Natural radionuclides in Austrian mineral water and their sequential measurement by fast methods

Ten samples of Austrian mineral water were investigated with regard to the natural radionuclides (228)Ra, (226)Ra, (210)Pb, (210)Po, (238)U and (234)U. The radium isotopes as well as (210)Pb were measured by liquid scintillation counting (LSC) after separation on a membrane loaded with element-selective particles (Empore Radium Disks) and (210)Po was determined by alpha-spectroscopy after spontaneous deposition onto a copper planchette. Uranium was determined by ICP-MS as well as by alpha-spectroscopy after ion separation and microprecipitation with NdF(3). From the measured activity concentrations the committed effective doses for adults and babies were calculated and compared to the total indicative dose of 0.1 mSv/a given in the EC Drinking Water Directive as a maximum dose. The dominant portion of the committed effective dose was due to the radium isotopes; the dose from (228)Ra in most samples clearly exceeded the dose from (226)Ra.     

Invariance of isotope ratios of lithogenic radionuclides: more evidence for their use as sediment source tracers

Activities of radionuclides in the 238U (230Th, 226Ra, 210Pb) and 232Th (232Th, 228Th, 228Ra) decay series were determined in sediments from an east Texas watershed and examined with isotope ratios and compared to particulate organic carbon (POC), % fines (<63 microm) and total concentrations of Al, Fe and Mn. The objective was to elucidate the presence or absence of relationships affecting the effectiveness of these radionuclides in modeling sediment transport. Strong positive correlations were observed between radionuclides and Mn (Th) and % fines (Ra and Th). Isotope ratios effectively reduce these influences, supporting the contention that isotope ratios offset extrinsic variability in terrestrial sediments. Strong associations of 210Pbxs (excess 210Pb) and 226Ra/230Th with POC agree with data from marine and terrestrial settings, indicating that the role of POC in isotope fractionation, transport and sequestration merits further investigation.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast

The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210Pb/226Ra and 234U/238U were 1.67, 1.22 and 1.0, respectively. The relationship between 226Ra/228Ra activity ratio and sample locations along the coastal shoreline indicates the increase of this ratio in the direction of the Shuqeir in the north and Safaga in the south where the oil exploration and phosphate mining activities are located. These activities may contribute a high flux of 226Ra. The concentration and distribution pattern of 226Ra in sediment can be used to trace the radiological impact of the non-nuclear industries on the Red Sea coast.     

Radiological impacts of natural radioactivity in Abu-Tartor phosphate deposits, Egypt.

Phosphate and environmental samples were collected from Abu Tartor phosphate mine and the surrounding region. The activity concentration of 226Ra (238U) series, 232Th series and 40K were measured using a gamma-ray spectrometer. The activities of uranium isotopes (238U, 235U and 234U) and 210Pb were measured using an alpha spectrometer and a low-background proportional gas counting system, respectively, after radiochemical separation. The results are discussed and compared with the levels in phosphate rocks from different countries. It seems that the Abu Tartor phosphate deposit has the lowest radioactivity level of exploited phosphate of sedimentary origin. 226Ra/238U, 210Pb/226Ra, 234U/238U and 226Ra/228Ra activity ratios were calculated and are discussed. The radioactivity levels in the surrounding region and the calculated exposure dose (nGy/h) will be considered as a pre-operational baseline to estimate the possible radiological impacts due to mining, processing and future phosphate industrial activities. To minimize these impacts, the processing wastes should be recycled to the greatest possible extent.     

Daily ingestion of 232Th, 238U, 226Ra, 228Ra and 210Pb in vegetables by inhabitants of Rio de Janeiro City

The concentrations of the naturally occurring radionuclides 232Th, 238U, 210Pb, 226Ra and 238Ra were determined in the vegetables (leafy vegetables, fruit, root, bean and rice) and derived products (sugar, coffee, manioc flour, wheat flour, corn flour and pasta) consumed most by the adult inhabitants of Rio de Janeiro City. A total of 88 samples from 26 different vegetables and derived products were analyzed. The highest contribution to radionuclide intake arises from bean, wheat flour, manioc flour, carrot, rice, tomato and potato consumption. The estimated daily intakes due to the consumption of vegetables and derived products are 1.9 mBq of 232Th (0.47 microg), 2.0 mBq of 238U (0.17 microg), 19 mBq of 236Ra, 26 mBq of 210Pb and 47 mBq of 228Ra. The estimated annual effective dose due to the ingestion of vegetables and their derived products with the long-lived natural radionuclides is 14.5 microSv. Taking into account literature data for water and milk from Rio de Janeiro the dose value increases to 29 microSv, with vegetables and derived products responsible for 50% of the dose and water for 48%. 210Pb (62%) and 228Ra (24%) were found to be the main sources for internal irradiation.     

