Assessment of potential migration of radionuclides and trace elements from the White Mesa uranium mill to the Ute Mountain Ute Reservation and surrounding areas, southeastern Utah

USGS Publications Warehouse

Naftz, David L.; Ranalli, Anthony J.; Rowland, Ryan C.; Marston, Thomas M.

2011-01-01

In 2007, the Ute Mountain Ute Tribe requested that the U.S. Environmental Protection Agency and U.S. Geological Survey conduct an independent evaluation of potential offsite migration of radionuclides and selected trace elements associated with the ore storage and milling process at an active uranium mill site near White Mesa, Utah. Specific objectives of this study were (1) to determine recharge sources and residence times of groundwater surrounding the mill site, (2) to determine the current concentrations of uranium and associated trace elements in groundwater surrounding the mill site, (3) to differentiate natural and anthropogenic contaminant sources to groundwater resources surrounding the mill site, (4) to assess the solubility and potential for offsite transport of uranium-bearing minerals in groundwater surrounding the mill site, and (5) to use stream sediment and plant material samples from areas surrounding the mill site to identify potential areas of offsite contamination and likely contaminant sources.

Uranium Release from Acidic Weathered Hanford Sediments: Single-Pass Flow-Through and Column Experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Guohui; Um, Wooyong; Wang, Zheming

The reaction of acidic radioactive waste with sediments can induce mineral transformation reactions that, in turn, control contaminant fate. Here, sediment weathering by synthetic uranium-containing acid solutions was investigated using bench-scale experiments to simulate waste disposal conditions at Hanford’s cribs, USA. During acid weathering, the presence of phosphate exerted a strong influence over uranium mineralogy and a rapidly precipitated, crystalline uranium phosphate phase (meta-ankoleite [K(UO2)(PO4)·3H2O]) was identified using spectroscopic and diffraction-based techniques. In phosphate-free system, uranium oxyhydroxide minerals such as K-compreignacite [K2(UO2)6O4(OH)6·7H2O] were formed. Single-pass flow-through (SPFT) and column leaching experiments using synthetic Hanford pore water showed that uranium precipitatedmore » as meta-ankoleite during acid weathering was strongly retained in the sediments, with an average release rate of 2.67E-12 mol g-1 s-1. In the absence of phosphate, uranium release was controlled by dissolution of uranium oxyhydroxide (compreignacite-type) mineral with a release rate of 1.05-2.42E-10 mol g-1 s-1. The uranium mineralogy and release rates determined for both systems in this study support the development of accurate U-release models for prediction of contaminant transport. These results suggest that phosphate minerals may be a good candidate for uranium remediation approaches at contaminated sites.« less

Uranium Release from Acidic Weathered Hanford Sediments: Single-Pass Flow-Through and Column Experiments.

PubMed

Wang, Guohui; Um, Wooyong; Wang, Zheming; Reinoso-Maset, Estela; Washton, Nancy M; Mueller, Karl T; Perdrial, Nicolas; O'Day, Peggy A; Chorover, Jon

2017-10-03

The reaction of acidic radioactive waste with sediments can induce mineral transformation reactions that, in turn, control contaminant fate. Here, sediment weathering by synthetic uranium-containing acid solutions was investigated using bench-scale experiments to simulate waste disposal conditions at Hanford's cribs (Hanford, WA). During acid weathering, the presence of phosphate exerted a strong influence over uranium mineralogy and a rapidly precipitated, crystalline uranium phosphate phase (meta-ankoleite [K(UO 2 )(PO 4 )·3H 2 O]) was identified using spectroscopic and diffraction-based techniques. In phosphate-free system, uranium oxyhydroxide minerals such as K-compreignacite [K 2 (UO 2 ) 6 O 4 (OH) 6 ·7H 2 O] were formed. Single-pass flow-through (SPFT) and column leaching experiments using synthetic Hanford pore water showed that uranium precipitated as meta-ankoleite during acid weathering was strongly retained in the sediments, with an average release rate of 2.67 × 10 -12 mol g -1 s -1 . In the absence of phosphate, uranium release was controlled by dissolution of uranium oxyhydroxide (compreignacite-type) mineral with a release rate of 1.05-2.42 × 10 -10 mol g -1 s -1 . The uranium mineralogy and release rates determined for both systems in this study support the development of accurate U-release models for the prediction of contaminant transport. These results suggest that phosphate minerals may be a good candidate for uranium remediation approaches at contaminated sites.

Transport of U(VI) through sediments amended with phosphate to induce in situ uranium immobilization.

PubMed

Mehta, Vrajesh S; Maillot, Fabien; Wang, Zheming; Catalano, Jeffrey G; Giammar, Daniel E

2015-02-01

Phosphate amendments can be added to U(VI)-contaminated subsurface environments to promote in situ remediation. The primary objective of this study was to evaluate the impacts of phosphate addition on the transport of U(VI) through contaminated sediments. In batch experiments using sediments (<2 mm size fraction) from a site in Rifle, Colorado, U(VI) only weakly adsorbed due to the dominance of the aqueous speciation by Ca-U(VI)-carbonate complexes. Column experiments with these sediments were performed with flow rates that correspond to a groundwater velocity of 1.1 m/day. In the absence of phosphate, the sediments took up 1.68-1.98 μg U/g of sediments when the synthetic groundwater influent contained 4 μM U(VI). When U(VI)-free influents were then introduced with and without phosphate, substantially more uranium was retained within the column when phosphate was present in the influent. Sequential extractions of sediments from the columns revealed that uranium was uniformly distributed along the length of the columns and was primarily in forms that could be extracted by ion exchange and contact with a weak acid. Laser induced fluorescence spectroscopy (LIFS) analysis along with sequential extraction results suggest adsorption as the dominant uranium uptake mechanism. The response of dissolved uranium concentrations to stopped-flow events and the comparison of experimental data with simulations from a simple reactive transport model indicated that uranium adsorption to and desorption from the sediments was not always at local equilibrium. Copyright © 2014 Elsevier Ltd. All rights reserved.

Sensitivity of geological, geochemical and hydrologic parameters in complex reactive transport systems for in-situ uranium bioremediation

NASA Astrophysics Data System (ADS)

Yang, G.; Maher, K.; Caers, J.

2015-12-01

Groundwater contamination associated with remediated uranium mill tailings is a challenging environmental problem, particularly within the Colorado River Basin. To examine the effectiveness of in-situ bioremediation of U(VI), acetate injection has been proposed and tested at the Rifle pilot site. There have been several geologic modeling and simulated contaminant transport investigations, to evaluate the potential outcomes of the process and identify crucial factors for successful uranium reduction. Ultimately, findings from these studies would contribute to accurate predictions of the efficacy of uranium reduction. However, all these previous studies have considered limited model complexities, either because of the concern that data is too sparse to resolve such complex systems or because some parameters are assumed to be less important. Such simplified initial modeling, however, limits the predictive power of the model. Moreover, previous studies have not yet focused on spatial heterogeneity of various modeling components and its impact on the spatial distribution of the immobilized uranium (U(IV)). In this study, we study the impact of uncertainty on 21 parameters on model responses by means of recently developed distance-based global sensitivity analysis (DGSA), to study the main effects and interactions of parameters of various types. The 21 parameters include, for example, spatial variability of initial uranium concentration, mean hydraulic conductivity, and variogram structures of hydraulic conductivity. DGSA allows for studying multi-variate model responses based on spatial and non-spatial model parameters. When calculating the distances between model responses, in addition to the overall uranium reduction efficacy, we also considered the spatial profiles of the immobilized uranium concentration as target response. Results show that the mean hydraulic conductivity and the mineral reaction rate are the two most sensitive parameters with regard to the overall uranium reduction. But in terms of spatial distribution of immobilized uranium, initial conditions of uranium concentration and spatial uncertainty in hydraulic conductivity also become important. These analyses serve as the first step of further prediction practices of the complex uranium transport and reaction systems.

Effect of Co-Contaminants Uranium and Nitrate on Iodine Remediation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Szecsody, James E.; Lee, Brady D.; Lawter, Amanda R.

The objective of this study is to evaluate the significance of co-contaminants on the migration and transformation of iodine species in the Hanford subsurface environment. These impacts are relevant because remedies that target individual contaminants like iodine, may not only impact the fate and transport of other contaminants in the subsurface, but also inhibit the effectiveness of a targeted remedy. For example, iodine (as iodate) co-precipitates with calcite, and has been identified as a potential remedy because it immobilizes iodine. Since uranium also co-precipitates with calcite in field sediments, the presence of uranium may also inhibit iodine co-precipitation. Another potentiallymore » significant impact from co-existing contaminants is iodine and nitrate. The presence of nitrate has been shown to promote biogeochemical reduction of iodate to iodide, thereby increasing iodine species subsurface mobility (as iodide exhibits less sorption). Hence, this study reports on both laboratory batch and column experiments that investigated a) the change in iodate uptake mass and rate of uptake into precipitating calcite due to the presence of differing amounts of uranium, b) the amount of change of the iodate bio-reduction rate due to the presence of differing nitrate concentrations, and c) whether nitrite can reduce iodate in the presence of microbes and/or minerals acting as catalysts.« less

Field Evaluation of the Restorative Capacity of the Aquifer Downgradient of a Uranium In-Situ Recovery Mining Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reimus, Paul William

A two-part field study was conducted in Smith Ranch-Highland in-situ recovery (ISR) near Douglas, Wyoming, to evaluate the restorative capacity of the aquifer downgradient (i.e., hydrologically downstream) of a Uranium ISR mining site with respect to the transport of uranium and other potential contaminants in groundwater after mining has ceased. The study was partially conducted by checking the Uranium content and the alkalinity of separate wells, some wells had been restored and others had not. A map and in-depth procedures of the study are included.

Decontamination of uranium-contaminated waste oil using supercritical fluid and nitric acid.

PubMed

Sung, Jinhyun; Kim, Jungsoo; Lee, Youngbae; Seol, Jeunggun; Ryu, Jaebong; Park, Kwangheon

2011-07-01

The waste oil used in nuclear fuel processing is contaminated with uranium because of its contact with materials or environments containing uranium. Under current law, waste oil that has been contaminated with uranium is very difficult to dispose of at a radioactive waste disposal site. To dispose of the uranium-contaminated waste oil, the uranium was separated from the contaminated waste oil. Supercritical R-22 is an excellent solvent for extracting clean oil from uranium-contaminated waste oil. The critical temperature of R-22 is 96.15 °C and the critical pressure is 49.9 bar. In this study, a process to remove uranium from the uranium-contaminated waste oil using supercritical R-22 was developed. The waste oil has a small amount of additives containing N, S or P, such as amines, dithiocarbamates and dialkyldithiophosphates. It seems that these organic additives form uranium-combined compounds. For this reason, dissolution of uranium from the uranium-combined compounds using nitric acid was needed. The efficiency of the removal of uranium from the uranium-contaminated waste oil using supercritical R-22 extraction and nitric acid treatment was determined.

Ammonia Gas Transport and Reactions in Unsaturated Sediments: Implications for Use as an Amendment to Immobilize Inorganic Contaminants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhong, Lirong; Szecsody, James E.; Truex, Michael J.

Use of gas-phase amendments for in situ remediation of inorganic contaminants in unsaturated sediments of the vadose zone may be advantageous, but there has been limited development and testing of gas remediation technologies. Treatment with ammonia gas has been studied and has a potential for use in treating inorganic contaminants such as uranium because it induces a high pore-water pH causing mineral dissolution and subsequent formation of stable precipitates that decrease the mobility of some contaminants. For field application, knowledge of ammonia transport and the geochemical reactions induced by ammonia is needed. Laboratory studies were conducted to support calculations neededmore » for field treatment design, to quantify advective and diffusive ammonia transport in unsaturated sediments, to evaluate reactions among gas, sediment, and water, and to study reaction-induced pore-water chemistry changes as a function of ammonia delivery conditions. Ammonia gas quickly partitions into sediment pore water and increases pH up to 13.2. Injected ammonia gas front movement can be reasonably predicted by gas flow rate and equilibrium partitioning. The ammonia gas diffusion rate is a function of the water content in the sediment. Measured diffusion front movement was 0.05, 0.03, and 0.02 cm/hr. in sediments with 2.0%, 8.7%, and 13.0% water content, respectively. Sodium, aluminum, and silica pore-water concentrations increase on exposure to ammonia and then decline as aluminosilicates precipitate with declining pH. When uranium is present in the sediment and pore water, up to 85% of the water-leachable uranium was immobilized by ammonia treatment.« less

Spectroscopic confirmation of uranium(VI)-carbonato adsorption complexes on hematite

USGS Publications Warehouse

Bargar, John R.; Reitmeyer, Rebecca; Davis, James A.

1999-01-01

Evaluating societal risks posed by uranium contamination from waste management facilities, mining sites, and heavy industry requires knowledge about uranium transport in groundwater, often the most significant pathway of exposure to humans. It has been proposed that uranium mobility in aquifers may be controlled by adsorption of U(VI)−carbonato complexes on oxide minerals. The existence of such complexes has not been demonstrated, and little is known about their compositions and reaction stoichiometries. We have used attenuated total reflectance Fourier transform infrared (ATR-FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopies to probe the existence, structures, and compositions of ≡FeOsurface−U(VI)−carbonato complexes on hematite throughout the pH range of uranyl uptake under conditions relevant to aquifers. U(VI)−carbonato complexes were found to be the predominant adsorbed U(VI) species at all pH values examined, a much wider pH range than previously postulated based on analogy to aqueous U(VI)−carbonato complexes, which are trace constituents at pH < 6. This result indicates the inadequacy of the common modeling assumption that the compositions and predominance of adsorbed species can be inferred from aqueous species. By extension, adsorbed carbonato complexes may be of major importance to the groundwater transport of similar actinide contaminants such as neptunium and plutonium.

