Natural radionuclides in bottled water in Austria

Concentration levels of 226Ra, 222Rn and 210Pb were analyzed in domestic bottled waters commercially available in Austria. Concentrations up to 0.23 Bq/l, with a geometric mean of 0.041 Bq/l were found for 226Ra. Concentrations for 222Rn ranged from <0.12-18 Bq/l, the geometric mean being 0.54 Bq/l. Lead-210 was analyzed in selected samples, the concentrations ranging from <2 to 34 mBq/l, with a geometric mean of 4.7 mBq/l. Ingestion doses resulting from consumption of these waters were calculated for the geometric mean and the maximum concentrations of the three radionuclides. The effective dose equivalents for different age groups of the population due to the intake of 226Ra range from 0.001 to 0.22 mSv/y and of 210Pb from 0.0003 to 0.05 mSv/y. Ingestion doses from 222Rn are low compared to those from 226Ra and 210Pb, ranging from 0.0001 to 0.011 mSv/y for adults and children, respectively. The doses are compared to the total ingestion dose from dietary intake of natural radionuclides on an annual basis.     

Natural radionuclides in drinking water supplies of São Paulo State, Brazil and consequent population doses

The activity concentrations of 228Ra, 226Ra and 222Rn have been analysed in 452 drinking water supplies of S?o Paulo State. This study started in 1994 and covered 54% of the 574 existing counties. Concentrations up to 235 and 131 mBq l-1 were observed for 226Ra and 228Ra, respectively, whereas 222Rn concentrations reached 315 Bq l-1. Radiation doses up to 0.3, 0.6 and 3.2 mSv yr-1 were estimated for the critical organs, for the ingestion of 226Ra, 226Ra and 222Rn, respectively. The corresponding committed effective doses reached values of 6 x 10(-3), 2 x 10(-2) and 3 x 10(-1) mSv yr-1, for the same radionuclides. These results indicate that 222Rn makes the highest contribution to the total effective dose.     

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.     

Natural radioactivity in the scale of water well pipes

The natural radioactivity of 226Ra and 228Ra in scale samples taken from pipes used in several local water wells was investigated. The results showed 226Ra activities to be varying from 1284 to 3613 Bq/kg whereas, the 228Ra concentrations did not show any significant variation, all being low, below 30 Bq/kg. The 222Rn exhalations from these scale samples were also measured and compared with the 226Ra contents. The average ratio of 222Rn/226Ra was 31%. Chemical analyses showed that the main constituent of the scale samples was iron. The radiation dose rates from the pipes and scale were up to 100nSv/h. Although not a major hazard this could present a long-term risk if the scale materials were handled indiscriminately.     

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.     

A study on natural radiation exposure in different realistic living rooms

In the first part of the paper, the factors affecting 222Rn properties in 25 different realistic living rooms (with low ventilation rates) of different houses in El-Minia City (Upper Egypt) have been studied; they included the activity concentration of 222Rn gas (C(o)), the unattached fraction (f(p)) of 218Po and 214Pb, the unattached potential alpha energy concentration (PAEC) and the equilibrium factor (F). The activity distributions of unattached 218Po and 214Pb as well as for the PAEC were determined. With a dosimetric model calculation [ICRP, 1994b. Human Respiratory Tract Model For Radiological Protection. Pergamon Press, Oxford. ICRP Publication 66] the total deposition fraction of unattached 218Po and 214Pb in human respiratory tract was evaluated to determine the total equivalent dose. An electrostatic precipitation method and a wire screen diffusion battery technique were both employed for the determination of 222Rn gas concentration and its unattached decay products, respectively. The mean activity concentration of 222Rn gas (C(o)) was found to be 110+/-20 Bq m(-3). The mean unattached activity concentrations of 218Po and 214Pb were found to be 0.6 and 0.35 Bq m(-3), respectively. A mean unattached fraction (f(p)) of 0.09+/-0.01 was obtained at a mean aerosol particle concentration (Z) of (2.9+/-0.23) x 10(3)cm(-3). The mean equilibrium factor (F) was determined to be 0.31+/-0.02. The mean PAEC of unattached 218Po and 214Pb was found to be 8.74+/-2.1 Bq m(-3). The activity distributions of 218Po and 214Pb show mean activity median diameters (AMD) of 1.5 and 1.85 nm with mean geometric standard deviations (SD) of 1.33 and 1.45, respectively. The mean activity distribution of the PAEC shows an AMD of 1.65 nm with a geometric standard deviation of 1.25. At a total deposition fraction of about 97% the total equivalent dose to the lung was determined to be about 133 microSv. The second part of this paper deals with a study of natural radionuclide contents of samples collected from the building materials of the rooms under investigations in part one. Analyses were performed in Marinelli beakers with a gamma multichannel analyzer equipped with a NaI(Tl) detector. The samples revealed the presence of the uranium-radium and thorium radioisotopes as well as 40K. Nine gamma-lines of the natural radioisotopes corresponding to 212Pb, 214Pb, 214Bi, 228Ac, 40K and 208Tl were detected and measured. The activity concentrations of 226Ra, 232Th and 40K were determined with mean activity concentrations of 58+/-19, 31+/-11 and 143+/-62 Bq kg(-1), respectively. These activities amount to a radium equivalent (Ra(eq)) of 113 Bq kg(-1) and to a mean value of external hazard index of 0.31.     

