Isotopic evidence of natural uranium and spent fuel uranium releases into the environment

Uranium and plutonium isotopes were measured in soils, sediments and waters in an area subject to the past and present discharges from the uranium conversion plant of Malvési (France). The isotopes (236)U and (239)Pu are well known activation products of uranium and they prove to be powerful tracers of spent fuel releases in soils and sediments. On the other hand (234)U and (238)U activities measured in waters can be used to distinguish between releases and background uranium sources. Such findings contribute to improve the monitoring of the actinides releases by nuclear fuel facilities (mining sites, conversion, enrichment and fuel plants, reprocessing plants).     

Uranium oxide and other airborne particles deposited on cypress leaves close to a nuclear facility

Enhanced activity of actinides and some decay products has been reported for the leaves of cypress trees (Chamaecyparis nootkatensis) at the edge of the Malvési uranium-processing facility, southwestern France. The enhanced activity is due to the release of actinides via the smokestacks and from artificial ponds inside the facility. This study was conducted to characterize airborne particulate matter deposited on the leaf surfaces and to investigate whether or not radioactive particles may be identified. Air-dried leaf samples were examined by scanning electron microscopy, in combination with energy-dispersive X-ray spectrometry. The samples were scanned systematically in both secondary and backscattered electron modes. Particles ranging in size from <200 nm to ~40 μm were found on most portions of the adaxial leaf surface, but they are especially abundant at the boundary between facial and lateral leaves. The majority of the analyzed particles could be attributed to five principal classes: carbonates, silicates, sulfates, oxides/hydroxides, and halides. In addition, other types of particles were found, including Fe alloys; scheelite-group phases; phosphates; sulfides; and fly ash spheres. Similar particles were also observed on the surface of a wheat sample used for comparison. Of special interest are U-rich particles, which were observed on the cypress leaves only and which were identified as U oxides, except for one particle, which was a U-oxide-fluoride. These U-rich particles were released into the atmosphere by the nuclear facility prior to their deposition on the leaf surfaces. As most of the U-rich particles are <2.5 μm across, they are respirable. Once inhaled, particles containing alpha-emitting isotopes represent a potentially long-term source of ionizing radiation inside the lungs and thus, pose a threat to the health of people living nearby.     

Uranium series radionuclides in surface waters from the Shu river (Kazakhstan)

The concentrations of (238)U, (234)U, (226)Ra, (210)Po and (210)Pb have been determined in surface waters collected along the course of the Shu River, lying on the border between Kazakhstan and Kyrgyzstan. In the study area, the river runs through some of the largest uranium deposits worldwide, which were actively exploited during the nuclear weapons and nuclear energy programmes of the former Soviet Union. The data show an increasing trend in uranium concentrations downstream the river from the city of Tokmak to the city of Shu, with good correlation between total uranium concentrations and total dissolved solids. Data on uranium isotopes disequilibrium show the presence of technogenic uranium inputs into the Shu River downstream from the city of Karasu, evidenced by a decrease in the measured (234)U/(238)U isotopic ratio from 1.63 in uncontaminated sites to 1.29 in sites affected by past mining activities.     

Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS

The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.     

Impact of Pollution Caused by Uranium Production on Soil Macrofauna

Thirty years of mining and milling activities of the Priargunsky Mining-Chemical Production Company (South-Eastern Siberia, Russia) have resulted in an enrichment of uranium in adjacent steppe soils by a factor of up to 600. A number of attendant pollutants (thorium, arsenic and heavy metals) also have high concentrations in the soil. To estimate the effects of this pollution on soil-living macroinvertebrates, pitfall trapping and core sampling were applied. The element composition of four beetle species was analysed. Soil macroinvertebrates had 3–37 times lower abundance and biodiversity at the contaminated sites compared with the control. Ground beetle communities at the contaminated sites were reduced compared to the control site. The concentrations of uranium and arsenic in beetles collected at the contaminated sites were 2–41 and 2–26 times higher, respectively, than at the control site. There is strong evidence that the contamination caused by uranium production has severe negative biological effects on important groups of the soil food web.     

