Radiological characterization and environmental impact in northwestern coast of Egypt

A study of environmental radioactivity along the northwestern coast of Egypt was performed by the Central Laboratory for Environmental Radioactivity Measurements Inter-comparison and Training within the framework of the research project: Radiological Studies/Measurements of Natural and Man-made Radionuclides in the Environment. The present paper contains important conclusions, correlations and interpretations of the environmental measurements. The samples collection and measurements were conducted according to the Egyptian Atomic Energy Authority monitoring plan for locations along the northwestern coast of Egypt and its main tributaries of interest. The specific activities of ²²⁶Ra (²³⁸U series), ²²⁸Ra (²³²Th series), ⁴⁰K and ¹³⁷Cs (Bq/kg dry weight) were measured using gamma-ray spectrometers based on hyper-pure germanium detectors. 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 were calculated for evaluation of the geo-chemical behavior of these radionuclides. Samples textures and CaCO₃ and total organic matter contents of sediments were also determined while the pH, major cations and anions such as Na⁺, K⁺, Ca⁺⁺, Mg⁺⁺and Cl^?, SO₄ ^– and HCO₃, respectively were also determined in water samples.     

Leaching of uranium,radium and thorium from vertisol soil by ground water

Shallow land burial is routinely used for the disposal of low-level radioactive waste. Natural processes causing leaching of radionuclides can lead to contamination of surrounding ground water and soil by the radionuclides. The comparative leachability of radionuclides U_(nat), ²²⁶Ra, ²²⁸Ra and Th_(nat) from the soil of a radioactive waste disposal site, by ground water was evaluated. The probability of leaching was obtained in the following order Ra (≈77%) > U (≈40%) > Th (≈20%). Observed ratios (OR) were calculated to correlate leachability of radionuclides to that of major cations Ca²⁺ and Mg²⁺. The leaching of the radionuclides was seen to be dependent on Ca²⁺ and SO₄²⁻ leached from the soil. This study provides sitespecific leachability of radionuclides, that can be used as indicator of the tendency for migration or retention in soil. It can play an important role during an unforeseen accident like breach of containment at the waste disposal site leading to contamination of soil and ground water and causing hazard to public via drinking water route.     

Transfer of 226Ra, 85Sr and 137Cs from milk to milk products</p> </p>

Summary Transfer of ²²⁶Ra, ⁸⁵Sr and ¹³⁷Cs from cow and sheep milk to various Syrian dairy products has been evaluated. Dairy products include Kashkivan cheese, braided cheese, Haloom cheese, Sircassian cheese, liquid cheese, native cheese, cottage, thick yogurt, butter and milk cream. The results showed that the percentage of ²²⁶Ra, ⁸⁵Sr and ¹³⁷Cs transferred from cow milk to milk cream (P_t=food processing retention factor′processing efficiency′100%) has reached 32%, 16% and 7%, respectively. Butter and liquid cheese were found to have the lowest percentage of transferred 226Ra, ⁸⁵Sr and ¹³⁷Cs. Most of the obtained P_t values of the studied radionuclides in thick yogurt were relatively low in spite of the high processing efficiencies of thick yogurt. Moreover, the transfer, P_t, of the studied radionuclides from cow milk to the prepared cheese was higher than those values determined for sheep milk. This is due to differences in chemical compositions of each type of milk. On the other hand, the treatment of Native cheese, most commonly consumed cheese in Syria, with different concentrations of NaCl solutions showed that ¹³⁷Cs was completely removed from cheese soaking in 5% NaCl solution (soaking time of 48 hours), while 40% of ²²⁶Ra and 80% of ⁸⁵Sr were also decontaminated using 0-2.5% NaCl solutions and soaking time of 48 hours. Based on the obtained results, industrialization processes of the dairy products that resulted the removal of radionuclides have been identified.</p> </p>     

Determination of natural radioactivity in Euphrates river

Levels of naturally occuring radionuclides (radium isotopes, U isotopes, ²¹⁰Po and ²¹⁰Pb) in water, sediments and biota samples collected from Euphrates river during the 1999–2000 period have been determined. Results have shown that the water contained relatively high levels of ²²⁶Ra; the largest value of 1150 mBq·l^–1 was observed. These relatively high levels of ²²⁶Ra, which is one of the main radioactive contaminants in the oil industry, may be due to past discharges of production water from the oil fields situated near the river banks. ²²⁶Ra/²³⁸U activity ratio was found to be more than unity in all water samples varying between 13 and 242. In addition, the results of sediment analyses have also shown lower values for ²²⁸Ra/²²⁶Ra activity ratio than unity in those samples collected nearby the oil fields. Moreover, concentrations of other naturally occurring radionuclides such as uranium isotopes, ²¹⁰Po and ²¹⁰Pb for most samples (water, sediments and biota) were found to be within the natural levels and in agreement with those values reported for other local and international studies. Only mussel species were found to contain high levels of ²¹⁰Po, about 1335 Bq·kg^–1 dry mass was observed in Anodonta sp species. However, the results of this study can be considered a baseline for monitoring of future changes. A regional research project (including Turkey, Syria and Iraq) to study this river (from the Anatolia Mountains to the Arabian Gulf) is necessary to determine the impact of all potential sources of contaminants.This revised version was published online in November 2005 with corrections to the Cover Date.     