Doses from 222Rn, 226Ra, and 228Ra in groundwater from Guarani aquifer, South America

Groundwater samples were analysed for 222Rn, 226Ra, and 228Ra in Guarani aquifer spreading around 1 million km2 within four countries in South America, and it was found that their activity concentrations are lognormally distributed. Population-weighted average activity concentration for these radionuclides allowed to estimate a value either slightly higher (0.13 mSv/year) than 0.1 mSv for the total effective dose or two times higher (0.21 mSv/year) than this limit, depending on the choice of the dose conversion factor. Such calculation adds useful information for the appropriate management of this transboundary aquifer that is socially and economically very important to about 15 million inhabitants living in Brazil, Argentina, Uruguay and Paraguay.     

A study of the technologically modified sources of 222Rn and its environmental impact in an Indian U mineralised belt

These investigations present qualitative and quantitative assessments of the 222Rn contributing potential of the technologically modified sources, e.g. mine exhausts and tailings piles, arising due to the mining and processing of uraniferous minerals at Jaduguda, India. The overall geometric mean of the 222Rn flux from low-grade uranium (U) mill tailings being 1.19 Bq m-2 s-1, requisite attenuation of 37.8% to the recommended limit of 0.74 Bq m-2 s-1 can be attained by a typical clay coverage of 20 cm. Theoretically, feasible options for selection of overburden materials for stabilisation of the tailings piles are examined. Extrapolation studies with a turbulent diffusion model yield an atmospheric dispersion pattern of 222Rn in reasonable correspondence with the prevailing concentrations, especially for locations beyond a 4 km radius. The overall 222Rn contribution of the U complex to the ambient air is the same as that contributed by the adjoining land mass of 2.75 km radius in this mineralised terrain.     

Simultaneous measurement of (226)Ra and (228)Ra in natural water by liquid scintillation counting

Several types of bottled drinking water originating from three different areas in Egypt are studied through measurement of radium activity, assessment of related annual dose for adults and finally to define the role of water quality on radium levels. The mean levels of (226)Ra activity range from 0.44 to 0.92 Bq/L and the mean levels of (228)Ra from 0.30 to 0.78 Bq/L, with related (226)Ra/(228)Ra ratios ranging from 2.61 to 0.56. Water types originating from the Eastern Nile Delta area are characterized by low (226)Ra levels and relatively high (228)Ra activity, presumably due to the muddy agricultural nature of this area, which is subject to water from several surface resources for irrigation. In general, the mean activity levels for both (226)Ra and (228)Ra are within those in drinking water in several other countries and the annual ingested dose is comparable with the typical range reported by UNSCEAR. Also, the effect of TDS, pH, calcium, bicarbonate, sulphate and chloride ion concentrations on radium levels is studied and discussed.     

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.     

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.     

Present status of 222Rn in groundwater in Extremadura

Radon-222 was measured in groundwater sources of Extremadura (Spain), analyzing 350 samples from private and public springs, wells, and spas by liquid scintillation counting (LSC) and gamma spectrometry. The (222)Rn activity concentrations ranged from 0.24 to 1168BqL(-1). The statistical analysis showed a log-normal distribution with a mean of (111+/-7)BqL(-1) and a median of (36+/-3)BqL(-1). A hydrogeological study revealed correlations between the activity concentration and the aquifer material's characteristics. A map of (222)Rn in groundwater was elaborated and compared with the natural gamma radiation map for this region. About 35% of the samples showed (222)Rn activity concentrations above the Euratom recommended limit of 100BqL(-1). Three uranium series radionuclides ((238)U, (234)U, and (226)Ra) were also assayed by alpha-particle spectrometry, estimating the annual effective dose due to the presence of these natural radionuclides in drinking water.     

