Radium removal from mine waters in underground treatment installations

The underground mining of hard coal is widespread in the Upper Silesian Coal Basin (southern Poland). In deep mines, inflows of highly mineralised waters containing radium isotopes are numerous. These waters cause severe damage to the natural environment due to the salinity, but additionally radioactive pollution occurs. The region is densely populated, therefore mitigation methods are very important. The method of radium removal has been applied in full technical scale in two coal mines with very good results - in one of the mines radium-bearing waters are treated at the rate of approximately 0.1m(3)s(-1), while in another mine salty waters are purified at the rate of 0.1m(3)s(-1). The purification takes place in special underground galleries without any contact of the mining crew with the radioactive deposits produced during the process. As a result, release of radium is significantly lower, more than 200MBq of (226)Ra and (228)Ra remains underground each day.     

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.     

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).     

Concentrations and environmental fate of Ra in cation-exchange regeneration brine waste disposed to septic tanks and accumulation in sludge, New Jersey Coastal Plain, USA

Concentrations of Ra in liquid and solid wastes generated from 15 softeners treating domestic well waters from New Jersey Coastal Plain aquifers (where combined Ra ((226)Ra plus (228)Ra) concentrations commonly exceed 0.185 Bq L(-1)) were determined. Softeners, when maintained, reduced combined Ra about 10-fold (<0.024 Bq L(-1)). Combined Ra exceeded 0.185 Bq L(-1) at 1 non-maintained system. Combined Ra was enriched in regeneration brine waste (maximum, 81.2 Bq L(-1)), but concentrations in septic-tank effluents receiving brine waste were less than in the untreated ground waters. The maximum combined Ra concentration in aquifer sands (40.7 Bq kg(-1) dry weight) was less than that in sludge from the septic tanks (range, 84-363 Bq kg(-1)), indicating Ra accumulation in sludge from effluent. The combined Ra concentration in sludge from the homeowners' septic systems falls within the range reported for sludge samples from publicly owned treatment works within the region.     

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.     

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.     

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.     

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.     

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.     

226Ra bioavailability to plants at the Urgeiriça uranium mill tailings site

Large amounts of solid wastes (tailings) resulting from the exploitation and treatment of uranium ore at the Urgeiri?a mine (north of Portugal) have been accumulated in dams (tailing ponds). To reduce the dispersion of natural radionuclides into the environment, some dams were revegetated with eucalyptus (Eucalyptus globolus) and pines (Pinus pinea). Besides these plants, some shrubs (Cytisus spp.) are growing in some of the dams. The objective of this study is to determine the 226Ra bioavailability from uranium mill tailings by quantifying the total and available fraction of radium in the tailings and to estimate its transfer to plants growing on the tailing piles. Plant and tailing samples were randomly collected and the activity concentration of 226Ra in plants (aerial part and roots) and tailings was measured by gamma-spectrometry. The exchangeable fraction of radium in tailings was quantified using one single step extraction with 1 mol dm-3 ammonium acetate (pH = 7) or 1 mol dm-3 calcium chloride solutions. The results obtained for 226Ra uptake by plants show that 226Ra concentration ratios for eucalyptus and pines decrease at low 226Ra concentrations in the tailings and appear relatively constant at higher radium concentrations. For shrubs, the concentration ratios increase at higher 226Ra solid waste concentrations approaching a saturation value. Percentage values of 16.0 +/- 8.3 and 12.9 +/- 8.9, for the fraction of radium extracted from the tailings, using 1 mol dm-3 ammonium acetate or calcium chloride solutions, respectively, were obtained. The 226Ra concentration ratios determined on the basis of exchangeable radium are one order of magnitude higher than those based on total radium. It can be concluded that, at a 95% confidence level, more consistent 226Ra concentration ratios were obtained when calculated on the basis of available radium than when total radium was considered, for all the dams.     

Soil to plant transfer of Radium-226

A study of the uptake of ²²⁶Ra by vegetables was carried out in zones contaminated by wastes from an abandoned radium salts factory and from uranium mines and in uncontaminated regions of purely natural radioactivity. Radium-226 uptake depends on its concentration in the soil, the logarithm of its concentration in the vegetables being a linear function of the logarithm of the concentration in the soil. Concentration factors for ²²⁶Ra uptake by cabbage leaves range from 0·007 to 0·11; for herbage, they range from 0·09 to 0·5.     

226Ra and 228Ra activities associated with agricultural drainage ponds and wetland ponds in the Kankakee Watershed, Illinois-Indiana, USA

Background radioactivity is elevated in many agricultural drainage ponds and also constructed wetland ponds in the Kankakee watershed. During 1995-1999, gross-alpha and -beta activities were measured up to 455 and 1650 mBq L-1, respectively. 226Ra and 228Ra averaged 139 and 192 mBq L-1 in controlled drainage ponds compared to 53 and 58 mBq L-1 for 226Ra and 228Ra, respectively, in native wetland ponds. Analyses of applied ammonium phosphate fertilizers near both native and controlled ponds indicate comparable 226Ra/228Ra and 228Ra/232Th activity ratios with only the surface waters in the controlled ponds. For example, 226Ra/228Ra activity ratios in controlled ponds ranged from 0.791 to 0.91 and group with a local fertilizer batch containing FL phosphate compounds with 226Ra/228Ra activity ratios of 0.831-1.04. Local soils of the Kankakee watershed have 226Ra/228Ra activity ratios of 0.541-0.70. Calculated Ra fluxes of waters, in drainage ditches associated with these controlled ponds, for 226Ra ranged from 0.77 to 9.00 mBq cm-2 d-1 and for 228Ra ranged from 1.22 to 8.43 mBq cm-2 d-1. Ra activity gradients were measured beneath these controlled ponds both in agricultural landscapes and in constructed wetlands, all being associated with drainage ditches. Ra had infiltrated to the local water table but was below regulatory maximum contaminant limits. Still, measurable Ra activity was measured downgradient of even the constructed wetlands in the Kankakee watershed, suggesting that the attenuation of Ra was low. However, no Ra excess was observed in the riparian zone or the Kankakee River downgradient of the native wetland ponds.     

