Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.     

A complimentary tool in the determination of activity concentrations of naturally occurring radionuclides

The determination of activity concentrations of radionuclides requires a reliable gamma spectrometry system, which also depends on the compulsory attainment of secular equilibrium amongst the progenies of the radionuclide of interest. This is often difficult to attain and hence a helium particle induced x-ray emission technique, not requiring the compulsory attainment of secular equilibrium, was used to determine the actual concentrations of the elemental content of tailings from the high background radiation tin mining area, Jos, Nigeria. The activity concentrations of the radionuclides of ⁴⁰K, ²³²Th and ²³⁸U were also calculated based on their elemental analyses, providing reliable information about the heads of uranium (²³⁸U) and thorium (²³²Th) series on the study area.     

Long-term investigation of anthropogenic and naturally occurring radionuclides at reference sites in western Sweden

In case of an accidental release of radioactive substances into the environment, it is important to quickly and reliably estimate the radiation dose received by people in the affected area, and to determine the extent of the contamination. Measurements of the extent of the release and the subsequent contamination can be facilitated if there are predetermined reference sampling sites with known background radiation and inventory of radionuclides. Since 1996, 34 reference sites for soil sampling, field gamma, and intensimeter measurements have been established in western Sweden. Time series data for dose rates and radioisotope inventory have been collected at these sites, allowing for the investigation of changes in these parameters over time. The mass activity densities for the uranium and thorium series elements varied approximately between 10 and 50 Bq/kg and between 10 and 40 Bq/kg, respectively. The mass activity density of ⁴⁰K was approximately in the range 300–800 Bq/kg. The radiation exposure due to ¹³⁷Cs was rather small in this area. The dose rates calculated from in situ measurement data showed that the contribution to the total dose rate was almost entirely due to naturally occurring radionuclides. The measured dose rate was about twice as high as the calculated rate, even after subtracting the contribution from cosmic radiation. This may be explained by the fact that intensimeters generally are calibrated to measure the quantity ambient dose equivalent, which should not underestimate the effective dose.     

Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Daily intakes of naturally occurring radioisotopes in typical Korean foods

The concentrations of naturally occurring radioisotopes ((232)Th, (228)Th, (230)Th, (228)Ra, (226)Ra, and (40)K) in typical Korean foods were evaluated. The daily intakes of these radioisotopes were calculated by comparing concentrations in typical Korean foods and the daily consumption rates of these foods. Daily intakes were as follows: (232)Th, 0.00-0.23; (228)Th, 0.00-2.04; (230)Th, 0.00-0.26; (228)Ra, 0.02-2.73; (226)Ra, 0.01-4.37 mBq/day; and (40)K, 0.01-5.71 Bq/day. The total daily intake of the naturally occurring radioisotopes measured in this study from food was 39.46 Bq/day. The total annual internal dose resulting from ingestion of radioisotopes in food was 109.83 muSv/y, and the radioisotope with the highest daily intake was (40)K. These values were same level compiled in other countries.     

Naturally occurring radionuclides in materials derived from urban water treatment plants in southeast Queensland, Australia

An assessment of radiologically enhanced residual materials generated during treatment of domestic water supplies in southeast Queensland, Australia, was conducted. Radioactivity concentrations of U-238, Th-232, Ra-226, Rn-222, and Po-210 in water, sourced from both surface water catchments and groundwater resources were examined both pre- and post-treatment under typical water treatment operations. Surface water treatment processes included sedimentation, coagulation, flocculation and filtration, while the groundwater was treated using cation exchange, reverse osmosis, activated charcoal or methods similar to surface water treatment. Waste products generated as a result of treatment included sediments and sludges, filtration media, exhausted ion exchange resin, backwash and wastewaters. Elevated residual concentrations of radionuclides were identified in these waste products. The waste product activity concentrations were used to model the radiological impact of the materials when either utilised for beneficial purposes, or upon disposal. The results indicate that, under current water resource exploitation programs, reuse or disposal of the treatment wastes from large scale urban water treatment plants in Australia do not pose a significant radiological risk.     

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.     