Seasonal variation of Ra/Ra ratio in seaweed: implications for water circulation patterns in coastal areas of the Noto Peninsula, Japan

To examine water circulation patterns of coastal water, 72 seaweed (Sargasso) samples and 27 coastal water samples were collected from coastal areas of the Noto Peninsula, Japan, during the period from December 1998 to June 2002. The (228)Ra and (226)Ra activities of those samples were measured by low-background gamma-ray spectrometry. There was a wide range of activities of (228)Ra (0.5-2Bq/kg-fresh) and (226)Ra (0.5-1.2Bq/kg-fresh) in the Sargasso samples. The (228)Ra/(226)Ra activity ratio of Sargasso samples exhibited seasonal variation with minimum values in June ((228)Ra/(226)Ra= approximately 1) and maximum values in December (1.5-2.5), which was mainly governed by changes in (228)Ra activity. It is also notable that the seasonal variation of the (228)Ra/(226)Ra ratio of Sargasso is in approximate agreement with that of the ambient coastal water. Sargasso samples appear to have retained the (228)Ra/(226)Ra ratio of the ambient coastal waters, and the temporal variations in that ratio provide insight into seasonal changes in water circulation in the Noto Peninsula coastal area.     

Natural radioactivity measurements in the city of Ptolemais (Northern Greece)

Specific activities of the natural radionuclides (238)U, (226)Ra, (232)Th and (40)K were measured by means of gamma-ray spectrometry in surface soil samples collected from the city of Ptolemais, which is located near lignite-fired power plants. The mean activity values for (238)U, (226)Ra, (232)Th and (40)K were found to be 42+/-11, 27+/-6, 36+/-5 and 496+/-56 Bq kg(-1), respectively. These values fall within the range of typical world and Greek values for soil. The indoor radon concentration levels, which were also measured in 66 dwellings by means of SSNTD, ranged from 12 to 129 Bq m(-3), with an average value of 36+/-2 Bq m(-3). This value is close to world and Greek average values for indoor radon concentrations. The total effective dose due to outdoor external irradiation of terrestrial origin and to indoor internal irradiation from the short-lived decay products of (222)Rn was estimated to be 1.2 mSv y(-1) for adults, which is lower than the global effective dose due to natural sources of 2.4 mSv y(-1).     

Seasonal variation of 228Ra/226Ra ratio in seaweed: implications for water circulation patterns in coastal areas of the Noto Peninsula, Japan

To examine water circulation patterns of coastal water, 72 seaweed (Sargasso) samples and 27 coastal water samples were collected from coastal areas of the Noto Peninsula, Japan, during the period from December 1998 to June 2002. The (228)Ra and (226)Ra activities of those samples were measured by low-background gamma-ray spectrometry. There was a wide range of activities of (228)Ra (0.5-2Bq/kg-fresh) and (226)Ra (0.5-1.2Bq/kg-fresh) in the Sargasso samples. The (228)Ra/(226)Ra activity ratio of Sargasso samples exhibited seasonal variation with minimum values in June ((228)Ra/(226)Ra= approximately 1) and maximum values in December (1.5-2.5), which was mainly governed by changes in (228)Ra activity. It is also notable that the seasonal variation of the (228)Ra/(226)Ra ratio of Sargasso is in approximate agreement with that of the ambient coastal water. Sargasso samples appear to have retained the (228)Ra/(226)Ra ratio of the ambient coastal waters, and the temporal variations in that ratio provide insight into seasonal changes in water circulation in the Noto Peninsula coastal area.     

Natural radioactivity measurements in building materials in Southern Lebanon

Using gamma-spectroscopy and CR-39 detector, concentration C of naturally occurring radioactive nuclides (226)Ra, (222)Rn, (214)Bi, (228)Ac, (212)Pb, (212)Bi and (40)K, has been measured in sand, cement, gravel, gypsum, and paint, which are used as building materials in Lebanon. Sand samples were collected from 10 different sandbank locations in the southern part of the country. Gravel samples of different types and forms were collected from several quarries. White and gray cement fabricated by Shaka Co. were obtained. gamma-spectroscopy measurements in sand gave Ra concentration ranging from 4.2+/-0.4 to 60.8+/-2.2 Bq kg(-1) and Ra concentration equivalents from 8.8+/-1.0 to 74.3+/-9.2 Bq kg(-1). The highest Ra concentration was in gray and white cement having the values 73.2+/-3.0 and 76.3+/-3.0 Bq kg(-1), respectively. Gravel results showed Ra concentration between 20.2+/-1.0 and 31.7+/-1.4 Bq kg(-1) with an average of 27.5+/-1.3 Bq kg(-1). Radon concentration in paint was determined by CR-39 detector. In sand, the average (222)Rn concentration ranged between 291+/-69 and 1774+/-339 Bq m(-3) among the sandbanks with a total average value of 704+/-139 Bq m(-3). For gravel, the range was found to be from 52+/-9 to 3077+/-370 Bq m(-3) with an average value of 608+/-85 Bq m(-3). Aerial and mass exhalation rates of (222)Rn were also calculated and found to be between 44+/-7 and 2226+/-267 mBq m(-2)h(-1), and between 0.40+/-0.07 and 20.0+/-0.3 mBq kg(-1)h(-1), respectively.     

