The application of phosphogypsum in agriculture and the radiological impact

Radium-226 in phosphogypsum produced in a phosphate industry, SICNG operating at Thessaloniki, Northern Greece since May 1966, varied from 261 to 688 Bq kg(-1) (mean value 508 Bq kg(-1)). This radionuclide in soil tilled with phosphogypsum used for agricultural purposes varied from 50 to 479 Bq kg(-1) (average 205 Bq kg(-1)), while in the regular soil of cultivated fields it varied from 37 to 54 Bq kg(-1) (average 48 Bq kg(-1)). Radium-226 in rice originated from cultivated fields tilled with phosphogypsum or not varied from 0.36 to 1.98 Bq kg(-1) (average 1.53 Bq kg(-1)) with the higher values observed in samples originated from cultivated fields tilled with phosphogypsum. Radium-226 transfer factors, TF, from soil tilled with phosphogypsum to plants for the case of rice varied from 6.5 x 10(-3) to 2.0 x 10(-2) (geometric mean: 1.1 x 10(-2)). A mean (226)Ra content in rice 1.53 Bq kg(-1) results in a daily intake of (226)Ra by humans in Greece 0.0084 Bq day(-1) leading to an annual effective dose for adults 0.86 microSv y(-1) which is much less in contributing to the average exposure to natural radiation sources (2.4 mSv y(-1)) and particularly to the part due to ingestion (0.29 mSv y(-1)). It is necessary to continuously control (monitoring) (226)Ra in phosphogypsum before any use for agricultural purposes.     

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.     

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.     

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).     

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

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

Natural radioactivity in phosphates, phosphogypsum and natural waters in Morocco

The contents of natural radionuclides (uranium, actinium and thorium series) were measured in sedimentary phosphate rock samples using high-resolution gamma spectrometry. Data obtained for uranium content (ppm) were compared with the results obtained by a method based on the measurements using solid-state nuclear track detectors (SSNTD) in the same samples. The potential leaching of radionuclides from sedimentary phosphate rock during the industrial production of the phosphoric acid was studied. The process of leaching of the radioisotopes from phosphogypsum was discussed. A method for the direct alpha counting of 226Ra thin source, elaborated by the deposition of Ra from aqueous solutions on manganese oxides film deposited on polyvinyl support, have been developed and applied for the determination of 226Ra in natural water samples. The results show that only the water sample from the mine area reveals the presence of 226Ra at a level of about 0.2 Bq l-1.     

Concentrations of natural radionuclides in imported mineral substances

Levels of natural radionuclides, such as thorium-232 (232Th), radium-226 (226Ra) and potassium-40 (40K), were determined in about 2,000 samples of imported mineral substances using gamma spectrometry. The maximum concentration levels of 232Th, 226Ra and 40K were 1,260 +/- 54, 13,400 +/- 94 and 1,256 +/- 260 Bq kg(-1), respectively, in zirconium compounds. Due to relatively high concentrations of the above-mentioned radionuclides in some imported mineral substances, the National Radiation Protection Department (NRPD), as the competent authority, has established national limits (900 Bq kg(-1) for 232Th, 1800 Bq kg(-1) for 226Ra and 11,000 Bq kg(-1) for 40K), based on the external exposures, for general importation permits of these materials.     

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.     

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.     

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.     

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.     

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.     

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.     

Norm and associated radiation hazards in bricks fabricated in various localities of the North-West Frontier Province (Pakistan).

The activity concentrations of natural gamma-emitting radionuclides and associated radiation hazards due to 40K, 226Ra and 232Th have been measured in baked brick samples, collected from six highly populated areas of the North-West Frontier Province (NWFP) of Pakistan. For the detection, analysis and data acquisition, a high purity germanium (HPGe) detector coupled with a high resolution multichannel analyser (MCA) was used. The range of the average values of the activity concentrations due to 40K, 226Ra and 232Th were found to be 680.3 +/- 22.2-784.4 +/- 30.7 Bq kg(-1), 36.9 +/- 3.5-51.9 +/- 3.3 Bq kg(-1) and 52.5 +/- 3.6-67.6 +/- 3.1 Bq kg(-1), respectively. Radium equivalent (Ra(eq)) activities and various hazard indices were also calculated to assess the radiation hazards. All the brick samples showed Ra, activities within the limit (370 Bq kg(-1)) set by the Organization for Economic Cooperation and Development (OECD) countries. The results of different criterion formulae also complemented each other in this study. The derived data have been compared with the reported values for other countries of the world.     