Joint ecotoxicology of cadmium and metsulfuron-methyl in wheat (Triticum aestivum)

Herbicide is indispensable for crop production. However, substantial usage of herbicide has led to its increasing accumulation in soils and crops. In addition, cadmium has become one of the widely occurring contaminants in soils due to its significant release into environment via anthropogenic activities. In this study, ecotoxicological investigations were made by exposing the food crop wheat to joint contaminations of Cd and metsulfuron-methyl, a sulfonylurea herbicide. We analyzed growth and physiological and molecular responses in wheat exposed to 0.5 mg kg^?1 Cd and 0.02 mg kg^?1 metsulfuron-methyl (MSM). Soils contaminated with Cd and MSM complex caused significantly detrimental effect on wheat growth and physiological process. Combinative treatments with Cd and MSM damage more severely the plant cells as compared with Cd or MSM treatment alone. Compared with the growth parameter, the biochemical and molecular responses of wheat appeared more pronounced to Cd and MSM complex. Furthermore, compared with control, wheat plants exposed to Cd?+?MSM generated more O^2?.and H₂O₂, both of which were shown to be the cause of enhanced activity of several antioxidant enzymes. Native polyacrylamide gel eletrophoresis and molecular response analyses were performed to validate the results indicated above. Our results indicated that joint contamination with Cd and MSM was more toxic to wheat than a single contamination. These sensitive biological parameters can be used as biomarkers monitoring the ecotoxicological process in plants.     

Carbonate induced dissolution of uranium containing precipitates under cement leachate conditions

The effects of carbonate on uranium (VI) solubility under aerobic and cementitious conditions have been investigated. The information is of relevance to low level nuclear waste disposal. Aqueous NaOH, KOH, Ca(OH)2 and a cement leachate solution were added to uranyl nitrate solution. Afterwards, increasing amounts of ammonium carbonate were added to re-dissolve the precipitates. The precipitates were characterised by means of X-ray powder diffraction (XRPD) measurements and modelling studies. The model calculations were performed using the MINTEQA2 speciation code, with an expanded database incorporating uranium stability constants taken from the HATCHES database. The measured and predicted amounts of CO3(2-) needed to dissolve the precipitates were compared. The knowledge gained from the 'pure' systems was used to rationalise the precipitation and re-dissolution behaviour observed in the leachate system. The lack of uranium solubility at low carbonate levels brought into question literature formation constants for UO2(OH)3- and UO2(OH)4(2-). An approximate log K value of 26.8 for K2U2O7 formation was estimated from the KOH results at pH 12. Generally, uranium solubilities are expected to be insignificant at low level nuclear waste sites because anaerobic conditions should persist. However, this study has demonstrated that solubility in leachate could rise at high pH and high carbonate levels, if aerobic conditions were to develop. Soluble U(VI) species would be formed. The novel part of the study has been to reproduce the effects and to correlate enhanced solubilities with model predictions. Consequently, the study has re-emphasised the need for appropriate environmental monitoring of such sites.     

Uranium bioassay and radioactive dust measurements at some uranium processing sites in Egypt--health effects

The safety of radiation workers in the uranium mining industry requires close and continuous monitoring of their working conditions. In this study, external radiation surveillance, radioactive dust monitoring and the bioassay of uranium were carried out in some processing sites. As dust represents one of the most important sources of radiation exposure in mills and mines, dust monitoring and bioassays were performed for a sample of workers on the production lines. The concentration of uranium in air ranged from 22.6 x 10(-7) to 11.1 x 10(-5) Bq cm-3, and the exposure levels ranged from 1 to 80 microSv h-1. Laser fluorimetric determination of uranium in urine samples showed concentrations in the range 8.4-29.2 micrograms L-1. Renal function parameters, such as serum creatinine and urea, and hematological parameters were determined in an attempt to correlate them with radiation exposure and the health status of the workers. Urine specimens collected from workers at the ore crushing and separation site showed elevated concentrations of uranium (up to 29.2 micrograms L-1) and a strong correlation between these concentrations and the registered serum creatinine. The mean uranium excretion in the investigated group was more than 20 times the occupational exposure decision level for urine uranium of 0.8 microgram L-1.     