Microbial Reduction of Fe(III) and U(VI) in Aquifers: Simulations Exploring Coupled Effects of Heterogeneity and Fe(II) Sorption

NASA Astrophysics Data System (ADS)

Scheibe, T. D.; Fang, Y.; Roden, E. E.; Brooks, S. C.; Chien, Y.; Murray, C. J.

2004-05-01

Uranium is a significant groundwater contaminant at many former mining and processing sites. In its oxidized state, U(VI) is soluble and mobile, although strongly retarded by sorption to natural iron oxide surfaces. It has been demonstrated that commonly occurring subsurface microorganisms can reduce uranium and other metals when provided sufficient carbon as an electron donor. Reduced U(IV) precipitates as a solid phase; therefore biostimulation provides a potential strategy for in situ removal from contaminated groundwater. However, these biogeochemical reactions occur in the context of a complex heterogeneous environment in which flow and transport dynamics and abiotic reactions can have significant impacts. We have constructed a high-resolution numerical model of groundwater flow and multicomponent reactive transport that incorporates heterogeneity in hydraulic conductivity and initial Fe(III) distribution, microbial growth and transport dynamics, and effects of sorption or precipitation of biogenic Fe(II) on availability of Fe(III) as an electron acceptor. The biogeochemical reaction models and their parameters are based on laboratory experiments; the heterogeneous field-scale property distributions are based on interpretations of geophysical and other observations at a highly characterized field site. The model is being run in Monte Carlo mode to examine the controls that these factors exert on 1) the initial distribution of sorbed uranium in an oxic environment and 2) the reduction and immobilization of uranium upon introduction of a soluble electron donor.

Reactive transport of uranium in a groundwater bioreduction study: Insights from high-temporal resolution 238U/235U data

NASA Astrophysics Data System (ADS)

Shiel, A. E.; Johnson, T. M.; Lundstrom, C. C.; Laubach, P. G.; Long, P. E.; Williams, K. H.

2016-08-01

We conducted a detailed investigation of U isotopes in conjunction with a broad geochemical investigation during field-scale biostimulation and desorption experiments. This investigation was carried out in the uranium-contaminated alluvial aquifer of the Rifle field research site. In this well-characterized setting, a more comprehensive understanding of U isotope geochemistry is possible. Our results indicate that U isotope fractionation is consistently observed across multiple experiments at the Rifle site. Microbially-mediated reduction is suggested to account for most or all of the observed fractionation as abiotic reduction has been demonstrated to impart much smaller, often near-zero, isotopic fractionation or isotopic fractionation in the opposite direction. Data from some time intervals are consistent with a simple model for transport and U(VI) reduction, where the fractionation factor (ε = +0.65‰ to +0.85‰) is consistent with experimental studies. However, during other time intervals the observed patterns in our data indicate the importance of other processes in governing U concentrations and 238U/235U ratios. For instance, we demonstrate that departures from Rayleigh behavior in groundwater systems arise from the presence of adsorbed species. We also show that isotope data are sensitive to the onset of oxidation after biostimulation ends, even in the case where reduction continues to remove contaminant uranium downstream. Our study and the described conceptual model support the use of 238U/235U ratios as a tool for evaluating the efficacy of biostimulation and potentially other remedial strategies employed at Rifle and other uranium-contaminated sites.

Newly recognized hosts for uranium in the Hanford Site vadose zone

USGS Publications Warehouse

Stubbs, J.E.; Veblen, L.A.; Elbert, D.C.; Zachara, J.M.; Davis, J.A.; Veblen, D.R.

2009-01-01

Uranium contaminated sediments from the U.S. Department of Energy's Hanford Site have been investigated using electron microscopy. Six classes of solid hosts for uranium were identified. Preliminary sediment characterization was carried out using optical petrography, and electron microprobe analysis (EMPA) was used to locate materials that host uranium. All of the hosts are fine-grained and intergrown with other materials at spatial scales smaller than the analytical volume of the electron microprobe. A focused ion beam (FIB) was used to prepare electron-transparent specimens of each host for the transmission electron microscope (TEM). The hosts were identified as: (1) metatorbernite [Cu(UO2)2(PO4)2??8H2O]; (2) coatings on sediment clasts comprised mainly of phyllosilicates; (3) an amorphous zirconium (oxyhydr)oxide found in clast coatings; (4) amorphous and poorly crystalline materials that line voids within basalt lithic fragments; (5) amorphous palagonite surrounding fragments of basaltic glass; and (6) Fe- and Mn-oxides. These findings demonstrate the effectiveness of combining EMPA, FIB, and TEM to identify solid-phase contaminant hosts. Furthermore, they highlight the complexity of U geochemistry in the Hanford vadose zone, and illustrate the importance of microscopic transport in controlling the fate of contaminant metals in the environment. ?? 2008 Elsevier Ltd.

Simplified behaviors from increased heterogeneity: I. 2-D uranium transport experiments at the decimeter scale.

PubMed

Miller, Andrew W; Rodriguez, Derrick R; Honeyman, Bruce D

2013-05-01

Intermediate scale tank studies were conducted to examine the effects of physical heterogeneity of aquifer material on uranium desorption and subsequent transport in order to bridge the scaling gap between bench and field scale systems. Uranium contaminated sediment from a former uranium mill field site was packed into two 2-D tanks with internal dimensions of 2.44×1.22×0.076 m (tank 1) and 2.44×0.61×0.076 m (tank 2). Tank 1 was packed in a physically homogenous manner, and tank 2 was packed with long lenses of high and low conductivities resulting in different flow fields within the tanks. Chemical gradients within the flow domain were altered by temporal changes in influent water chemistry. The uranium source was desorption from the sediment. Despite the physical differences in the flow fields, there were minimal differences in global uranium leaching behavior between the two tanks. The dominant uranium species in both tanks over time and space was Ca2UO2(CO3)3(0). However, the uranium/alkalinity relationships varied as a function of time in tank 1 and were independent of time in tank 2. After planned stop-flow events, small, short-lived rebounds were observed in tank 1 while no rebound of uranium concentrations was observed in tank 2. Despite appearing to be in local equilibrium with respect to uranium desorption, a previously derived surface complexation model was insufficient to describe uranium partitioning within the flow domain. This is the first in a pair of papers; the companion paper presents an intermediate scale 3-D tank experiment and inter-tank comparisons. For these systems, physical heterogeneity at or above the decimeter scale does not affect global scale uranium desorption and transport. Instead, uranium fluxes are controlled by chemistry dependent desorption patterns induced by changing the influent ionic composition. Published by Elsevier B.V.

Simplified behaviors from increased heterogeneity: I. 2-D uranium transport experiments at the decimeter scale

NASA Astrophysics Data System (ADS)

Miller, Andrew W.; Rodriguez, Derrick R.; Honeyman, Bruce D.

2013-05-01

Intermediate scale tank studies were conducted to examine the effects of physical heterogeneity of aquifer material on uranium desorption and subsequent transport in order to bridge the scaling gap between bench and field scale systems. Uranium contaminated sediment from a former uranium mill field site was packed into two 2-D tanks with internal dimensions of 2.44 × 1.22 × 0.076 m (tank 1) and 2.44 × 0.61 × 0.076 m (tank 2). Tank 1 was packed in a physically homogenous manner, and tank 2 was packed with long lenses of high and low conductivities resulting in different flow fields within the tanks. Chemical gradients within the flow domain were altered by temporal changes in influent water chemistry. The uranium source was desorption from the sediment. Despite the physical differences in the flow fields, there were minimal differences in global uranium leaching behavior between the two tanks. The dominant uranium species in both tanks over time and space was Ca2UO2(CO3)30. However, the uranium/alkalinity relationships varied as a function of time in tank 1 and were independent of time in tank 2. After planned stop-flow events, small, short-lived rebounds were observed in tank 1 while no rebound of uranium concentrations was observed in tank 2. Despite appearing to be in local equilibrium with respect to uranium desorption, a previously derived surface complexation model was insufficient to describe uranium partitioning within the flow domain. This is the first in a pair of papers; the companion paper presents an intermediate scale 3-D tank experiment and inter-tank comparisons. For these systems, physical heterogeneity at or above the decimeter scale does not affect global scale uranium desorption and transport. Instead, uranium fluxes are controlled by chemistry dependent desorption patterns induced by changing the influent ionic composition.

Application of Optical Imaging Techniques for Quantification of pH and O2 Dynamicsin Porous Media

NASA Astrophysics Data System (ADS)

Li, B.; Seliman, A. F.; Pales, A. R.; Liang, W.; Sams, A.; Darnault, C. J. G.; DeVol, T. A.

2016-12-01

Understanding the spatial and temporal distribution of physical and chemical parameters (e.g. pH, O2) is imperative to characterize the behavior of contaminants in a natural environment. The objectives of this research are to calibrate pH and O2 sensor foils, to develop a dual pH/O2 sensor foil, and to apply them into flow and transport experiments, in order to understand the physical and chemical parameters that control contaminant fate and transport in an unsaturated sandy porous medium. In addition, demonstration of a sensor foil that quantifies aqueous uranium concentration will be presented. Optical imaging techniques will be conducted with 2D tanks to investigate the influence of microbial exudates and plant roots on pH and O2 parameters and radionuclides transport. As a non-invasive method, the optical imaging technique utilizes optical chemical sensor films and either a digital camera or a spectrometer to capture the changes with high temporal and spatial resolutions. Sensor foils are made for different parameters by applying dyes to generate favorable fluorescence that is proportional to the parameter of interest. Preliminary results suggested that this method could detect pH ranging from 4.5 to 7.5. The result from uranium foil test with different concentrations in the range of 2 to 8 ppm indicated that a higher concentration of uranium resulted in a greater color intensity.

A record of uranium-series transport at Nopal I, Sierra Pena Blanca, Mexico: Implications for natural uranium deposits and radioactive waste repositories

DOE PAGES

Denton, J. S.; Goldstein, S. J.; Paviet, P.; ...

2016-04-10

Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less

Fate of Uranium in Wetlands: Impact of Drought Followed by Re-flooding

NASA Astrophysics Data System (ADS)

Gilson, E.; Huang, S.; Koster van Groos, P. G.; Scheckel, K.; Peacock, A. D.; Kaplan, D. I.; Jaffe, P. R.

2014-12-01

Uranium contamination in groundwater can be mitigated in anoxic zones by iron-reducing bacteria that reduce soluble U(VI) to insoluble U(IV) and by uranium immobilization through complexation and sorption. Wetlands often link ground and surface-waters, making them strategic systems for potentially limiting migration of uranium contamination. Little is known about how drought periods that result in the drying of wetland soils, and consequent redox changes, affect uranium fate and transport in wetlands. In order to better understand the fate and stability of immobilized uranium in wetland soils, and how dry periods affect the uranium stability, we dosed saturated wetland mesocosms planted with Scirpus acutus with low levels of uranyl-acetate for 5 months before imposing a 9-day drying period followed by a 13-day rewetting period. Concentrations of uranium in mesocosm effluent increased after rewetting, but the cumulative amount of uranium released in the 13 days following the drying constituted less than 1% of the uranium immobilized in the soil during the 5 months prior to the drought. This low level of remobilization suggests that the uranium immobilized in these soils was not primarily bioreduced U(IV), which could have been oxidized to soluble U(VI) during the drought and released in the effluent during the subsequent flood. XANES analyses confirm that most of the uranium immobilized in the mesocosms was U(VI) sorbed to iron oxides. Compared to mesocosms that did not experience drying or rewetting, mesocosms that were sacrificed immediately after drying and after 13 days of rewetting had less uranium in soil near roots and more uranium on root surfaces. Metal-reducing bacteria only dominated the bacterial community after 13 days of rewetting and not immediately after drying, indicating that these bacteria are not responsible for this redistribution of uranium after the drying and rewetting. Results show that short periods of drought conditions in a wetland may impact uranium distribution, but these conditions may not cause large losses of immobilized uranium from the wetland.

Understanding Uranium Behavior in a Reduced Aquifer

NASA Astrophysics Data System (ADS)

Janot, N.; Lezama-Pacheco, J. S.; Williams, K. H.; Bernier-Latmani, R.; Long, P. E.; Davis, J. A.; Fox, P. M.; Yang, L.; Giammar, D.; Cerrato, J. M.; Bargar, J.

