Concentration of 226Ra in Hungarian bottled mineral water

Concentration of the radionuclide 226Ra was determined in almost every type of bottled mineral water commercially available in Hungary. Determination of the radon coming from the radium dissolved in the water was used for activity measurement. As the results show, the 226Ra concentrations exceed the level of 100 mBq l(-1) in six cases out of the 28 types of mineral water investigated. In one case 3 Bq l(-1) was measured, which provides 0.3 mSv year(-1) committed effective dose for adults in the case of a consumption rate of 1 l day(-1). In soft drinks produced from mineral water a concentration of 2.6 Bq l(-1) was determined, which means 1.4 mSv year(-1) effective dose in the age group 12-17 years in the case of permanent daily drinking of 1 l of these beverages.     

Occurrence of 222Rn, 226Ra, 228Ra and U in groundwater in Fujian Province, China

222Rn, 226Ra, 228Ra and U were determined in a total of 552 groundwater samples collected throughout Fujian Province of China. The geometric mean concentrations of 222Rn, 226Ra, 228Ra and total U in the groundwater were 147.8 kBq m-3, 12.7 Bq m-3, 30.2 Bq m-3 and 0.54 microgram kg-1, respectively. High groundwater 222Rn was explained by the predominantly granitic rock aquifers in Fujian. A lifetime risk of 1.7 x 10(-3) was estimated for the ingestion of groundwater 222Rn. High ratios of 228Ra to 226Ra contents (geometric mean of 2.4) and their disproportion suggest that 228Ra should also be measured in the assessment of population doses from drinking water in the regions of high rock or soil 232Th. No significant correlation between the 222Rn concentrations in groundwater and air was found.     

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.     

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.     

Dissolution characteristics of 226Ra from phosphogypsum

The paper presents the results of the dissolution characteristics of 226Ra from phosphogypsum, a by-product from phosphate fertilizer industries. Leachability of 226Ra in distilled water and rainwater have been examined under different leaching conditions such as contact time, solid:liquid ratio and simulating natural conditions. The concentration of 226Ra activity in the leachates ranged from 0.07 to 0.53 Bq l(-1). Study indicated that leaching of radium may be slow in field conditions near the phosphogypsum stock piles.     

Abnormal high natural radium concentration in surface waters

Unexpected high 228Ra concentrations, up to 2 Bq 1(-1), were found in waters of a coastal lagoon close to a monazite sand separation plant. Due to their use as process waters in this plant, the initial supposition was a contamination related to its operation. However, it was concluded that these abnormal radium concentrations had a natural origin, springs at the lagoon head area with high 228Ra and 226Ra concentrations. The strong relationship among radium and light rare-earth elements (LREEs), the observed 228Ra/226Ra activity ratio and the rare-earth element pattern in the spring waters suggested that monazite is the main source of nuclides for water, indicating the disturbance of monazite chemical stability by the combined effects of low pH and high salinity. Both factors combined allow relatively low mobility of thorium, but, on the other hand, a relatively high mobility of radium and LREEs.     

Determination of 228Ra, 226Ra and 224Ra in natural water via adsorption on MnO2-coated discs

A fast procedure based on sorption of Ra on MnO2 coated polyamide discs is presented for determination of radium isotopes (i.e. 228Ra, 226Ra, 224Ra) in aqueous samples. The sample discs can be used directly for low-level alpha-spectrometry without the need for further separation and preparation methods to produce planar sample sources. While the activity of alpha-emitting 224Ra and 226Ra can be determined during a first measurement, beta-emitting 228Ra is obtained via ingrowth of the progeny 228Th on the same sample disc after a standing time of about six months. Calculations are presented for optimizing the analytical accuracy as well as for predicting the sorption yield or chemical recovery of radium on the sample disc as a function of exposure time because the sorption uptake proceeds with first-order kinetics. The analyses can be carried out on small samples of 0.5-11 and, for long counting times of one week and use of high-purity silicon surface barrier detectors, a detection limit of 0.15 mBq l-1 is obtained for 226Ra. Since the half-life of 224Ra is only 3.7 d and since 228Th (as a measure for 228Ra) is built up only partially on the sample disc, a slightly higher detection limit of 0.24 mBq l-1 results for the latter isotopes. The procedure is therefore sufficiently sensitive to allow the investigation of Ra isotope relationships in aquifers at typical environmental levels.     