Influence of freezing on physicochemical forms of natural and technogenic radionuclides in Chernozem soil

Sharp variations of different climatic parameters influence the transport, transfer, and deposition of contaminants in nature. Investigations of the impact of environmental temperature on the fractionation of radionuclides in soil are necessary for adequate assessment of their distribution and bioavailability in case of a nuclear accident. The impact of a sharp decrease of environmental temperature shortly after radioactive contamination on the physicochemical fractionation of natural and technogenic radionuclides in Chernozem soil and its influence on their potential migration ability and bioavailability in case of subsequent warming were evaluated. The soil was contaminated in a laboratory with ²⁴¹Am, ⁶⁰Co, ¹³⁷Cs, ²²⁸Ra, ²³⁴Th, and U and two temperature regimes were used for storage. Changes of the radionuclides association with various soil phases in the first weeks after contamination were studied. Physicochemical forms of ²⁴¹Am, ⁶⁰Co, ²²⁸Ra, ²³⁴Th, and U were determined using two sequential extraction procedures. The ion-exchangeable forms of ¹³⁷Cs were evaluated by single extraction with 1 M NH₄NO₃. The data showed that the freezing, following the radioisotope contamination of the soil, causes an increase of the amount of potentially mobile forms of radiocobalt, radiocesium, radium, and thorium and has an insignificant impact on the fractionation of americium and uranium.     

Accurate determination of naturally occurring radionuclides in Philippine coal-fired thermal power plants using inductively coupled plasma mass spectrometry and γ-spectroscopy

There is an increased interest in measuring naturally occurring radioactive materials (NORM) like coal, fly ash considering health hazards caused by naturally occurring radionuclides. This paper presents activity concentration (AC) of ²²⁶Ra, ²²⁸Ra, ²³²Th, ²³⁸U and ⁴⁰K in feed coal, bottom and fly ash samples from Philippines coal-fired thermal power plants using inductively coupled plasma mass spectrometry (ICP-MS) and high-purity germanium gamma spectroscopy (HPGe γ-spectroscopy). Coal, bottom and fly ash samples were digested using a microwave oven with a mixture of HNO₃, HClO₄ and HF. Uranium (²³⁸U) and thorium (²³²Th) ACs were also analyzed from samples using ICP-MS. A good correlation was found for the measurement of U and Th using both techniques (R² = 0.97 and 0.94 respectively). ICP-MS measurements showed the highest AC of ²³²Th and ²³⁸U in fly ash and lowest for feed coal samples. With HPGe γ-spectroscopy measurements, highest AC (in Bq kg^{− 1}) of ²²⁶Ra, ²²⁸Ra, ²²⁸Th and ⁴⁰K, were noticed in fly ash followed by bottom ash and feed coal. ICP-MS method is rapid for the measurement of uranium and thorium in comparison to γ-spectroscopy as secular equilibrium is not required. Activity concentrations of bottom and fly ash samples were found to be within the reported values worldwide and below the International Atomic Energy Agency recommended values for regulatory control.     

Influence of geology and soil particle size on the surface-area/volume activity ratio for natural radionuclides

The radioactive concentrations of²²⁶Ra,²³²Th,²³⁵U and⁴⁰K in surface soil of the province of Cáceres (Spain) were studied as a function of the geology and grain size. The activities of the four radionuclides in granitic and metamorphic soils have normal frequency distributions, with the mean value being significantly higher for the granitic soils than for the metamorphic soils. Sedimentary soils present asymmetric distributions, and their activities lie between the previous two types. The specific activities of the four radionuclides rises as the particle radius decreases. The equationA _e =(P ₁/R)+P ₂ describes the dependence of the specific activityA _e on radiusR, P ₁ andP ₂ being parameters that are related to the surface area and volume activities of the grains. The isotopes²²⁶Ra,²³²Th and²³⁵U accumulate with greater intensity on the surface of the grains than⁴⁰K. This effect is more pronounced in granitic and sedimentary soils than in metamorphic soils.     