2012-12-01

Uranium contamination of groundwater is a concern at several US Department of Energy sites, such Old Rifle, CO. Uranium transport in the environment is mainly controlled by its oxidation state, since oxidized U(VI) is relatively mobile, whereas U(IV) is relatively insoluble. Bio-remediation of contaminated aquifers aims at immobilizing uranium in a reduced form. Previous laboratory and field studies have shown that adding electron donor (lactate, acetate, ethanol) to groundwater stimulates the activity of metal- and sulfate-reducing bacteria, which promotes U(VI) reduction in contaminated aquifers. However, obtaining information on chemical and physical forms of U, Fe and S species for sediments biostimulated in the field, as well as kinetic parameters such as U(VI) reduction rate, is challenging due to the low concentration of uranium in the aquifers (typically < 10 ppm) and the expense of collecting large number of cores. An in-situ technique has been developed for studying uranium, iron and sulfur reduction dynamics during such bioremediation episodes. This technique uses in-well columns to obtain direct access to chemical and physical forms of U(IV) produced in the aquifer, evolving microbial communities, and trace and major ion groundwater constituents. While several studies have explored bioreduction of uranium under sulfate-reducing conditions, less attention has been paid to the initial iron-reducing phase, noted as being of particular importance to uranium removal. The aim of this work was to assess the formation of U(IV) during the early stages of a bio-remediation experiment at the Old Rifle site, CO, from early iron-reducing conditions to the transition to sulfate-reducing conditions. Several in-well chromatographic columns packed with sediment were deployed and were sampled at different days after the start of bio-reduction. X-ray absorption spectroscopy and X-ray microscopy were used to obtain information on Fe, S and U speciation and distribution. Chemical extractions of the reduced sediments have also been performed, to determine the rate of Fe(II) and U(IV) accumulation.

Processes affecting transport of uranium in a suboxic aquifer

USGS Publications Warehouse

Davis, J.A.; Curtis, G.P.; Wilkins, M.J.; Kohler, M.; Fox, P.; Naftz, D.L.; Lloyd, J.R.

2006-01-01

At the Naturita site in Colorado, USA, groundwaters were sampled and analyzed for chemical composition and by culture and culture-independent microbiological techniques. In addition, sediments were extracted with a dilute sodium carbonate solution to determine quantities of labile uranium within the sediments. Samples from the upgradient portion of the contaminated aquifer, where very little dissolved Fe(II) is found in the groundwater, have uranium content that is controlled by U(VI) adsorption and few metal-reducing bacteria are observed. In the extreme downgradient portion of the aquifer, where dissolved Fe(II) is observed, uranium content of the sediments includes significant quantities of reduced U(IV) and diverse populations of Fe(III)-reducing bacteria were present in the subsurface with the potential of reducing U(VI) to U(IV). ?? 2006 Elsevier Ltd. All rights reserved.

Exogenous contamination of uranium in human scalp hair.

PubMed

Muikku, Maarit; Heikkinen, Tarja

2012-06-01

The use of human scalp hair as a bioindicator of occupational or environmental exposure has been the subject of some debate over the years. One problem is how to distinguish internal contamination from external contamination. In this study, possibility that elevated levels of natural uranium in human hair are partly due to the exogenously bound uranium from uranium-rich household water was tested. Hair samples from six adult volunteers were cut and then exposed externally to uranium by using washing water with highly elevated levels of natural uranium. After that, and before making the analysis using inductively coupled plasma mass spectrometry (ICP-MS), the samples were washed using two commonly used washing procedures in order to remove external contamination. No quantitative information was gained in the tests, but it was shown that the use of uranium-rich water when washing hair affects the uranium concentration in hair. Although the samples were cleaned according to widely used washing procedures before the analysis, the uranium concentrations in hair were about three orders of magnitude higher after the tests. The possibility of external contamination should be kept in mind, especially when considering hair as an excretion pathway for estimating internal dose.

Geochemical investigations by the U.S. Geological Survey on uranium mining, milling, and environmental restoration

USGS Publications Warehouse

Landa, Edward R.; Cravotta, Charles A.; Naftz, David L.; Verplanck, Philip L.; Nordstrom, D. Kirk; Zielinski, Robert A.

2000-01-01

Recent research by the U.S. Geological Survey has characterized contaminant sources and identified important geochemical processes that influence transport of radionuclides from uranium mining and milling wastes. 1) Selective extraction studies indicated that alkaline earth sulfates and hydrous ferric oxides are important hosts of 226Ra in uranium mill tailings. The action of sulfate-reducing and ironreducing bacteria on these phases was shown to enhance release of radium, and this adverse result may temper decisions to dispose of uranium mill tailings in anaerobic environments. 2) Field studies have shown that although surface-applied sewage sludge/wood chip amendments aid in revegetating pyritic spoil, the nitrogen in sludge leachate can enhance pyrite oxidation, acidification of groundwater, and the consequent mobilization of metals and radionuclides. 3) In a U.S. Environmental Protection Agencyfunded study, three permeable reactive barriers consisting of phosphate-rich material, zero-valent iron, or amorphous ferric oxyhydroxide have been installed at an abandoned uranium upgrader facility near Fry Canyon, UT. Preliminary results indicate that each of the permeable reactive barriers is removing the majority of the uranium from the groundwater. 4) Studies on the geochemistry of rare earth elements as analogues for actinides such as uranium and thorium in acid mine drainage environments indicate high mobility under acid-weathering conditions but measurable attenuation associated with iron and aluminum colloid formation. Mass balances from field and laboratory studies are being used to quantify the amount of attenuation. 5) A field study in Colorado demonstrated the use of 234U/238U isotopic ratio measurements to evaluate contamination of shallow groundwater with uranium mill effluent.

TRANSPORT AND FATE OF AMMONIUM AND ITS IMPACT ON URANIUM AND OTHER TRACE ELEMENTS AT A FORMER URANIUM MILL TAILING SITE

PubMed Central

Miao, Ziheng; Nihat, Hakan; McMillan, Andrew Lee; Brusseau, Mark L.

2013-01-01

The remediation of ammonium-containing groundwater discharged from uranium mill tailing sites is a difficult problem facing the mining industry. The Monument Valley site is a former uranium mining site in the southwest US with both ammonium and nitrate contamination of groundwater. In this study, samples collected from 14 selected wells were analyzed for major cations and anions, trace elements, and isotopic composition of ammonium and nitrate. In addition, geochemical data from the U.S. Department of Energy (DOE) database were analyzed. Results showing oxic redox conditions and correspondence of isotopic compositions of ammonium and nitrate confirmed the natural attenuation of ammonium via nitrification. Moreover, it was observed that ammonium concentration within the plume area is closely related to concentrations of uranium and a series of other trace elements including chromium, selenium, vanadium, iron, and manganese. It is hypothesized that ammonium-nitrate transformation processes influence the disposition of the trace elements through mediation of redox potential, pH, and possibly aqueous complexation and solid-phase sorption. Despite the generally relatively low concentrations of trace elements present in groundwater, their transport and fate may be influenced by remediation of ammonium or nitrate at the site. PMID:24357895

A new formulation containing calixarene molecules as an emergency treatment of uranium skin contamination.

PubMed

Spagnul, Aurélie; Bouvier-Capely, Céline; Phan, Guillaume; Rebière, François; Fattal, Elias

2010-09-01

Cutaneous contamination represents the second highest contamination pathway in the nuclear industry. Despite that the entry of actinides such as uranium into the body through intact or wounded skin can induce a high internal exposure, no specific emergency treatment for cutaneous contamination exists. In the present work, an innovative formulation dedicated to uranium skin decontamination was developed. The galenic form consists in an oil-in-water nanoemulsion, which contains a tricarboxylic calixarene known for its high uranium affinity and selectivity. The physicochemical characterization of this topical form revealed that calixarene molecules are located at the surface of the dispersed oil droplets of the nanoemulsion, being thus potentially available for uranium chelation. It was demonstrated in preliminary in vitro experiments by using an adapted ultrafiltration method that the calixarene nanoemulsion was able to extract and retain more than 80% of uranium from an aqueous uranyl nitrate contamination solution. First ex vivo experiments carried out in Franz diffusion cells on pig ear skin explants during 24 h showed that the immediate application of the calixarene nanoemulsion on a skin contaminated by a uranyl nitrate solution allowed a uranium transcutaneous diffusion decrease of about 98% through intact and excoriated skins. The calixarene nanoemulsion developed in this study thus seems to be an efficient emergency system for uranium skin decontamination.

Remediation of uranium contaminated soils with bicarbonate extraction and microbial U(VI) reduction

USGS Publications Warehouse

Philips , Elizabeth J.P.; Landa, Edward R.; Lovely, Derek R.

1995-01-01

A process for concentrating uranium from contaminated soils in which the uranium is first extracted with bicarbonate and then the extracted uranium is precipitated with U(VI)-reducing microorganisms was evaluated for a variety of uranuum-contaminated soils. Bicarbonate (100 mM) extracted 20–94% of the uranium that was extracted with nitric acid. The U(VI)-reducing microorganism,Desulfovibrio desulfuricans reduced the U(VI) to U(IV) in the bicarbonate extracts. In some instances unidentified dissolved extracted components, presumably organics, gave the extract a yellow color and inhibited U(VI) reduction and/or the precipitation of U(IV). Removal of the dissolved yellow material with the addition of hydrogen peroxide alleviated this inhibition. These results demonstrate that bicarbonate extraction of uranium from soil followed by microbial U(VI) reduction might be an effective mechanism for concentrating uranium from some contaminated soils.

Column Testing and 1D Reactive Transport Modeling to Evaluate Uranium Plume Persistence Processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Raymond H.; Morrison, Stan; Morris, Sarah

Motivation for Study: Natural flushing of contaminants at various U.S. Department of Energy Office of Legacy Management sites is not proceeding as quickly as predicted (plume persistence) Objectives: Help determine natural flushing rates using column tests. Use 1D reactive transport modeling to better understand the major processes that are creating plume persistence Approach: Core samples from under a former mill tailings area Tailings have been removed. Column leaching using lab-prepared water similar to nearby Gunnison River water. 1D reactive transport modeling to evaluate processes

High frequency EMI sensing for estimating depleted uranium radiation levels in soil

NASA Astrophysics Data System (ADS)

Shubitidze, Fridon; Barrowes, Benjamin E.; Ballard, John; Unz, Ron; Randle, Adam; Larson, Steve L.; O'Neill, Kevin A.

2018-04-01

This paper studies high (100 kHz up to 15 MHz) frequency electromagnetic responses (HFEMI) for DU metallic pieces and DU contaminated soils and derives a simple empirical expression from the measured HFEMI data for estimating DU contamination levels in soil. Depleted uranium (DU) is the byproduct of uranium enrichment and contains 33% less radioactive isotopes than natural uranium. There are at least thirty facilities at fourteen separate locations in the US, where munitions containing DU have been evaluated or used for training. At these sites, which vary in size, evaluation studies have been conducted with and without catch boxes. In addition, the DoD used DU at open firing ranges as large as thousands of acres (hundreds of hectares), for both artillery and aircraft training. These activities have left a legacy of DU contamination. Currently at military sites where DU munitions have been or are being used, cleanup activities mainly are done by excavating and shipping large volumes of site soil and berm materials to a hazardous material radiation disposal site. This approach is very time consuming, costly, and associated with the potential for exposure of personnel performing excavation and transportation. It also limits range use during the operation. So, there is an urgent need for technologies for rapid surveying of large areas to detect, locate, and removal of DU contaminants at test sites. Additionally, the technologies are needed to detect material at a depth of at least 30 cm as well as discriminate between DU metals and oxides from natural uranium and from other conductive metals such as natural and man-made range clutter. One of the potential technologies for estimating DU radiation levels in soils is HFEMI sensing. In this paper, HFEMI signals are collected for DU metal pieces, sodium diunarate (Na2U2 O3) and tri-uranium octoxide (U3O8). The EMI signal's sensitivity with respect to DU material composition and conditions are illustrated and analyzed. A new scheme for extracting near-surface soil's EM parameters is formulated.

Uranium Bioreduction and Biomineralization.

PubMed

Wufuer, Rehemanjiang; Wei, Yongyang; Lin, Qinghua; Wang, Huawei; Song, Wenjuan; Liu, Wen; Zhang, Daoyong; Pan, Xiangliang; Gadd, Geoffrey Michael

2017-01-01

Following the development of nuclear science and technology, uranium contamination has been an ever increasing concern worldwide because of its potential for migration from the waste repositories and long-term contaminated environments. Physical and chemical techniques for uranium pollution are expensive and challenging. An alternative to these technologies is microbially mediated uranium bioremediation in contaminated water and soil environments due to its reduced cost and environmental friendliness. To date, four basic mechanisms of uranium bioremediation-uranium bioreduction, biosorption, biomineralization, and bioaccumulation-have been established, of which uranium bioreduction and biomineralization have been studied extensively. The objective of this review is to provide an understanding of recent developments in these two fields in relation to relevant microorganisms, mechanisms, influential factors, and obstacles. Copyright © 2017 Elsevier Inc. All rights reserved.

Radon as a natural tracer for gas transport within uranium waste rock piles.