The impact of a disused mine on uranium transport in the River Fal, South West England

Unfiltered and filtered (0.45 and 0.2 microm) water samples and sediment samples (sieved to <180 microm and 180-1000 microm) were collected along an approximately 15 km transect of the River Fal, Cornwall, UK, to examine the impact of the disused South Terras uranium mine on the uranium concentrations of the river water and underlying sediments. The uranium concentration of the water samples fluctuated along the river, with the 0.45 microm filtered water showing the largest, seven-fold, difference between minimum (0.19 microg L(-1)) and maximum (1.34 microg L(-1)) concentrations. The historical uranium mine and spoil heaps were not a significant source of uranium to the river water, as water concentrations were low next to the site, but a highly elevated uranium concentration (1000 mg kg(-1)) was found in sediment below an outflow pipe from this mine. Operationally defined "colloidal" (0.2-0.45 microm) and "dissolved" (<0.2 microm) uranium were the predominant forms of the element in the river water (35 and 45% respectively). The uranium concentration in the dissolved phase showed a correlation coefficient of 0.83 (n= 9) with the total cation concentration, suggesting that the uranium concentration in this fraction is directly linked to weathering of rocks and minerals. The observation that weathering is the dominant mechanism delivering uranium to the river water explains the low uranium concentrations in the river water close to South Terras mine, despite the proximity of the spoil heaps, and the maximum uranium concentrations close to a china clay mining area.     

Element Levels in Snakes in South Carolina: Differences Between a Control Site and Exposed Site on the Savannah River Site

Levels of 18 elements, including lead, mercury, selenium, and uranium, were examined in three species of snakes from an exposed and reference site on the Department of Energy's Savannah River Site in South Carolina. We tested the hypotheses that there were no differences as a function of species, and there were no difference between the exposed and control site for blood and muscle (tail) samples for banded water snake (Nerodia fasciata), brown water snake (N. taxispilota) and cottonmouth (Akistrodon piscivorous). The banded water snakes collected were significantly smaller than the other two species. For blood, there were significant species differences only for barium, copper, selenium, uranium and zinc, while for muscle tissue there were significant interspecific differences in aluminum, arsenic, barium, cobalt, cesium, copper, iron, lead, mercury, manganese, strontium, vanadium and zinc, suggesting that muscle tissue in the tail is a better indicator of potential interspecific differences. It is also easier logistically to collect tail tissue than blood. Where one species had significantly higher levels than the other species in muscle tissue levels, cottonmouth had higherlevels of five elements (aluminum, cobalt, lead, mercury, vanadium), brown water snake had two (lead, strontium), and banded water snake had only barium. There were few significant differences between the control and reference site for levels of blood, but several for muscle tissue. All three species had significantly higher levels of arsenic and manganese at Tim's Branch than the reference site, and nickel and uranium were significantly higher for banded watersnake and cottonmouth, the larger species. Individuals with high exposure of one element were exposed to high levels of other elements.     

Trace Element Contamination in Benthic Macroinvertebrates from a Small Stream Near a Uranium Mill Tailings Site

