The importance of physico-chemical parameters on the speciation of natural radionuclides in riverine ecosystems

External gamma radiation levels were measured in the catchment areas of the Sharavathi River and the dose rates in air were found to be in the range 26.0-61.0 nGy h⁻¹. Soil and sediment samples of the riverine environment were analysed for natural radionuclides such as ²²⁶Ra, ²³²Th and ⁴⁰K using a NaI(Tl) gamma spectrometer. The activity concentration of ²¹⁰Pb and ²¹⁰Po in soil and sediment samples was determined by radiochemical separation techniques. Evaluation of the activity concentration of radionuclides with grain size revealed an increase in the activity of ²²⁶Ra, ²³²Th and ⁴⁰K towards fine grain size. The activity concentrations for all isotopes in all samples were not significantly correlated with pH. However, the activity of ²¹⁰Po and ²¹⁰Pb in sediment showed a moderate positive correlation with organic matter content and a good correlation with clay content of sediment.     

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.     

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.].     

Study of 210Po and 210Pb in the riverine environments of coastal Karnataka

Activity of ²¹⁰Po and ²¹⁰Pb were measured in soil and sediment samples collected from the major rivers Kali, Sharavathi and Netravathi of Coastal Karnataka. The activity of these two radionuclides were determined by radiochemical separation of ²¹⁰Po and counting the activity using a ZnS(Ag) Alpha counter. The activity of ²¹⁰Pb was higher than that of ²¹⁰Po in the riverine environs. The ²¹⁰Po and ²¹⁰Pb content in sediment was found to increase with silt/clay and organic matter contents. However no significant correlation was found between the activity ²¹⁰Po and ²¹⁰Pb with pH in sediments. The activity of ²¹⁰Po and ²¹⁰Pb and influence of physico-chemical parameters on these radionuclides were studied and discussed in this paper.     

Natural radioactivity in farm soil and phosphate fertilizer and its environmental implications in Qena governorate, Upper Egypt

Samples of phosphate fertilizers and farm soils, taken to a depth of up to 30 cm in cultivated land, were collected over the Qena governorate, Upper Egypt. Activity concentration of background radionuclides such as (226)Ra, (232)Th and (40)K of these samples were determined by gamma-ray spectrometry. The results show that these radionuclides were present in concentrations of 366+/-10.5, 66.7+/-7.3 and 4+/-2.6 Bq/kg for phosphate fertilizers. For farm soil and Nile island's soil the corresponding values were 13.7+/-7, 12.3+/-4.6, 1233+/-646 and 11.9+/-6.7, 10.5+/-6.1, 1636+/-417 Bq/kg, respectively. The radium equivalent activity (Ra(eq)), the representative level index, I(gamma r), and absorbed dose in air for all samples were calculated. The data were discussed and compared with those given in the literature.     

Measurement of natural radioactivity in building materials in Qena city, Upper Egypt

Building materials cause direct radiation exposure because of their radium, thorium and potassium content. In this paper, samples of commonly used building materials (bricks, cement, gypsum, ceramics, marble, limestone and granite) in Qena city, Upper Egypt have been collected randomly over the city. The samples were tested for their radioactivity contents by using gamma spectroscopic measurements. The results show that the highest mean value of (226)Ra activity is 205+/-83 Bqkg(-1) measured in marble. The corresponding value of (232)Th is 118+/-14 Bqkg(-1) measured in granite. For (40)K this value is (8.7+/-3.9)x10(2) Bqkg(-1) measured in marble. The average concentrations of the three radionuclides in the different building materials are 116+/-54, 64+/-34 and (4.8+/-2.2)x10(2) Bqkg(-1) for (226)Ra, (232)Th and (40)K, respectively. Radium equivalent activities and various hazard indices were also calculated to assess the radiation hazard. The maximum mean of radium equivalent activity Ra(eq) is 436+/-199 Bqkg(-1) calculated in marble. The highest radioactivity level and dose rate in air from these materials were calculated in marble.     

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.     

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.     