Biomagnification of 7Be, 234Th, and 228Ra in marine organisms near the northern Pacific coast of Japan

Enrichment of natural radionuclides of thorium, radium and beryllium in several kinds of marine organisms was investigated near the Pacific coast of Miyagi Pref., Japan. The radioactivity of 7Be, 210Pb, 234Th, 238U, 228Ra and 137Cs was measured using gamma spectrometry. High concentrations of 234Th were observed in ascidian livers (50-400 Bq/kg dry) and excrement (2000-2900 Bq/kg dry), although the parent 238U concentrations were less than 3 Bq/kg dry. Such extreme disequilibrium between 238U and 234Th activity was observed in other organisms (barnacles, mussels and brown algae). Relatively high concentrations of 228Ra were detected in ascidian livers and were observed to decrease according to its half-life (5.75 year), suggesting disequilibrium with its parent 232Th. High concentrations (about 1900-5000 Bq/kg dry) of 7Be were detected in ascidian liver. Possible mechanisms for the observed biomagnification and bioaccumulation of these radionuclides in the organisms analyzed were proposed.     

The temporal variations of (7)Be, (210)Pb and (210)Po in air in England

We have conducted measurements of naturally occurring radionuclides (7)Be, (210)Pb and (210)Po in air at ground level at Chilton, Oxfordshire, England. The sampling and analysis regime for the latter two isotopes has been optimised to minimise uncertainties in measurement due to decay of (210)Po and in-growth of (210)Pb during the sampling and analysis period. Analysis times were reduced by using Cerenkov counting to assay the (210)Bi daughter of (210)Pb. Monthly data collected over a four-year period are presented and discussed. (7)Be activity concentrations appear to peak in spring. (210)Pb activity concentrations also follow a seasonal trend reflecting different (222)Rn emanation rates from soil during winter and summer. Data for (210)Po show no such trend.     

Distribution of (226)Ra-(210)Pb-(210)Po in marine biota and surface sediments of the Red Sea, Sudan

Activity concentration levels and ratios of (226)Ra, (210)Pb and (210)Po are presented in multicellular marine algae, molluscs, coral as well as in surface marine sediments collected from the shallower waters of the fringing reefs area extending towards north and south (Flamingo bay) of PortSudan harbour, Sudan. The analyses were performed adopting alpha-spectrometry, liquid scintillation and Cerenkov counting techniques. Surface sediments from this coastal region are poor in their radioactivity content in contrast to similar data reported from different coastal areas around the globe. There is surface enrichment of (210)Pb and (210)Po with respect to their progenitor (226)Ra as it is evident from the activity ratios of (210)Pb/(226)Ra (3.03+/-1.79) and (210)Po/(226)Ra (2.23+/-1.56). Among marine plants and animals investigated, the green algae species, Halimeda, and coral species, Favites, show substantial concentration of radium at 8.2Bq/kg and 21.9Bq/kg dry weight, respectively. Similarly, the highest concentration of (210)Po was met in Favites at 38.7Bq/kg followed by brown algae, Cystoseria sp., at 32.6Bq/kg. There is no variation seen among algal species for (210)Pb uptake, however, converse to radium and polonium, Favites (coral) was found to contain the minimum concentration of lead (3.88Bq/kg). In most species there is preferential accumulation of polonium over its parent radium as indicated by (210)Po:(226)Ra activity ratio with Cystoseria (brown algae) showing the highest value at 8.81. On the other hand, (210)Po:(210)Pb activity concentration ratio revealed that coral species Favites (9.97) and the brown algae Sargassum (1.85) have a greater tendency to accumulate (210)Po over (210)Pb, while in the rest of species; this ratio is less than unity.     

Distribution of natural radionuclides in the production and use of phosphate fertilizers in Brazil