A review of the studies on environmental transport and speciation analysis of radionuclides in India

Department of Atomic Energy, India, has a systematic environmental monitoring program to ensure that the impact of radionuclides on human and environment is well within the limits, stipulated by the regulatory body. Concentrations of radionuclides are estimated in air, water, soil, sediment and biota in the environment around the power plant site on a regular basis. The environmental migration pattern and impact of radionuclides in the environment depends upon not only on the total concentration but the physico-chemical nature of radionuclide also. This paper presents a brief review of the studies of environmental transportation of radionuclides and influence of speciation with special reference to Indian conditions. A fairly good amount of results are available on the influence of speciation of radionuclides on the wet and dry deposition and preliminary results are available on the speciation analysis in dietary items, in soil and in ground water. Initial studies are concentrated on tritium, ¹³⁷Cs, Uranium, ⁹⁰Sr and their chemical analogues.     

Performance of HPGe gamma spectrometry system for the measurement of low level radioactivity

Comprehensive quality assurance/quality control procedure is very much necessary to obtain accurate and precise analytical measurement result. This paper discusses the quality control aspects of the High-Purity Germanium (HPGe) based gamma spectrometry system, which has been used for the measurement of low-level radioactivity in environmental samples. The gamma spectrometry system consisting of coaxial n-type HPGe detector having 50% relative efficiency with respect to 7.62 cm x 7.62 cm NaI (Tl), Nuclear Instrumentation Module (NIM) based pulse processing electronic accessories and 8 k MCA. To reduce the background contribution, 7.5 cm thick lead has been placed surrounding the detector. The minimum detectable activities (MDA) with 95% confidence level (for 300 g soil sample and 100,000 s counting time) for important radionuclides such as ²³⁸U, ²²⁶Ra, ²³²Th, ⁴⁰K, and ¹³⁷Cs are 10.4, 4.3, 4.1, 16.9 and 0.1 Bq kg^?1, respectively. The Quality control (X bar R) charts were plotted using ¹³⁷Cs and ⁴⁰K background counts observed periodically, which showed that the fluctuation is well within the confidence limit and confirms the stability of the system. The laboratory has been participating in the proficiency tests (PTs) of the International Atomic Energy Agency (IAEA). In recently concluded PTs, the samples include soil, spiked standard solution, spinach, phosphogypsum and spiked air filter were analysed for the natural, fission and activation products radionuclides. The performance evaluation of the IAEA PTs showed that the laboratory results were in good agreement with the target value, which confirms the reliability and traceability of the gamma spectrometric measurement result of the laboratory.     

Comparison of transfers for natural radionuclides (238U, 234Th, 226Ra, 210Pb & 210Po) from five different soils to four different barley genotypes

Transfer Factors (Fv) of ²³⁸U, ²²⁶Ra, ²³⁴Th, ²¹⁰Po and ²¹⁰Pb from five different agricultural soils in semi-arid region (Syria) to four different barley genotypes were studied in an agricultural potted experiment. The geometric mean of the Fv values were (0.08) for ²¹⁰Pb, and (0.02) for ²¹⁰Po, while it ranged from 0.18 to 0.42 ,from 0.08 to 0.15 and from 0.22 to 0.4 for ²³⁸U, ²³⁴Th and ²²⁶Ra, respectevily. The Fv values of ²³⁸U and ²²⁶Ra were within the recommended global medians, while the Fv values of ²³⁴Th, ²¹⁰Pb and ²¹⁰Po were higher. There is no clear relationship between the soil properties and Fv of all studied radionuclides to barley genotypes. Moreover, the expression of glutathione (GSH) gene, which is belived to be involoved in heavy metal removal was generally low in all studied varieties grown in all soil types.

     

Preparation of in-house calibration source for the use in radioactivity analysis of the environmental samples: consideration of homogeneity

