Ra–Po–Pb isotope systematics in waters of Sambhar Salt Lake,Rajasthan (India): geochemical characterization and particulate reactivity

The Sambhar Salt Lake hydrological system, including river waters, groundwaters, evaporating pans and sub-surface brines, has been analyzed for the salt content (TDS) and naturally occurring radionuclides (²¹⁰Po, ²¹⁰Pb and ^226,228Ra). The abundance of these radionuclides and their activity ratios show a wide variation in different hydrological regimes, which helps to geochemically characterize the lake system. A significantly lower Ra to total dissolved solids (TDS) ratio in the brines (by two to three orders of magnitude), when compared to the groundwaters and river waters, suggests removal of dissolved Ra by co-precipitation with Ca–Mg minerals at an early stage of the brine evolution. The concentration of Ra in evaporating lake/pan waters saturates at a value of about 35 Bq L⁻¹ over the salinity range of 100–370 g L⁻¹; attributable to its equilibration with the clay minerals. The two distinct regimes, saline lake system (lake water, evaporating pans and sub-surface brines) and groundwaters have been identified based on their differences in the distribution of ^226,228Ra isotopes. This observation points to the conclusion that the groundwaters and the lake brines are not intimately coupled in terms of their origin and evolution. The abundances of ²¹⁰Po and ²¹⁰Pb along with their activity ratios (²¹⁰Po/²¹⁰Pb) are markedly different among the surface lake waters/evaporating pans, sub-surface lake brines and groundwaters. These differences are explained in terms of different geochemical behaviour of these nuclides in presence of algae and organic matter present in these water regimes.     

Review of Russian language studies on radionuclide behaviour in agricultural animals: 3. Transfer to muscle

Over 150 publications reporting studies conducted in the former USSR were reviewed to provide transfer coefficients (F_f) to the muscle of domestic animals from experiments using chronic administration, often for long timescales in large scale experiments. Only a few of these studies were made available in the English language literature or taken into account in international reviews. The values derived have been compared with expected values reported by the IAEA's Handbook of parameter values for the prediction of radionuclide transfer in temperate environments (TRS 364) where possible. The information presented here has been used in the current updating of parameters recommended for environmental assessments by the IAEA. Many of the reported values are for Sr due to the Mayak accident and Cs due to the Chernobyl accident. Nevertheless, the reported data for a wide range of radionuclides, in particular for Ru, Sb, and Zn markedly improve the extent of available data.     

Americium,plutonium and uranium contamination and speciation in well waters,streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site,Kazakhstan

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that ²⁴¹Am, ^239,240Pu and ²³⁸U concentrations in well waters within the study area are in the range 0.04–87 mBq dm⁻³, 0.7–99 mBq dm⁻³, and 74–213 mBq dm⁻³, respectively, and for ²⁴¹Am and ^239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm⁻³, 0.08 mBq dm⁻³ and 0.32 mBq dm⁻³ for ²⁴¹Am, ^239,240Pu and ²³⁸U, respectively. The ²³⁵U/²³⁸U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.     

Radionuclide transfer to animal products: revised recommended transfer coefficient values

A compilation has been undertaken of data which can be used to derive animal product transfer coefficients for radionuclides, including an extensive review of Russian language information. The resultant database has been used to provide recommended transfer coefficient values for a range of radionuclides to (i) cow, sheep and goat milk, (ii) meat (muscle) of cattle, sheep, goats, pigs and poultry and (iii) eggs. The values are used in a new IAEA handbook on transfer parameters which replaces that referred to as ‘TRS 364’. The paper outlines the approaches and procedures used to identify and collate data, and assumptions used. There are notable differences between the TRS 364 ‘expected’ values and the recommended values in the revised Handbook from the new database. Of the recommended values, three milk values are at least an order of magnitude higher than the TRS 364 values (Cr, Pu (cow) Pu (sheep)) and one milk value is lower (Ni (cow)). For meat, four values (Am, Cd, Sb (beef) I (pork)) are at least an order of magnitude higher than the TRS 364 values and eight values are at least an order of magnitude lower (Ru, Pu (beef), Ru, Sr, Zn (sheep), Ru, Sr (pork), Mn (poultry)). Many data gaps remain.     