Direct measurement of the accumulation of non-radioactive traceelements in aquatic biota near uranium mining or processing sites has been relatively rare, with greater focus on the radiological activity in the adjacent soils and groundwater. To evaluate the potential ecological concern associated with trace elements at a former uranium mill site in southeasternUtah, benthic macroinvertebrates were collected and analyzed for 17 trace elements from multiple locations within a small on-site stream, Montezuma Creek, and a nearby reference stream. Key questions of this study relate to the spatial and temporalextent of contamination in aquatic biota, the potential ecological risks associated with that contamination, and the usefulness of benthic macroinvertebrates as a monitoring tool at this site. Composite samples of similar macroinvertebrate taxa and functional feeding groups were collected from each site over atwo year period that was representative of normal and dry-yearconditions. In both years, mean concentrations of arsenic,molybdenum, selenium, and vanadium were significantly higher (afactor of 2–4 times; P < 0.05) in macroinvertebrates collectedfrom one or both of the two Montezuma Creek sites immediatelydownstream of the mill tailing site in comparison toconcentrations from reference locations. Mean uraniumconcentrations in invertebrates immediately downstream of themill site were more than 10 times higher than at reference sites.The site-to-site pattern of contamination in Montezuma Creekinvertebrates was similar in 1995 and 1996, with mill-relatedtrace elements showing a downstream decreasing trend. However,nine of seventeen contaminant concentrations were higher in thesecond year of the study, possibly due to a higher influx of deepgroundwater during the drier second year of the study. Apreliminary assessment of ecological risks, based on the benthicmacroinvertebrate bioaccumulation data, suggests that aquatic andterrestrial population risks are low. Benthic macroinvertebratesappeared to be sensitive integrators of trace element inputs tothe aquatic environment from a former uranium mill tailing site,and provided useful spatial and temporal patterns ofcontamination not easily obtained using conventional surfacewater or groundwater measures.     

TiO2 and ZnO nanoparticles negatively affect wheat growth and soil enzyme activities in agricultural soil

The properties of nanoparticles and their increased use have raised concerns about their possible harmful effects within the environment. Most studies on their effects have been in aqueous systems. Here we investigated the effect of TiO(2) and ZnO nanoparticles on wheat growth and soil enzyme activities under field conditions. Both of the nanoparticles reduced the biomass of wheat. The TiO(2) nanoparticles were retained in the soil for long periods and primarily adhered to cell walls of wheat. The ZnO nanoparticles dissolved in the soil, thereby enhancing the uptake of toxic Zn by wheat. The nanoparticles also induced significant changes in soil enzyme activities, which are bioindicators of soil quality and health. Soil protease, catalase, and peroxidase activities were inhibited in the presence of the nanoparticles; urease activity was unaffected. The nanoparticles themselves or their dissolved ions were clearly toxic for the soil ecosystem.     

Extractable Hydrocarbons, Nickel and Vanadium Contents of Ogbodo-Isiokpo Oil Spill Polluted Soils in Niger Delta, Nigeria

An oil spill polluted site at Ogbodo-Isiokpo in Ikwere Local Government Area of Rivers State in southern Nigeria, was identified for study following three successive reconnaissance surveys of oil fields in the Agbada west plain of Eastern Niger Delta. A sampling area of 200 m × 200 m was delimited at the oil spill impacted site using the grid technique and soils were collected at surface (0–15 cm) and subsurface (15–30 cm) depths from three replicate quadrats. A geographically similar, unaffected area, located 50 m adjacent to the polluted site, was chosen as a control (reference) site. Total extractable hydrocarbon contents of the polluted soils ranged from 3.02–4.54 and 1.60–4.20 mg/kg (no overlap in standard errors) at surface and subsurface depths respectively. The concentrations of two “diagnostic” trace heavy metals, nickel (Ni) and vanadium (V), which are normal constituents of crude oil, were also determined in the soils by atomic absorption spectrophotometric method after pre-extraction of cations with dithionite–citrate carbonate. Ni varied from 0.15 to 1.65 mg/kg in the polluted plots and from 0.18 to 0.82 mg/kg in the unpolluted plots; vanadium varied from 0.19 to 0.70 mg/kg in the polluted plots and from 0.14 to 0.38 mg/kg in the unpolluted plots. Ni and V were more enhanced (p < 0.05) in the oil-polluted soils, especially at subsurface depth. Whilst the oil spillage could be said to be indirectly responsible for the enhanced concentrations of nickel and vanadium via the injection and availability of the petroleum hydrocarbons that might have increased the activities of biodegradation on site, the physico-chemical properties of the soils and inherent mobility of metals, as well as the intense rainfall and flooding that characterized the period of study, may have also contributed, at least in part, to these enhanced concentrations. Such levels of Ni and V may result to enhanced absorption by plants, which may bring about possible bioaccumulation in such plants and the animals that depend on them for survival and all of these may lead to toxic reactions along the food chain.     

