface 137Cs and (239,240)Pu concentrations in the Pacific

The present levels of anthropogenic radionuclides, 137Cs and (239,240)Pu, in surface waters of the Pacific are estimated using the HAM database, which is a comprehensive data set of 137Cs, (239,240)Pu and other anthropogenic radionuclides. The time-series data of surface 137Cs and (239,240)Pu suggests that surface 137Cs and (239,240)Pu concentrations in the Pacific since 1971 decrease exponentially in each sea area, although the temporal changes of surface 137Cs and (239,240)Pu differed between sea areas of the Pacific. The calculated 137Cs concentrations in the Pacific surface waters in 2000 are homogeneous in the Pacific, comparing with that in the 1960s and 1970s, although they are still high in the North Pacific and low in the South Pacific. The biogeochemical and physical processes are significant factors to control present levels of surface (239,240)Pu concentrations, which are high in the Subarctic and equatorial Pacific and low in the mid-latitude region of the eastern North Pacific.     

Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model

We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect.     

Modelling the distribution of plutonium in the Pacific Ocean

An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well.     

Temporal variation of 137Cs water column inventory in the North Pacific since the 1960s

The temporal variation of water column inventories of 137Cs in the North Pacific since the 1960s was examined based on the analysis of the 137Cs profiles in HAM database. 137Cs in seawater in the North Pacific have originated mainly from global fallout from atmospheric nuclear weapons tests, which occurred in the early 1960s. In the 1960s, both the meridional distribution of 137Cs inventory in the North Pacific and that of fallout on land stations showed mid-latitude maximum. The region with higher deposition at land stations, however, was more northern than the latitudes where the 137Cs inventory in the North Pacific showed a maximum. The difference of the latitude where maximum 137Cs deposition/inventory was observed reflects the difference of the geographical distribution of the precipitation amount in the Pacific and Atlantic Oceans followed by the different warm current systems in each ocean. A good positive relation between 137Cs inventory and annual precipitation amount was discovered in the ocean stations at the middle latitude in the North Pacific. The horizontal distribution of 137Cs inventories at the middle latitudes in the North Pacific is characterized as west-high and east-low in the early 1960s, which was basically controlled by the distribution of annual precipitation amount. Eastward advection, then, modified it to be less difference in 1966-1967 after the highest deposition periods in 1963-1965. In the 1970s and 1980s, increases of the 137Cs inventory at the lower latitude of 10-20 deg. N are found. Surface and subsurface southward transports are considered as the source of this increasing 137Cs inventory.     

Ventomod: a dynamic model for leaf to fruit transfer of radionuclides in processing tomato plants (Lycopersicon esculentum Mill.) following a direct contamination event

This paper presents results on the calibration and validation of a model (Ventomod) for leaf to fruit transfer of (134)Cs, (85)Sr and (65)Zn in processing tomato plants after leaf contamination. Several models (e.g. FARMLAND) that deal specifically with the transfer of radionuclides to fruits are adaptations of models that were developed for agricultural crops such as leafy green vegetables. "Ventomod" represents a dynamic evaluation model exclusively built for the short-term behaviour of radionuclide depositions. It forecasts the level of radionuclide contamination in ripe processing tomato fruits following an accidental radionuclide release into the atmosphere. A validation of the developed model by data sets from an independent experiment showed that the model successfully reproduced the observed radionuclide distribution and dynamics in tomato fruits. The level of uncertainty was within the normal range of similar assessment models. For a more general use of this model further testing with independent data sets from experiments obtained under different environmental conditions and data from other horticulturally important plant species would be desirable.     

Activity concentration of caesium-137 in agricultural soils

In this study, we measured 137Cs activity concentrations in the soil samples taken from agricultural lands in the Buyuk Menderes Basin in Turkey in 1997 and 1998. The soil samples were collected from 42 sites in this Basin. The activity concentration of 137Cs was found to range between 2.81+/-0.17 Bq.kg(-1) and 20.75+/-0.29 Bq.kg(-1). The effect of organic matter, clay, silt and sand contents and pH of the soil on the relative adsorption of the 137Cs on the soil surface were also studied.     

Human exposure to dioxins through the diet in Catalonia,Spain: carcinogenic and non-carcinogenic risk

The main objectives of this study were to estimate the dietary intake of dioxins by the population of Catalonia, Spain, to determine which food groups showed the greatest contribution to this intake, and to assess the health risks potentially associated with the dietary dioxin intake. From June to August 2000, food samples were randomly acquired in seven cities of Catalonia. Dioxin concentrations were determined in 108 samples belonging to the following groups: vegetables, fruits, pulses, cereals, fish and shellfish, meats and meat products, eggs, milk and dairy products, and oils and fats. Estimates of average daily food consumption were obtained from recent studies. Total dietary intake of dioxins for the general population of Catalonia was estimated to be 95.4 pg WHO-TEQ/day (78.4 pg I-TEQ/day), with fish and shellfish (31%), diary products (25%), cereals (14%) and meat (13%) showing the greatest percentages of contribution to dioxin intake. The contribution of all the rest of food groups to the total dietary intake was under 20%. The non-carcinogenic risk index of dioxin intake through the diet was in the range 0.34-1.36, while the carcinogenic risk level was 1,360 excess cancer over a lifetime of 70 years. Our results corroborate the decreasing tendency in dietary intake of dioxins found in recent studies (2000-2001) from various countries.     

Influence of heavy metals on the formation and the distribution behavior of PAH and PCDD/F during simulated fires

Combustion experiments were performed with an artificial fire load (polystyrene and quartz powder) in a laboratory scale incinerator in the presence of gaseous HCl to simulate accidental fire conditions. The aim of this investigation was to trace back the alterations of the formation and the distribution behavior of PAH and PCDD/PCDF to the presence of CuO or a mixture of metal oxides (CdO, CuO, Fe(2)O(3), PbO, MoO(3), ZnO). The total amount of the 16 PAH target compounds was reduced by the factor of 5-9 when the mixture of metal oxides was present rather than merely CuO. PAH patterns as well as their distribution behavior were significantly influenced by these oxides. In general, transportation inside the installation was enhanced for most of the 16 analyzed PAH. Only fluorene and dibenzo[a,h]anthracene were transported to a smaller extent. In contrast to PAH, total concentrations of PCDD were increased by factor 9 and of PCDF by factor 10, respectively, when CuO was present. Adding the mixture of metal oxides resulted in an increase of PCDD by factor 14 and of PCDF by factor 7. CuO and the mixture of metal oxides had a different influence on the PCDD/F homologue patterns. For instance, the HxCDF to OCDF ratio after incineration without any metal oxide was 1 to 6, whereas addition of CuO or the mixture of the metal oxides shifted the HxCDF to OCDF ratios towards 1 to 40 or 1 to 17, respectively. Combustion along with CuO increased transportation of higher chlorinated PCDF congeners, whereas the mixture of the metal oxides caused a strong decrease of PCDF distribution throughout the system.