Efficiency of aluminum-pillared montmorillonite on the removal of cesium and copper from aqueous solutions.

Aluminum-pillared-layered montmorillonites (PILMs) were tested for their potential application in the removal of copper or cesium from aqueous solutions. By varying the initial conditions, several PILMs were prepared and characterized by means of X-ray fluorescence (XRF), proton induced gamma-ray emission (PIGE), X-ray diffraction (XRD) and sorption isotherms. Uptake of metals was studied by means of XRF spectrometry for copper sorption or gamma-ray spectrometry for cesium, using 137Cs as radiotracer. The sorption kinetics and capacity of PILMs were determined in relation to the effects of factors such as the initial metal concentration, initial pH of the solution and the presence of competitive cations. Kinetic studies showed that an equilibrium time of few minutes was needed for the adsorption of metal ions on PILMs. A pseudo-first-order equation was used to describe the sorption process for either copper or cesium. The most effective pH range for the removal of copper and cesium was found to be 4.0-6.0 and 3.0-8.0, respectively. Cesium sorption isotherms were best represented by a two-site Langmuir model while copper isotherms followed the Freundlich or the two-site Langmuir model. Cesium sorption experiments with inorganic or organic competitive cations as blocking agents revealed that the high selective sites of PILMs for cesium sorption (1-2% of total) are surface and edge sites in addition to interlayer exchange sites. In copper sorption, the two sites were determined as interlayer sites of PILMs after restoring their cation exchange capacity and sites associated with the pillar oxides.

Use of HPGe gamma-ray spectrometry to assess the isotopic compositiion of uranium in soils.

Gamma-ray spectrometry was used to determine uranium activity and investigate the presence of depleted uranium in soil samples collected from camping sites of the Greek expeditionary force in Kosovo. Assessment of 238U concentrations was based on measurements of the 63.3 keV and 92.38 keV emissions of its first daughter nuclide, 234Th. To determine the isotopic ratio of 238U/235U, secular equilibrium along the two radioactive series was first ensured and thereby the contribution of 235U under the 186 keV peak was deduced. The uranium activity in the samples varied from 48 to 112 Bq kg(-1), whereas the activity ratio of 238U/235U averaged 23.1+/-4.3.

Strontium adsorption properties of an aluminum-pillared montmorillonite carrying carboxylate functional groups.

Strontium adsorption was studied in an aluminum-pillared montmorillonite (PILC) carrying organic acid groups. The in situ dissociation of these groups increases the number of negative sites in the modified PILC, promoting thus the uptake of cations from an exchange solution. To investigate the role of solution pH and acid strength in cation uptake phenomena, base titrations were performed for PILCs carrying either oxalate or acetate groups. Comparison with the pristine PILC showed that extra Sr(2+) uptake initiated at pH 6 and 8 in the presence of oxalate and acetate, respectively. The overall increase in Sr(2+) uptake was higher in the presence of oxalate and amounted to about 136% as compared with the pristine PILC, at pH slightly above 8. The effect of the acid's strength was further probed through strontium adsorption isotherms, taken at a constant pH for PILC samples carrying acetate, oxalate, malonate, or citrate groups. The results demonstrate that cation uptake can be optimized by tuning the pH conditions to the acid's strength or vice versa.

Strontium-90 concentration measurements in human bones and teeth in Greece.

Strontium-90 concentration was measured in human bones and teeth collected in Greece during the period 1992-1996. One hundred and five bone samples, mainly cancellous bone, and 108 samples, taken from a total of 896 individual teeth were processed. Samples were classified according to the age and sex of the donors. Samples were chemically pre-treated according to a specially devised method to enable extraction of 90Y, at equilibrium with 90Sr in the original sample. Subsequently, 90Y beta activity was measured with a gas proportional counter. Radiostrontium concentration in bone samples showed small variations with respect to age or sex, with an average value of 30 mBq 90Sr/g Ca. However, 90Sr concentration measurements in teeth demonstrated a pronounced structure, which clearly reflects contamination from the 1960s atmospheric nuclear weapons tests and the more recent Chernobyl accident. This difference is attributed to the different histological structure of skeletal bones and teeth, the later consisting mainly of compact bone. An age-dependent model for radiostrontium concentration in human bones and teeth is developed which is able to successfully reproduce the experimental data. Through a fitting process, the model also yielded calcium turnover rates for compact bone, as a function of age, as well as an estimate of radiostrontium contamination of foodstuffs in Greece for the past four decades. The results obtained in this study indicate that radiostrontium environmental contamination which resulted from the atmospheric nuclear weapons tests in the 1960s, exceed by far that caused by the Chernobyl accident.