PubMed

Silva, N C; Chagas, E G L; Abreu, C B; Dias, D C S; Lopez, D; Guerreiro, E T Z; Alberti, H L C; Braz, M L; Branco, O; Fleming, P

2014-07-01

Acid mine drainage (AMD) has been identified as the main cause for outflow of acid water and radioactive/non-radioactive contaminants. AMD encompasses pyrites oxidation when water and oxygen are available. AMD was identified in uranium waste rock piles (WRPs) of Indústrias Nucleares do Brasil-Caldas facility (Brazilian uranium mine), resulting in high costs for water treatment. AMD reduction is the main challenge, and scientific investigation has been conducted to understand oxygen and water transportation within WRPs, where 222Rn is used as natural tracer for oxygen transportation. The study consists of soil radon gas mapping in the top layer of WRP4 using active soil gas pumping, radon adsorption in active charcoal and 222Rn determination using high-resolution gamma-ray spectrometry. A sampling network of 71 points was built where samples were collected at a depth of 40 cm. Soil radon gas concentration ranged from 33.7 to 1484.2 kBq m(-3) with mean concentration of 320.7±263.3 kBq m(-3). © The Author 2014. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

Mineral solubility and free energy controls on microbial reaction kinetics: Application to contaminant transport in the subsurface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taillefert, Martial; Van Cappellen, Philippe

Recent developments in the theoretical treatment of geomicrobial reaction processes have resulted in the formulation of kinetic models that directly link the rates of microbial respiration and growth to the corresponding thermodynamic driving forces. The overall objective of this project was to verify and calibrate these kinetic models for the microbial reduction of uranium(VI) in geochemical conditions that mimic as much as possible field conditions. The approach combined modeling of bacterial processes using new bioenergetic rate laws, laboratory experiments to determine the bioavailability of uranium during uranium bioreduction, evaluation of microbial growth yield under energy-limited conditions using bioreactor experiments, competitionmore » experiments between metabolic processes in environmentally relevant conditions, and model applications at the field scale. The new kinetic descriptions of microbial U(VI) and Fe(III) reduction should replace those currently used in reactive transport models that couple catabolic energy generation and growth of microbial populations to the rates of biogeochemical redox processes. The above work was carried out in collaboration between the groups of Taillefert (batch reactor experiments and reaction modeling) at Georgia Tech and Van Cappellen (retentostat experiments and reactive transport modeling) at University of Waterloo (Canada).« less

Microbial reduction of uranium

USGS Publications Warehouse

Lovley, D.R.; Phillips, E.J.P.; Gorby, Y.A.; Landa, E.R.

1991-01-01

REDUCTION of the soluble, oxidized form of uranium, U(VI), to insoluble U(IV) is an important mechanism for the immobilization of uranium in aquatic sediments and for the formation of some uranium ores1-10. U(VI) reduction has generally been regarded as an abiological reaction in which sulphide, molecular hydrogen or organic compounds function as the reductant1,2,5,11. Microbial involvement in U(VI) reduction has been considered to be limited to indirect effects, such as microbial metabolism providing the reduced compounds for abiological U(VI) reduction and microbial cell walls providing a surface to stimulate abiological U(VI) reduction1,12,13. We report here, however, that dissimilatory Fe(III)-reducing microorganisms can obtain energy for growth by electron transport to U(VI). This novel form of microbial metabolism can be much faster than commonly cited abiological mechanisms for U(VI) reduction. Not only do these findings expand the known potential terminal electron acceptors for microbial energy transduction, they offer a likely explanation for the deposition of uranium in aquatic sediments and aquifers, and suggest a method for biological remediation of environments contaminated with uranium.

Evaluation of residual uranium contamination in the dirt floor of an abandoned metal rolling mill.

PubMed

Glassford, Eric; Spitz, Henry; Lobaugh, Megan; Spitler, Grant; Succop, Paul; Rice, Carol

2013-02-01

A single, large, bulk sample of uranium-contaminated material from the dirt floor of an abandoned metal rolling mill was separated into different types and sizes of aliquots to simulate samples that would be collected during site remediation. The facility rolled approximately 11,000 tons of hot-forged ingots of uranium metal approximately 60 y ago, and it has not been used since that time. Thirty small mass (≈ 0.7 g) and 15 large mass (≈ 70 g) samples were prepared from the heterogeneously contaminated bulk material to determine how measurements of the uranium contamination vary with sample size. Aliquots of bulk material were also resuspended in an exposure chamber to produce six samples of respirable particles that were obtained using a cascade impactor. Samples of removable surface contamination were collected by wiping 100 cm of the interior surfaces of the exposure chamber with 47-mm-diameter fiber filters. Uranium contamination in each of the samples was measured directly using high-resolution gamma ray spectrometry. As expected, results for isotopic uranium (i.e., U and U) measured with the large-mass and small-mass samples are significantly different (p < 0.001), and the coefficient of variation (COV) for the small-mass samples was greater than for the large-mass samples. The uranium isotopic concentrations measured in the air and on the wipe samples were not significantly different and were also not significantly different (p > 0.05) from results for the large- or small-mass samples. Large-mass samples are more reliable for characterizing heterogeneously distributed radiological contamination than small-mass samples since they exhibit the least variation compared to the mean. Thus, samples should be sufficiently large in mass to insure that the results are truly representative of the heterogeneously distributed uranium contamination present at the facility. Monitoring exposure of workers and the public as a result of uranium contamination resuspended during site remediation should be evaluated using samples of sufficient size and type to accommodate the heterogeneous distribution of uranium in the bulk material.

Ecotoxicity literature review of selected Hanford Site contaminants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Driver, C.J.

1994-03-01

Available information on the toxicity, food chain transport, and bioconcentration of several Hanford Site contaminants were reviewed. The contaminants included cesium-137, cobalt-60, europium, nitrate, plutonium, strontium-90, technetium, tritium, uranium, and chromium (III and VI). Toxicity and mobility in both aquatic and terrestrial systems were considered. For aquatic systems, considerable information was available on the chemical and/or radiological toxicity of most of the contaminants in invertebrate animals and fish. Little information was available on aquatic macrophyte response to the contaminants. Terrestrial animals such as waterfowl and amphibians that have high exposure potential in aquatic systems were also largely unrepresented in themore » toxicity literature. The preponderance of toxicity data for terrestrial biota was for laboratory mammals. Bioconcentration factors and transfer coefficients were obtained for primary producers and consumers in representative aquatic and terrestrial systems; however, little data were available for upper trophic level transfer, particularly for terrestrial predators. Food chain transport and toxicity information for the contaminants were generally lacking for desert or sage brush-steppe organisms, particularly plants and reptiles« less

Effect of pH and Pressure on Uranium Removal from Drinking Water Using NF/RO Membranes.

PubMed

Schulte-Herbrüggen, Helfrid M A; Semião, Andrea J C; Chaurand, Perrine; Graham, Margaret C

2016-06-07

Groundwater is becoming an increasingly important drinking water source. However, the use of groundwater for potable purposes can lead to chronic human exposure to geogenic contaminants, for example, uranium. Nanofiltration (NF) and reverse osmosis (RO) processes are used for drinking water purification, and it is important to understand how contaminants interact with membranes since accumulation of contaminants to the membrane surface can lead to fouling, performance decline and possible breakthrough of contaminants. During the current study laboratory experiments were conducted using NF (TFC-SR2) and RO (BW30) membranes to establish the behavior of uranium across pH (3-10) and pressure (5-15 bar) ranges. The results showed that important determinants of uranium-membrane sorption interactions were (i) the uranium speciation (uranium species valence and size in relation to membrane surface charge and pore size) and (ii) concentration polarization, depending on the pH values. The results show that it is important to monitor sorption of uranium to membranes, which is controlled by pH and concentration polarization, and, if necessary, adjust those parameters controlling uranium sorption.

Calixarene-entrapped nanoemulsion for uranium extraction from contaminated solutions.

PubMed

Spagnul, Aurélie; Bouvier-Capely, Céline; Phan, Guillaume; Rebière, François; Fattal, Elias

2010-03-01

Accidental cutaneous contamination by actinides such as uranium occurring to nuclear power plant workers can lead to their dissemination in other tissues and induce severe damages. Until now, no specific emergency treatment for such contamination has been developed. The aim of the present work was to formulate a tricarboxylic calix[6]arene molecule, known to exhibit good affinity and selectivity for complexing uranium, within a topical delivery system for the treatment of skin contamination. Since calixarene was shown to reduce oil/water interfacial tension, we have designed an oil-in-water nanoemulsion, taking advantage of the small droplet size offering a high contact surface with the contaminated aqueous medium. Characterization of the calixarene nanoemulsion was performed by determination of the oily droplet size, zeta potential and pH, measured as a function of the calixarene concentration. The obtained results have confirmed the surface localization of calixarene molecules being potentially available to extract uranyl ions from an aqueous contaminated solution. In a preliminary experiments, the calixarene nanoemulsion was used for the removal of free uranium from an aqueous contaminated solution. Results showed that the calixarene nanoemulsion extracted up to 80 +/- 5% of uranium, which demonstrates the potential interest of this delivery system for uranium skin decontamination. 2009 Wiley-Liss, Inc. and the American Pharmacists Association

Fission- and alpha-track study of biogeochemistry of plutonium and uranium in carbonates of bikini and enewetak atolls. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Levy, Y.; Friedman, G. M.; Miller, D. S.

1978-12-31

Results of the analysis of uranium concentrations in the 8 coral heads sampled from the Bikini and Enewetak lagoons lead to the following conclusions: (1) no parallel increase in uranium concentration was found in the corals contaminated by Pu and Am; (2) in the noncontaminated corals, the fission track analysis shows wider ranges of uranium concentrations (1.8 to 3.1). Thus, in the corals not contaminated by Pu and Am, uranium concentrations similar to the uranium concentration in the contaminated corals were found; (3) uranium content in all corals analyzed was rather homogeneously distributed, i.e., no hot spots, stars, or areasmore » differing in concentration by more than a few percent were detected by the fission track analyses.« less

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

PubMed Central

Zhang, Ping; Wu, Linwei; Rocha, Andrea M.; Shi, Zhou; Wu, Bo; Qin, Yujia; Wang, Jianjun; Yan, Qingyun; Curtis, Daniel; Ning, Daliang; Van Nostrand, Joy D.; Wu, Liyou; Watson, David B.; Adams, Michael W. W.; Alm, Eric J.; Adams, Paul D.; Arkin, Adam P.

2018-01-01

ABSTRACT Contamination from anthropogenic activities has significantly impacted Earth’s biosphere. However, knowledge about how environmental contamination affects the biodiversity of groundwater microbiomes and ecosystem functioning remains very limited. Here, we used a comprehensive functional gene array to analyze groundwater microbiomes from 69 wells at the Oak Ridge Field Research Center (Oak Ridge, TN), representing a wide pH range and uranium, nitrate, and other contaminants. We hypothesized that the functional diversity of groundwater microbiomes would decrease as environmental contamination (e.g., uranium or nitrate) increased or at low or high pH, while some specific populations capable of utilizing or resistant to those contaminants would increase, and thus, such key microbial functional genes and/or populations could be used to predict groundwater contamination and ecosystem functioning. Our results indicated that functional richness/diversity decreased as uranium (but not nitrate) increased in groundwater. In addition, about 5.9% of specific key functional populations targeted by a comprehensive functional gene array (GeoChip 5) increased significantly (P < 0.05) as uranium or nitrate increased, and their changes could be used to successfully predict uranium and nitrate contamination and ecosystem functioning. This study indicates great potential for using microbial functional genes to predict environmental contamination and ecosystem functioning. PMID:29463661

Trace elements and Pb isotopes in soils and sediments impacted by uranium mining.

PubMed

Cuvier, A; Pourcelot, L; Probst, A; Prunier, J; Le Roux, G

2016-10-01

The purpose of this study is to evaluate the contamination in As, Ba, Co, Cu, Mn, Ni, Sr, V, Zn and REE, in a high uranium activity (up to 21,000Bq∙kg(-1)) area, downstream of a former uranium mine. Different geochemical proxies like enrichment factor and fractions from a sequential extraction procedure are used to evaluate the level of contamination, the mobility and the availability of the potential contaminants. Pb isotope ratios are determined in the total samples and in the sequential leachates to identify the sources of the contaminants and to determine the mobility of radiogenic Pb in the context of uranium mining. In spite of the large uranium contamination measured in the soils and the sediments (EF≫40), trace element contamination is low to moderate (2

Modeling the effectiveness of U(VI) biomineralization in dual-porosity porous media

NASA Astrophysics Data System (ADS)

Rotter, B. E.; Barry, D. A.; Gerhard, J. I.; Small, J. S.

2011-05-01

SummaryUranium contamination is a serious environmental concern worldwide. Recent attention has focused on the in situ immobilization of uranium by stimulation of dissimilatory metal-reducing bacteria (DMRB). The objective of this work was to investigate the effectiveness of this approach in heterogeneous and structured porous media, since such media may significantly affect the geochemical and microbial processes taking place in contaminated sites, impacting remediation efficiency during biostimulation. A biogeochemical reactive transport model was developed for uranium remediation by immobile-region-resident DMRB in two-region porous media. Simulations were used to investigate the parameter sensitivities of the system over wide-ranging geochemical, microbial and groundwater transport conditions. The results suggest that optimal biomineralization is generally likely to occur when the regional mass transfer timescale is less than one-thirtieth the value of the volumetric flux timescale, and/or the organic carbon fermentation timescale is less than one-thirtieth the value of the advective timescale, and/or the mobile region porosity ranges between equal to and four times the immobile region porosity. Simulations including U(VI) surface complexation to Fe oxides additionally suggest that, while systems exhibiting U(VI) surface complexation may be successfully remediated, they are likely to display different degrees of remediation efficiency over varying microbial efficiency, mobile-immobile mass transfer, and porosity ratios. Such information may aid experimental and field designs, allowing for optimized remediation in dual-porosity (two-region) biostimulated DMRB U(VI) remediation schemes.

The combined effect of uranium and gamma radiation on biological responses and oxidative stress induced in Arabidopsis thaliana.

