Radioactive contamination of the environment as a result of uranium production: a case study at the abandoned Lincang uranium mine,Yunnan Province,China

The distribution of radioactive pollutants, such as²²²Rn, U, Th and²²⁶Ra in the air, surface waters, soils and crops around the Lincang uranium mine, Yunnan Province, China, is studied. The mechanical, geochemical and biogeochemical processes responsible for the transport and fate of the radioactive elements are discussed based on the monitoring data. The pollutants concentrations of effluents from the mine tunnels were dependent on pH and which were controlled by biochemical oxidation of sulfide in the ore/host rocks. Radon anomalies in air reached 4 km from the tailings pile depending on radon release from the site, topography and climate.²³⁸U and²²⁶Ra abnormities in stream sediments and soil were 40—90 cm deep and 790—800 m away downstream. Anomalies of radioactive contaminants of surface watercourses extended 7.5—13 km from the discharge of effluents of the site mainly depending on mechanical and chemical processes. There were about 2.86 ha rice fields and 1.59 km stream sediments contaminated. Erosion of tailings and mining debris with little or no containment or control accelerated the contamination processes.

     

Radioactive contamination of the environment as a result of uranium production: a case study at the abandoned Lincang uranium mine,Yunnan Province,China

The distribution of radioactive pollutants, such as²²²Rn, U, Th and²²⁶Ra in the air, surface waters, soils and crops around the Lincang uranium mine, Yunnan Province, China, is studied. The mechanical, geochemical and biogeochemical processes responsible for the transport and fate of the radioactive elements are discussed based on the monitoring data. The pollutants concentrations of effluents from the mine tunnels were dependent on pH and which were controlled by biochemical oxidation of sulfide in the ore/host rocks. Radon anomalies in air reached 4 km from the tailings pile depending on radon release from the site, topography and climate.²³⁸U and²²⁶Ra abnormities in stream sediments and soil were 40—90 cm deep and 790—800 m away downstream. Anomalies of radioactive contaminants of surface watercourses extended 7.5—13 km from the discharge of effluents of the site mainly depending on mechanical and chemical processes. There were about 2.86 ha rice fields and 1.59 km stream sediments contaminated. Erosion of tailings and mining debris with little or no containment or control accelerated the contamination processes.     

Radioecology around a closed uranium mine

The uranium mine and mill at ?irovski vrh, Slovenia, operated from 1982 to 1990. After processing, the uranium mill tailings were deposited onto the Bor?t waste pile lying close to the mine. Radioecological studies focused on assessing the mobility and bioavailability of deposited radionuclides were initiated some five years ago. The mobility of ²³⁸U, ²³⁴U, ²³⁰Th and ²²⁶Ra in soil was studied by applying sequential extraction protocols. The highest activity concentrations were found at the bottom of the waste pile. Uranium isotopes were the most mobile, followed by ²²⁶Ra whose mobility appeared to be suppressed by high sulphate concentrations and ²³⁰Th. The wetland plants grown in soils contaminated with seepage waters from the tailings contained higher levels of ²³⁸U, ²²⁶Ra and ²³⁰Th compared to plants from a control site. The activity concentration of ²²⁶Ra was the highest in all studied plant species. The radiological risk to wildlife around the mine area as assessed by the ERICA Tool was negligible. Activity concentrations in bovine milk from the area of ?irovski vrh were comparable to the reference location, except for uranium where the content was higher. The combined annual effective dose for adults consuming milk from the ?irovski vrh area is 13.0 ± 1.7 μSv a^?1.     

Analyses of radionuclides in soil,water, and agriculture products near the Urgeiriça uranium mine in Portugal

Analyses of soils, irrigation waters, agriculture products (lettuce), green pasture, and cheese were performed in samples collected in the area of the old Urgeiriça uranium mine and milling facilities, Centre-North of Portugal, in order to assess the transfer of uranium series radionuclides in the environment and to man. Soils close to milling tailings display an enhancement of radioactivity. In the drainage basin of the stream Ribeira da Pantanha, receiving drainage from the tailings piles and discharges from the acid mine water treatment plant, there was enhancement of uranium series radionuclide concentrations in water and suspended matter. Agriculture products from kitchen gardens irrigated with water from the Ribeira da Pantanha show an increase of radioactivity, mainly due to uranium isotopes. Agriculture products from other kitchen gardens in this area, irrigated with groundwater, as well pasture and cheese produced locally from sheep milk did not show enhanced radionuclide concentrations. In the Urgeiriça area, some soils display radionuclide concentrations higher than soils in reference areas and, in agriculture products grown there, ²²⁶Ra was the radionuclide more concentrated by vegetables. Through ingestion of these products ²²⁶Ra may be the main contributor to the increment of radiation dose received by local population.     