Development and testing of a revised dynamic model of radiocaesium transfer to sheep tissues.

The model of radiocaesium transfer to sheep presented by Galer et al. provides reliable predictions only for sheep of a similar body weight to those used in the development of the model (approximately 30 kg). To extend the applicability of the model, it was necessary to re-parameterise it in terms of activity concentrations in tissues rather than total activities within them (although for gut compartments the use of activity has been retained). The rate coefficients for the new model have been estimated by fitting the model to the data used by Galer et al. which was derived from a single "calibration" experiment. The new model was found to account for 94% of the observed variation in the data (n = 42), a result similar to that obtained by Galer et al. The model has also been tested against data not used in its development but obtained from four separate experiments undertaken by three different laboratories. Good agreement between the predictions of the new model and observations was found for most circumstances and for several breeds of sheep with different body weights. It is concluded that the new model provides a useful dynamic description of radiocaesium transfers to the tissues of sheep of different breeds and under different contamination scenarios.

Radiostrontium transfer to sheep's milk as a result of soil ingestion.

Soil ingestion as a source of radiostrontium contamination of ruminant milk products was studied by measuring the transfer coefficient to ovine milk. This is a follow-up report from a previous experiment (Assimakopoulos et al., 1993), which investigated radiocaesium transfer to sheep's milk as a result of soil ingestion. Milk samples from three lactating ewes, housed in individual metabolism cages, were used. Fifty grams per day of heavily contaminated sandy topsoil, collected in the Chernobyl area, were administered orally to the animals for a period of 1 week. The daily intake of 90Sr was 78 Bq day-1. During this contamination period, daily milk production and excreta output were measured. Excreta and milk was collected for an additional 7-day decontamination period, while they were fed on uncontaminated feed. The transfer coefficient was obtained through a best fit (minimum chi 2) of the data to predictions of a linear compartment model. The value obtained was fm = 0.041 +/- 0.016 d kg-1 for radiostrontium transport to milk. This result suggests that soil ingestion can be a major source of radiostrontium contamination in sheep and other free-grazing ruminants.

Ratios of transfer coefficients for radiocesium transport in ruminants.

A corollary of the multiple-compartment model for the transport of trace elements through animals was tested for cows, goats, and sheep. According to this corollary, for a given body "compartment" k of the animal (soft tissue, lung, liver, etc.), the ratio a(k) = f(k)/f(blood) of the transfer coefficients f, should exhibit similar values for physiologically similar animals. In order to verify this prediction, two experiments were performed at the Agricultural Research Station of Ioannina and at the facilities of Ria Pripyat in Pripyat, Ukraine. Eight animals in the first experiment and eighteen in the second were housed in individual pens and were artificially contaminated with a constant daily dose of radiocesium until equilibrium was reached. The animals were then sacrificed and transfer coefficients f(k) to twelve body "compartments" k were measured. These data were used to calculate the ratios a(k). The results were in accordance with predictions of the model and average values of a(k) were extracted for ruminants. It is concluded that these values may be employed for the prediction of animal contamination in any body compartment through the measurement of blood samples.

Strontium-90 concentrations in human teeth in south Ukraine, 5 years after the Chernobyl accident.

Approximately 1000 human teeth, collected in South Ukraine, in 1990-1991, were measured for 90Sr concentration. The teeth were grouped into 18 samples according to the age and sex of the donors. Measured levels of 90Sr concentrations were lower by a factor of 10 than measurements taken in the mid-1960s and mid-1970s. An interesting feature of the data is a 3-fold enhancement of contamination levels in the 25-45 year-old age group of the male population. A possible explanation for this anomaly is that this age group contains a significant number of men who were mobilized immediately after the Chernobyl accident for clean-up operations within the 30-km zone around the damaged nuclear power plant.

Transport of radiocaesium from a sheep's diet to its tissues.

Transfer coefficients for radiocaesium transport from a sheep's diet to blood, muscle, lung, liver, kidney, spleen heart, brain, rumen, intestines and fat were measured in a controlled experiment involving 50 adult ewes. The animals were fed dry grass and wheat, both contaminated with Chernobyl fallout debris, for a period of 60 days. During this period half of the animals were killed at regular intervals and samples of their blood and tissues were measured for radiocaesium concentration. The rest of the animals were returned to uncontaminated food and were monitored for radiocaesium concentration through periodic slaughtering for an additional 60 days. Transfer coefficients were extracted from the plateau reached at the end of the contamination phase. The data were also analyzed by means of a recently proposed linear multiple compartment model and transport rate parameters for each compartment were extracted. Transfer coefficients computed through the model's transport rate parameters show remarkable agreement with the experimentally obtained values.