The influence of pH and temperature on the aqueous geochemistry of neodymium in near surface conditions

Geochemical calculations were employed for the solubility and speciation of neodymium in a model soil solution as a function of pH. The calculations were based on the recently determined stability constants for Nd and solubility product for the Nd end-member of mineral monazite (NdPO(4)). Simulations were carried out at near neutral pH (pH 6.0 to pH 7.5) and 25 degrees C at the atmospheric CO(2) partial pressure. Additional calculations were also performed to assess Nd mobility at the extreme temperature conditions (300 degrees C) at neutral pH. Our results suggest that relatively dilute (Ionic Strength, I = 0.1), low-temperature waters may transport very small quantities of rare earth elements and actinides to the surficial environment at near neutral pH conditions. Evidently, higher temperature or extreme fluid composition may have a greater potential for mobilization of these elements. The results are pertinent to researchers interested in engineering applications for the precipitation of Nd and surrogate actinides from aqueous nuclear wastes.     

Derivation and Use of Sediment Quality Guidelines for Ecological Risk Assessment of Metals and Radionuclides Released to the Environment from Uranium Mining and Milling Activities in Canada

The Screening Level Concentration (SLC) approach was used to derive Lowest Effect Level (LEL) and Severe Effect Level (SEL) concentrations for nine metals (As, Cr, Cu, Pb, Mo, Ni, Se, U and V) and three radionuclides (²²⁶Ra, ²¹⁰Pb, and ²¹⁰Po) released to the aquatic environment during the mining and milling of uranium ore. This method was chosen because it allowed for the best use of the considerable historical and current data collected for diverse purposes in the uranium mining and milling regions of Canada (20,606 data points used in the analysis). Except for Cr, all the LELs derived in this study using the weighted method and published sediment quality guidelines (SQGs) were highly reliable (> 85%) in predicting sites unimpacted by uranium mining/milling defined as sites where reductions in the abundance and species richness of benthic invertebrate communities were < 20%. The derived SEL values and corresponding published SQGs (with the exception of Ni) were not reliable predictors (≤60%) of severe impacts on benthic invertebrate communities when severe impacts are defined as a reduction in abundance and species richness ≥40%. Most of the severely impacted sites had sediment contaminant concentrations well below the SEL values. It is concluded that LELs derived using the weighted method can reliably be used in ecological risk assessments as concentrations below which adverse effects on benthic invertebrate communities are not expected. In contrast, it is recommended that SELs not be used in assessments of uranium mining/milling activities as concentrations above which adverse effects are anticipated.     

Microbial activities and trace element contents in an urban soil

Soil biological properties are influenced by trace metals. The main sources of these pollutants in the urban areas are industrial plants, power stations, domestic heating systems and motor vehicles. The aim of this work was to evaluate, in relation to distance from urban roads, soil trace metal concentrations (Pb, Cu, Cr, Cd and V) and their influence on C-microbial biomass as well as on soil respiration and enzyme activities (phosphatase glucosidase, galactosidase, xylanase, cellulase, trealase, protease and invertase). The samplings were carried out at four sites, along a route that goes from Giannone Street to Passionisti Street, two heavily travelled roads at two different times of the year (spring and autumn). Heavy metal contents and microbial activities were highest at the sites near the roads. The highest values of microbial activities were found in the inner site; here, on the contrary, the lowest concentrations of heavy metals were measured. Significant and negative correlations were found between microbial activity and heavy metal contents.     

