Environmental assessment of arsenic released from potential pollution sources

An assessment study of the environmental pathways of arsenic released from a coal-fired power plant (CFPP) or introduced into soil as a contaminant by phosphatic fertilizers has been carried out using a time-dependent forecasting model.The long-term predictions indicate that arsenic can be taken up by plants and that it can migrate into the groundwater system through soil layers. However, arsenic exhibits such a high degree of mobility that its retention and accumulation in biota should remain low. This fact may explain the relatively low concentrations of arsenic in environmental media as well as in groundwater systems.     

Leachable 226Ra in Philippine phosphogypsum and its implication in groundwater contamination in Isabel, Leyte, Philippines

Phosphogypsum (PG), the major waste material in phosphate fertilizer processing, has been known to contain enhanced levels of naturally-occurring radionuclides especially (226)Ra.The lack of radioactivity data regarding Philippine phosphogypsum and its environmental behavior in the Philippine setting has brought concern on possible contamination of groundwater beneath the phosphogypsum ponds in Isabel, Leyte, Philippines. The radioactivity of Philippine phosphogypsum was determined and the leaching of (226)Ra from phosphogypsum and through local soil was quantified. Level of (226)Ra in groundwater samples in Isabel, Leyte, Philippines was also quantified to address the primary concern. It was found that the (226)Ra activity in Philippine phosphogypsum is distributed in a wide range from 91.5 to 935 Bq/kg. As much as 5% of (226)Ra can be leached from Philippine PG with deionized water. In vitro soil leach experiments suggest that the soil in the phosphate fertilizer plant area would be able to deter the intrusion of (226)Ra into the water table. Compared to reported values of natural groundwater levels of (226)Ra, the concentration of this radionuclide in Isabel, Leyte groundwater suggest that there is no (226)Ra intrusion brought about by the presence of phosphogypsum ponds in the area.     

Edaphic factors affecting the vertical distribution of radionuclides in the different soil types of Belgrade, Serbia

The specific activities of natural radionuclides ((40)K, (226)Ra and (232)Th) and Chernobyl-derived (137)Cs were measured in soil profiles representing typical soil types of Belgrade (Serbia): chernozems, fluvisols, humic gleysols, eutric cambisols, vertisols and gleyic fluvisols. The influence of soil properties and content of stable elements on radionuclide distribution down the soil profiles (at 5 cm intervals up to 50 cm depth) was analysed. Correlation analysis identified associations of (40)K, (226)Ra and (137)Cs with fine-grained soil fractions. Significant positive correlations were found between (137)Cs specific activity and both organic matter content and cation exchange capacity. Saturated hydraulic conductivity and specific electrical conductivity were also positively correlated with the specific activity of (137)Cs. The strong positive correlations between (226)Ra and (232)Th specific activities and Fe and Mn indicate an association with oxides of these elements in soil. The correlations observed between (40)K and Cr, Ni, Pb and Zn and also between (137)Cs and Cd, Cr, Pb and Zn could be attributed to their common affinity for clay minerals. These results provide insight into the main factors that affect radionuclide migration in the soil, which contributes to knowledge about radionuclide behaviour in the environment and factors governing their mobility within terrestrial ecosystems.     

Radioactivity levels in major French rivers: summary of monitoring chronicles acquired over the past thirty years and current status