Nationwide survey on the natural radionuclides in industrial raw minerals in South Korea

A Nationwide survey on the natural radioactivity in industrial raw mineral commodities (17 kinds of domestic and 18 kinds of imported) that are representative minerals used in production and consumption in South Korea was conducted. The target industrial minerals can be categorized into two groups. The first group covers non-metallic and metallic raw minerals with low levels of radioactivity such as clay, silica sand, carbonates, bituminous and anthracite coal, iron ores, ilmenite, rutile, and phosphate ore. The other group comprises minerals with high levels of radioactivity including zircon and monazite. One hundred and sixty-four domestic and imported samples were analysed by gamma-ray spectroscopy using an HPGe detector. The (40)K content ranges from <0.00131 to 2.69Bq g(-1), and (226)Ra and (232)Th range over <0.0006 to 0.630 and <0.0008 to 0.474Bq g(-1), respectively. There was no anthropogenic radioactive signal in any of the samples.     

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 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.     

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.     

Radium equivalent activity concentrations in concrete building blocks in eight cities in Southwestern Nigeria

The radioactivity concentrations of (226)Ra, (232)Th and (40)K were measured by using gamma ray spectroscopy in 130 concrete building blocks collected from block making sites in eight cities in Southwestern Nigeria. The results were used to compute the radium equivalent activity concentration for each city. The values of the concentrations of the primordial radionuclides varied widely within each city and among the cities. The weighted means for the cities range between 13.3 and 18.4, 28.2 and 71.6, and 176.2 and 336.8 Bq/kg for (226)Ra, (232)Th and (40)K, respectively. The city weighted means of radium equivalent activity concentrations for the eight cities range from 81 to 145 with a mean of 101 Bq/kg. The maximum for external hazard index was determined as 0.39. All the values are within the safety limits recommended by UNSCEAR [United Nations Scientific Committee on the Effects of Atomic Radiation 1982. Report to the General Assembly, with annexes. New York, United Nations.].     

Natural radioactivity in some major rivers of coastal Karnataka on the southwest coast of India

Systematic studies on radiation level and distribution of radionuclides have been carried out in riverine environs of three major rivers of coastal Karnataka, viz. Kali, Sharavathi and Netravathi. The ambient gamma radiation levels along three rivers were measured using a portable plastic scintillometer. Activity concentrations of (226)Ra, (232)Th and (40)K in soil, sediment and rock were measured using a NaI(Tl) gamma-ray spectrometer. In the Kali, Sharavathi and Netravathi riverbanks, the median values of absorbed gamma dose rates in air were found to be 44 nGy h(-1), 35 nGy h(-1) and 57 nGy h(-1), respectively. The highest activity of (226)Ra was found in riverbank soil samples of Sharavathi River. The highest activities of (232)Th and (40)K were found in riverbank soil and sediment samples of Netravathi River. In Kali River, the highest (226)Ra activity was recorded for rock samples. To assess the radiological hazard of natural radioactivity in the samples, absorbed gamma dose rates in air, radium equivalent activity, representative level index, external hazard index and internal hazard index associated with the radionuclides were calculated and compared with internationally recommended values. The representative level index (I(gammar)) values are high in sediment samples of Netravathi River. The radium equivalent activity (Ra(eq)), external hazard index (H(ex)) and internal hazard index (H(in)) values are high in rock samples of Kali River. The results of these investigations are presented and discussed in this paper.     

Determination and comparison of uranium and radium isotopes activities and activity ratios in samples from some natural water sources in Morocco.

Radiochemical results (238U, 226Ra and 228Ra activities; 234U/238U, 228Ra/226Ra and 226Ra/238U activity ratios) are reported for 42 natural water samples collected from wells, hot mineral springs, rivers, tap water, lakes and irrigation water in 15 Moroccan locations. Results show that 238U activity varies between 4.5 and about 309 mBq l(-1) in wells, 0.6 and 8.5 mBq l(-1) in hot springs, 9.7 and 28 mBq l(-1) in rivers, 2.5 and 16 mBq l(-1) in tap waters and between 6 and 24 mBq l(-1) in lakes. The 234U/238U activity ratio varies in the range 0.87-3.35 in all analyzed water samples except for hot springs where it reaches values higher than 7. Unlike well water, mineral water samples present low 238U activities and high 234U/238U activity ratios and 226Ra activities. The highest activity of radium in mineral water is 150 times higher than the highest activity of 226 Ra found in well water. 226Ra/238U activity ratios are in the ranges 0.07-1.14 in wells, 0.04-0.38 in rivers, 0.04-2.48 in lakes, and 1.79-2115 in springs. The calculated equivalent doses to all the measured activities are inferior to the maximum contaminant levels recommended by the International Commission of Radioprotection and they do not present any risk for public health in Morocco.     

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.