Characterisation of airborne uranium and thorium contamination in northern England through measurement of U, Th and 235U/238U in tree bark

Samples of tree bark were collected from four locations in Northern England (a typical rural site, a coal-fired power station, a uranium (isotopic) enrichment plant and a nuclear fuel fabrication facility), to assess the nature and extent of airborne uranium and thorium contamination. The U and Th concentrations of bark were determined by inductively coupled plasma mass spectrometry after conventional nebulisation of bark digests, whilst measurement of 235U/238U isotopic ratio utilised high efficiency nebulisation. Uranium concentrations varied between and within the sites (range, 0.01-12 micrograms g-1), with maximum values recorded within 1 km of the nuclear fuel fabrication plant (Springfields). In comparison, the concentration of Th in bark was low (mean, 0.018 microgram g-1) at all sites with the exception of the area affected by coal combustion (0.2-0.8 microgram g-1). The U/Th ratio varied from 0.5 to 3900 compared with the average crustal ratio of 0.3. Low values (< 2) were recorded at the 'coal' and 'rural' sites whilst Capenhurst and Springfields showed high values indicating the relative magnitude of uranium elevation. Significant enrichment of the natural 235U/238U ratio (0.00725) was observed near the nuclear installations, in particular, the enrichment plant (Capenhurst).     

Metal pollution assessment of sediment and water in the Shur River

Intensified industrialization and human activities have resulted in the release of various contaminants into the environment. Among them, heavy metals are often present as a result of mining, milling and industrial manufacturing. In the present investigation, bulk concentrations Pb, Cd, Zn, Cu, Fe, Ca and Al in Shur River (Iran) bed sediments and water around the Sarcheshmeh copper mine were measured from several sample locations. In addition, partitioning was assessed to determine the proportions of metals in different forms. The degree of sediment contamination was evaluated using an Enrichment Factor (EF) and geo-accumulation index (I (geo)) and a newly developed pollution index (I (POLL)). Elevated metals in sediment and water were found to be correlated with areas of the river that were proximal to direct and indirect mining activities. Cadmium and Zn showed the highest pollution index. Cluster analysis was performed in order to assess heavy metal interactions between water and sediment. Chemical partitioning studies revealed that organic metallic bonds were not significantly present in the sediment of the Shur River.     

Distribution of natural radionuclides in surface soils in the vicinity of abandoned uranium mines in Serbia

The activity concentrations of natural radionuclides in soils from the area affected by uranium mining at Stara Planina Mountain in Serbia were studied and compared with the results obtained from an area with no mining activities (background area). In the affected area, the activity concentrations ranged from 1.75 to 19.2 mg kg^?1 for uranium and from 1.57 to 26.9 mg kg^?1 for thorium which is several-fold higher than those in the background area. The Th/U, K/U, and K/Th activity ratios were also determined and compared with data from similar studies worldwide. External gamma dose rate in the air due to uranium, thorium, and potassium at 1 m above ground level in the area affected by uranium mining was found to be 91.3 nGy h^?1, i.e., about two-fold higher than that in background area. The results of this preliminary study indicate the importance of radiological evaluation of the area and implementation of remedial measures in order to prevent further dispersion of radionuclides in the environment.     

Application of artificial neural networks for classification of uranium distribution in the Central Rand goldfield,South Africa

Mine tailings generate significant environmental impacts and contribute to water pollution. The Central Rand goldfield, South Africa is replete with gold mine tailings which have contributed significantly to water pollution as a result of acid mine drainage (AMD). Water quality is affected by mine tailings and spillages, especially from active slimes dams, currently reprocessed tailings, as well as footprints left behind after reprocessing. The release and distribution of uranium from these sites was studied. Correlation matrices show a strong link between different variables as a result of AMD produced. Principal component analysis (PCA) was used to identify very influential variables which account for the pollution trends. Artificial neural networks (ANN) using the Kohonen algorithm were applied to visualise these trends and patterns in the distribution of uranium. High concentrations of this radionuclide were detected in streams in the vicinity of the tailings dumps, active slimes and reprocessing areas. The concentrations are reduced drastically in dams and wetlands as a result of precipitation and dilution effects.