The Brazilian phosphate fertilizer is obtained by wet reaction of igneous phosphate rock with concentrated sulphuric acid, giving as final product, phosphoric acid and dehydrated calcium sulphate (phosphogypsum) as by-products. Phosphoric acid is the starting material for triple superphosphate (TSP), single superphosphate (SSP), monoammonium phosphate (MAP) and diammonium phosphate (DAP). The phosphate rock used as raw material presents in its composition radionuclides of the U and Th natural series. Taking this into account, the main aim of this paper is to evaluate the fluxes of natural radionuclides and radioactive disequilibria involved in the Brazilian industrial process of phosphoric acid production; to determine the content of radioactivity in several commercial fertilizers produced by this industry; to estimate their radiological impact in crop soils and the long term exposure due to their application. Radiological characterization of phosphate rock, phosphogypsum and phosphate fertilizers was performed by alpha and gamma spectrometry. The fertilizer samples, which are derived directly from phosphoric acid, MAP and DAP, presented in their composition low activity concentrations for 226Ra, 228Ra and 210Pb. As for U and Th, the concentrations found in MAP and DAP are more significant, up to 822 and 850Bqkg(-1), respectively. SSP and TSP, which are obtained by mixing phosphoric acid with different amounts of phosphate rock, presented higher concentrations of radionuclides, up to 1158Bqkg(-1) for (238)U, 1167Bqkg(-1) for (234)U, 1169Bqkg(-1) for 230Th, 879Bqkg(-1) for 226Ra, 1255Bqkg(-1) for 210Pb, 521Bqkg(-1) for 232Th, 246Bqkg(-1) for 228Ra and 302Bqkg(-1) for 228Th. Long term exposure due to successive fertilizer applications was evaluated. Internal doses due to the application of phosphate fertilizer for 10, 50 and 100 years were below 1mSvy(-1), showing that the radiological impact of such practice is negligible.     

Concentration levels of 210Pb and 210Po in dry tobacco leaves in Greece

Tobacco leaves are large and have sticky exudates that retain the radon decay products once they deposit on the leaves. The study of 210Po in tobacco is required, because of the cumulative alpha-radiation dose delivered to humans from inhaled 210Po in cigarette smoke. 210Pb is the other element of interest since it is the 210Po precursor in the radioactive decay chain. In the present study, the concentrations of these two radionuclides were determined in tobacco samples from seven regions in Greece. 210Po was determined by alpha spectrometry using a surface barrier detector after radiochemical separation and spontaneous deposition of polonium on a nickel disk. The 210Pb activity in the samples was determined via the 210Po resulting from the decay of 210Pb. The results of the present study indicate that 210Po concentrations ranged from 3.6 to 17.0 mBqg(-1) (average 13.1 mBqg(-1)) of dry tobacco, while 210Pb concentrations ranged from 7.3 to 18.0 mBqg(-1) (average 13.4 mBqg(-1)). The mean value of the annual committed effective dose for smokers (20 cigarettes per day) of Greek tobacco was estimated to be 287 microSv (124 microSv from 210Po and 163 microSv from 210Pb). The inhalation dose for smokers is on average about 12 times higher than for non-smokers living in the mid-latitudes of the northern hemisphere.     

Radiological characteristics and investigation of the radioactive equilibrium in the ashes produced in lignite-fired power plants

Coal- and lignite-fired power plants produce significant amounts of ashes, which are quite often being used as additives in cement and other building materials. In many cases, coal and lignite present high concentrations of naturally occurring radionuclides, such as 238U, 226Ra, 210Pb, 232Th and 40K. During the combustion process, the produced ashes are enriched in the above radionuclides. The different enrichment of the various radionuclides within a radioactive series, such as that of 238U, results in the disturbance of radioactive secular equilibrium. An extensive research project for the determination of the natural radioactivity of lignite and ashes from Greek lignite-fired power plants is in progress in the Nuclear Engineering Department of the National Technical University of Athens (NED-NTUA) since 1983. This paper presents detailed results for the natural radioactivity, the secular radioactive equilibrium disturbance and the radon exhalation rate of the fly-ash collected at the different stages along the emission control system of a lignite-fired power plant as well as of the bottom-ash. From the results obtained so far, it may be concluded that 226Ra radioactivity of fly-ash in some cases exceeds 1 kBq kg(-1), which is much higher than the mean 226Ra radioactivity of surface soils in Greece (25 Bq kg(-1)). Furthermore, the radioactivity of 210Pb in fly-ash may reach 4 kBq kg(-1). These results are interpreted in relation to the physical properties of the investigated nuclides, the temperature in the flue-gas pathway, as well as the fly-ash grain size distribution. It is concluded that towards the coldest parts of the emission control system of the power plant, the radioactivity of some natural nuclides is gradually enhanced, secular radioactive equilibrium is significantly disturbed and the radon exhalation rate tends to increase.     