(238)U, (234)U, (226)Ra, (210)Po concentrations of bottled mineral waters in Italy and their dose contribution

Due to the importance of bottled mineral water in human diet with special regard to children in lactation period, a monitoring of natural radioactivity in some bottled mineral waters produced in Italy was performed. Gross alpha and beta activities and (226)Ra, (238)U, (234)U, and (210)Po concentrations were measured. Gross alpha and beta activities were determined by standards ISO 9696 and ISO 9697; for (226)Ra determination liquid scintillation was used. The (238)U and (234)U concentrations were determined by alpha spectrometry after their separation from matrix by extraction chromatography and electroplating. (210)Po was measured by alpha spectrometry. The results revealed that the concentrations (mBqL(-1)) of (226)Ra, (238)U, (234)U, and (210)Po ranged from <10.00 to 52.50, from <0.17 to 89.00, from <0.17 to 79.00, and from <0.04 to 21.01, respectively. Uranium and radium concentrations do not reach the relevant recommended derived activity concentration (DWC). For polonium concentration, none of the samples reaches the relevant DWC in the case of adults and children, but one sample exceeds this value for infants. The dose contribution for different classes of age was calculated using the dose coefficient factors reported by EC Directive 96/29 EURATOM and certain annual intake. For children and adult age class, the calculated doses are quite similar and lower than 0.1mSvy(-1); for infants (<1y) in three cases the calculated dose ranges from 0.11 to 0.17mSvy(-1).     

Distribution and correlation of the natural radionuclides in a coal mine of the West Macedonia Lignite Center (Greece)

The distribution and correlation of six natural nuclides in the West Macedonia Lignite Center, Northern Greece were studied. Fifty-five samples of lignite, aged from 1.8 to 5 million years, and corresponding steriles, beds of marls, clays and sands alternating with the lignite, were collected perpendicular to the mine benches and measured spectroscopically. The mean concentrations of (238)U and (226)Ra in lignites were found to be higher than that in steriles since these nuclides are associated with the organic material of lignite, whereas (238)U/(226)Ra equilibrium was not observed in either lignites or steriles. Finally, the ratio (226)Ra/(228)Ra in lignites was approximately double of that in steriles, confirming the affinity of the (238)U series with the coal matrix in contrast to the (232)Th series. No correlation was found between radionuclide concentrations and the depth of the sample, nor with the ash content of lignite.     

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 mine's 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.     

Radon (222Rn) level variations on a regional scale: influence of the basement trace element (U, Th) geochemistry on radon exhalation rates

The approach proposed in this study provides insight into the influence of the basement geochemistry on the spatial distribution of radon (222Rn) levels both at the soil/atmosphere interface and in the atmosphere. We combine different types of in situ radon measurements and a geochemical classification of the lithologies, based on 1/50,000 geological maps, and on their trace element (U, Th) contents. The advantages of this approach are validated by a survey of a stable basement area of Hercynian age, located in South Brittany (western France) and characterized by metamorphic rocks and granitoids displaying a wide range of uranium contents. The radon source-term of the lithologies, their uranium content, is most likely to be the primary parameter which controls the radon concentrations in the outdoor environment. Indeed, the highest radon levels (> or = 100 Bq m-3 in the atmosphere, > or = 100 mBq m-2 s-1 at the surface of the soil) are mostly observed on lithologies whose mean uranium content can exceed 8 ppm and which correspond to peraluminous leucogranites or metagranitoids derived from uraniferous granitoids.     

Liquid discharges from the use of radionuclides in medicine (diagnosis)

The production and discharge of liquid radioactive wastes as excreta from patients undergoing Nuclear Medicine Diagnostic (NMD) in a hospital were studied. Instantaneous and accumulated activity, discharged from the hospital to the sewage system, has been estimated keeping in mind radionuclide decay. This study would enable estimation of the environmental impact due to NMD procedures. Annual accumulated activities of 2.2GBq ((131)I), 1.847GBq ((99m)Tc), 0.743GBq ((123)I), 0.337GBq ((67)Ga), 0.169GBq ((111)In) and 0.033GBq ((201)Tl) result from our model when applied to a European hospital. A comparison is made with calculations by other authors that do not consider the radionuclide decay and who overestimate by two orders of magnitude. Doses to critical people as sewage treatment workers are also significantly reduced. So, our results stress the importance of including the decay in the calculations.     

Occurrence and behaviour of radionuclides in the Moselle River-Part II: Distribution of radionuclides between aqueous phase and suspended matter

Most of the radionuclides released from nuclear power plants ( NPPs) into rivers are primarily adsorbed onto suspended matter. To describe this nuclide transfer, a model was used which takes the total suspended matter load as solid phase into account. The necessary partition factors of various radionuclides were determined in river water/suspended matter of the Moselle in laboratory investigations. By use of this model, a conservative estimate of the radionuclide concentration of the solid phase could be obtained which proved to be more realistic than the results based on the distribution law.Furthermore, the influence of grain-size on the specific activity of single fractions of a Moselle sediment was demonstrated using ¹³⁷Cs, ¹⁰⁶Ru and ¹⁴⁴Ce from the Chernobyl nuclear accident as tracers. The grain-size pattern is considered to be a main factor which may seriously distort the determination of distribution coefficients and concentration factors that are needed in applying the model based on the distribution law.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Quantification of transfer of U, Ra, Th, K and Cs in mosses of a semi-natural ecosystem

There is a lack of appropriate data on transfer of some radionuclides on many terrestrial biota groups. To expand the available data concentration ratios of ²³⁸U, ²²⁶Ra, ²³²Th, ⁴⁰K and ¹³⁷Cs in mosses are presented in this paper. The relationship between concentration ratios of radionuclides and physicochemical characteristics of the underlying soil was also investigated. The data on concentration ratios obtained here will provide a useful addition to the currently used database of transfer parameters, particularly for natural radionuclides.     