Spatial variability and radiation assessment of the radionuclides in soils and sediments around a uranium tailings reservoir,south of China

Journal of Radioanalytical and Nuclear Chemistry - The concentrations of 238U, 226Ra, 232Th and 40K and gross α, β were measured in soils and sediments around a uranium tailings reservoir...     

Radioanalytical assessment of environmental contamination around non-remediated uranium mining legacy site and radium mobility

During the past century extensive uranium mining took place in Portugal for radium and uranium production. One such uranium mine was the Boco Mine, in operation during the 1960s and 70s. Mining waste and open pits were left uncovered since mine closure. During the nineties a quarry for sand extraction was operated in the same site and water from a local stream was extensively used in sand sieving. Downstream the mine area, agriculture soil is used for cattle grazing. Water from the stream, water wells, soil, pasture and sheep meat were now analyzed for radionuclides of uranium natural series. The U-series radionuclide ²²⁶Ra was generally the highest in concentrations especially in soil, pasture, and in internal organs of sheep. ²²⁶Ra concentrations were 1,093 ± 96 Bq/kg (dry weight, dw) in soil, 43 ± 3 Bq/kg (dw) in pasture, and 193 ± 84 mBq/kg (wet weight, ww) in muscle tissue of sheep. Other sheep internal organs displayed much higher ²²⁶Ra concentrations, such as the brain and kidneys with 1,850 ± 613 mBq/kg (ww) and 6,043 ± 6,023 mBq/kg (ww), respectively. Results of analyses of tissue samples from sheep grown in a comparison area were 2 to 16 times lower, depending on the organ. Absorbed radiation doses for internal organs were computed and may exceed 5.2 mGy/y in the case of kidneys, near three times higher than in animals from the reference area, but below the threshold for biological effects. Radionuclide transfer in the terrestrial food chain and radiation exposure of the human population is discussed.     

Radium accumulation in animal thyroid glands a possible method for uranium and thorium prospecting

A method of prospecting for uranium and thorium is proposed based on uptake of their radioactive daughters²²⁶Ra and²²⁸Ra by plants, the collection of plant material by herbivores, the concentration of the radioactive species by specific animal tissues, and the subsequent gamma-ray analysis of the tissues. This paper is based on work performed under United States Energy Research and Development Administration (formerly U.S.A.E.C.), Contract EY-76-C-06-1830.     

Uranium, thorium and potassium contents and radioactive equilibrium states of the uranium and thorium series nuclides in phosphate rocks and phosphate fertilizers

Uranium, thorium and potassium contents and radioactive equilibrium states of the uranium and thorium series nuclides have been studied for 2 phosphate rocks and 7 phosphate fertilizers. Uranium contents were found to be rather high (39-117 ppm) except for phosphate rock from Kola. The uranium series nuclides were found to be in various equilibration states, which can be grouped into following three categories. Almost in the equilibrium state, 238U approximately 230Th greater than 210Pb greater than 226Ra and 238U greater than 230Th greater than 210Pb greater than 226Ra. Thorium contents were found to be, in general, low and appreciable disequilibrium of the thorium series nuclides was not observed except one sample. Potassium contents were also very low (less than 0.3% K2O) except for complex fertilizers. Based on the present data, discussions were made for the radiation exposure due to phosphate fertilizers.     