Radiocaesium transfer to sheep's milk as a result of soil ingestion.

Soil ingestion as a source of radiocaesium contamination to ruminants was studied by measuring the transfer coefficient to sheep milk. Eight lactating ewes, housed in individual metabolism cages, were used. Fifty grams per day of heavily contaminated sandy topsoil, collected in 1990 from the Chernobyl area, were administered orally to the animals for a period of 1 week. The daily dose intake in 137Cs was 1835 Bq day-1. During this contamination period, daily milk production and excreta output were measured. The ewes were monitored for an additional 7 day decontamination period, while they fed on uncontaminated feed. Transfer coefficients were obtained through a best fit (minimum chi 2) of the data to predictions of a linear compartment model. The values obtained were fm = (2.6 +/- 0.7) x 10(-2) and f mu = (5 +/- 2) x 10(-2) days kg-1 for radiocaesium transport to milk and urine, respectively. These results suggest that soil ingestion can be a major source of radiocontamination for sheep and other free-grazing ruminants. Comparison of our results with soil-to-milk transfer coefficient values derived in two recent independent experiments suggests that there might be a strong dependence of radiocaesium availability on soil composition.

A general multiple-compartment model for the transport of trace elements through animals.

Multiple-compartment models employed in the analysis of trace element transport in animals are often based on linear differential equations which relate the rate of change of contaminant (or contaminant concentration) in each compartment to the amount of contaminant (or contaminant concentration) in every other compartment in the system. This has the serious disadvantage of mixing intrinsic physiological properties with the geometry of the animal. The basic equations on which the model presented here is developed are derived from the actual physical process under way and are capable of separating intrinsic physiological properties from geometry. It is thus expected that rate coefficients determined through this model will be applicable to a wider category of physiologically similar animals. A specific application of the model for the study of contamination of sheep--or indeed for any ruminant--is presented, and the temporal evolution of contaminant concentration in the various compartments of the animal is calculated. The application of this model to a system of compartments with changing geometry is also presented.

A study of radiocesium contamination and decontamination of sheep's milk.

The radiocesium contamination and decontamination of sheep's milk were studied under a constant level of activity concentration in the sheep's diet. Two sets of experiments were performed: one at the end of the animal's lactating period and one during the main lactating period. The data were in satisfactory agreement with the predictions of a simple two-compartment model. At the stage of equilibrium the data yielded the transfer coefficient fm with an average value of fm = 0.063 +/- 0.005 d L-1. In the second experiment a detailed study of the decontamination phase revealed a two-component decay with amplitudes 53% and 43% and half-lives 1.5 d and 6.9 d, respectively. A small 4% long-lived (T1/2 = 170 d) third component could not be distinguished from an overall background decay, measured in control animals.

The propagation of the Chernobyl 131I impulse through the air- grass- animal- milk pathway in northwestern Greece.

A three-compartment (air- grass-milk) milk contamination model for 131I has been applied to atmospheric, grass and milk data, following the April 1986 nuclear accident at Chernobyl. Samples of ovine and bovine milk collected daily by a large dairy company in Ioannina (northwestern Greece), throughout the month of May 1986 have been employed. The contamination impulse in the area, which provides the input to the model, has been approximated by a first order gamma-variate curve. Transfer rates and decay constants have been extracted by fitting predictions of the model independently to each set of data (air, grass and milk). All model parameters obtained from more than one set of data show remarkable consistency. These parameters are used to calculate the transfer coefficients fm for the transport of radioiodine at equilibrium for sheep and cows.

Processes that contribute to radiocesium decontamination of feta cheese.