Since the beginning of the 1990 s, liquid releases of gamma-emitting radionuclides from French nuclear facilities have generally fallen by almost 85%. Almost 65% of gamma-emitting liquid effluents released into freshwater rivers concerned the River Rh?ne (Southeast France), with around 85% of this originating from the Marcoule spent fuel reprocessing plant. Upstream of French nuclear plants, artificial radionuclides still detected by gamma spectrometry in 2006, include (137)Cs, (131)I as well as (60)Co, (58)Co and (54)Mn in the case of the Rhine (Switzerland nuclear industries). In the wake of the fallout from the Chernobyl accident, (103)Ru, (106)Rh-Ru, (110 m)Ag, (141)Ce and (129)Te were detected in rivers in the east of France. Some of these radionuclides were found in aquatic plants until 1989. In eastern France, (137)Cs activity in river sediments and mosses is still today two to three times greater than that observed in similar environments in western France. No (134)Cs has been detected upstream of nuclear plants in French rivers since 2001. Downstream of nuclear plants, the gamma emitters still detected regularly in rivers in 2006 are (137)Cs, (134)Cs, (60)Co, (58)Co, (110 m)Ag, (54)Mn, (131)I, together with (241)Am downstream of the Marcoule spent fuel reprocessing plant. Alpha and beta emitters such as plutonium isotopes and (90)Sr first entered freshwaters at the early 1950s due to the leaching of soils contaminated by atmospheric fallout from nuclear testing. These elements were also introduced, in the case of the Rh?ne River, via effluent from the Marcoule reprocessing plant. Until the mid 1990 s, plutonium isotope levels observed in the lower reaches of the Rh?ne were 10 to 1000 times higher than those observed in other French freshwaters. Data gathered over a period of almost thirty years of radioecological studies reveal that the only radionuclides detected in fish muscles are (137)Cs, (90)Sr, plutonium isotopes and (241)Am. At the scale of the French territory, there is no significant difference since the mid 1990 s between (137)Cs activity observed downstream of nuclear facilities and that observed upstream, whether in sediments, mosses and fish. Finally, this study highlights that the natural radioactivity of surface freshwaters are around 25 times greater than artificial radioactivity from gamma emitters. However, non gamma emitters released by nuclear industries, such as (3)H, may lead to artificial activity levels 2 to 20 times higher than natural levels.     

Study on transfers of uranium, thorium and decay products from grain, water and soil to chicken meat and egg contents

Activity concentrations of the uranium and thorium series radionuclides were determined in chicken meat and eggs as well as in soil, water and other dietary intakes of poultry at five sites of the French territory. These data allow the calculation of transfer coefficients which enrich the database given by the technical report series no. 472 of the IAEA. In egg contents, the highest activity concentrations (in mBq kg(-1) fresh weight) are for (226)Ra, ranging between 136 and 190 and are much lower for uranium (between 0.51 and 1.30 for (238)U). In chicken meat, (238)U activity concentration is higher than in egg contents and ranges between 1.7 and 9.7. Concerning (232)Th, its activity concentration is lower than uranium and ranges between 0.5 and 4.9. Daily ingested activity concentration by the animals was assessed taking into account the activity concentrations measured in the grains, in the soil and in the drinking water. The activity concentration in grains and the daily intakes allow the calculation of concentration ratios and transfer coefficients for chicken meat and egg contents. In chicken meat the transfer coefficients (d kg(-1)) range between 0.0018 and 0.0073 for (238)U and between 0.0008 and 0.0028 for (232)Th. In egg contents they range from 0.00018 to 0.0018 for (238)U and are much higher for radium isotopes (0.10-0.23 for (226)Ra and 0.07-0.11 for (228)Ra).     

Radium equivalent activity in the light of UNSCEAR report

Radium equivalent activity (Ra ( eq )) has been in practice for the last 40 years for the assessment of radiological hazard of radioactivity in environmental materials. The in-practice model for the calculation of the Ra ( eq ) has been critically reviewed in the light of the UNSCEAR 2000 report. Annual effective dose (E) values of (232)Th and (40)K were found to be not equal to that of (226)Ra derived from the activity concentrations of these radionuclides used in the expression for the Ra ( eq ). Therefore, a modified model has been proposed for the determination of the Ra ( eq ) for outdoor external exposure to gamma rays. The relation between the E and Ra ( eq ) has been explored. It is recommended that while describing the radiological hazard of the materials containing radioactivity, there should be no need to calculate the Ra ( eq ) if the E has already been determined or vice versa.     