Comparative plant uptake and environmental behavior of U-series radionuclides at a uranium mine-mill

Concentrations of U, Th, Ra, Pb, and Po were determined in native vegetation and underlying substrate (soil and tailings) at various sites around a conventional open pit, acid leach uranium production operation in the Western United States. Radionuclide concentrations in substrate and vegetation were generally elevated above background at all sites disturbed by mining and milling activities. Observed plant/soil CR values for vegetation growing on exposed, weathered tailings were ordered as follows:²³⁸U>²³⁰Th>²¹⁰Po,²²⁶Ra>²¹⁰Pb. We suspect that in the case of sulfuric acid leached tailings, Ra and Pb are sequestered as sulfates, which are highly insoluble relative to U and Th sulfates, resulting in reduced availability for plant uptake. Soil acidity and the saturation condition at the tailings impoundment edge tend to enhance radionuclide availability for plant uptake. The transport of radionuclides to foliage and subsequent retention and absorption may play a role in plant contamination.     

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.     

Radium-226 in uranium mill tailings

A study of the physical state of²²⁶Ra in uranium mill tailings was undertaken by Chemex Laboratories Ltd. under contract to NUTP. A test portion of a leached uranium ore was collected just prior to neutralization with lime and subjected to repetitive batch water leaching. The leachates were analyzed for barium, lead,²²⁶Ra, iron and sulphate. The experimental results suggest that²²⁶Ra is co-precipitated with lead sulphate during uranium leaching of the ore with sulphuric acid. The attainment of equilibrium conditions in the pore water of the leached ore then allows a re-proportioning of²²⁶Ra between solid lead and barium sulphates resulting in a depletion of²²⁶Ra in the outer layers of the crystals of solid lead sulphate and an enrichment in²²⁶Ra in the outer layers of solid barium sulphate.     

Radioactive series disequilibria in underground uranium deposits of the Singhbhum Shear Zone, Eastern India

Radionuclides of the ²³⁸U series (²²⁶Ra, ²¹⁰Pb, ²³⁴Th and ²³⁴U), ²³⁵U series (²²⁷Ac and ²³¹Pa) and ²³²Th series (²²⁸Th and ²²⁸Ra) series were measured by High Resolution Gamma Spectrometry system in twenty-five uranium ore samples from underground uranium deposits in the Singhbhum Shear Zone of Eastern India. The activity concentrations were observed to vary within a wide range in most of the deposits, as is the case in most rocks of crustal origin. The uranium ore from these deposits were not of high ore grade (U concentrations ranged from 0.015 to 0.082%). Activity ratios of key daughter–parent pairs from the decay chains, viz. ²²⁶Ra/²³⁸U, ²²⁶Ra/²¹⁰Pb, ²³¹Pa/²³⁵U, ²²⁷Ac/²³⁵U, ²³⁰Th/²³⁸U, ²³⁴U/²³⁸U, ²²⁶Ra/²³⁰Th and ²²⁸Th/²²⁸Ra indicated migration/accumulation of uranium and radium in some samples. The ²²⁶Ra/²³⁰Th ARs suggested that the deposits were not closed to groundwater movement for a maximum time period of 8ky. Thiel plot of the ²³⁴U/²³⁸U vs. ²³⁰Th/²³⁸U activity ratios indicated uranium accumulation and complex processes of uranium redistribution.     

Assessment of natural uranium and 226Ra concentration in ground water around the uranium mine at Narwapahar, Jharkhand, India and its radiological significance

A brief study on dissolved radionuclides in aquatic environment, especially in ground water, constitutes the key aspect for assessment and control of natural exposure. In the present study the distribution of natural uranium and ²²⁶Ra concentration were measured in ground water samples collected within a 10 km radius around the Narwapahar uranium mine in the Singhbhum thrust belt of Jharkhand, India in 2007–2008. The natural uranium content in the ground water samples in this region was found to vary from 0.1 to 3.75 μg L^?1 with an average of 0.87 ± 0.73 μg L^?1 and ²²⁶Ra concentration was found to vary from 5.2 to 38.1 mBq L^?1 with an average of 13.73 ± 7.34 mBq L^?1. The mean annual ingestion dose due to intake of natural uranium and ²²⁶Ra through drinking water pathway to male and female adults population was estimated to be 6.55 and 4.78 μSv y^?1, respectively, which constitutes merely a small fraction of the reference dose level of 100 μSv y^?1 as recommended by WHO.     