Environmental impact studies of barium and radium discharges by produced waters from the "Bacia de Campos" oil-field offshore platforms,Brazil

Produced water samples from different E&P offshore petroleum platforms, belonging to the Bacia de Campos oil field, Brazil, were analyzed for barium, 226Ra and 'Ra. The concentrations measured are in the range of 0.36-25.7 mg l(-1) for barium, 0.012-6.0 Bq l(-1) for 226Ra and <0.05-12.0 Bq l(-1) for 1Ra. A strong correlation between the concentration of barium and radium isotopes was observed (226Ra: r2=0.926: 228Ra: r2=0.785). Additionally, seawater and sediment samples were taken at different distances (from 250 to 1,000 m) from the two selected platforms. Water samples were analyzed for dissolved and particulate barium, 226Ra and 225Ra and the sediment samples for total and leachable barium, 226Ra and 228Ra. The results showed that even for the shortest sampling distance (250 m) from the discharge point, barium, 226Ra and 228Ra concentrations are similar to the local background, indicating that dispersion by local currents is enough to minimize environmental impacts.     

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.     

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.     

Distribution of gamma-ray emitting radionuclides in the environment of Burullus Lake: I. Soils and vegetations

The concentrations and distribution of gamma-ray emitting isotopes in Burullus Lake were investigated with the aim of evaluating the environmental radioactivity. Particularly in wetlands, natural properties of the environment can cause the actual inventory to be different from the activity originally deposited. The mean concentrations of (226)Ra, (232)Th and (40)K were 14.3, 15.5 and 224 Bq/kg, respectively, in the coastal soils. On the other hand, soil samples from the islands had mean concentrations of 13.5, 17.4 and 341 Bq/kg for (226)Ra, (232)Th and (40)K, respectively. Samples from coast and islands show evidence of possible transfer and accumulation of the (137)Cs radionuclide. The mean (137)Cs activity concentrations in the soil samples were 1.2 and 15.1 Bq/kg in the coast and islands, respectively. The vertical migration of (137)Cs was studied based on its content in the consequently located three soil layers down to 30 cm depth. The radium equivalent, dose rate in air and annual dose equivalent from the terrestrial natural gamma-radiation were evaluated. The mean activity concentrations of the gamma-ray emitting radionuclides in vegetation were relatively low.     

Radionuclide and chemical concentrations in mineral waters at Saratoga Springs, New York

A project to characterize the radionuclide and chemical components in natural spring waters in the vicinity of Saratoga Springs, New York (USA) has been completed. As a result of the measured radionuclide and chemical content, eight springs were labeled as mineral waters, whereas three springs contained very low concentrations of these components. The mineral waters were highly enriched in alkaline and alkaline-earth elements, as well as chloride ions. Three isotopes of radium ((224)Ra, (226)Ra, (228)Ra) were detected in the mineral waters and reached concentrations of 1, 20, and 2 Bq/L, respectively. Overall, the (226)Ra isotope constituted about 80% of the total radioactivity measured in the water samples. Dissolved uranium concentrations in the mineral waters were very low (mean approximately 50 mBq/L).     

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.     

Radionuclide content of concrete building blocks and radiation dose rates in some dwellings in Ibadan, Nigeria

Thirty-two samples of concrete building blocks were collected from different block making industries in Ibadan. The radioactivity concentrations of the natural radionuclides in the samples were determined by gamma-ray spectrometry with a NaI(Tl) detector. The radioactivity concentrations varied from 6.2 to 57.5 Bq kg(-1), 12.4 to 64.9 Bq kg(-1) and 95.3 to 766.1 Bq kg(-1) for 226Ra, 232Th and 40K, respectively. The radium equivalent activities of the 32 samples varied from 51.3 to 175.7 Bq kg(-1). Radiation exposure levels in 30 dwellings were determined using LiF thermoluminescent dosimeters. The annual equivalent dose rates varied from 0.318 to 0.657 mSv y(-1) with a mean of 0.433 mSv y(-1). The annual effective dose rate to the whole body was calculated as 0.236 mSv y(-1), which is less than that (mean) estimated by UNSCEAR for normal background areas.     