An in-house reference material has been prepared in Kuwait Institute for Scientific Research radioecology laboratory, for quality control purposes of gamma spectrometer systems. The material contains a known amount of uranium ore reference material (prepared by the International Atomic Energy Agency and coded as IAEA-RGU-1) which is mixed with marine sediment collected from Kuwait bay. The IAEA-RGU-1 has been certified that it is in equilibrium state with the decay daughters, and stable to be used for quality control purposes. Nevertheless, the homogeneous distribution of the doped material with the prepared source should be verified. This has been examined using gamma spectrometry measurements in conjunction with analysis of variance statistical tools, Dixon, box plots and Grubbs tests. The calculated total uncertainty has been utilized to establish the recommended specific activity ranges of ²²⁶Ra, ²²⁴Th, ²¹⁴Pb, ²¹⁴Bi and ²¹⁰Pb radioisotopes in the prepared source. The obtained results showed that the estimated uncertainty arising from the sample inhomogeneity has a significant contribution in the total uncertainty. The stability control charts of the ultra-low background gamma spectrometry system demonstrated the suitability of the prepared material for the purpose of quality control. However, the emitted gamma-rays from the prepared source covers the required energy range for determination of natural and artificial radionuclides in different species of environmental samples such as marine sediment, soil samples, and samples contaminated by naturally occurring radioactive material produced by oil industry. In addition, the material might be used for system calibration in case its traceability is proven. The experimental data revealed the significance of the homogeneity in preparing environmental samples for radioactivity measurements; in particular when small sample quantities of environmental samples are required to be analyzed.     

Transfer of naturally occurring radionuclides to wheat under laboratory controlled conditions

Knowledge of soil–plant transfer of naturally occurring radionuclides can be essential to assure an adequate radiological protection. Available data are mainly for anthropogenic radionuclides and biased for temperate climates. Wheat plantlets were grown using soil collected in Mediterranean regions and transfer factors, TF, for ^234,238U, ²²⁶Ra, ²¹⁰Po and stable elements (K, Na, Ca and Mg) were determined. U, Ra and Po were mainly located in roots. Calcium presented the highest TF values, whereas for radionuclides were much lower. Uranium TFs were correlated with total and exchangeable potassium concentration in soil. Calcium and radium TFs were correlated with total calcium concentration in soil.

     

Assessment of radioactivity contribution and transfer characteristics of natural radionuclides in agroecosystem

Taking into account the importance of distribution and transfer of radionuclides in the soil–plant system, especially in agricultural fields, the aim of this research was assessment of radioactivity contribution and transfer characteristics of natural radionuclides in agroecosystem. The measurement of the natural radioactivity distribution was conducted in organic and sustainable farming management systems. Statistical evaluation of the physical and chemical properties of soils subjected to different farming systems, revealed the existence of differences in some parameters. Balanced distribution of natural radionuclides in soil-crop system was observed. Radionuclide ⁴⁰K was the most accessible to the investigated crops via uptake from the soil, then ²³²Th and ²²⁶Ra. The obtained results are useful for understanding the behavior of the radionuclides and provide an insight into the cumulative deposition of radioactivity in the agroecosystem.

     

Improvement of quality in the evaluation of radium isotopes 224,226,228Ra in oil scale samples

Elevated concentrations of the radium isotopes ^224,226,228Ra exist in the scale and produced water in oil exploration. The activity concentration of ²²⁶Ra was calculated from 186.2 keV peak with no usual spectral interference of 185.7 from ²³⁵U. The activity concentration of ²²⁸Ra was calculated from its first daughter product ²²⁸Ac using the 911.2 keV gamma rays since it is a pure beta emitter. The activity concentration of ²²⁴Ra was calculated from ²¹²Pb using the 238.6 keV gamma-ray and the secular equilibrium equation with ²²⁸Ra. The IAEA 448 (oil contaminated field soil) reference material was used as a quality control for ^226,228Ra and but was unreliable for ²²⁴Ra using ²¹²Pb.

     

Influence of the physico-chemical properties of Selangor soil series on the distribution coefficient (<Emphasis Type="Italic">K</Emphasis><Subscript>d</Subscript>-value) of <Superscript>226</Superscript>Ra

²²⁶Ra is a member of the ²³⁸U natural decay series and is one of the most important isotope to be determined among the naturally occurring nuclides in environmental samples. In order to evaluate the radiation dose from ²²⁶Ra, it is important to know its mobility in different types of soils. The aim of the present study is to quantify the influence of physico-chemical soil properties on ²²⁶Ra adsorption. The distribution coefficients (K _d-value) of ²²⁶Ra in Selangor soil series samples were measured in one core, at three depth levels to evaluate the adsorbability of ²²⁶Ra. The soil samples were spiked with ²²⁶Ra tracer and the activities of ²²⁶Ra in the separated phase from batch sorption test were measured by a low background but high efficiency well-type HPGe detector. Several physico-chemical soil properties were also characterised for each soil samples. Pearson’s correlation and stepwise multiple regression test were applied at the 0.05 level of significance throughout all analysis to determine the relationships and influences between distribution coefficients (K _d-value) of ²²⁶Ra with physicochemical soil properties for the Selangor soil series. The observed K _d value was in the range of 50.55–172.28 mL g⁻¹ (mean: 93.20 ± 46.99 mL g⁻¹). The regression showed that the highest positive correlations were observed for organic matter (OM) and cation exchange capacity (CEC) (r = 0.96**, 0.81**, respectively) with K _d-values. The results indicate that the stepwise multiple regression model incorporating the soil’s OM and CEC accounts for 98% of the variability in distribution coefficients of ²²⁶Ra.     