Distribution of long-lived radionuclides of the 238U series in the sediments of a small river in a uranium mineralized region of Spain

A study is presented on the distribution and mobilization of the natural U isotopes (238U and 234U), 230Th, and 226Ra in the sediments of a small river crossing an uranium mineralized zone where a disused uranium mine is located. Due to the preferential directions for surface run-off waters and to the mine's situation, one sampling point along the river bed was identified as a point of accumulation of radionuclides. The average values of the activity concentrations (Bq/kg) in this sediment sample were 5,025, 5,055, 5,915 and 1,694 for 238U, 234U, 230Th and 226Ra, respectively, while the respective average values of the activity concentrations (Bq/kg) for the sediment sample considered to give the background level were 125, 124, 131 and 370. Isotopic ratios between the descendants of 238U served to clarify some paths of distribution, involving the soils nearest to the sampling points and the location of these points with respect to the disused mine. The differences in behaviour found between the uranium, thorium and radium isotopes were associated to the mobility of these radionuclides in the fluvial system studied. Correlations between the radionuclide activity concentration ratios and stable element concentrations in the sediment samples were also investigated.     

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.     

Origin and transport of U and Ra in riverine,estuarine and marine sediments of the Krka River,Croatia

Spatial distribution of ²³⁸U and ²²⁶Ra activities in sediment columns along the Krka River and estuary, were studied using gamma spectrometry. Markedly different ²³⁸U and ²²⁶Ra activities between riverine, estuarine and marine sediments were observed. Distribution of these radionuclides, as well as their anthropogenic and natural origin, was evaluated by activity measurements, taking into account sedimentation rates estimated by ¹³⁷Cs distribution in sediment columns.     

Specific activity and hazards of granite samples collected from the Eastern Desert of Egypt

Fifty granitic rock samples were collected from different plutons in the central part of the Eastern Desert of Egypt and were analyzed for specific concentrations of (238)U, (232)Th and (40)K radionuclei. The measurements were carried out using a high performance and stability Nomad Plus spectroscopy system attached to a 1.7 keV (FWHM) HPGe detector. The spectra were analyzed using the direct gamma counting comparison method as well as the traditional absolute efficiency curve method. The highest average value of (238)U concentration (1184 Bq kg(-1)) was observed at EI Misikat region whereas the highest average values of (40)K and (232)Th concentration (2301.8 and 162.5 Bq kg(-1) respectively), were detected at Gabal Homret Waggat area. The radium equivalent activity (Ra(eq)), the absorbed dose rate (D), the external hazard index (H(ex)) and the annual gonadal dose equivalent were also calculated and compared to the international recommended values. Radon exhalation rate from the rock samples were measured using the activated charcoal canister method. The average value of radon exhalation varies from 0.052 to 0.69 Bq m(-2) h(-1) and depends on the specific concentration of uranium.     

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.     

Assessment of the natural radioactivity and radiological hazards in Turkish cement and its raw materials

The natural radioactivity due to presence of (226)Ra, (232)Th and (40)K radionuclides in raw materials, intermediate products (clinker) and end products (22 different cement types) was measured using a gamma-ray spectrometry with HPGe detector. The specific radioactivity of (226)Ra, (232)Th and (40)K in the analyzed cement samples ranged from 12.5+/-0.3 to 162.5+/-1.7Bqkg(-1) with a mean of 40.5+/-26.7Bqkg(-1), 6.7+/-0.3 to 124.9+/-2.5Bqkg(-1) with a mean of 26.1+/-18.9Bqkg(-1) and 64.4+/-2.3 to 679.3+/-18.2Bqkg(-1) with a mean of 267.1+/-102.4Bqkg(-1), respectively. The radium equivalent activity (Ra(eq)), the gamma-index, the emanation coefficient, the (222)Rn mass exhalation rate and the indoor absorbed dose rate were estimated for the radiation hazard of the natural radioactivity in all samples. The calculated Ra(eq) values of cement samples (37.2+/-8.7-331.1+/-15.5Bqkg(-1) with a mean of 98.3+/-53.8) are lower than the limit of 370Bqkg(-1) set for building materials. The Ra(eq) values were compared with the corresponding values for cement of different countries. The mean indoor absorbed dose rate is slightly higher than the population-weighted average of 84nGyh(-1).     

Coupled anthropogenic anomalies of radionuclides and major elements in estuarine sediments

Concentrations of fertilizer industry-derived P (up to 3.4%), Ca (up to 6.1%), (226)Ra (up to 744 Bq kg(-1)) and (210)Pb (up to 1317 Bq kg(-1)) at least one order of magnitude above natural levels were recorded in a sediment core from Morr?o River estuary (SE Brazil). Unsupported (210)Pb (= total (210)Pb-(226)Ra) activities unexplained by atmospheric fallout and deviations from the radionuclides secular equilibrium also indicated strong anomalies. Anomalous constituents were positively correlated with each other and negatively correlated with clay mineral-bearing elements. These negative correlations were explained by a depletion of natural sediment constituents due to a dilution caused by elevated inputs of steel industry-derived elements (mainly by Fe levels up to 24%). Absolute data and normalizations by a proxy for clays (Al) and anthropogenic Fe evidenced variabilities in the quality of coastal and land-derived sediment inputs, mainly due to changes in the relative contributions from industrial sources.     