Partitioning of natural radionuclides in sediments around a former uranium mine and mill

Partitioning of natural radionuclides in sediments from streams affected by the waste piles of the former uranium mine and mill located at ?irovski vrh, Slovenia, was performed by applying a sequential extraction procedure. The sediments were collected at three sites located upstream and three sites located downstream of the waste piles. Then the four-step Community Bureau of Reference (BCR) sequential extraction protocol was applied to the samples and the natural radionuclides ²³⁸U, ²³⁰Th, ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po were analysed in each extraction fraction. It was expected that the fractionation of natural radionuclides originating from the waste piles would differ from that upstream of the influence of waste piles because their chemical environment had been altered during the processes of uranium extraction. This difference could allow tracing of the radionuclides coming from the waste piles downstream of the affected watercourses. The results definitely showed that the total activity concentrations at sites downstream of the influence of the waste piles were higher than at sites upstream of the piles. However, this difference was geographically very limited and could no longer be detected already at a distance of about 5 km downstream. Unexpectedly, the fractionation of radionuclides upstream and downstream of the area of influence of the waste piles did not appear to be significantly altered. The sole differences found were for ²³⁸U and ²²⁶Ra in the second fraction (the “Fe/Mn oxides” fraction) and for ²¹⁰Po in the fourth fraction (the “residue” fraction) of the BCR sequential extraction protocol.     

Activity concentration of226Ra and238U in various soils

The distribution of²²⁶Ra and²³⁸U in various soils has been studied. Supposing that radioactive equilibrium were in existence, the average activities of²²⁶Ra and²³⁸U would show a nearly 11 correlation. As weathering affects radioactive equilibrium in surface soil, radioactive equilibrium was not in existence. Therefore, four kinds of soil were selected from different weathering conditions, viz. river bed soil, paddy field soil, field soil and uncropped soil. The²²⁶Ra/²³⁸U ratio of various soils lies in the range of 1.63 to 2.41. The activity concentrations of²²⁶Ra were greater than²³⁸U in various soils. The ratio²²⁶Ra/²³⁸U can be shown to be a quantitative index of weathering. Phosphatic manure contains²³⁸U and its daughter isotopes in concentrations far exceeding the average abundance in the earth's crust. But the cultivated soils (paddy field soil, field soil) are not affected by fertilizers in Kamisaibara.     

A device for uranium series leaching from glass fiber in HEPA filter

For the disposal of a high efficiency particulate air (HEPA) glass filter into the environment, the glass fiber should be leached to lower its radioactive concentration to the clearance level. To derive an optimum method for the removal of uranium series from a HEPA glass fiber, five methods were applied in this study. That is, chemical leaching by a 4.0?M HNO₃?C0.1?M Ce(IV) solution, chemical leaching by a 5 wt% NaOH solution, chemical leaching by a 0.5?M H₂O₂?C1.0?M Na₂CO₃ solution, chemical consecutive chemical leaching by a 4.0?M HNO₃ solution, and repeated chemical leaching by a 4.0?M HNO₃ solution were used to remove the uranium series. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 5?h by the 4.0?M HNO₃?C0.1?M Ce(IV) solution were 2.1, 0.3, 1.1, and 1.2?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 36?h by 4.0?M HNO₃?C0.1?M Ce(IV) solution were 76.9, 3.4, 63.7, and 71.9?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 8?h by a 0.5?M H₂O₂?C1.0?M Na₂CO₃ solution were 8.9, 0.0, 1.91, and 6.4?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after consecutive leaching for 8?h by the 4.0?M HNO₃ solution were 2.08, 0.12, 1.55, and 2.0?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after three repetitions of leaching for 3?h by the 4.0?M HNO₃ solution were 0.02, 0.02, 0.29, and 0.26?Bq/g. Meanwhile, the removal efficiencies of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th from the waste solution after its precipitation?Cfiltration treatment with NaOH and alum for reuse of the 4.0?M HNO₃ waste solution were 100, 100, 93.3, and 100%.     