PubMed

Vanhoudt, Nathalie; Vandenhove, Hildegarde; Horemans, Nele; Wannijn, Jean; Van Hees, May; Vangronsveld, Jaco; Cuypers, Ann

2010-11-01

Uranium never occurs as a single pollutant in the environment, but always in combination with other stressors such as ionizing radiation. As effects induced by multiple contaminants can differ markedly from the effects induced by the individual stressors, this multiple pollution context should not be neglected. In this study, effects on growth, nutrient uptake and oxidative stress induced by the single stressors uranium and gamma radiation are compared with the effects induced by the combination of both stressors. By doing this, we aim to better understand the effects induced by the combined stressors but also to get more insight in stressor-specific response mechanisms. Eighteen-day-old Arabidopsis thaliana seedlings were exposed for 3 days to 10 muM uranium and 3.5 Gy gamma radiation. Gamma radiation interfered with uranium uptake, resulting in decreased uranium concentrations in the roots, but with higher transport to the leaves. This resulted in a better root growth but increased leaf lipid peroxidation. For the other endpoints studied, effects under combined exposure were mostly determined by uranium presence and only limited influenced by gamma presence. Furthermore, an important role is suggested for CAT1/2/3 gene expression under uranium and mixed stressor conditions in the leaves.

The dendroanalysis of oak trees as a method of biomonitoring past and recent contamination in an area influenced by uranium mining.

PubMed

Märten, Arno; Berger, Dietrich; Köhler, Mirko; Merten, Dirk

2015-12-01

We reconstructed the contamination history of an area influenced by 40 years of uranium mining and subsequent remediation actions using dendroanalysis (i.e., the determination of the elemental content of tree rings). The uranium content in the tree rings of four individual oak trees (Quercus sp.) was determined by laser ablation with inductively coupled plasma mass spectrometry (LA-ICP-MS). This technique allows the investigation of trace metals in solid samples with a spatial resolution of 250 μm and a detection limit below 0.01 μg/g for uranium. The investigations show that in three of the four oaks sampled, there were temporally similar uranium concentrations. These were approximately 2 orders of magnitude higher (0.15 to 0.4 μg/g) than those from before the period of active mining (concentrations below 0.01 μg/g). After the mining was terminated and the area was restored, the uranium contents in the wood decreased by approximately 1 order of magnitude. The similar radial uranium distribution patterns of the three trees were confirmed by correlation analysis. In combination with the results of soil analyses, it was determined that there was a heterogeneous contamination in the forest investigated. This could be confirmed by pre-remediation soil uranium contents from literature. The uranium contents in the tree rings of the oaks investigated reflect the contamination history of the study area. This study demonstrates that the dendrochemical analysis of oak tree rings is a suitable technique for investigating past and recent uranium contamination in mining areas.

Method to remove uranium/vanadium contamination from groundwater

DOEpatents

Metzler, Donald R.; Morrison, Stanley

2004-07-27

A process for removing uranium/vanadium-based contaminants from groundwater using a primary in-ground treatment media and a pretreatment media that chemically adjusts the groundwater contaminant to provide for optimum treatment by the primary treatment media.

FLUORIDE VOLATILITY PROCESS FOR THE RECOVERY OF URANIUM

DOEpatents

Katz, J.J.; Hyman, H.H.; Sheft, I.

1958-04-15

The separation and recovery of uraniunn from contaminants introduced by neutron irradiation by a halogenation and volatilization method are described. The irradiated uranium is dissolved in bromine trifluoride in the liquid phase. The uranium is converted to the BrF/sub 3/ soluble urmium hexafluoride compound whereas the fluorides of certain contaminating elements are insoluble in liquid BrF/sub 3/, and the reaction rate of the BrF/sub 3/ with certain other solid uranium contamirnnts is sufficiently slower than the reaction rate with uranium that substantial portions of these contaminating elements will remain as solids. These solids are then separated from the solution by a distillation, filtration, or centrifugation step. The uranium hexafluoride is then separated from the balance of the impurities and solvent by one or more distillations.

Influence of mineral colloids and humic substances on uranium(VI) transport in water-saturated geologic porous media

NASA Astrophysics Data System (ADS)

Wang, Qing; Cheng, Tao; Wu, Yang

2014-12-01

Mineral colloids and humic substances often co-exist in subsurface environment and substantially influence uranium (U) transport. However, the combined effects of mineral colloids and humic substances on U transport are not clear. This study is aimed at quantifying U transport and elucidating geochemical processes that control U transport when both mineral colloids and humic acid (HA) are present. U-spiked solutions/suspensions were injected into water-saturated sand columns, and U and colloid concentrations in column effluent were monitored. We found that HA promoted U transport via (i) formation of aqueous U-HA complexes, and (ii) competition against aqueous U for surface sites on transport media. Illite colloids had no influence on U transport at pH 5 in the absence of HA due to low mobility of the colloids. At pH 9, U desorbed from mobile illite and the presence of illite decreased U transport. At pH 5, high U transport occurred when both illite colloids and HA were present, which was attributed to enhanced U adsorption to illite colloids via formation of ternary illite-HA-U surface complexes, and enhanced illite transport due to HA attachment to illite and transport media. This study demonstrates that the combined effects of mineral colloids and HA on contaminant transport is different from simple addition of the individual effect.

Uranium removal from a contaminated effluent using a combined microbial and nanoparticle system.

PubMed

Baiget, Mar; Constantí, Magda; López, M Teresa; Medina, Francesc

2013-09-25

Reduction of soluble uranium(VI) to insoluble uranium(IV) for remediating a uranium-contaminated effluent (EF-03) was examined using a biotic and abiotic integrated system. Shewanella putrefaciens was first used and reduced U(VI) in a synthetic medium but not in the EF-03 effluent sample. Subsequently the growth of autochthonous microorganisms was stimulated with lactate. When lactate was supported on active carbon 77% U(VI) was removed in 4 days. Separately, iron nanoparticles that were 50 nm in diameter reduced U(VI) by 60% in 4 hours. The efficiency of uranium(VI) removal was improved to 96% in 30 min by using a system consisting of lactate and iron nanoparticles immobilized on active carbon. Lactate also stimulated the growth of potential uranium-reducing microorganisms in the EF-03 sample. This system can be efficiently used for the bioremediation of uranium-contaminated effluents. Copyright © 2013 Elsevier B.V. All rights reserved.

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

DOE Office of Scientific and Technical Information (OSTI.GOV)

He, Zhili; Zhang, Ping; Wu, Linwei

Contamination from anthropogenic activities has significantly impacted Earth’s biosphere. However, knowledge about how environmental contamination affects the biodiversity of groundwater microbiomes and ecosystem functioning remains very limited. Here, we used a comprehensive functional gene array to analyze groundwater microbiomes from 69 wells at the Oak Ridge Field Research Center (Oak Ridge, TN), representing a wide pH range and uranium, nitrate, and other contaminants. We hypothesized that the functional diversity of groundwater microbiomes would decrease as environmental contamination (e.g., uranium or nitrate) increased or at low or high pH, while some specific populations capable of utilizing or resistant to those contaminantsmore » would increase, and thus, such key microbial functional genes and/or populations could be used to predict groundwater contamination and ecosystem functioning. Our results indicated that functional richness/diversity decreased as uranium (but not nitrate) increased in groundwater. In addition, about 5.9% of specific key functional populations targeted by a comprehensive functional gene array (GeoChip 5) increased significantly (P < 0.05) as uranium or nitrate increased, and their changes could be used to successfully predict uranium and nitrate contamination and ecosystem functioning. Here, this study indicates great potential for using microbial functional genes to predict environmental contamination and ecosystem functioning.« less

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

DOE PAGES

He, Zhili; Zhang, Ping; Wu, Linwei; ...

2018-02-20

Contamination from anthropogenic activities has significantly impacted Earth’s biosphere. However, knowledge about how environmental contamination affects the biodiversity of groundwater microbiomes and ecosystem functioning remains very limited. Here, we used a comprehensive functional gene array to analyze groundwater microbiomes from 69 wells at the Oak Ridge Field Research Center (Oak Ridge, TN), representing a wide pH range and uranium, nitrate, and other contaminants. We hypothesized that the functional diversity of groundwater microbiomes would decrease as environmental contamination (e.g., uranium or nitrate) increased or at low or high pH, while some specific populations capable of utilizing or resistant to those contaminantsmore » would increase, and thus, such key microbial functional genes and/or populations could be used to predict groundwater contamination and ecosystem functioning. Our results indicated that functional richness/diversity decreased as uranium (but not nitrate) increased in groundwater. In addition, about 5.9% of specific key functional populations targeted by a comprehensive functional gene array (GeoChip 5) increased significantly (P < 0.05) as uranium or nitrate increased, and their changes could be used to successfully predict uranium and nitrate contamination and ecosystem functioning. Here, this study indicates great potential for using microbial functional genes to predict environmental contamination and ecosystem functioning.« less

Bioremediation of uranium contamination with enzymatic uranium reduction

USGS Publications Warehouse

Lovley, D.R.; Phillips, E.J.P.

1992-01-01

Enzymatic uranium reduction by Desulfovibrio desulfuricans readily removed uranium from solution in a batch system or when D. desulfuricans was separated from the bulk of the uranium-containing water by a semipermeable membrane. Uranium reduction continued at concentrations as high as 24 mM. Of a variety of potentially inhibiting anions and metals evaluated, only high concentrations of copper inhibited uranium reduction. Freeze-dried cells, stored aerobically, reduced uranium as fast as fresh cells. D. desulfuricans reduced uranium in pH 4 and pH 7.4 mine drainage waters and in uraniumcontaining groundwaters from a contaminated Department of Energy site. Enzymatic uranium reduction has several potential advantages over other bioprocessing techniques for uranium removal, the most important of which are as follows: the ability to precipitate uranium that is in the form of a uranyl carbonate complex; high capacity for uranium removal per cell; the formation of a compact, relatively pure, uranium precipitate.

Bioremediation of Uranium-Contaminated Groundwater using Engineered Injection and Extraction

NASA Astrophysics Data System (ADS)

Greene, J. A.; Neupauer, R.; Ye, M.; Kasprzyk, J. R.; Mays, D. C.; Curtis, G. P.

2017-12-01

During in-situ remediation of contaminated groundwater, a treatment chemical is injected into the contaminated groundwater to react with and degrade the contaminant, with reactions occurring where the treatment chemical contacts the contaminant. Traditional in-situ groundwater remediation relies on background groundwater flow for spreading of treatment chemicals into contaminant plumes. Engineered Injection and Extraction (EIE), in which time-varying induced flow fields are used to actively spread the treatment chemical into the contaminant plume, has been developed to increase contact between the contaminant and treatment chemical, thereby enhancing contaminant degradation. EIE has been investigated for contaminants that degrade through irreversible bimolecular reaction with a treatment chemical, but has not been investigated for a contaminant governed by reversible reactions. Uranium primarily occurs in its aqueous, mobile form, U(VI), in the environment but can be bioreduced to its sparingly soluble, immobile form, U(IV), by iron reducing bacteria stimulated by an acetate amendment. In this study, we investigate the ability of EIE to facilitate and sustain favorable conditions to immobilize uranium during remediation, and to prevent re-mobilization of uranium into the aqueous phase after active remediation has ended. Simulations in this investigation are conducted using a semi-synthetic model based on physical and chemical conditions at the Naturita Uranium Mill Tailings Remedial Action (UMTRA) site in southwestern Colorado and the Old Rifle UMTRA site in western Colorado. The EIE design is optimized for the synthetic model using the Borg multi-objective evolutionary algorithm.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Denton, J. S.; Goldstein, S. J.; Paviet, P.

Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning.

PubMed

He, Zhili; Zhang, Ping; Wu, Linwei; Rocha, Andrea M; Tu, Qichao; Shi, Zhou; Wu, Bo; Qin, Yujia; Wang, Jianjun; Yan, Qingyun; Curtis, Daniel; Ning, Daliang; Van Nostrand, Joy D; Wu, Liyou; Yang, Yunfeng; Elias, Dwayne A; Watson, David B; Adams, Michael W W; Fields, Matthew W; Alm, Eric J; Hazen, Terry C; Adams, Paul D; Arkin, Adam P; Zhou, Jizhong

2018-02-20

Contamination from anthropogenic activities has significantly impacted Earth's biosphere. However, knowledge about how environmental contamination affects the biodiversity of groundwater microbiomes and ecosystem functioning remains very limited. Here, we used a comprehensive functional gene array to analyze groundwater microbiomes from 69 wells at the Oak Ridge Field Research Center (Oak Ridge, TN), representing a wide pH range and uranium, nitrate, and other contaminants. We hypothesized that the functional diversity of groundwater microbiomes would decrease as environmental contamination (e.g., uranium or nitrate) increased or at low or high pH, while some specific populations capable of utilizing or resistant to those contaminants would increase, and thus, such key microbial functional genes and/or populations could be used to predict groundwater contamination and ecosystem functioning. Our results indicated that functional richness/diversity decreased as uranium (but not nitrate) increased in groundwater. In addition, about 5.9% of specific key functional populations targeted by a comprehensive functional gene array (GeoChip 5) increased significantly ( P < 0.05) as uranium or nitrate increased, and their changes could be used to successfully predict uranium and nitrate contamination and ecosystem functioning. This study indicates great potential for using microbial functional genes to predict environmental contamination and ecosystem functioning. IMPORTANCE Disentangling the relationships between biodiversity and ecosystem functioning is an important but poorly understood topic in ecology. Predicting ecosystem functioning on the basis of biodiversity is even more difficult, particularly with microbial biomarkers. As an exploratory effort, this study used key microbial functional genes as biomarkers to provide predictive understanding of environmental contamination and ecosystem functioning. The results indicated that the overall functional gene richness/diversity decreased as uranium increased in groundwater, while specific key microbial guilds increased significantly as uranium or nitrate increased. These key microbial functional genes could be used to successfully predict environmental contamination and ecosystem functioning. This study represents a significant advance in using functional gene markers to predict the spatial distribution of environmental contaminants and ecosystem functioning toward predictive microbial ecology, which is an ultimate goal of microbial ecology. Copyright © 2018 He et al.

Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Campbell, Kate M.; Kukkadapu, Ravi K.; Qafoku, Nikolla

2012-05-23

Localized zones or lenses of naturally reduced sediments have the potential to play a significant role in the fate and transport of redox-sensitive metals and metalloids in aquifers. To assess the mineralogy, microbiology, and redox processes that occur in these zones, we examined several cores from a region of naturally occurring reducing conditions in a uranium-contaminated aquifer (Rifle, CO). Sediment samples from a transect of cores ranging from oxic/suboxic Rifle aquifer sediment to naturally reduced sediment were analyzed for uranium and iron content, oxidation state, and mineralogy, reduced sulfur phases, and solid phase organic carbon content using a suite ofmore » analytical and spectroscopic techniques on bulk sediment and size fractions. Solid-phase uranium concentrations were higher in the naturally reduced zone, with a high proportion of the uranium present as reduced U(IV). The sediments were also elevated in reduced sulfur phases and Fe(II), indicating it is very likely that U(VI), Fe(III), and sulfate reduction occurred or is occurring in the sediment. The microbial community was assessed using lipid- and DNA-based techniques, and statistical redundancy analysis was performed to determine correlations between the microbial community and the geochemistry. Increased concentration of solid phase organic carbon and biomass in the naturally reduced sediment suggests that natural bioreduction is stimulated by a zone of increased organic carbon concentration associated with fine-grained material and lower permeability to groundwater flow. Characterization of the naturally bioreduced sediment provides an understanding of the natural processes that occur in the sediment under reducing conditions and how they may impact natural attenuation of radionuclides and other redox sensitive materials. Results also suggest the importance of recalcitrant organic carbon for maintaining reducing conditions and uranium immobilization.« less

Estimates of radiological risk from depleted uranium weapons in war scenarios.

PubMed

Durante, Marco; Pugliese, Mariagabriella

2002-01-01

Several weapons used during the recent conflict in Yugoslavia contain depleted uranium, including missiles and armor-piercing incendiary rounds. Health concern is related to the use of these weapons, because of the heavy-metal toxicity and radioactivity of uranium. Although chemical toxicity is considered the more important source of health risk related to uranium, radiation exposure has been allegedly related to cancers among veterans of the Balkan conflict, and uranium munitions are a possible source of contamination in the environment. Actual measurements of radioactive contamination are needed to assess the risk. In this paper, a computer simulation is proposed to estimate radiological risk related to different exposure scenarios. Dose caused by inhalation of radioactive aerosols and ground contamination induced by Tomahawk missile impact are simulated using a Gaussian plume model (HOTSPOT code). Environmental contamination and committed dose to the population resident in contaminated areas are predicted by a food-web model (RESRAD code). Small values of committed effective dose equivalent appear to be associated with missile impacts (50-y CEDE < 5 mSv), or population exposure by water-independent pathways (50-y CEDE < 80 mSv). The greatest hazard is related to the water contamination in conditions of effective leaching of uranium in the groundwater (50-y CEDE < 400 mSv). Even in this worst case scenario, the chemical toxicity largely predominates over radiological risk. These computer simulations suggest that little radiological risk is associated to the use of depleted uranium weapons.

In situ effects of metal contamination from former uranium mining sites on the health of the three-spined stickleback (Gasterosteus aculeatus, L.).

PubMed

Le Guernic, Antoine; Sanchez, Wilfried; Bado-Nilles, Anne; Palluel, Olivier; Turies, Cyril; Chadili, Edith; Cavalié, Isabelle; Delahaut, Laurence; Adam-Guillermin, Christelle; Porcher, Jean-Marc; Geffard, Alain; Betoulle, Stéphane; Gagnaire, Béatrice

2016-08-01

Human activities have led to increased levels of various pollutants including metals in aquatic ecosystems. Increase of metallic concentrations in aquatic environments represents a potential risk to exposed organisms, including fish. The aim of this study was to characterize the environmental risk to fish health linked to a polymetallic contamination from former uranium mines in France. This contamination is characterized by metals naturally present in the areas (manganese and iron), uranium, and metals (aluminum and barium) added to precipitate uranium and its decay products. Effects from mine releases in two contaminated ponds (Pontabrier for Haute-Vienne Department and Saint-Pierre for Cantal Department) were compared to those assessed at four other ponds outside the influence of mine tailings (two reference ponds/department). In this way, 360 adult three-spined sticklebacks (Gasterosteus aculeatus) were caged for 28 days in these six ponds before biomarker analyses (immune system, antioxidant system, biometry, histology, DNA integrity, etc.). Ponds receiving uranium mine tailings presented higher concentrations of uranium, manganese and aluminum, especially for the Haute-Vienne Department. This uranium contamination could explain the higher bioaccumulation of this metal in fish caged in Pontabrier and Saint-Pierre Ponds. In the same way, many fish biomarkers (antioxidant and immune systems, acetylcholinesterase activity and biometric parameters) were impacted by this environmental exposure to mine tailings. This study shows the interest of caging and the use of a multi-biomarker approach in the study of a complex metallic contamination.

Absorption, accumulation and biological effects of depleted uranium in Peyer's patches of rats.

PubMed

Dublineau, I; Grison, S; Grandcolas, L; Baudelin, C; Tessier, C; Suhard, D; Frelon, S; Cossonnet, C; Claraz, M; Ritt, J; Paquet, P; Voisin, P; Gourmelon, P

2006-10-29

The digestive tract is the entry route for radionuclides following the ingestion of contaminated food and/or water wells. It was recently characterized that the small intestine was the main area of uranium absorption throughout the gastrointestinal tract. This study was designed to determine the role played by the Peyer's patches in the intestinal absorption of uranium, as well as the possible accumulation of this radionuclide in lymphoid follicles and the toxicological or pathological consequences on the Peyer's patch function subsequent to the passage and/or accumulation of uranium. Results of experiments performed in Ussing chambers indicate that the apparent permeability to uranium in the intestine was higher (10-fold) in the mucosa than in Peyer's patches ((6.21+/-1.21 to 0.55+/-0.35)x10(-6)cm/s, respectively), demonstrating that the small intestinal epithelium was the preferential pathway for the transmucosal passage of uranium. A quantitative analysis of uranium by ICP-MS following chronic contamination with depleted uranium during 3 or 9 months showed a preferential accumulation of uranium in Peyer's patches (1355% and 1266%, respectively, at 3 and 9 months) as compared with epithelium (890% and 747%, respectively, at 3 and 9 months). Uranium was also detected in the mesenteric lymph nodes ( approximately 5-fold after contamination with DU). The biological effects of this accumulation of depleted uranium after chronic contamination were investigated in Peyer's patches. There was no induction of the apoptosis pathway after chronic DU contamination in Peyer's patches. The results indicate no change in the cytokine expression (Il-10, TGF-beta, IFN-gamma, TNF-alpha, MCP-1) in Peyer's patches and in mesenteric lymph nodes, and no modification in the uptake of yeast cells by Peyer's patches. In conclusion, this study shows that the Peyer's patches were a site of retention for uranium following the chronic ingestion of this radionuclide, without any biological consequences of such accumulation on Peyer's patch functions.

Immobilization of uranium in contaminated soil by natural apatite addition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mrdakovic Popic, Jelena; Stojanovic, Mirjana; Milosevic, Sinisa

2007-07-01

Available in abstract form only. Full text of publication follows: The goal of this study was to evaluate the effectiveness of Serbian natural mineral apatite as soil additive for reducing the migration of uranium from contaminated sediments. In laboratory study we investigated the sorption properties of domestic apatite upon different experimental conditions, such as pH, adsorbent mass, reaction period, concentration of P{sub 2}O{sub 5} in apatite, solid/liquid ratio. In second part of study, we did the quantification of uranium in soil samples, taken from uranium mine site 'Kalna', by sequential extraction method. The same procedure was, also, used for uraniummore » determination in contaminated soil samples after apatite addition, in order to determine the changes in U distribution in soil fraction. The obtained results showed the significant level of immobilization (96.7%) upon certain conditions. Increase of %P{sub 2}O{sub 5} in apatite and process of mechano-chemical activation led to increase of immobilization capacity from 17.50% till 91.64%. The best results for uranium binding were obtained at pH 5.5 and reaction period 60 days (98.04%) The sequential extraction showed the presence of uranium (48.2%) in potentially available soil fractions, but with the apatite addition uranium content in these fractions decreased (30.64%), what is considering environmental aspect significant fact. In situ immobilization of radionuclide using inexpensive sequestering agents, such as apatite, is very adequate for big contaminated areas of soil with low level of contamination. This investigation study on natural apatite from deposit 'Lisina' Serbia was the first one of this type in our country. Key words: apatite, uranium, immobilization, soil, contamination. (authors)« less

Biogeochemical behaviour and bioremediation of uranium in waters of abandoned mines.

PubMed

Mkandawire, Martin

2013-11-01

The discharges of uranium and associated radionuclides as well as heavy metals and metalloids from waste and tailing dumps in abandoned uranium mining and processing sites pose contamination risks to surface and groundwater. Although many more are being planned for nuclear energy purposes, most of the abandoned uranium mines are a legacy of uranium production that fuelled arms race during the cold war of the last century. Since the end of cold war, there have been efforts to rehabilitate the mining sites, initially, using classical remediation techniques based on high chemical and civil engineering. Recently, bioremediation technology has been sought as alternatives to the classical approach due to reasons, which include: (a) high demand of sites requiring remediation; (b) the economic implication of running and maintaining the facilities due to high energy and work force demand; and (c) the pattern and characteristics of contaminant discharges in most of the former uranium mining and processing sites prevents the use of classical methods. This review discusses risks of uranium contamination from abandoned uranium mines from the biogeochemical point of view and the potential and limitation of uranium bioremediation technique as alternative to classical approach in abandoned uranium mining and processing sites.

From dust to dose: Effects of forest disturbance on increased inhalation exposure.

PubMed

Whicker, Jeffrey J; Pinder, John E; Breshears, David D; Eberhart, Craig F

2006-09-15

Ecosystem disturbances that remove vegetation and disturb surface soils are major causes of excessive soil erosion and can result in accelerated transport of soils contaminated with hazardous materials. Accelerated wind erosion in disturbed lands that are contaminated is of particular concern because of potential increased inhalation exposure, yet measurements regarding these relationships are lacking. The importance of this was highlighted when, in May of 2000, the Cerro Grande fire burned over roughly 30% of Los Alamos National Laboratory (LANL), mostly in ponderosa pine (Pinus ponderosa) forest, and through areas with soils containing contaminants, particularly excess depleted and natural uranium. Additionally, post-fire thinning was performed in burned and unburned forests on about 25% of LANL land. The first goal of this study was to assess the potential for increased inhalation dose from uranium contaminated soils via wind-driven resuspension of soil following the Cerro Grande Fire and subsequent forest thinning. This was done through analysis of post-disturbance measurements of uranium air concentrations and their relationships with wind velocity and seasonal vegetation cover. We found a 14% average increase in uranium air concentrations at LANL perimeter locations after the fire, and the greatest air concentrations occurred during the months of April-June when wind velocities are highest, no snow cover, and low vegetation cover. The second goal was to develop a methodology to assess the relative contribution of each disturbance type towards increasing public and worker exposure to these resuspended soils. Measurements of wind-driven dust flux in severely burned, moderately burned, thinned, and unburned/unthinned forest areas were used to assess horizontal dust flux (HDF) in these areas. Using empirically derived relationships between measurements of HDF and respirible dust, coupled with onsite uranium soil concentrations, we estimate relative increases in inhalation doses for workers ranging from 15% to 38%. Despite the potential for increased doses resulting from these forest disturbances, the estimated annual dose rate for the public was <1 microSv yr(-1), which is far below the dose limits for public exposures, and the upper-bound dose rate for a LANL worker was estimated to be 140 microSv yr(-1), far below the 5 x 10(4) microSv yr(-1) occupational dose limit. These results show the importance of ecosystem disturbance in increasing mobility of soil-bound contaminants, which can ultimately increase exposure. However, it is important to investigate the magnitude of the increases when deciding appropriate strategies for management and long-term stewardship of contaminated lands.

Wind Transport of Radionuclide- Bearing Dust, Peña Blanca, Chihuahua, Mexico

NASA Astrophysics Data System (ADS)

Velarde, R.; Goodell, P. C.; Gill, T. E.; Arimoto, R.