Radiochemical characterization of mineral waters in the Eastern Black Sea Region, Turkey

This study has evaluated the levels of natural radionuclides and chemical components of mineral waters in the Eastern Black Sea Region (Turkey). The mean activity concentrations of (226)Ra, (232)Th, (137)Cs, (40)K, gross alpha and gross beta were found as 129, 33, 28, 714, 125 and 170 mBq L(-1), respectively. Due to consumption of mineral waters, the radiological impact of them on the inhabitants was calculated by taking the annual intake into account through ingestion of aforementioned radionuclides. The estimated effective doses from mineral water were found to be 13.20 μSv year(-1) ((226)Ra), 2.74 μSv year(-1) ((232)Th), 0.13 μSv year(-1) ((137)Cs) and 1.62 μSv year(-1) ((40)K). The overall contribution of these radionuclides to the committed effective dose from a year's consumption of mineral water in the region is therefore estimated to be only 17.69%, which is in concordance with the recommended WHO value (100 μSv year(-1)). The chemical analysis results showed that these waters contain Na, Al, P, Cl, K, Ca, V, Mn, Fe, Ni, Cu and Zn elements. These values were evaluated and compared with the internationally verified values. This study provides important information for consumers and authorities because of their internal radiochemical exposure risk from mineral water intake.     

Radioactivities related to coal mining

Natural radioactivity concentrations due to the coal mining in Gabal El-Maghara, North Sinai, Egypt, were determined using gamma-ray spectroscopy. Coal, water and soil samples were investigated in this study. The (226)Ra, (232)Th and (40)K activity concentrations in coal before extraction were 18.5 +/- 0.5, 29.5 +/- 1.2 and 149.0 +/- 8.4 Bq kg(-1), respectively. These concentrations were reduced to 18-22% after extraction due to the clay removal of the coal ore. The activity contents of the water and soil samples collected from the surrounding area did not show any evidence of enhancement due to the mining activities. Absorbed dose rate and effective dose equivalent in the mine environment were 29.4 nGy h(-1) and 128.0 microSv a(-1), respectively. The measured activity concentrations in the mine environment and the surrounding areas (5 km away from the mine) are similar to that found in other regions in North and South Sinai. Based on the measurements of gamma-ray emitting radionuclides, the mine activity does not lead to any enhancement in the local area nor represents any human risk.     

Actinides and decay products in selected produce and bioindicators in the vicinity of a uranium plant

Cypress needles collected at the edge of the Malvési uranium facility (SW France) exhibit enhanced activities of actinides and some decay products (uranium, americium, plutonium, (230)Th, (226)Ra) compared to a remote site. These enhanced activities resulted from the release of U via smokestacks and passive release from former artificial ponds located inside the nuclear site. Enhanced activities are also observed in selected produce (wheat, lettuce, fruits) sampled from the edge of the site. However, excess actinides measured in wheat grains in 2007 are inconsistent with the activities and the uranium ratio measured in the soils. This result suggests that the studied annual crops were contaminated mainly through the short-term release of airborne actinides, and that other transfer pathways, such as, uptake through the roots or adhesion of soil particles, were negligible.     

Implementation of Neural Networks for Classification of Moss and Lichen Samples on the Basis of Gamma-Ray Spectrometric Analysis

Mosses and lichens have an important role in biomonitoring. The objective of this study is to develop a neural network model to classify these plants according to geographical origin. A three-layer feed-forward neural network was used. The activities of radionuclides ((226)Ra, (238)U, (235)U, (40)K, (232)Th, (134)Cs, (137)Cs and (7)Be) detected in plant samples by gamma-ray spectrometry were used as inputs for neural network. Five different training algorithms with different number of samples in training sets were tested and compared, in order to find the one with the minimum root mean square error. The best predictive power for the classification of plants from 12 regions was achieved using a network with 5 hidden layer nodes and 3,000 training epochs, using the online back-propagation randomized training algorithm. Implementation of this model to experimental data resulted in satisfactory classification of moss and lichen samples in terms of their geographical origin. The average classification rate obtained in this study was (90.7 +/- 4.8)%.     