Radium,uranium and thorium concentrations in low specific activity scales and in waters of some oil and gas production plants

Low specific activity scales consisting of alkaline earth metal carbonates and sulfates are often present in some gaseous and liquid hydrocarbon plants; these scales contain a certain concentration of radium, uranium and thorium, which can cause a risk of -irradiation and of internal radiocontamination when they must be mechanically removed. That being stated,²³⁸U,²³²Th and²²⁶Ra were determined in scales, sludges and waters coming from different plants.²³⁸U and²³²Th concentrations were found very low; the isotopes²³⁸U and²³⁴U resulted in radioactive equilibrium, whilst²³²Th and²²⁸Th were not always in equilibrium.²²⁶Ra concentration was higher in scales and sludges than in waters.     

Radiochemical characterization of spring waters in Balaton Upland, Hungary, estimation of radiation dose to members of public

Hungary is rich in spring waters. A survey studying the naturally occurring alpha emitter radionuclides in 30 frequently visited and regularly consumed spring waters was conducted out in the Balaton Upland region of Hungary.²²⁶Ra, ²²⁴Ra, ²³⁴U, ²³⁸U and ²¹⁰Po activity concentrations were determined by using alpha spectrometry after separation from matrix elements. Average concentration (mBq L^{− 1}) of ²²⁶Ra, ²²⁴Ra, ²³⁴U, ²³⁸U and ²¹⁰Po in the spring waters is varied from 2.1 to 601, from < 1.1 to 65.4, from 3.9 to 741.9, from < 0.44 to 274.3 and from 2 to 15.2 respectively. In most cases radioactive disequilibrium was observed between uranium and radium isotopes. The doses for the analyzed samples of spring water are in the range 3.59–166.73 μSv y^{− 1} with an average 18.2 μSv y^{− 1} .This is well below the 100 μSv y^{− 1} reference level of the committed effective dose recommended by WHO. Only one water sample had a dose higher than 100 μSv y^{− 1}, mainly due to the contribution from radium (²²⁶Ra, ²²⁴Ra) and ²¹⁰Po isotopes. This study provides important information for consumers and authorities about their internal radiological exposure risk from spring water intake.     

Natural radioactivity levels in mineral,therapeutic and spring waters in Tunisia

Radioactivity measurements were carried out in 26 groundwater samples from Tunisia. Activity concentrations of uranium were studied by radiochemical separation procedures followed by alpha spectrometry and that for radium isotopes by gamma-ray spectrometry.The results show that, the concentrations in water samples range from 1.2 to 69 mBq/L.1, 1.3 to 153.4 mBq/L, 2.0 to 1630.0 mBq/L and 2.0 to 1032.0 mBq/L for ²³⁸U, ²³⁴U, ²²⁶Ra and ²²⁸Ra, respectively. The U and Ra activity concentrations are low and similar to those published for other regions in the world. The natural radioactivity levels in the investigated samples are generally increased from mineral waters through therapeutic to the spring waters.The results show that a correlation between total dissolved solids (TDS) values and the ²²⁶Ra concentrations was found to be high indicating that ²⁶⁶Ra has a high affinity towards the majority of mineral elements dissolved in these waters. High correlation coefficients were also observed between ²²⁶Ra content and chloride ions for Cl^?–Na⁺ water types. This can be explained by the fact that radium forms a complex with chloride and in this form is more soluble.The isotopic ratio of ²³⁴U/²³⁸U and ²²⁶Ra/²³⁴U varies in the range from 0.8 to 2.6 and 0.6 to 360.8, respectively, in all investigated waters, which means that there is no radioactive equilibrium between the two members of the ²³⁸U series. The fractionation of isotopes of a given element may occur because of preferential leaching of one, or by the direct action of recoil during radioactive decay.The annual effective doses due to ingestion of the mineral waters have been estimated to be well below the 0.1 mSv/y reference dose level.     

Solvent extraction of uranium(VI) with benzyloctadecyldimethylammonium chloride (BODMAC) from highly concentrated chloride solution

The ²²²Rn emanation fraction (EF) released from the technically enhanced naturally occurring radioactive material (TE-NORM) wastes at certain sites of petroleum and gas production was determined. The samples were analyzed by γ-ray spectrometry to determine the activity concentration of the ²²⁶Ra content, of which the ²²²Rn emanation fraction was calculated. The results showed that the ²²²Rn emanation fraction differs in the oil and gas production sites and it is independent of the activity concentration of ²²⁶Ra. This revised version was published online in August 2006 with corrections to the Cover Date.