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.     

Soil-to-plant transfer factors for natural radionuclides and stable elements in a Mediterranean area

The transfer factors (TF) for natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 228Th), and 226Ra were obtained in plant samples (grass-pasture) growing in granitic and alluvial soils around a disused uranium mine located in the Extremadura region in the south-west of Spain. Affected and non-affected areas of the mine presented large differences in the activity concentrations of radionuclides of the uranium series. We also determined transfer factors for several stable elements (essential and non-essential). A set of statistical tests were applied to validate the data. The results showed that the transfer factors for both the natural radionuclides and the stable elements are independent of the two substrate types involved and also of the two areas considered in the study.     

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.     

Influence of soil texture on the distribution and availability of 238U, 230Th, and 226Ra in soils

The influence of soil texture on the distribution and availability of (238)U, (230)Th, and (226)Ra in soils was studied in soil samples collected at a rehabilitated uranium mine located in the Extremadura region in south-west Spain. The activity concentration (Bqkg(-1)) in the soils ranged from 60 to 750 for (238)U, from 60 to 260 for (230)Th, and from 70 to 330 for (226)Ra. The radionuclide distribution was determined in three soil fractions: coarse sand (0.5-2mm), medium-fine sand (0.067-0.5mm), and silt and clay (<0.067 mm). The relative mobility of the natural radionuclides in the different fractions was studied by comparison of the activity ratios between radionuclides belonging to the same radioactive series. The lability of these radionuclides in each fraction was also studied through selective extraction from the soils using a one-step sequential extraction scheme. Significant correlations were found for (238)U, (230)Th, and (226)Ra between the activity concentration per fraction and the total activity concentration in the bulk soil. Thus, from the determination of the activity concentration in the bulk soil, one could estimate the activity concentration in each fraction. Correlations were also found for (238)U and (226)Ra between the labile activity concentration in each fraction and the total activity concentration in bulk soil. Assuming that there is some particle-size fraction that predominates in the process of soil-to-plant transfer, the parameters obtained in this study should be used as correction factors for the transfer factors determined from the bulk soil in previous studies.     

The influence of a coal-fired power plant operation on radionuclide concentrations in soil

Fifty-two soil samples in the vicinity of a coal-fired power plant (CFPP) in Figueira (Brazil) were analyzed. The radionuclide concentration for the uranium and thorium series in soils ranged from <9 to 282 Bq kg(-1). The range of 40K concentration in soils varied from <59 to 412 Bq kg(-1). The CFPP (10 MWe) has been operating for 35 years and caused a small increment in natural radionuclide concentration in the surroundings. This technologically enhanced natural radioactivity (TENR) was mainly due to the uranium series (234Th, 226Ra and 210Pb) and was observable within the first kilometer from the power plant. The CFPP influence was only observed in the 0-25 cm soil horizon. The soil properties prevent the radionuclides of the 238U-series from reaching deeper soil profiles. The same behavior was observed for 40K as well. No influence was observed for 232Th, which was found in low concentrations in the coal.     

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.     

Radiological impacts of natural radioactivity in Abu-Tartor phosphate deposits, Egypt.

Phosphate and environmental samples were collected from Abu Tartor phosphate mine and the surrounding region. The activity concentration of 226Ra (238U) series, 232Th series and 40K were measured using a gamma-ray spectrometer. The activities of uranium isotopes (238U, 235U and 234U) and 210Pb were measured using an alpha spectrometer and a low-background proportional gas counting system, respectively, after radiochemical separation. The results are discussed and compared with the levels in phosphate rocks from different countries. It seems that the Abu Tartor phosphate deposit has the lowest radioactivity level of exploited phosphate of sedimentary origin. 226Ra/238U, 210Pb/226Ra, 234U/238U and 226Ra/228Ra activity ratios were calculated and are discussed. The radioactivity levels in the surrounding region and the calculated exposure dose (nGy/h) will be considered as a pre-operational baseline to estimate the possible radiological impacts due to mining, processing and future phosphate industrial activities. To minimize these impacts, the processing wastes should be recycled to the greatest possible extent.     

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.     