Natural radioactivity in Brazilian groundwater

More than 220 groundwater samples were analyzed for 228Ra, 226Ra, 222Rn, 210Pb, U(nat), Th(nat), pH, conductivity, fluoride and some additional elements determined by ICP-MS. Since samples from several Brazilian states were taken, involving areas with quite different geologies, no general trend was observed relating the chemical composition and the natural radionuclide content. On the other hand, 210Pb strongly depends on the water content of its progenitor, 222Rn. The values obtained during the present work were compared with those reported by Hainberger et al. [Hainberger, P.L., de Oliveira Paiva, I.R., Salles Andrade, H.A., Zundel, G., Cullen, T.L., 1974. Radioactivity in Brazilian mineral waters. Radiation Data and Reports, 483-488.], when more than 270 groundwater samples were analyzed, mainly, for 226Ra. Based on the results of both works, it was possible to build a database including the results of both works, generating a set with the radium content of circa 350 groundwater sources. It was demonstrated that 228Ra, 226Ra, 222Rn, 210Pb and U(nat) content in Brazilian groundwater follows a lognormal distribution and the obtained geometric mean were 0.045, 0.014, 57.7, 0.040 BqL(-1) and 1.2 microgL(-1), respectively.     

Characterization of the TE-NORM waste associated with oil and natural gas production in Abu Rudeis, Egypt

The present study was conducted to characterize the Technically Enhanced Naturally Occurring Radioactive Materials (TE-NORM) waste generated from oil and gas production. The waste was characterized by means of dry screening solid fractionation, X-ray analysis (XRF and XRD) and gamma-ray spectrometry. Sediment of the TE-NORM waste was fractionated into ten fractions with particle sizes varying from less than 100 microm to more than 3 mm. The results showed that the TE-NORM waste contains mainly radionuclides of the 238U, 235U and 232Th series. The mean activity concentrations of 226Ra (of U-series), 228Ra (of Th-series) and 40K in the waste samples before fractionation (i.e. 3 mm) were found to amount to 68.9, 24 and 1.3 Bq/g (dry weight), respectively. After dry fractionation, the activity concentrations were widely distributed and enriched in certain fractions. This represented a 1.48 and 1.82-fold enrichment of 226Ra and 228Ra, respectively, in fraction F8 (2.0-2.5 mm) over those in bulk TE-NORM waste samples. The activity ratios of 238U/226Ra, 210Pb/226Ra, 223Ra/226Ra and 228Ra/224Ra were calculated and evaluated. Activity of the most hazardous radionuclide 226Ra was found to be higher than the exemption levels established by IAEA [International Atomic Energy Agency, 1994. International Basic Safety Standards for the Protection against Ionizing Radiation and for the Safety of Radiation Sources. GOV/2715/94, Vienna]. The radium equivalent activity (Ra-eq), radon (222Rn) emanation coefficient (EC) and absorbed dose rate (Dgammar) were estimated and these are further discussed.     

Genotoxicity and toxicity assay of water sampled from a radium production industry storage cell territory by means of Allium-test

Water from natural reservoirs located near the radium production industry storage cell were analyzed using the anaphase-telophase chromosome aberration assay that was carried out on Allium schoenoprasum L. meristematic root tip cells. (262)Ra, (228)U, (232)Th, (210)Pb and (210)Po concentrations in all samples were found not to exceed the radioactivity concentration guides. The concentrations of 10 heavy metal ions were measured in water samples, but only Zn and Mn levels exceeded the maximum permissible concentration for the natural reservoirs. All water samples caused a significant increase of the chromosome aberration frequency as compared to control. The chromosome aberration spectrum analysis shows that the genotoxic effect was a result of chemical toxicity mainly. Two samples from the brook springhead were found to be toxic. The regression analysis results show that the mitotic index increased in parallel to Zn ion levels, and decreased with higher (238)U concentrations. The water samples genotoxicity positively correlated with the Zn concentration. The present work demonstrates that in order to achieve pollutant screening, it is not sufficient to determine the pollutants concentration only. Adequate conclusions on the risk due to environment contamination need to be based on the additional simultaneous use of toxicity and genotoxicity tests. When bioassays indicate some genotoxic and toxic effects, the determination of the chemical composition of the samples is then required. A combination of these two methods allows the identification of the elements that require constant biological monitoring. In the study reported here, those elements are Zn and (238)U.     

Radiological hazards of Narghile (hookah, shisha, goza) smoking: activity concentrations and dose assessment