Natural radioactivity and chemical concentrations in Egyptian groundwater

Measurements of natural radioactivity in drinking water have been performed in many parts of the world, mostly for assessment of the doses and risk resulting from consuming water. A study of the radionuclide and chemical components in groundwater from Beni Suef Governate, Egypt has been carried out. Fifty water samples were analyzed by gamma ray spectroscopy to determine the ²²⁶Ra, ²³²Th, and ⁴⁰K concentrations; major elements, pH, alkalinity, and conductivity were also measured. The specific activity values ranged from 0.008 to 0.040 Bq/l for ²²⁶Ra, from 0.003 to 0.019 Bq/l for ²³²Th, and from 0.025 to 0.344 Bq/l for ⁴⁰K. The annual ingestions of these radionuclides, using local consumption rates (average over the whole population) of 1.5 l day^???1, were estimated to be 8.59, 4.86, and 83.47 Bq year^???1 for ²²⁶Ra, ²³²Th, and ⁴⁰K, respectively. The estimated values and weighted means of these radionuclides compare well with the world average. The estimated effective doses from drinking water were found to be 2.4 ??Sv year^???1 (²²⁶Ra), 1.1 ??Sv year^???1 (²³²Th), and 0.51 ??Sv year^???1 (⁴⁰K). Contribution of these radionuclides to the committed effective dose from 1 year consumption of drinking water is estimated to be only 4%.     

Distribution of gamma-ray emitting radionuclides in the marine environment of the Burullus Lake: II. Bottom sediments

The sediment compartment has the ability to trap large amounts of radionuclides and to indicate the radiological impact of pollution. The present work shows the results obtained related to the concentrations of ¹³⁷Cs and natural radionuclides in sediment in the Burullus Lake, Egypt. The average values of ²²⁶Ra, ²³²Th, and ⁴⁰K in the bottom sediments collected from the east of the Burullus Lake ranged from 10.3 to 21.8 Bq/kg, from 11.9 to 34.4 Bq/kg, and from 268 to 401 Bq/kg, respectively. The study has shown that ⁴⁰K concentration is nearly uniform throughout the studied area while ²²⁶Ra and ²³²Th are more concentrated in the northeastern shore. Lake sediments showed contamination with ¹³⁷Cs (2.7–15.9 Bq/kg). The ¹³⁷Cs sediment activities indicated higher concentrations in the off-shore sites. Concentrations of all γ -ray emitting radionuclides except ⁴⁰K in water samples were below the detection limits. The ⁴⁰K sediment–water distribution coefficients of the near-shore samples were higher than the off-shore samples.     

Radiological study of exposure levels in El Maghara underground coal mine

Coal is largely composed of organic matter, but it is the inorganic matter in coal minerals and trace elements that have been cited as possible causes of health, environmental and technological problems associated with the use of coal. Some trace elements in coal are naturally radioactive. These radioactive elements include uranium (U), thorium (Th) and their numerous decay products, including radium (Ra) and radon (Rn). Although these elements are less chemically toxic than other coal constituents, such as arsenic, selenium or mercury, questions have been raised concerning the possible risk from radiation. In order to accurately address these questions and to predict the mobility of radioactive elements during the coal fuel cycle, it is important to determine the specific activity, distribution and form of radioactive elements in coal. The assessment of the radiation exposure from coal burning is critically dependent on the specific activity of radioactive elements in coal and in the fly ash that remains after combustion. The El-Maghara coal mine is the only producing coal mine in Egypt. It is located in the middle of the Sinai desert about 250 km north-east of Cairo, where a coal-fired power plant is intended to be built. In this study, a pre-operational radiological baseline of the site and the occupational radiation exposures due to radon progeny in the mine were determined. The specific activities of 226Ra, 232Th and 40K in soil and coal dust samples collected along the main gallery ranges were found to be 6-22.9, 9.6-47.3 and 77-489 Bq kg-1, respectively. Soil samples collected around the mine showed concentrations of 226Ra, 232Th and 40K in the ranges 2.7-20.2, 3.2-12.6 and 14.6-201 Bq kg-1, respectively. All of the mean values of radon progeny were lower than the action levels for working places recommended in the International Commission on Radiological Protection (ICRP) 65.     

226Ra in Tap and Mineral Water and Related Health Risk in the Republic of Croatia

The presence of 226Ra in drinking water may sometimes make important contribution to natural background radiation exposures. The paper describes the study of 226Ra content in drinking water of Croatia: tap water from the public supply system of several major towns and bottled mineral water from two selected mineral water springs. 226Ra was determined by alpha-spectrometric measurement after radiochemical separation. The radiation doses originating from drinking tap water and bottled mineral water were estimated. The annual dose from consumption of bottled mineral water was compared to that received from ingestion of public system tap water. The study showed that 226Ra content for investigated categories of waters is below the levels at which any unacceptable dose due to ingestion would arise.     