Deposition rates of unattached and attached radon progeny in room with turbulent airflow and ventilation

In this paper deposition rate coefficients for unattached and attached radon progeny were estimated according to a particle deposition model for turbulent indoor airflow described by Zhao and Wu [2006. Modeling particle deposition from fully developed turbulent flow in ventilation duct. Atmos. Environ. 40, 457–466]. The parameter which characterizes turbulent indoor airflow in this model is friction velocity, u*. Indoor ventilation changes indoor airflow and friction velocity and influences deposition rate coefficients. Correlation between deposition and ventilation rate coefficients in the room was determined. It was shown that deposition rate coefficient increases with ventilation rate coefficient and that these parameters of the Jacobi room model cannot be assumed to be independent. The values of deposition rate coefficients were presented as functions of friction velocity and ventilation rate coefficient. If ventilation rate coefficient varies from 0.1 up to 1 h⁻¹, deposition rate coefficients for unattached and attached fractions were estimated to be in the range 3–110 h⁻¹ and 0.015–0.35 h⁻¹, respectively.     

A review and test of predictive models for the bioaccumulation of radiostrontium in fish

Empirical relations between the ⁹⁰Sr concentration factor (CF) and the calcium concentration in freshwater aquatic systems have previously been determined in studies based on data obtained prior to the Chernobyl accident. The purpose of the present research is to review and compare these models, and to test them against a database of post-Chernobyl measurements from rivers and lakes in Ukraine, Russia, Belarus and Finland. It was found that two independently developed models, based on pre-Chernobyl empirical data, are in close agreement with each other, and with empirical data. Testing of both models against new data obtained after the Chernobyl accident confirms the models’ predictive ability. An investigation of the influence of fish size on ⁹⁰Sr accumulation showed no significant relationship, though the data set was somewhat limited.     

Exposure to inhaled THM: Comparison of continuous and event-specific exposure assessment for epidemiologic purposes

Trihalomethanes (THMs) (chloroform, bromoform, dibromochloromethane, and bromodichloromethane) are the most abundant by-products of chlorination. People are exposed to THMs through ingestion, dermal contact and inhalation. The objective of this study was to compare two methods for assessing THM inhalation: a direct method with personal monitors assessing continuous exposure and an indirect one with microenvironmental sampling and collection of time–activity data during the main event exposures: bathing, showering and swimming. This comparison was conducted to help plan a future epidemiologic study of the effects of THMs on the upper airways of children. 30 children aged from 4 to 10 years were included. They wore a 3M^™ 3520 organic vapor monitor for 7 days. We sampled air in their bathrooms (during baths or showers) and in the indoor swimming pools they visited and recorded their time–activity patterns. We used stainless steel tubes full of Tenax^® to collect air samples. All analyses were performed with Gas Chromatography and Mass Spectrometry (GC-MS). Chloroform was the THM with the highest concentrations in the air of both bathrooms and indoor swimming pools. Its continuous and event exposure measurements were significantly correlated (r_s = 0.69 p < 0.001). Continuous exposures were higher than event exposures, suggesting that the event exposure method does not take into account some influential microenvironments. In an epidemiologic study, this might lead to random exposure misclassification, thus underestimation of the risk, and reduced statistical power. The continuous exposure method was difficult to implement because of its poor acceptability and the fragility of the personal monitors. These two points may also reduce the statistical power of an epidemiologic study. It would be useful to test the advantages and disadvantages of a second sample in the home or of modeling the baseline concentration of THM in the home to improve the event exposure method.     

Radiological maps for Trabzon, Turkey

The activity concentrations and absorbed gamma dose rates due to primordial radionuclides and ¹³⁷Cs have been ascertained in 222 soil samples in 18 counties of the Trabzon province of Turkey using a HPGe detector. The mean activity concentrations of ²³⁸U, ²³²Th, ⁴⁰K and ¹³⁷Cs in soil samples were 41, 35, 437 and 21 Bq kg⁻¹, respectively. Based on the measured concentrations of these radionuclides, the mean absorbed gamma dose in air was calculated as 59 nGy h⁻¹ and hence, the mean annual effective dose due to terrestrial gamma radiation was calculated as 72 μSv y⁻¹. In addition, outdoor in situ gamma dose rate (D) measurements were performed in the same 222 locations using a portable NaI detector and the annual effective dose was calculated to be 66 μSv y⁻¹ from these results. The results presented in this study are compared with other parts of Turkey. Radiological maps of the Trabzon province were composed using the results obtained from the study.     