Distribution and environmental impacts of some radionuclides in sedimentary rocks at Wadi Naseib area, southwest Sinai, Egypt

The present study examines the natural radioactivity in some sedimentary rocks and their associated environmental impacts at Wadi Naseib area. Exposure rate (ER), dose rate (DR), radium equivalent activity (Ra(eq)), external hazard index (H(ex)), internal hazard index (H(in)) and radioactivity level index (I(gamma)) were calculated. Wadi Naseib area is covered with sedimentary rocks of early to late Paleozoic age. These rocks are classified into two types: mineralized and non-mineralized sediments. The radiometric investigations revealed that uranium and thorium contents reached up to 710 and 520 ppm, respectively, in the mineralized rocks. This was attributed to the presence of some secondary uranium minerals. All sediments had low values of eTh and K content. The exposure and dose rates exceeded public permissible values in the mineralized sediments. Exposure and dose rates were within the safety range for workers and the public in the non-mineralized sediments. The expected environmental impacts may be low due to the limited occurrence of U-mineralization and corresponding areas for radiation exposure. Some precautions and recommendations were suggested to avoid any possible environmental impacts from areas and/or raw materials of high intensity of natural radiation sources.     

Diffusion of (226)Ra and (40)K radionuclides reproduced in underwater sedimentary columns in laboratory

The potential radiological impact of the increase of radioactive substances in the environment makes interesting the study of the migration of the contaminant radionuclides in soils and sediments, which are the last receiver system of these substances. By using a battery of sedimentary columns controlled in the laboratory, the diffusion of the (226)Ra and (40)K radionuclides has been studied, assessing their respective effective diffusion coefficients in a similar sedimentary medium. A decreasing temporal evolution is obtained, associated to the progressive 'fixation' of the radionuclides by the clay minerals of the sediment, followed by a constant tendency. A timescale of the 'fixation' by the sediment is determined, being of the order of days for (226)Ra and of the order of months for (40)K, so the progressive 'fixation' of (40)K by the clay minerals of the sediments is slower than in the case of (226)Ra.     

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.     

Predicting soil-to-plant transfer of radionuclides with a mechanistic model (BioRUR)

BioRUR model has been developed for the simulation of radionuclide (RN) transfer through physical and biological compartments, based on the available information on the transfer of their nutrient analogues. The model assumes that radionuclides are transferred from soil to plant through the same pathways as their nutrient analogues, where K and Ca are the analogues of Cs and Sr, respectively. Basically, the transfer of radionuclide between two compartments is calculated as the transfer of nutrient multiplied by the ratio of concentrations of RN to nutrient, corrected by a selectivity coefficient. Hydroponic experiments showed the validity of this assumption for root uptake of Cs and Sr and reported a selectivity coefficient around 1.0 for both. However, the application of this approach to soil-to-plant transfer raises some questions on which are the effective concentrations of RN and nutrient detected by the plant uptake mechanism. This paper describes the evaluation of two configurations of BioRUR, one which simplifies the soil as an homogeneous pool, and the other which considers that some concentration gradients develop around roots and therefore ion concentrations at the root surface are different from those of the bulk soil. The results show a good fit between the observed Sr transfer and the mechanistic simulations, even when a homogeneous soil is considered. On the other hand, Cs transfer is overestimated by two orders of magnitude if the development of a decreasing K profile around roots is not taken into account.     

Natural and anthropogenic radionuclides in airborne particulate samples collected in Barcelona (Spain)

Results for naturally occurring ⁷Be, ²¹⁰Pb, ⁴⁰K, ²¹⁴Bi, ²¹⁴Pb, ²¹²Pb, ²²⁸Ac and ²⁰⁸Tl and anthropogenic ¹³⁷Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The ²¹²Pb and ²⁰⁸Tl, ²¹⁴Bi and ²¹⁴Pb, ⁷Be and ²¹⁰Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The ⁷Be and ²¹⁰Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the ⁷Be, ²¹⁰Pb, ⁴⁰K and ¹³⁷Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.