Soil to plant transfer of 238U, 226Ra and 232Th on a uranium mining-impacted soil from southeastern China

Both soil and plant samples of nine different plant species grown in soils from southeastern China contaminated with uranium mine tailings were analyzed for the plant uptake and translocation of 238U, 226Ra and 232Th. Substantial differences were observed in the soil-plant transfer factor (TF) among these radionuclides and plant species. Lupine (Lupinus albus) exhibited the highest uptake of 238U (TF value of 3.7x10(-2)), while Chinese mustard (Brassica chinensis) had the least (0.5x10(-2)). However, in the case of 226Ra and 232Th, the highest TFs were observed for white clover (Trifolium pratense) (3.4x10(-2)) and ryegrass (Lolium perenne) (2.1x10(-3)), respectively. 232Th in the tailings/soil mixture was less available for plant uptake than 226Ra or 238U, and this was especially evident for Chinese mustard and corn (Zea mays). The root/shoot (R/S) ratios obtained for different plants and radionuclides shown that Indian mustard had the smallest R/S ratios for both 226Ra (5.3+/-1.2) and 232Th (5.3+/-1.7), while the smallest R/S ratio for 238U was observed in clover (2.8+/-0.9).     

Fractionation of natural radionuclides in soils from the vicinity of a former uranium mine ?irovski vrh, Slovenia

As a result of former uranium mining and milling activities at ?irovski vrh, Slovenia, 0.6 million tons of uranium mill tailings (UMT) were deposited onto a nearby waste pile Boršt. Resulting enhanced levels of natural radionuclides in UMT could pose threat for the surrounding environment. Therefore, sequential extraction protocol was performed to assess mobility and bioavailability of ²³⁸U, ²³⁴U, ²³⁰Th and ²²⁶Ra in soils from the waste pile and its surrounding. The radionuclides associated with exchangeable, organic, carbonate, Fe/Mn oxides and residual fraction, respectively, were determined. Results showed that the highest activity concentrations for the studied radionuclides were on the bottom of the waste pile. In non-contaminated locations, about 80% of all radionuclides were in the residual fraction. Considering activity concentrations in the UMT, ²³⁸U and ²³⁴U are the most mobile. Mobility of ²²⁶Ra is suppressed by high sulphate concentrations and is similar to mobility of ²³⁰Th.     

Biomagnification of 7Be, 234Th, and 228Ra in marine organisms near the northern Pacific coast of Japan

Enrichment of natural radionuclides of thorium, radium and beryllium in several kinds of marine organisms was investigated near the Pacific coast of Miyagi Pref., Japan. The radioactivity of 7Be, 210Pb, 234Th, 238U, 228Ra and 137Cs was measured using gamma spectrometry. High concentrations of 234Th were observed in ascidian livers (50-400 Bq/kg dry) and excrement (2000-2900 Bq/kg dry), although the parent 238U concentrations were less than 3 Bq/kg dry. Such extreme disequilibrium between 238U and 234Th activity was observed in other organisms (barnacles, mussels and brown algae). Relatively high concentrations of 228Ra were detected in ascidian livers and were observed to decrease according to its half-life (5.75 year), suggesting disequilibrium with its parent 232Th. High concentrations (about 1900-5000 Bq/kg dry) of 7Be were detected in ascidian liver. Possible mechanisms for the observed biomagnification and bioaccumulation of these radionuclides in the organisms analyzed were proposed.     

Natural radioactivity, dose assessment and uranium uptake by agricultural crops at Khan Al-Zabeeb, Jordan

Khan Al-Zabeeb, an irrigated cultivated area lies above a superficial uranium deposits, is regularly used to produce vegetables and fruits consumed by the public. Both soil and plant samples collected from the study area were investigated for their natural radioactivity to determine the uranium uptake by crops and hence to estimate the effective dose equivalent to human consumption. Concentrations of (238)U, (235)U, (232)Th, (226)Ra, (222)Rn, (137)Cs and (40)K in nine soil profiles were measured by gamma-ray spectrometry whereas watermelon and zucchini crops were analyzed for their uranium content by means of alpha spectrometry after radiochemical separation. Correlations between measured radionuclides were made and their activity ratios were determined to evaluate their geochemical behavior in the soil profiles. Calculated soil-plant transfer factors indicate that the green parts (leaves, stems and roots) of the studied crops tend to accumulate uranium about two orders of magnitude higher than the fruits. The maximum dose from ingestion of 1 kg of watermelon pulp was estimated to be 3.1 and 4.7 nSv y(-1) for (238)U and (234)U, respectively. Estimations of the annual effective dose equivalent due to external exposure showed extremely low values. Radium equivalent activity and external hazard index were seen to exceed the permissible limits of 370 Bq kg(-1) and 1, respectively.     