Effect of americium-241 on luminous bacteria. Role of peroxides

The effect of americium-241 (²⁴¹Am), an alpha-emitting radionuclide of high specific activity, on luminous bacteria Photobacterium phosphoreum was studied. Traces of ²⁴¹Am in nutrient media (0.16-6.67 kBq/L) suppressed the growth of bacteria, but enhanced luminescence intensity and quantum yield at room temperature. Lower temperature (4 °C) increased the time of bacterial luminescence and revealed a stage of bioluminescence inhibition after 150 h of bioluminescence registration start. The role of conditions of exposure the bacterial cells to the ²⁴¹Am is discussed. The effect of ²⁴¹Am on luminous bacteria was attributed to peroxide compounds generated in water solutions as secondary products of radioactive decay. Increase of peroxide concentration in ²⁴¹Am solutions was demonstrated; and the similarity of ²⁴¹Am and hydrogen peroxide effects on bacterial luminescence was revealed. The study provides a scientific basis for elaboration of bioluminescence-based assay to monitor radiotoxicity of alpha-emitting radionuclides in aquatic solutions.     

Sorption of selenate on soils and pure phases: kinetic parameters and stabilisation

This study was conducted to identify the principle selenate carrier phases for two selected soils, by comparing their reactivity with selenate to that of pure phases of the solids. Silica, calcium carbonate, aluminium hydroxide, goethite, bentonite and humic acid were selected as the main soil carrier phases. Comparisons were made first on the parameter values obtained with the best fit of a kinetic sorption model which can discriminate instantaneous sorption from kinetically limited sorption. Then comparisons were made of the ability for each solid to stabilise selenate by measuring the ratio of the partition coefficient for sorption (Kd_sorption) over that of the desorption (Kd_desorption). Kinetics and stabilisation were used to help elucidate the nature of interactions with the test solid phases for a large range of selenate concentrations. The experiments were conducted over 165 h in batch reactors, the solid being isolated from the solution by dialysis tubing, at two pH (5.4 and 8) and three selenate concentrations (1 × 10⁻³, 1 × 10⁻⁶ and 1 × 10⁻⁸ mol L⁻¹). The results obtained showed that only aluminium hydroxide can sorb selenate throughout the studied pH range (pH 5.4 to 8.0). The sorption capacity on this mineral was high (Kd_sorption > 100 to 1 × 10⁴ L kg⁻¹) and the selenate was mainly stabilized by the formation of inner sphere complexes. The sorption on goethite occurred at pH 5.4 (Kd_sorption 52 L kg⁻¹), mainly as outer sphere complexes, and was null at pH 8. On silica, a weak sorption was observed only at pH 5.4 and at 165 h (Kd_sorption 4 L kg⁻¹). On bentonite, calcium carbonate and humic acid no significant sorption was observed. Concerning the two soils studied, different behaviours were observed for selenate. For soil Ro (pH 5.4), Kd_sorption was low (8 L kg⁻¹) compared to soil Bu (pH 8) (70 L kg⁻¹). The sorption behaviour of selenate on soil Ro was mainly due to outer sphere complexes, as for goethite, whereas for soil Bu the sorption was mainly attributed to inner sphere complexes followed by reduction mechanisms, probably initiated by microorganisms, in which no steady state was reached at the end of the 165 h experiments. The sorption of selenate decreased when concentrations reached 1 × 10⁻³ mol L⁻¹, due to solid saturation, except for aluminium hydroxide. Reduction of selenate seemed also to occur on goethite and soil Ro, for the same concentration, but without preventing a decrease in sorption. Thus, this work shows that the comparison of selenate behaviour between soil and pure phases helps to elucidate the main carrier phases and sorption mechanisms in soil.