J.C. Lozano

Soil-to-plant transfer factors for natural radionuclides and stable elements in a Mediterranean area

The transfer factors (TF) for natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 228Th), and 226Ra were obtained in plant samples (grass-pasture) growing in granitic and alluvial soils around a disused uranium mine located in the Extremadura region in the south-west of Spain. Affected and non-affected areas of the mine presented large differences in the activity concentrations of radionuclides of the uranium series. We also determined transfer factors for several stable elements (essential and non-essential). A set of statistical tests were applied to validate the data. The results showed that the transfer factors for both the natural radionuclides and the stable elements are independent of the two substrate types involved and also of the two areas considered in the study.

About the assumption of linearity in soil-to-plant transfer factors for uranium and thorium isotopes and 226Ra

The linearity assumption for soil and plant concentrations of radionuclides is usually a good approximation for use in food-chain models. To verify this assumption, different samples of plant and substrate were collected from a granitic zone located near a disused uranium mine in order to cover a large range of concentrations. In all of the samples, the activity concentration of 226Ra and of different isotopes of uranium (238U and 234U) and thorium (232Th, 230Th and 228Th) were determined. The results indicate that the linearity assumption can be considered valid when the range of concentrations taken into account is large (approx. two orders of magnitude). Otherwise, there is a clear deviation from linearity. Also, the influence of different stable elements on the soil-plant transfer factors was studied by using multivariate regression methods. The uptake of uranium, thorium and radium was found to be mainly associated with the concentration of iron in the plant and the phosphorus and alkaline earths in the substrate.

Distribution and mobilization of U, Th and 226Ra in the plant-soil compartments of a mineralized uranium area in south-west Spain.

The activity concentrations of natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 225Th) and 226Ra were studied in soil and vegetation samples from a disused uranium mine located in the Extremadura region in the south-west of Spain. The results allowed us to characterize radiologically the area close to the installation and one affected zone was clearly manifest as being dependent on the direction of the surface water flow from the mine. The activity concentration mean values (Bq/kg) in this zone were: 10,924, 10,900, 10,075 and 5,289 for 238U, 234U, 230Th and 226Ra, respectively, in soil samples and 1,050, 1,060, 768 and 1,141 for the same radionuclides in plant samples. In an unaffected zone, the activity concentration mean values (Bq/kg) were: 184, 190, 234 and 7251 for 235U, 234U, 230Th and 226Ra, respectively, in soil samples and 28. 29, 31 and 80 in plant samples. The activity concentrations obtained for 232Th and 228Th showed that the influence of the mine was only important for the uranium series radionuclides. The relative radionuclide mobilities were determined from the activity ratios. Correlations between radionuclide activity concentrations and stable element concentrations in the soil samples helped to understand the possible distribution paths for the natural radionuclides.

Distribution of long-lived radionuclides of the 238U series in the sediments of a small river in a uranium mineralized region of Spain

A study is presented on the distribution and mobilization of the natural U isotopes (238U and 234U), 230Th, and 226Ra in the sediments of a small river crossing an uranium mineralized zone where a disused uranium mine is located. Due to the preferential directions for surface run-off waters and to the mines situation, one sampling point along the river bed was identified as a point of accumulation of radionuclides. The average values of the activity concentrations (Bq/kg) in this sediment sample were 5,025, 5,055, 5,915 and 1,694 for 238U, 234U, 230Th and 226Ra, respectively, while the respective average values of the activity concentrations (Bq/kg) for the sediment sample considered to give the background level were 125, 124, 131 and 370. Isotopic ratios between the descendants of 238U served to clarify some paths of distribution, involving the soils nearest to the sampling points and the location of these points with respect to the disused mine. The differences in behaviour found between the uranium, thorium and radium isotopes were associated to the mobility of these radionuclides in the fluvial system studied. Correlations between the radionuclide activity concentration ratios and stable element concentrations in the sediment samples were also investigated.

Determination of radium isotopes by BaSO4 coprecipitation for the preparation of alpha-spectrometric sources

A coprecipitation procedure for the preparation of α-spectrometric sources for radium, using BaSO4 as carrier, has been applied to the determination of alpha radium isotopes in water samples. The use of133Ba as a suitable tracer for radium determination and possible losses of radon isotopes from the sources are studied and discussed.

The ability of Helianthus annuus L. and Brassica juncea to uptake and translocate natural uranium and 226Ra under different milieu conditions.