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

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

Fractionation of natural radionuclides in soils from a uranium mineralized area in the south-west of Spain

A new version of a classical method was applied to study the distribution of natural radionuclides (238U, 230Th, and 226Ra) in the soil fractions obtained by a sequential extraction procedure. The potential significance of the fractions obtained with this method was tested on two very similar soils but with very different contents of the three radionuclides, collected in the proximity of a disused uranium mine located in the Extremadura region in the south-west of Spain. The results confirmed that, if only non-residual fractions are considered, the sequential method applied shows a characteristic speciation pattern of these natural radionuclides in this soil matrix, i.e., the distribution of each of the three radionuclides was very similar for the two soil samples.     

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.     

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.     

Radionuclides in hot mineral spring waters in Jordan

Hot mineral springs in Jordan are very attractive to people who seek physical healing but they are unaware of natural radioactive elements that may be contained in the hot mineral water. The activities of the natural radioactive isotopes were measured and the concentrations of the parents of their natural radioactive series were calculated. The measured radionuclides were 234Th, 226Ra, 214Pb, 214Bi, 228Ac, 228Th, 212Pb, 212Bi and 208Tl. In addition the activities of 235U and 40K were measured. The activities ranged from 0.14 to 34.8 Bq/l, while the concentrations of parent uranium and thorium isotopes ranged from 3.0 x 10(-3) to 0.59 mg/l. The results were compared with those for drinking water.     

Invariance of isotope ratios of lithogenic radionuclides: more evidence for their use as sediment source tracers

Activities of radionuclides in the 238U (230Th, 226Ra, 210Pb) and 232Th (232Th, 228Th, 228Ra) decay series were determined in sediments from an east Texas watershed and examined with isotope ratios and compared to particulate organic carbon (POC), % fines (<63 microm) and total concentrations of Al, Fe and Mn. The objective was to elucidate the presence or absence of relationships affecting the effectiveness of these radionuclides in modeling sediment transport. Strong positive correlations were observed between radionuclides and Mn (Th) and % fines (Ra and Th). Isotope ratios effectively reduce these influences, supporting the contention that isotope ratios offset extrinsic variability in terrestrial sediments. Strong associations of 210Pbxs (excess 210Pb) and 226Ra/230Th with POC agree with data from marine and terrestrial settings, indicating that the role of POC in isotope fractionation, transport and sequestration merits further investigation.     

Natural radionuclides and (137)Cs distributions and their relationship with sedimentological processes in Patras Harbour, Greece

Surficial and subsurficial sediment samples derived from gravity cores, selected from the harbour of Patras, Greece, were analyzed for grain size, water content, bulk density, specific gravity, organic carbon content and specific activities of natural radionuclides and (137)Cs. The specific activities of (232)Th, (226)Ra, (40)K and (137)Cs were measured radiometrically. The radionuclides (238)U and (232)Th were also analyzed using the INAA. The differences found between the specific activities of the natural radionuclides measured by the two methods are of no statistical significance. The sediment cores selection was based on a detailed bathymetric and marine seismic survey. Through the study of the detailed bathymetric map and the seismic profiles it was shown that ship traffic is highly influential to the harbour bathymetry. The granulometric and geotechnical properties of the sediments and therefore the specific activities of the natural radionuclides and (137)Cs seem to be controlled by the ship traffic. Relationship between radionuclide activity concentrations and granulometric/geotechnical parameters was defined after the treatment of all the analyses using R-mode factor analysis. The natural radionuclide activities are related to the fine fraction and bulk density of the sediments, while (137)Cs is mainly influenced by the organic carbon content. In addition, (238)U and (226)Ra seem to be in close relation with the heavy minerals fraction in coarse-grained sediments with high specific gravity.     

Natural activities of 40K, 238U and 232Th in elephant grass (Pennisetum purpureum) in Ibadan metropolis, Nigeria

Samples of elephant grass collected at some pasturing farmlands across different locations in Ibadan metropolis were analyzed for their natural radioactivity concentrations due to 40K, 238U and 232Th radionuclides. Radioactivity measurements were carried out using gamma-ray spectroscopy. The average radioactivity concentration of 40K was found to be 25.7+/-5.5 Bq kg(-1) for 238U and 33.4+/-3.9 Bq kg(-1) for 232Th. The radiological health implication to the population that may result from these values is found to be very low and almost insignificant. No artificial radionuclide, however, was detected in any of the samples, hence, measurements have been taken as representing baseline values of these radionuclides in the grass in the metropolis.