2007-05-01

This investigation evaluates radionuclide fractionation during wind erosion of high-grade uranium ore storage piles at Peña Blanca (50km north of Chihuahua City), Chihuahua, Mexico. The aridity of the local environment promotes dust resuspension by high winds. Although active operations ceased in 1983, the Peña Blanca mining district is one of Mexico`s most important uranium ore reserves. The study site contains piles of high grade ore, left loose on the surface, and separated by the specific deposits from which they were derived (Margaritas, Nopal I, and Puerto I). Similar locations do not exist in the United States, since uranium mining sites in the USA have been reclaimed. The Peña Blanca site serves as an analog for the Yucca Mountain project. Dust deposition is collected at Peña Blanca with BSNE sediment catchers (Fryrear, 1986) and marble dust traps (Reheis, 1999). These devices capture windblown sediment; subsequently, the sample data will help quantify potentially radioactive short term field sediment loss from the repository surface and determine sediment flux. Aerosols and surface materials will be analyzed and radioactivity levels established utilizing techniques such as gamma spectroscopy. As a result, we will be able to estimate how much radionuclide contaminated dust is being transported or attached geochemically to fine grain soils or minerals (e.g., clays or iron oxides). The high-grade uranium-bearing material is at secular equilibrium, thus the entire decay series is present. Of resulting interest is not only the aeolian transport of uranium, but also of the other daughter products. These studies will improve our understanding of geochemical cycling of radionuclides with respect to sources, transport, and deposition. The results may also have important implications for the geosciences and homeland security, and potential applications to public health. Funding for this project is provided in part via a NSF grant to Arimoto.

Baseline risk assessment of ground water contamination at the uranium mill tailings site near Durango, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1995-02-01

This risk assessment evaluates the possibility of health and environmental risks from contaminated ground water at the uranium mill tailings site near Durango, Colorado. The former uranium processing site`s contaminated soil and material were removed and placed at a disposal site located in Body Canyon, Colorado, during 1986--1991 by the US Departments of Energy`s Uranium Mill Tailings Remedial Action (UMTRA) Project. Currently, the UMTRA Project is evaluating the nature and extent of ground water contamination at the site. This risk assessment follows an approach similar to that used by the US Environmental Protection Agency. The first step is to determinemore » what site-related contaminants are found in ground water samples. The next step in the risk assessment is to determine how much of these contaminants people might ingest if they got their drinking water from a well on the site. In accordance with standard practice for this type of risk assessment, the highest contaminant concentrations from the most contaminated wells are used. The risk assessment then explains the possible health problems that could result from this amount of contamination.« less

Laser removal of loose uranium compound contamination from metal surfaces

NASA Astrophysics Data System (ADS)

Roberts, D. E.; Modise, T. S.

2007-04-01

Pulsed laser removal of surface contamination of uranyl nitrate and uranium dioxide from stainless steel has been studied. Most of the loosely bound contamination has been removed at fluence levels below 0.5 J cm -2, leaving about 5% fixed contamination for uranyl nitrate and 15% for uranium dioxide. Both alpha and beta activities are then sufficiently low that contaminated objects can be taken out of a restricted radiation area for re-use. The ratio of beta to alpha activity is found to be a function of particle size and changes during laser removal. In a separate experiment using technetium-99m, the collection of removed radioactivity in the filter was studied and an inventory made of removed and collected contamination.

Compared in vivo efficiency of nanoemulsions unloaded and loaded with calixarene and soapy water in the treatment of superficial wounds contaminated by uranium.

PubMed

Grivès, Sophie; Phan, Guillaume; Bouvier-Capely, Céline; Suhard, David; Rebière, François; Agarande, Michelle; Fattal, Elias

2017-04-01

No emergency decontamination treatment is currently available in the case of radiological skin contamination by uranium compounds. First responders in the workplace or during an industrial nuclear accident must be able to treat internal contamination through skin. For this purpose, a calixarene nanoemulsion was developed for the treatment of intact skin or superficial wounds contaminated by uranium, and the decontamination efficiency of this nanoemulsion was investigated in vitro and ex vivo. The present work addresses the in vivo decontamination efficiency of this nanoemulsion, using a rat model. This efficiency is compared to the radio-decontaminant soapy water currently used in France (Trait rouge ® ) in the workplace. The results showed that both calixarene-loaded nanoemulsion and non-loaded nanoemulsion allowed a significant decontamination efficiency compared to the treatment with soapy water. Early application of the nanoemulsions on contaminated excoriated rat skin allowed decreasing the uranium content by around 85% in femurs, 95% in kidneys and 93% in urines. For skin wounded by microneedles, mimicking wounds by microstings, nanoemulsions allowed approximately a 94% decrease in the uranium retention in kidneys. However, specific chelation of uranium by calixarene molecules within the nanoemulsion was not statistically significant, probably because of the limited calixarene-to-uranium molar ratio in these experiment conditions. Moreover, these studies showed that the soapy water treatment potentiates the transcutaneous passage of uranium, thus making it bioavailable, in particular when the skin is superficially wounded. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

The application of illite supported nanoscale zero valent iron for the treatment of uranium contaminated groundwater.

PubMed

Jing, C; Landsberger, S; Li, Y L

2017-09-01

In this study, nanoscale zero valent iron I-NZVI was investigated as a remediation strategy for uranium contaminated groundwater from the former Cimarron Fuel Fabrication Site in Oklahoma, USA. The 1 L batch-treatment system was applied in the study. The result shows that 99.9% of uranium in groundwater was removed by I-NZVI within 2 h. Uranium concentration in the groundwater stayed around 27 μg/L, and there was no sign of uranium release into groundwater after seven days of reaction time. Meanwhile the release of iron was significantly decreased compared to NZVI which can reduce the treatment impact on the water environment. To study the influence of background pH of the treatment system on removal efficiency of uranium, the groundwater was adjusted from pH 2-10 before the addition of I-NZVI. The pH of the groundwater was from 2.1 to 10.7 after treatment. The removal efficiency of uranium achieved a maximum in neutral pH of groundwater. The desorption of uranium on the residual solid phase after treatment was investigated in order to discuss the stability of uranium on residual solids. After 2 h of leaching, 0.07% of the total uranium on residual solid phase was leached out in a HNO 3 leaching solution with a pH of 4.03. The concentration of uranium in the acid leachate was under 3.2 μg/L which is below the EPA's maximum contaminant level of 30 μg/L. Otherwise, the concentration of uranium was negligible in distilled water leaching solution (pH = 6.44) and NaOH leaching solution (pH = 8.52). A desorption study shows that an acceptable amount of uranium on the residuals can be released into water system under strong acid conditions in short terms. For long term disposal management of the residual solids, the leachate needs to be monitored and treated before discharge into a hazardous landfill or the water system. For the first time, I-NZVI was applied for the treatment of uranium contaminated groundwater. These results provide proof that I-NZVI has improved performance compared to NZVI and is a promising technology for the restoration of complex uranium contaminated water resources. Copyright © 2017 Elsevier Ltd. All rights reserved.

Plutonium Decontamination of Uranium using CO2 Cleaning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Blau, M

A concern of the Department of Energy (DOE) Environmental Management (EM) and Defense Programs (DP), and of the Los Alamos National Laboratory (LANL) and the Lawrence Livermore National Laboratory (LLNL), is the disposition of thousands of legacy and recently generated plutonium (Pu)-contaminated, highly enriched uranium (HEU) parts. These parts take up needed vault space. This presents a serious problem for LLNL, as site limit could result in the stoppage of future weapons work. The Office of Fissile Materials Disposition (NN-60) will also face a similar problem as thousands of HEU parts will be created with the disassembly of site-return pitsmore » for plutonium recovery when the Pit Disassembly and Conversion Facility (PDCF) at the Savannah River Site (SRS) becomes operational. To send HEU to the Oak Ridge National Laboratory and the Y-12 Plant for disposition, the contamination for metal must be less than 20 disintegrations per minute (dpm) of swipable transuranic per 100 cm{sup 2} of surface area or the Pu bulk contamination for oxide must be less than 210 parts per billion (ppb). LANL has used the electrolytic process on Pu-contaminated HEU weapon parts with some success. However, this process requires that a different fixture be used for every configuration; each fixture cost approximately $10K. Moreover, electrolytic decontamination leaches the uranium metal substrate (no uranium or plutonium oxide) from the HEU part. The leaching rate at the uranium metal grain boundaries is higher than that of the grains and depends on the thickness of the uranium oxide layer. As the leaching liquid flows past the HEU part, it carries away plutonium oxide contamination and uranium oxide. The uneven uranium metal surface created by the leaching becomes a trap for plutonium oxide contamination. In addition, other DOE sites have used CO{sub 2} cleaning for Pu decontamination successfully. In the 1990's, the Idaho National Engineering Laboratory investigated this technology and showed that CO{sub 2} pellet blasting (or CO{sub 2} cleaning) reduced both fixed and smearable contamination on tools. In 1997, LLNL proved that even tritium contamination could be removed from a variety of different matrices using CO{sub 2}cleaning. CO{sub 2} cleaning is a non-toxic, nonconductive, nonabrasive decontamination process whose primary cleaning mechanisms are: (1) Impact of the CO{sub 2} pellets loosens the bond between the contaminant and the substrate. (2) CO{sub 2} pellets shatter and sublimate into a gaseous state with large expansion ({approx}800 times). The expanding CO{sub 2} gas forms a layer between the contaminant and the substrate that acts as a spatula and peels off the contaminant. (3) Cooling of the contaminant assists in breaking its bond with the substrate. Thus, LLNL conducted feasibility testing to determine if CO{sub 2} pellet blasting could remove Pu contamination (e.g., uranium oxide) from uranium metal without abrading the metal matrix. This report contains a summary of events and the results of this test.« less

In situ remediation of uranium contaminated groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dwyer, B.P.; Marozas, D.C.

1997-02-01

In an effort to develop cost-efficient techniques for remediating uranium contaminated groundwater at DOE Uranium Mill Tailing Remedial Action (UMTRA) sites nationwide, Sandia National Laboratories (SNL) deployed a pilot scale research project at an UMTRA site in Durango, CO. Implementation included design, construction, and subsequent monitoring of an in situ passive reactive barrier to remove Uranium from the tailings pile effluent. A reactive subsurface barrier is produced by emplacing a reactant material (in this experiment various forms of metallic iron) in the flow path of the contaminated groundwater. Conceptually the iron media reduces and/or adsorbs uranium in situ to acceptablemore » regulatory levels. In addition, other metals such as Se, Mo, and As have been removed by the reductive/adsorptive process. The primary objective of the experiment was to eliminate the need for surface treatment of tailing pile effluent. Experimental design, and laboratory and field results are discussed with regard to other potential contaminated groundwater treatment applications.« less

In situ remediation of uranium contaminated groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dwyer, B.P.; Marozas, D.C.

1997-12-31

In an effort to develop cost-efficient techniques for remediating uranium contaminated groundwater at DOE Uranium Mill Tailing Remedial Action (UMTRA) sites nationwide, Sandia National Laboratories (SNL) deployed a pilot scale research project at an UMTRA site in Durango, CO. Implementation included design, construction, and subsequent monitoring of an in situ passive reactive barrier to remove Uranium from the tailings pile effluent. A reactive subsurface barrier is produced by emplacing a reactant material (in this experiment - various forms of metallic iron) in the flow path of the contaminated groundwater. Conceptually the iron media reduces and/or adsorbs uranium in situ tomore » acceptable regulatory levels. In addition, other metals such as Se, Mo, and As have been removed by the reductive/adsorptive process. The primary objective of the experiment was to eliminate the need for surface treatment of tailing pile effluent. Experimental design, and laboratory and field preliminary results are discussed with regard to other potential contaminated groundwater treatment applications.« less

Attenuation and Transport Mechanisms of Depleted Uranium in Groundwater at Lawrence Livermore National Laboratory Site 300

NASA Astrophysics Data System (ADS)

Danny, K. R.; Taffet, M. J.; Brusseau, M. L. L.; Chorover, J.

2015-12-01

Lawrence Livermore National Laboratory (LLNL) Site 300 was established in 1955 to support weapons research and development. Depleted uranium was used as a proxy for fissile uranium-235 (235U) in open-air explosives tests conducted at Building 812. As a result, oxidized depleted uranium was deposited on the ground, eventually migrating to the underlying sandstone aquifer. Uranium (U) groundwater concentrations exceed the California and Federal Maximum Contaminant Level of 20 pCi L-1 (30 ug L-1). However, the groundwater plume appears to attenuate within 60 m of the source, beyond which no depleted U is detected. This study will determine the relative contribution of physical (e.g. dilution), chemical (e.g. surface adsorption, mineral precipitation), and biological (e.g. biotransformation) processes that contribute to the apparent attenuation of U, which exists as uranyl (UO22+) complexes, at the site. Methods of investigation include evaluating 15 yr of hydrogeologic and chemical data, creating a site conceptual model, and applying equilibrium (e.g. aqueous species complexation, mineral saturation indices) and reactive transport models using Geochemist's WorkbenchTM. Reactive transport results are constrained by direct field observations, including U major ion, and dissolved O2 concentrations, pH, and others, under varying chemical and hydraulic conditions. Aqueous speciation calculations indicate that U primarily exists as anionic CaUO2(CO3)32- or neutral Ca2UO2(CO3)30 species. Additionally, nucleation and growth of Ca/Mg uranyl carbonate solids are predicted to affect attenuation. Initial reactive transport results suggest surface adsorption (e.g. ion exchange, surface complexation) to layer silicate clays is limited under the aqueous geochemical conditions of the site. Current and future work includes XRD analysis of aquifer solids to constrain iron and aluminum (oxy)hydroxides, and coupling advective-dispersive transport with the chemical and physical processes. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-ABS-675707.

Surface Water-Groundwater Interactions as a Critical Component of Uranium Plume Persistence

NASA Astrophysics Data System (ADS)

Williams, K. H.; Christensen, J. N.; Hobson, C.