Total effective dose equivalent assessment after exposure to high-level natural radiation using the RESRAD code

The current work reports the activity concentrations of several natural radionuclides (²²⁶Ra, ²³²Th, and ⁴⁰K) in Khak-Sefid area of Ramsar, Iran. An evaluation of total effective dose equivalent (TEDE) from exposure to high-level natural radiations is also presented. Soil samples were analyzed using a high-purity germanium detector with 80 % relative efficiency. The TEDE was calculated on a land area of 40,000 m² with 1.5-m thickness of contaminated zone for the member of three critical groups of farmer, construction worker, and resident using Residual Radioactive Material Guidelines (RESRAD) modeling program. It was found that the mean activity concentrations (in Bq/kg) were 23,118?±?468, 25.8?±?2.3, and 402.6?±?16.5 for ²²⁶Ra, ²³²Th, and ⁴⁰K, respectively. The maximum calculated TEDE during 1,000 years was 107.1 mSv/year at year 90, 92.42 mSv/year at year 88, and 22.09 mSv/year at year 46 for farmer, resident, and construction worker scenarios, respectively. The maximum TEDE in farmer scenario can be reduced to the level below the dose limit of 1 mSv/year which is safe for public health using soil cover with thickness of 50 cm or more on the contaminated zone. According to RESRAD prediction, the TEDE received by individuals for all exposure scenarios considerably exceed the set dose limit, and it is mainly due to ²²⁶Ra.     

Distribution of radionuclides in surface soils, Singhbhum Shear Zone, India and associated dose

Gamma emitters were estimated in surface soils from a mineralized zone in Eastern India using high purity Germanium detector-based high resolution gamma spectrometry system. Activities of ²³⁸U, ²²⁶Ra, ²³²Th, ²³⁵U, ²²⁷Th, ^234mPa, ²¹⁰Pb, ⁴⁰K, and ¹³⁷Cs were 79?±?50, 81?±?53, 65?±?23, 4?±?2, 5?±?4, 92?±?50, 97?±?45, 517?±?201, and 4?±?2 Bq/kg, respectively. Most radionuclides were observed to follow log-normal distribution. The correlation between physicochemical properties of the samples, like pH, organic matter content, particle size, and moisture content were also studied. Activity ratios of ²²⁶Ra/²³⁸U, ²¹⁰Pb/²²⁶Ra, and ²²⁷Th/²³⁵U indicated deviation from secular equilibrium in some samples. The associated annual effective dose ranged from 0.07 to 0.24 mSv and the mean was calculated to be 0.12?±?0.04 mSv for this region, indicating it to be one of normal natural background radiation.     

An independent review and prioritization of past radionuclide and chemical releases from the Los Alamos National Laboratory--implications for future dose reconstruction studies

From 1999 through 2010, a team of scientists and engineers systematically reviewed approximately eight million classified and unclassified documents at Los Alamos National Laboratory (LANL) that describe historical off-site releases of radionuclides and chemicals in order to determine the extent to which a full-scale dose reconstruction for releases is warranted and/or feasible. As a part of this effort, a relative ranking of historical airborne and waterborne radionuclide releases from LANL was established using priority index (PI) values that were calculated from estimated annual quantities released and the maximum allowable effluent concentrations according to The U.S. Nuclear Regulatory Commission (USNRC). Chemical releases were ranked based on annual usage estimates and U.S. Environmental Protection Agency (USEPA) toxicity values. PI results for airborne radionuclides indicate that early plutonium operations were of most concern between 1948 and 1961, in 1967, and again from 1970 through 1973. Airborne releases of uranium were found to be of most interest for 1968, from 1974 through 1978, and again in 1996. Mixed fission products yielded the highest PI value for 1969. Mixed activation product releases yielded the highest PI values from 1979 to 1995. For waterborne releases, results indicate that plutonium is of most concern for all years evaluated with the exception of 1956 when (90)Sr yielded the highest PI value. The prioritization of chemical releases indicate that four of the top five ranked chemicals were organic solvents that were commonly used in chemical processing and for cleaning. Trichloroethylene ranked highest, indicating highest relative potential for health effects, for both cancer and non-cancer effects. Documents also indicate that beryllium was used in significant quantities, which could have lead to residential exposures exceeding established environmental and occupational exposure limits, and warrants further consideration. In part because of the close proximity of residents to LANL, further study of historical LANL releases and the potential impact to public health is recommended for those materials with the largest priority index values; namely, plutonium, uranium, and selected chemicals.     