Radioactive impact of a bauxite beneficiation plant in the Itea Gulf (Gulf of Corinth, Greece)

Activity concentration measurements of natural radionuclides performed by γ-ray spectrometry and ICP-MS in sediment samples from the Gulf of Itea and in surface soil samples collected from the surrounding area of a bauxite beneficiation plant, showed that (1) the breaker zone of the Itea Gulf, in the vicinity of the bauxite beneficiation plant, is contaminated with ²³⁸U, ²³²Th and ²²⁶Ra, (2) the activities in sediment samples from the rest of the Gulf were at the background level, and (3) enhanced activities of the ²³⁸U, ²³²Th and ²²⁶Ra were found in a number of soil samples due to bauxite dust deposition from the nearby beneficiation plant. The application of the optimized BCR sequential extraction procedure on the surface sediment samples showed that the U and Th were strongly bound to the sediments.     

226Ra translocation from soil to selected vegetation in the Crucea (Romania) uranium mining area

A two year field survey of ²²⁶Ra translocation from soil to selected spontaneous plants growing in the Crucea (Romania) uranium mining area is presented. Since Crucea is a large and relatively highly contaminated area, an easy and cheap way for a desired lowering of radiopollution represents phytoremediation using plentifully occurring plant species. The ²²⁶Ra translocation from soil was affected by analyzed species, collecting sites and vegetation periods. The specific ²²⁶Ra activities of the roots were considerably higher than the aboveground parts confirming the root tropism of radioisotopes. Mentha piperita was found to be highly effective in phytoremediation, especially in autumn.     

Sub-10 nm Radiolabeled Barium Sulfate Nanoparticles as Carriers for Theranostic Applications and Targeted Alpha Therapy

The treatment of cancer patients with α-particle-emitting therapeutics continues to gain in importance and relevance. The range of radiopharmaceutically relevant α-emitters is limited to a few radionuclides, as stable chelators or carrier systems for safe transport of the radioactive cargo are often lacking. Encapsulation of α-emitters into solid inorganic systems can help to diversify the portfolio of candidate radionuclides, provided, that these nanomaterials effectively retain both the parent and the recoil daughters. We therefore focus on designing stable and defined nanocarrier-based systems for various clinically relevant radionuclides, including the promising α-emitting radionuclide ²²⁴Ra. Hence, sub-10 nm barium sulfate nanocontainers were prepared and different radiometals like ⁸⁹Zr, ¹¹¹In, ¹³¹Ba, ¹⁷⁷Lu or ²²⁴Ra were incorporated. Our system shows stabilities of >90 % regarding the radiometal release from the BaSO₄ matrix. Furthermore, we confirm the presence of surface-exposed amine functionalities as well as the formation of a biomolecular corona.     

Chemometry of the distribution and origin of 226Ra, 228Ra, 40K and 137Cs in the soil near the lignite fired plants of West Macedonia (Greece)

The distribution and origin of natural ⁴⁰K,²²⁶Ra and²²⁸Ra and artificial ¹³⁷Cs have been investigated in the surface soil of a West Macedonia basin at four lignite fired power plants. No significant increase in specific activity of soil due to natural radionuclides of coal has been found. The specific activities of ²²⁶Ra, ²²⁸Ra and ⁴⁰K are equal to those of Greek soils. Radiocesium activity is slightly higher in the first 10 cm layer. The application of chemometrical methods confirmed that the radionulides ²²⁶Ra, ²²⁸Ra and ⁴⁰K are natural components of the soil and they do not originate from fly ash. This revised version was published online in July 2006 with corrections to the Cover Date.     

Terrestrial absorbed dose rate measurement in the Jhangar valley of Pakistan

Specific activity of natural radionuclides; ²²⁶Ra, ²³²Th and ⁴⁰K were measured in the agricultural soil of eastern salt range of Pakistan using gamma ray spectrometry. The soil samples were collected within the ploughing region (up to 12 cm depth) and processed before analysis. The average specific activities of different radionuclides in the dry mass of soil samples were: ⁴⁰K, (666 Bq/kg), ²²⁶Ra (51 Bq/kg), and ²³²Th (59 Bq/kg). The average outdoor terrestrial absorbed dose rate in air from gamma radiation one meter above ground surface was found to be 93 nGy/h.