Narghile (hookah, shisha, goza, "water-pipe") smoking has become fashionable worldwide. Its tobacco pastes, known as moassel and jurak, are not standardized and generally contain about 30-50% (sometimes more) tobacco, molasses/juice of sugarcane, various spices and dried fruits (particularly in jurak) and, in the case of moassel, glycerol and flavoring essences. Tobacco contains minute amounts of radiotoxic elements such as (210)Pb, (210)Po and uranium, which are inhaled via smoking. Only very few data have been published on the concentrations of natural radionuclides in narghile tobacco mixtures. Consequently, the aim of this study was to draw first conclusions on the potential hazards of radioactivity in moassel tobacco in relation to narghile smoking. The results indicate the existence of a wide range in the radioactivity contents where the average (range) activity concentrations of (238)U, (234)Th (226)Ra, (210)Pb, (210)Po, (232)Th and (40)K, in Bq/kg dry weight were 55 (19-93), 11 (3-23), 3 (1.2-8), 14 (3-29), 13 (7-32), 7 (4-10) and 719 (437-1044)Bq/kg dry weight, respectively. The average concentrations of natural radionuclides in moassel tobacco pastes are comparable to their concentration in Greek cigarettes and tobacco leaves, and lower than that of Brazilian tobacco leaves. The distribution pattern of these radionuclides after smoking, between smoke, ash and filter, is unknown, except for (210)Po during cigarette smoking and from one existing study during moassel smoking. Radiological dose assessment due to intake of natural radionuclides was calculated and the possible radio-toxicity of the measured radionuclides is briefly discussed.     

Evaluation of 210Pb and 210Po in cigarette tobacco produced in Brazil

Cigarette smoking is one of the pathways that might contribute significantly to the increase in the radiation dose reaching man, due to the relatively large concentrations of 210Pb and 210Po found in tobacco leaves. In the present study, the concentrations of these two radionuclides were determined in eight of the most frequently sold cigarette brands produced in Brazil. 210Pb was determined by counting the beta activity of 210Bi with a gas flow proportional detector after radiochemical separation and precipitation of PbCrO4. 210Po was determined by alpha spectrometry using a surface barrier detector after radiochemical separation and spontaneous deposition of Po on a copper disk. The results showed concentrations ranging from 11.9 to 30.2 mBq per gram of dry tobacco for 210Pb and from 10.9 to 27.4 mBq per gram of dry tobacco for 210Po. The collective committed effective dose resulting from the use of cigarettes produced in Brazil per year is estimated to be 1.5 x 10(4) man-Sv.     

Direct comparison of 210Po, 234Th and POC particle-size distributions and export fluxes at the Bermuda Atlantic Time-series Study (BATS) site

Particle-reactive, naturally occurring radionuclides are useful tracers of the sinking flux of organic matter from the surface to the deep ocean. Since the Joint Global Ocean Flux Study (JGOFS) began in 1987, the disequilibrium between ²³⁴Th and its parent ²³⁸U has become widely used as a technique to measure particle export fluxes from surface ocean waters. Another radionuclide pair, ²¹⁰Po and ²¹⁰Pb, can be used for the same purpose but has not been as widely adopted due to difficulty with accurately constraining the ²¹⁰Po/²¹⁰Pb radiochemical balance in the ocean and because of the more time-consuming radiochemical procedures. Direct comparison of particle flux estimated in different ocean regions using these short-lived radionuclides is important in evaluating their utility and accuracy as tracers of particle flux. In this paper, we present paired ²³⁴Th/²³⁸U and ²¹⁰Po/²¹⁰Pb data from oligotrophic surface waters of the subtropical Northwest Atlantic and discuss their advantages and limitations. Vertical profiles of total and particle size-fractionated ²¹⁰Po and ²³⁴Th activities, together with particulate organic carbon (POC) concentrations, were measured during three seasons at the Bermuda Atlantic Time-series Study (BATS) site. Both ²¹⁰Po and ²³⁴Th reasonably predict sinking POC flux caught in sediment traps, and each tracer provides unique information about the magnitude and efficiency of the ocean's biological pump.     

Source of radium in a well-water-augmented Florida lake

A study of the lake waters of Saddleback Lake, Florida was undertaken with the goal of determining the source of elevated radium activities in the lake. Four radium isotopes, (226)Ra, (228)Ra, (223)Ra and (224)Ra, were measured and activities of all the four radium isotopes were substantially greater in the well water used to augment the lake as compared to the lake waters. In the surface water, radium activities were highest close to the well used for augmentation in the initial sampling. Activities initially decreased with time after augmentation from the well ceased. The (223)Ra/(226)Ra activity ratio decreased during the first month of sampling and closely followed an exponential decay curve based on the (223)Ra decay constant. Trends in the activities and the (223)Ra/(226)Ra activity ratios support the conclusion that the well used to augment the lake was the dominant source of (223)Ra and (226)Ra to Saddleback Lake during this study. The (224)Ra/(226)Ra activity ratio did not follow the expected trend of exponential decay based on the (224)Ra decay constant. While the augmentation well supplied some (224)Ra, these results suggest that there must be an additional source of (224)Ra to the lake. The most likely additional source of (224)Ra appears to be the ingrowth of (224)Ra on the sediment within the lake from (228)Ra (via (228)Th).     

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.