222Rn and 220Rn concentrations in soil gas of Karkonosze-Izera Block (Sudetes, Poland)

Soil gas 222Rn and 220Rn concentrations were measured at 18 locations in the Karkonosze-Izera Block area in southwestern Poland. Measurements were carried out in surface air and at sampling depths of 10, 40 and 80 cm. Surface air 222Rn concentrations ranged from 4 to 2160 Bq m(-3) and 220Rn ranged from 4 to 228 Bq m(-3). The concentrations for 10 and 40 cm varied from 142 Bq m(-3) to 801 kBq m(-3) and 102 Bq m(-3) to 64 kBq m(-3) for 222Rn and 220Rn, respectively. At 80 cm 222Rn concentrations ranged from 94 Bq m(-3) to >1 MBq m(-3). The 220Rn concentrations at 80 cm varied from 45 Bq m(-3) to 48 kBq m(-3). The concentration versus depth profiles for 222Rn differed for soils developed on fault zones, uranium deposits or both. Atmospheric air temperature and soil gas 222Rn and 220Rn were negatively correlated. At sampling sites with steep slopes, 220Rn concentrations decreased with depth.     

Aerial measurements on uranium ore mining, milling and processing areas in Germany

The paper describes aerial measurements at several sites containing residues from uranium mines, waste rock dumps and tailings ponds of the Wismut company in Saxony and Thuringia. For the measurements, a computerized gamma-ray spectrometer equipped with a HPGe-detector and a NaI(Tl)-detector array with a volume of 121 was used. Radioactive anomalies from natural radionuclides have been detected and mapped. The activity concentrations of 226Ra, 228Th and 40K in areas with elevated radioactivity from natural radionuclides were determined from aerial measurements. Ground-based measurements--as far as available--confirmed these results. The mean 226Ra activity concentrations in the different waste rock dumps were found to be in the range 370 to 1600 Bq kg-1. The highest mean 226Ra activity concentrations were measured for the tailings ponds with values up to 1300 Bq kg-1. For 40K and 208Tl, activity concentrations of 860 and 40 Bq kg-1, respectively, were obtained as averages of all measurements. These values are commonly found in the environment. In general, there is reasonable agreement between the results measured with different detectors and measuring methods.     

Significant radioactive contamination of soil around a coal-fired thermal power plant

Soil samples were collected around a coal-fired power plant from 81 different locations. Brown coal, unusually rich in uranium, is burnt in this plant that lies inside the confines of a small industrial town and has been operational since 1943. Activity concentrations of the radionuclides 238U, 226Ra, 232Th, 137Cs and 40K were determined in the samples. Considerably elevated concentrations of 238U and 226Ra have been found in most samples collected within the inhabited area. Concentrations of 235U and 226Ra in soil decreased regularly with increasing depth at many locations, which can be explained by fly-ash fallout. Concentrations of 235U and 226Ra in the top (0-5 cm depth) layer of soil in public areas inside the town are 4.7 times higher, on average, than those in the uncontaminated deeper layers, which means there is about 108 Bq kg(-1) surplus activity concentration above the geological background. A high emanation rate of 222Rn from the contaminated soil layers and significant disequilibrium between 238U and 226Ra activities in some kinds of samples have been found.     

An efficient and simple method for measuring (226)Ra using the scintillation cell in a delayed coincidence counting system (RaDeCC)

A delayed coincidence counter (RaDeCC), developed to determine ultra-low levels of (223)Ra (half life = 11.1 days) and (224)Ra (half life = 3.6 days) in seawater, was adapted to measure (226)Ra (half life = 1622 years). After pre-concentration of Ra from seawater onto MnO(2)-coated fiber we show in this study that the (226)Ra activity can be determined using the RaDeCC's ability to record alpha decay of its daughters as total counts. For sufficient ingrowth of (222)Rn, the Mn-fiber is hermetically sealed in a column for a few days. Then, the ingrown (222)Rn is circulated through the RaDeCC air-loop system followed by shutting down of the pump and closure of the scintillation cell for equilibration. Counting may be completed within a few hours for seawater samples. Sample measurements with this method agreed well with data obtained using gamma-ray spectrometry. This proves that a set of Ra isotopes ((223)Ra, (224)Ra, and (226)Ra), commonly used for geophysical studies such as mixing rates of different water masses and submarine groundwater discharge, can be efficiently and rapidly measured using the RaDeCC.