In a series of experiments, the transfer of radiocesium from ovine milk to feta cheese was investigated through modifications of the standard cheese making procedure. All variations explored showed no significant change in the percentage of radiocesium transfer and the milk-to-cheese transfer coefficient was determined as f=.79 plus/minus .04 L.kg-1. It is concluded that cesium, like the rest of the alkali metals, remains in the water phase and thus follows very closely the distribution of moisture into the products of cheese making. The possibility of radiocesium decontamination of mature feta during the customary storage of the product in brine was also explored in a second series of experiments. The theoretical model employed in the analysis of cesium transport from feta to brine is presented in the Appendix to this paper. Predictions of the model were validated by experiments. A procedure is thus proposed for decontaminating mature feta during storage through successive replacements of the storage medium. Nomograms are presented for the determination of the optimum time interval between changes of the brine and the radiocesium concentration remaining in the feta. Changes in the properties of the product induced by the proposed treatment were also investigated with respect to composition, taste, and overall quality.

Radiocesium levels measured in breast milk one year after the reactor accident at Chernobyl.

One hundred-two samples of colostral milk, collected during spring of 1987, approximately one year after the reactor accident at Chernobyl, were measured for radiocesium contamination. The data showed a normal-type distribution with a mean contamination concentration of 16.4 Bq L-1. A weak correlation of the data to the mothers' diet was established by taking into account four of the main staples in the area. The corresponding transfer coefficient was deduced with a value of fm = 0.06 +/- 0.03 d L-1. The resultant effective dose received by breast-feeding infants was estimated, on the average, as 0.012 mrem d-1.

The environmental behavior of 131I in northwestern Greece following the nuclear reactor accident at Chernobyl.

A three compartment (air-grass-milk) milk contamination model for 131I has been applied to atmospheric, grass and milk data, following the April 1986 nuclear accident at Chernobyl. Samples of ovine and bovine milk collected daily by a large dairy company in Ioannina (northwestern Greece), throughout the month of May 1986 have been employed. The contamination impulse in the area, which provides the input to the model, has been approximated by a first order gamma-variate curve. Transfer rates and decay constants have been extracted by fitting predictions of the model independently to each set of data (air, grass and milk). All model parameters obtained from more than one set of data show remarkable consistency. These parameters are used to calculate the transfer coefficients fm for the transport of radioiodine at equilibrium for sheep and cows. The results are also employed for the extraction of radiation dose estimates sustained through ingestion and inhalation by the population in the area.

Measurement of the transfer coefficient for radiocesium transport from a sheep's diet to its milk.

The rate of increase and decay of radio contamination secreted in sheep's milk, resulting from a constant level of radiocesium in the animals' diet, was investigated. Ten lactating ewes were used in the experiment. For a period of 12 d the animals fed on contaminated grass, resulting in a daily radiocesium intake of 832 Bq per animal. They were subsequently returned to a contamination-free diet and were monitored for another 9 d. Throughout the period of the experiment, 134Cs and 137Cs concentrations in the animals' milk were measured daily with an 18% efficiency, high-resolution Ge detector. The data were in satisfactory agreement with the predictions of a simple two-compartment theory. The transfer coefficient, describing the steady-state equilibrium in this model, was measured as fm = 0.058 +/- 0.007 dL-1.

Transport of the radioisotopes iodine-131, cesium-134, and cesium-137 from the fallout following the accident at the Chernobyl nuclear reactor into cheesemaking products.

The transport of radiation contamination from milk to products of the cheese making process has been studied. The concentration of radioactive iodine and cesium in samples of sheep milk and cheese (Gruyère) products was measured for 10 consecutive production d. Milk with concentration 100 Bq/L in each of the radionuclides 131I, 134Cs, and 137Cs cheese with concentration 82.2 +/- 3.9 Bq/kg in iodine and an average of 42.3 +/- 2.3 Bq/kg in the cesium isotopes is produced. The corresponding concentrations in cream extracted from the same milk are 26.7 +/- 2.8 Bq/kg (131I) and 18.6 +/- 1.9 Bq/kg (134Cs, 137Cs).

Flow measurements with a high-speed computed tomography scanner.

A high-speed computed tomography (CT) scanner with a scan time of 50 ms was used to measure flow in a phantom constructed to simulate both tissue and vessels. After a bolus injection of iodinated contrast medium, the phantom was scanned at a rate of up to 2 images/s. A gamma-variate curve was fit to the time-density data obtained from the inlet and outlet, as well as from the tissue-equivalent part of the phantom. Flow was then calculated using different curves and curve parameters according to the Stewart-Hamilton equation, the mean transit time, and a modification of the Sapirstein principle. Actual flow rates were assessed by timed sampling. The results demonstrated that high-speed CT can measure flow accurately by all these methods. Application of high-speed CT for flow measurements in experimental animals and patients is, therefore, promising. The limitations of each technique for clinical application are discussed.