226Ra, 40K and 7Be activity concentrations in plants in the environment of Kaiga,India

Leaves, stem and bark samples from several plant species were collected from tropical forest of Kaiga, in the west coast of India where two nuclear power reactors of 220 MW each have just been commissioned and another two are under construction, and analysed for their (226)Ra, (40)K and (7)Be concentrations. The activities of (226)Ra and (40)K in plants were found to vary in the range BDL-13.2 and 12.0-797.3 Bq kg(-1), respectively. Plants show significant (7)Be activity in leaves, the activity varies in 72.5-1,060.8 Bq kg(-1). Stem and bark of plants show higher levels of (226)Ra and (40)K when compared to leaves. Soil-to-plant transfer factor for (226)Ra and (40)K were found to vary in the range BDL-0.37 and 0.09-5.61, respectively for different plants. The concentration of (226)Ra and (40)K in leaves depends on the age of the leaves.     

Natural radioactivity and dose assessment for phosphate rocks from Wadi El-Mashash and El-Mahamid Mines, Egypt

The activity concentrations of (226)Ra, (232)Th and (40)K have been measured by gamma spectroscopy (sodium iodide NaI(Tl) detector) in phosphate rock samples, collected from the Wadi El-Mashash, a site located in the central eastern desert, and El-Mahamid in the Nile valley, Egypt. The average activity concentrations of (226)Ra, (232)Th and (40)K (Bq kg(-1)) in phosphate rocks were 665.8+/-33.4, 329.4+/-17 and 587.6+/-29.4 for Wadi El-Mashash and 566.8+/-28.6, 217.3+/-11.8 and 560.1+/-28 for El-Mahamid, respectively. The corresponding values for shale rocks were 85.2+/-5.7, 93.3+/-5.6 and 303.1+/-15.2 Bq kg(-1), respectively. As a measure of radiation hazard to the occupational workers and public, the Ra equivalent activities, representative level index and dose rates due to natural radionuclides at 1 m above the ground surface were estimated. The calculated external gamma-radiation dose received by the workers of the phosphate mine are 538 and 418 microSv/y, which is far below the permitted dose of 20 mSv/y recommended by the International Commission of Radiation Protection [ICRP-60, 1990. Radiation Protection: 1990 Recommendation of the International Commission on Radiological Protection, Oxford, Pergamon Preis.] for workers.     

Characteristics, spatial distribution and vertical profile of gamma-ray emitting radionuclides in the coastal environment of North Sinai

Radionuclide concentrations of beach and dune sand from various sites in Al-Arish city and surrounding area, North Sinai, Egypt, were measured. The sampling sites included locations in the local harbor, Al-Arish valley and Zaranik protected area. The results indicate that the activities of the products of (232)Th and (226)Ra series in samples from the harbor and along the beach were higher than those from non-coastal sites. The activity concentrations of (232)Th for beach sand ranged from 2.3 to 506.5 Bq/kg with an average of 83.4 Bq/kg, while that for dune sand ranged from 2.2 to 15.1 Bq/kg with an average of 6.4 Bq/kg. The average activity concentration of (226)Ra for beach sand was 56.0 Bq/kg (2.9-261.5 Bq/kg), while that for dune sand was 6.5 Bq/kg (3.0-14.7 Bq/kg). The average activity concentrations of (40)K for beach and dune sand were 88.1 Bq/kg and 178.4 Bq/kg, respectively. Six depth profiles in the harbor area were measured up to a depth of 1m within more than two years. These sets of measurements allowed the determination of the migration rate of black sand to be 0.094 cm/day. Samples with the smallest grain size (<0.2 mm) were found to have the highest level of activities, which were attributed to their high content of black sand. No risk exists for public health based on the calculated effective dose equivalent and the recommended limit of 5 mSv/y. On the other hand, local children and adults may receive doses higher than this recommended limit in two locations in the Zaranik protected area according to a model developed in this study.     

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.     

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.     

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.