Seedlings of Helianthus annuus L. (HA) and Brassica juncea (BJ) were used to test the effect of the pH, the presence of phosphates, and the addition of ethylene-diamine-tetraacetic acid (EDTA) or citrate on the uptake and the translocation of uranium isotopes ((238)U, (235)U, and (234)U) and (226)Ra. The results indicated that the presence of phosphates generally reduces the uptake and transfer of uranium from the roots to the shoots of HA. In the case of BJ, while phosphate enhanced the retention of uranium by roots, the translocation was poorer. Likewise, for (226)Ra, the best translocation was in the absence of phosphates for both species. The addition of citrate increased the translocation of uranium for both species, but had no clear effect on the transfer of (226)Ra. The effect of EDTA was much more moderate both for uranium and for (226)Ra, and for both plant species. Only noticeable was a slightly better uptake of (226)Ra by BJ at neutral pH, although the translocation was lower.

DETERMINATION OF 222RN AND 226RA IN AQUEOUS SAMPLES USING A LOW-LEVEL LIQUID SCINTILLATION COUNTER

Abstract A method for measuring 222 Rn and 226 Ra in aqueous samples has been studied. The technique uses low-level liquid scintillation counting from vials containing an insoluble high efficiency mineral oil scintillation cocktail. A Wallac 1220 TM Quantulus LS counter was used for all the experiments. The optimum pulse-shape discrimination value was evaluated by using the minimum detectable activity criterion for each condition of measurement. Experiments on the optimum volume and sample-cocktail ratio, the influence of shaking, type of vial and diffusion of radon from vials were carried out. The study was applied to the determination of very low levels of 222 Rn and 226 Ra from aqueous environmental samples. The results reached using this method were very satisfactory and even better than from other more laborious procedures.

Influence of soil texture on the distribution and availability of 238U, 230Th, and 226Ra in soils

The influence of soil texture on the distribution and availability of (238)U, (230)Th, and (226)Ra in soils was studied in soil samples collected at a rehabilitated uranium mine located in the Extremadura region in south-west Spain. The activity concentration (Bqkg(-1)) in the soils ranged from 60 to 750 for (238)U, from 60 to 260 for (230)Th, and from 70 to 330 for (226)Ra. The radionuclide distribution was determined in three soil fractions: coarse sand (0.5-2mm), medium-fine sand (0.067-0.5mm), and silt and clay (<0.067 mm). The relative mobility of the natural radionuclides in the different fractions was studied by comparison of the activity ratios between radionuclides belonging to the same radioactive series. The lability of these radionuclides in each fraction was also studied through selective extraction from the soils using a one-step sequential extraction scheme. Significant correlations were found for (238)U, (230)Th, and (226)Ra between the activity concentration per fraction and the total activity concentration in the bulk soil. Thus, from the determination of the activity concentration in the bulk soil, one could estimate the activity concentration in each fraction. Correlations were also found for (238)U and (226)Ra between the labile activity concentration in each fraction and the total activity concentration in bulk soil. Assuming that there is some particle-size fraction that predominates in the process of soil-to-plant transfer, the parameters obtained in this study should be used as correction factors for the transfer factors determined from the bulk soil in previous studies.

Enhancing radium solubilization in soils by citrate, EDTA, and EDDS chelating amendments.

The effect of three chelating agents (citrate, EDTA, and EDDS) on the solubilization of radium from a granitic soil was studied systematically, considering different soil pH values, chelating agent concentrations, and leaching times. For all the chelating agents tested, the amount of radium leached proved to be strongly dependent on the pH of the substrate: only for acidic conditions did the amount of radium released increase significantly relative to the controls. Under the best conditions, the radium released from the amended soil was greater by factors of 20 in the case of citrate, 18 for EDTA, and 14 for EDDS. The greatest improvement in the release of radium was obtained for the citrate amendment at the highest concentration tested (50 mmol kg(-1)). A slightly lower amount of radium was leached with EDTA at 5 mmol kg(-1) soil, but the solubilization over time was very different from that observed with citrate or EDDS. With EDTA, a maximum in radium leaching was reached on the first day after amendment, while with citrate, the maximum was attained on the fourth day. With EDDS, radium leaching increased slightly but steadily with time (until the sixth day), but the net effect for the period tested was the lowest of the three reagents.

Elimination of natural uranium and 226Ra from contaminated waters by rhizofiltration using Helianthus annuus L.

The elimination of natural uranium and (226)Ra from contaminated waters by rhizofiltration was tested using Helianthus annuus L. (sunflower) seedlings growing in a hydroponic medium. Different experiments were designed to determine the optimum age of the seedlings for the remediation process, and also to study the principal way in which the radionuclides are removed from the solution by the sunflower roots. In every trial a precipitate appeared which contained a major fraction of the natural uranium and (226)Ra. The results indicated that the seedlings themselves induced the formation of this precipitate. When four-week-old seedlings were exposed to contaminated water, a period of only 2 days was sufficient to remove the natural uranium and (226)Ra from the solution: about 50% of the natural uranium and 70% of the (226)Ra were fixed in the roots, and essentially the rest was found in the precipitate, with only very small percentages fixed in the shoots and left in solution.