Radioactivity concentration in liquid and solid phases of scale and sludge generated in the petroleum industry

Scales and sludge generated during oil extraction and production can contain uranium, thorium, radium and other natural radionuclides, which can cause exposure of maintenance personnel. This work shows how the oil content can influence the results of measurements of radionuclide concentration in scale and sludge. Samples were taken from a PETROBRAS unit in Northeast Brazil. They were collected directly from the inner surface of water pipes or from barrels stored in the waste storage area of the E&P unit. The oil was separated from the solids with a Soxhlet extractor by using aguarras at 90+/-5 degrees C as solvent. Concentrations of 226Ra and 228Ra in the samples were determined before and after oil extraction by using an HPGe gamma spectrometric system. The results showed an increase in the radionuclide concentration in the solid (dry) phase, indicating that the above radionuclides concentrate mostly in the solid material.     

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.     

Evaluation of technologically enhanced natural radiation near the coal-fired power plants in the Lodz region of Poland

Radionuclide releases together with escaping fly ashes (from 45 x 10(6) kg in previous decades to 8 x 10(6) kg annually in 1996) from the main local and several small coal-fired power plants resulted in a relatively small increase in natural radioactivity levels in the Lodz region. The natural gamma terrestrial radiation dose rates (1 m above ground level) were measured at 82 points including in the vicinity of power plants, in the center of the town and on edge of the town. The average dose rate value for the first area was 36 +/- 1.2 nGy h (-1), whereas the same dose rate for the edge of town was slightly lower 30 +/- 0.9 nGy h (-1) but this difference was statistically significant. Further confirmation of the technologically slightly enhanced exposure of the local population to natural radionuclides was achieved by gamma-spectrometry measurement of the uranium and thorium decay series radionuclides in the surface soil profiles (up to 30 cm depth). The average increase of 226Ra and 232Th radionuclides in the top layer of soil (0-10 cm) according to the 20+/-30 cm depth layer was 21% and 17%, respectively. However, due to the relatively low levels of 232Th (14.3 Bq kg (-1)) and 238U (16.8 Bq kg (-1)) in this area, the annual average effective dose from the natural terrestrial radiation for the local population is also relatively low, 0.28 mSv only.     

Radionuclide content of building materials and associated gamma dose rates in Egyptian dwellings

Studies have been carried out to determine the natural radioactivity in some building materials (bricks, tiles, marble and ceramics) and their associated radiation hazard. The radioactivity concentrations of ²²⁶Ra ²³²Th and ⁴⁰K were measured using a gamma spectrometer with a Hp–Ge detector. The activities of ²³⁸U and ²³⁴U were measured using an alpha-spectrometer with a surface barrier detector after applying a radiochemical procedure. The ²³⁴U/²³⁸U isotopic ratios were calculated. The radium equivalent activities and the radiation hazard index associated with the natural radionuclides were calculated. A computer program was developed and applied to calculate the dose rate a person will receive from the walls of a room constructed from the studied building materials.     

Natural radionuclides in Austrian mineral water and their sequential measurement by fast methods

Ten samples of Austrian mineral water were investigated with regard to the natural radionuclides (228)Ra, (226)Ra, (210)Pb, (210)Po, (238)U and (234)U. The radium isotopes as well as (210)Pb were measured by liquid scintillation counting (LSC) after separation on a membrane loaded with element-selective particles (Empore Radium Disks) and (210)Po was determined by alpha-spectroscopy after spontaneous deposition onto a copper planchette. Uranium was determined by ICP-MS as well as by alpha-spectroscopy after ion separation and microprecipitation with NdF(3). From the measured activity concentrations the committed effective doses for adults and babies were calculated and compared to the total indicative dose of 0.1 mSv/a given in the EC Drinking Water Directive as a maximum dose. The dominant portion of the committed effective dose was due to the radium isotopes; the dose from (228)Ra in most samples clearly exceeded the dose from (226)Ra.