Measuring the radium quartet (Ra, Ra, Ra, Ra) in seawater samples using gamma spectrometry

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While ²²⁸Ra and ²²⁶Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (²²⁴Ra and ²²³Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report ²²⁶Ra, ²²⁸Ra, ²²⁴Ra, ²²³Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The ²²³Ra and ²²⁴Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the ²²⁴Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low ²²³Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes.     

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.     

Contamination of settling ponds and rivers as a result of discharge of radium-bearing waters from Polish coal mines

Saline waters from underground coal mines in Poland often contain natural radioactive isotopes, mainly 226Ra from the uranium decay series and 228Ra from the thorium series. Approximately 40% of the total amount of radium remains underground as radioactive deposits, but 225 MBq of 226Ra and 400 MBq of 228Ra are released daily into the rivers along with the other mine effluents from all Polish coal mines. Technical measures such as inducing the precipitation of radium in gobs, decreasing the amount of meteoric inflow water into underground workings, etc. have been undertaken in several coal mines, and as a result of these measures, the total amount of radium released to the surface waters has diminished by about 60% during the last 5-6 years. Mine water can have a severe impact on the natural environment, mainly due to its salinity. However, associated high levels of radium concentration in river waters, bottom sediments and vegetation have also been observed. Sometimes radium concentrations in rivers exceed 0.7 kBq/m3, which is the permitted level for waste waters under Polish law. The extensive investigations described here were carried out for all coal mines and on this basis the total radium balance in the effluents has been calculated. Measurements in the vicinity of mine settling ponds and in rivers have given us an opportunity to study radium behaviour in river waters and to assess the degree of contamination. Solid waste materials with enhanced natural radioactivity have been produced in huge amounts in the power and coal industries in Poland. As a result of the combustion of coal in power plants, low-radioactive waste materials are produced, with 226Ra concentration seldom exceeding a few hundreds of Bq/kg. A different situation is observed in coal mines, where, as a result of precipitation of radium from radium-bearing waters, highly radioactive deposits are formed. Sometimes the radioactivity of such materials is extremely high; precipitates from coal mines may have radium concentrations of 400,000 Bq/kg--equivalent to 3% uranium ore. Usually, such deposition takes place underground, but sometimes co-precipitation of radium with barium takes place on the surface, in settling ponds and in rivers. Therefore management of solid waste with technologically enhanced natural radioactivity (TENR) is a very important subject.     

Environmental fate of Ra in cation-exchange regeneration brine waste disposed to septic tanks, New Jersey Coastal Plain, USA: migration to the water table

Fate of radium (Ra) in liquid regeneration brine wastes from water softeners disposed to septic tanks in the New Jersey Coastal Plain was studied. Before treatment, combined Ra (²²⁶Ra plus ²²⁸Ra) concentrations (maximum, 1.54 Bq L⁻¹) exceeded the 0.185 Bq L⁻¹ Maximum Contaminant Level in 4 of 10 studied domestic-well waters (median pH, 4.90). At the water table downgradient from leachfields, combined Ra concentrations were low (commonly ≤0.019 Bq L⁻¹) when pH was >5.3, indicating sequestration; when pH was ≤5.3 (acidic), concentrations were elevated (maximum, 0.985 Bq L⁻¹ - greater than concentrations in corresponding discharged septic-tank effluents (maximum, 0.243 Bq L⁻¹)), indicating Ra mobilization from leachfield sediments. Confidence in quantification of Ra mass balance was reduced by study design limitations, including synoptic sampling of effluents and ground waters, and large uncertainties associated with analytical methods. The trend of Ra mobilization in acidic environments does match observations from regional water-quality assessments.     

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).     

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.