Distributions of 210Pb around a uraniferous coal-fired power plant in Western Turkey

In the present study the spatial and the vertical distributions of 210Pb were investigated in the soils around a uranifereous coal fired power plant (CPP) in Yatagan Basin, in Western Turkey. The variation of 226Ra activity along the soil profiles was studied to assess the unsupported 210Pb distribution in the same samples. 226Ra was measured by gamma spectroscopy and 210Pb activities were determined from 210Po activities using radiochemical deposition and alpha spectroscopy. The total 210Pb activity concentrations in bulk core samples varied in the range of 38-250 Bq kg(-1) in the study sites and of 22-78 Bq kg(-1) in reference site. In the sectioned cores sampled from the study areas the ranges for activity concentrations of 226Ra, total 210Pb and unsupported 210Pb are 24-77; 39-344 and 4-313 Bq kg(-1), respectively. Corresponding ranges for reference site are 37-39; 39-122 and 1-83 Bq kg(-1).     

Monitoring DNA damage in wood small-reed (Calamagrostis epigejos) plants growing in a sediment reservoir with substrates from uranium mining

For most plant species growing in polluted areas genotoxicity assays are not available. We have studied the possibility of using the alkaline protocol of the Comet assay as a method for detecting induced DNA damage in a grass Calamagrostis epigejos, growing wild in highly polluted areas. To calibrate the Comet assay for C. epigejos, two model mutagens were applied: the monofunctional alkylating agent ethyl methanesulfonate (EMS) and gamma-rays. With increasing concentrations of EMS (0 to 10 mM, 18 h treatment at 26 degrees C) applied on excised leaves, the DNA damage, as expressed by the tail moment (TM) values, increased from 4.7 +/- 0.9 to 60.8 +/- 2.7 microns. After gamma irradiation (0 to 30 Gy) the TM value increased from 4.2 +/- 0.2 to 48.1 +/- 1.7 microns. A 24 to 72 h recovery of leaves after EMS treatment in an EMS-free medium did not result in a significant change in the induced EMS damage. By contrast, a 24 h recovery after gamma-irradiation led to a complete repair of DNA damage measurable by the Comet assay. We have measured the DNA damage in nuclei of leaves of C. epigejos plants growing in the area of a sediment reservoir with substrates from uranium mining, where the ore was exploited through leaching with sulfuric acid. The average specific activity of natural radionuclides measured in the substrate was for 226Ra = 11,818 Bq kg-1, for 232Th = 66 Bq kg-1 and for 40K = 75 Bq kg-1. No significant increase in the DNA damage in plants growing on the sediment substrate above the DNA damage in control plants was detected by the Comet assay.     

Determination of 226Ra at ultratrace level in mineral water samples by sector field inductively coupled plasma mass spectrometry

An analytical procedure has been proposed for the determination of (226)Ra at the low femtogram per ml concentration level in mineral water samples using double focusing sector field ICP-MS (ICP-SFMS). For the pre-concentration and separation of radium from the matrix elements in water a tandem of a laboratory-prepared filter, based on MnO(2), and Eichrom "Sr-specific" resin was used. The recovery of the method was determined to be 70.5%. The limit of detection for (226)Ra determination was 0.02 fg ml(-1), including a pre-concentration factor of 10. In addition, uranium concentration and uranium isotope ratios were measured by ICP-SFMS. In several mineral water samples with a relatively high uranium content, (226)Ra concentrations were found between 0.7-15 fg ml(-1). The effective dose of the contribution was calculated using the radionuclide concentration and dose conversion factors from the World Health Organization, WHO (1993). Assuming a mineral water consumption of 2 l d(-1), a slightly higher calculated dose than the suggested limit for drinking water (0.1 mSv y(-1)) was found in some samples.