2015-12-01

Residual contamination of soils, sediments and groundwater by uranium milling operations presents a lingering problem at former mill sites throughout the upper Colorado River Basin in the western USA. Remedial strategies predicated upon natural flushing by low uranium recharge waters have frequently failed to achieve target concentrations set by national and state regulators. Flushing times of tens of years have often yielded negligible decreases in groundwater uranium concentrations, with extrapolated trends suggesting multiple decades or longer may be required to achieve regulatory goals. The U.S. Department of Energy's Rifle, Colorado field site serves as a natural laboratory for investigating the underlying causes for uranium plume persistence, with recent studies there highlighting the important role that surface water-groundwater interactions play in sustaining uranium delivery to the aquifer. Annual snowmelt-driven increases in Colorado River discharge induce 1-2 m excursions in groundwater elevation at the Rifle site, which enables residual tailings-contaminated materials (so-called Supplemental Standards) to become hydrologically connected to the aquifer for short periods of time during peak discharge. The episodic contact between shallow groundwater and residual contamination leads to abrupt 20-fold increases in groundwater uranium concentration, which serve to seasonally replenish the plume given the location of the Supplemental Standards along the upgradient edge of the aquifer. Uranium isotope composition changes abruptly as uranium concentrations increase reflecting the contribution of a temporally distinct contaminant reservoir. The release of uranium serves to potentially replenish organic matter rich sediments located within the alluvial aquifer at downstream locations, which have been postulated to serve as a parallel contributor to plume persistence following the uptake, immobilization, and slow re-oxidation of uranium.

Sorption and bioreduction of hexavalent uranium at a military facility by the Chesapeake Bay.

PubMed

Dong, Wenming; Xie, Guibo; Miller, Todd R; Franklin, Mark P; Oxenberg, Tanya Palmateer; Bouwer, Edward J; Ball, William P; Halden, Rolf U

2006-07-01

Directly adjacent to the Chesapeake Bay lies the Aberdeen Proving Ground, a U.S. Army facility where testing of armor-piercing ammunitions has resulted in the deposition of >70,000 kg of depleted uranium (DU) to local soils and sediments. Results of previous environmental monitoring suggested limited mobilization in the impact area and no transport of DU into the nation's largest estuary. To determine if physical and biological reactions constitute mechanisms involved in limiting contaminant transport, the sorption and biotransformation behavior of the radionuclide was studied using geochemical modeling and laboratory microcosms (500 ppb U(VI) initially). An immediate decline in dissolved U(VI) concentrations was observed under both sterile and non-sterile conditions due to rapid association of U(VI) with natural organic matter in the sediment. Reduction of U(VI) to U(IV) occurred only in non-sterile microcosms. In the non-sterile samples, intrinsic bioreduction of uranium involved bacteria of the order Clostridiales and was only moderately enhanced by the addition of acetate (41% vs. 56% in 121 days). Overall, this study demonstrates that the migration of depleted uranium from the APG site into the Chesapeake Bay may be limited by a combination of processes that include rapid sorption of U(VI) species to natural organic matter, followed by slow, intrinsic bioreduction to U(IV).

Uranium plume persistence impacted by hydrologic and geochemical heterogeneity in the groundwater and river water interaction zone of Hanford site

NASA Astrophysics Data System (ADS)

Chen, X.; Zachara, J. M.; Vermeul, V. R.; Freshley, M.; Hammond, G. E.

2015-12-01

The behavior of a persistent uranium plume in an extended groundwater- river water (GW-SW) interaction zone at the DOE Hanford site is dominantly controlled by river stage fluctuations in the adjacent Columbia River. The plume behavior is further complicated by substantial heterogeneity in physical and geochemical properties of the host aquifer sediments. Multi-scale field and laboratory experiments and reactive transport modeling were integrated to understand the complex plume behavior influenced by highly variable hydrologic and geochemical conditions in time and space. In this presentation we (1) describe multiple data sets from field-scale uranium adsorption and desorption experiments performed at our experimental well-field, (2) develop a reactive transport model that incorporates hydrologic and geochemical heterogeneities characterized from multi-scale and multi-type datasets and a surface complexation reaction network based on laboratory studies, and (3) compare the modeling and observation results to provide insights on how to refine the conceptual model and reduce prediction uncertainties. The experimental results revealed significant spatial variability in uranium adsorption/desorption behavior, while modeling demonstrated that ambient hydrologic and geochemical conditions and heterogeneities in sediment physical and chemical properties both contributed to complex plume behavior and its persistence. Our analysis provides important insights into the characterization, understanding, modeling, and remediation of groundwater contaminant plumes influenced by surface water and groundwater interactions.

3D Geospatial Models for Visualization and Analysis of Groundwater Contamination at a Nuclear Materials Processing Facility

NASA Astrophysics Data System (ADS)

Stirewalt, G. L.; Shepherd, J. C.

2003-12-01

Analysis of hydrostratigraphy and uranium and nitrate contamination in groundwater at a former nuclear materials processing facility in Oklahoma were undertaken employing 3-dimensional (3D) geospatial modeling software. Models constructed played an important role in the regulatory decision process of the U.S. Nuclear Regulatory Commission (NRC) because they enabled visualization of temporal variations in contaminant concentrations and plume geometry. Three aquifer systems occur at the site, comprised of water-bearing fractured shales separated by indurated sandstone aquitards. The uppermost terrace groundwater system (TGWS) aquifer is composed of terrace and alluvial deposits and a basal shale. The shallow groundwater system (SGWS) aquifer is made up of three shale units and two sandstones. It is separated from the overlying TGWS and underlying deep groundwater system (DGWS) aquifer by sandstone aquitards. Spills of nitric acid solutions containing uranium and radioactive decay products around the main processing building (MPB), leakage from storage ponds west of the MPB, and leaching of radioactive materials from discarded equipment and waste containers contaminated both the TGWS and SGWS aquifers during facility operation between 1970 and 1993. Constructing 3D geospatial property models for analysis of groundwater contamination at the site involved use of EarthVision (EV), a 3D geospatial modeling software developed by Dynamic Graphics, Inc. of Alameda, CA. A viable 3D geohydrologic framework model was initially constructed so property data could be spatially located relative to subsurface geohydrologic units. The framework model contained three hydrostratigraphic zones equivalent to the TGWS, SGWS, and DGWS aquifers in which groundwater samples were collected, separated by two sandstone aquitards. Groundwater data collected in the three aquifer systems since 1991 indicated high concentrations of uranium (>10,000 micrograms/liter) and nitrate (> 500 milligrams/liter) around the MPB and elevated nitrate (> 2000 milligrams/ liter) around storage ponds. Vertical connectivity was suggested between the TGWS and SGWS, while the DGWS appeared relatively isolated from the overlying aquifers. Lateral movement of uranium was also suggested over time. For example, lateral migration in the TGWS is suggested along a shallow depression in the bedrock surface trending south-southwest from the southwest corner of the MPB. Another pathway atop the buried bedrock surface, trending west-northwest from the MPB and partially reflected by current surface topography, suggested lateral migration of nitrate in the SGWS. Lateral movement of nitrate in the SGWS was also indicated north, south, and west of the largest storage pond. Definition of contaminant plume movement over time is particularly important for assessing direction and rate of migration and the potential need for preventive measures to control contamination of groundwater outside facility property lines. The 3D geospatial property models proved invaluable for visualizing and analyzing variations in subsurface uranium and nitrate contamination in space and time within and between the three aquifers at the site. The models were an exceptional visualization tool for illustrating extent, volume, and quantitative amounts of uranium and nitrate contamination in the subsurface to regulatory decision-makers in regard to site decommissioning issues, including remediation concerns, providing a perspective not possible to achieve with traditional 2D maps. The geohydrologic framework model provides a conceptual model for consideration in flow and transport analyses.

Bioimmobilization of uranium-practical tools for field applications

NASA Astrophysics Data System (ADS)

Istok, J. D.

2011-12-01

Extensive laboratory and field research has conclusively demonstrated that it is possible to stimulate indigenous microbial activity and create conditions favorable for the reductive precipitation of uranium from groundwater, reducing aqueous U concentrations below regulatory levels. A wide variety of complex and coupled biogeochemical processes have been identified and specific reaction mechanisms and parameters have been quantified for a variety of experimental systems including pure, mixed, and natural microbial cultures, and single mineral, artificial, and natural sediments, and groundwater aquifers at scales ranging from very small (10s nm) to very large (10s m). Multicomponent coupled reactive transport models have also been developed to simulate various aspects of this process in 3D heterogeneous environments. Nevertheless, full-scale application of reductive bioimmobilization of uranium (and other radionuclides and metals) remains problematical because of the technical and logistical difficulties in creating and maintaining reducing environment in the many large U contaminated groundwater aquifers currently under aerobic and oxidizing conditions and often containing high concentrations of competing and more energetically favorable electron acceptors (esp. nitrate). This talk will discuss how simple tools, including small-scale in situ testing and geochemical reaction path modeling, can be used to quickly assess the feasibility of applying bioimmobilization to remediate U contaminated groundwater aquifers and provide data needed for full-scale design.

Nano-Scale Hydroxyapatite: Synthesis, Two-Dimensional Transport Experiments, and Application for Uranium Remediation

DOE PAGES

Kanel, S. R.; Clement, T. P.; Barnett, M. O.; ...

2011-01-01

Synthetic nano-scale hydroxyapatite (NHA) was prepared and characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM) methods. The XRD data confirmed that the crystalline structure and chemical composition of NHA correspond to Ca 5 OH(PO 4 ) 3 . The SEM data confirmed the size of NHA to be less than 50 nm. A two-dimensional physical model packed with saturated porous media was used to study the transport characteristics of NHA under constant flow conditions. The data show that the transport patterns of NHA were almost identical to tracer transport patterns. This result indicates that the NHA material can movemore » with water like a tracer, and its movement was neither retarded nor influenced by any physicochemical interactions and/or density effects. We have also tested the reactivity of NHA with 1 mg/L hexavalent uranium (U(VI)) and found that complete removal of U(VI) is possible using 0.5 g/L NHA at pH 5 to 6. Our results demonstrate that NHA has the potential to be injected as a dilute slurry for in situ treatment of U(VI)-contaminated groundwater systems.« less

Assessing the Vulnerability of Public-Supply Wells to Contamination: Central Valley Aquifer System near Modesto, California

USGS Publications Warehouse

Jagucki, Martha L.; Jurgens, Bryant C.; Burow, Karen R.; Eberts, Sandra M.

2009-01-01

This fact sheet highlights findings from the vulnerability study of a public-supply well in Modesto, California. The well selected for study pumps on average about 1,600 gallons per minute from the Central Valley aquifer system during peak summer demand. Water samples were collected at the public-supply well and at monitoring wells installed in the Modesto vicinity. Samples from the public-supply wellhead contained the undesirable constituents uranium, nitrate, arsenic, volatile organic compounds (VOCs), and pesticides, although none were present at concentrations exceeding drinking-water standards. Of these contaminants, uranium and nitrate pose the most significant water-quality risk to the public-supply well because human activities have caused concentrations in groundwater to increase over time. Overall, study findings point to four primary factors that affect the movement and (or) fate of contaminants and the vulnerability of the public-supply well in Modesto: (1) groundwater age (how long ago water entered, or recharged, the aquifer); (2) irrigation and agricultural and municipal pumping that drives contaminants downward into the primary production zone of the aquifer; (3) short-circuiting of contaminated water down the public-supply well during the low-pumping season; and (4) natural geochemical conditions of the aquifer. A local-scale computer model of groundwater flow and transport to the public-supply well was constructed to simulate long-term nitrate and uranium concentrations reaching the well. With regard to nitrate, two conflicting processes influence concentrations in the area contributing recharge to the well: (1) Beneath land that is being farmed or has recently been farmed (within the last 10 to 20 years), downward-moving irrigation waters contain elevated nitrate concentrations; yet (2) the proportion of agricultural land has decreased and the proportion of urban land has increased since 1960. Urban land use is associated with low nitrate concentrations in recharge (3.1 milligrams per liter). Results of the simulation indicate that nitrate concentrations in the public-supply well peaked in the late 1990s and will decrease slightly from the current level of 5.5 milligrams per liter during the next 100 years. A lag time of 20 to 30 years between peak nitrate concentrations in recharge and peak concentrations in the well is the result of the wide range of ages of water reaching the public-supply well combined with changing nitrogen input concentrations over time. As for uranium, simulation results show that concentrations in the public-supply well will likely approach the Maximum Contaminant Level of 30 micrograms per liter over time; however, it will take more than 100 years because of the contribution of old water at depth in the public-supply well that dilutes uranium concentrations in shallower water entering the well. This allows time to evaluate management strategies and to alter well-construction or pumping strategies to prevent uranium concentrations from exceeding the drinking-water standard.

Remote Sensing and GIS Methods to Detect Uranium Contamination in Watersheds on the Navajo Nation: A NASA/AIHEC Summer Research Experience

NASA Astrophysics Data System (ADS)

Chaco, E.; Robinson, D. K.; Carlson, M.; Rock, B. N.

2010-12-01

Using ground-based mapping of private drinking water wells contaminated with uranium, we developed Landsat Thematic Mapper (TM) band combinations which indicate possible contamination of extensive areas along the Polacca Wash, the Cottonwood Wash and the Balakai Wash below Black Mesa on the Navajo Nation. The project built on water quality samples taken on unregulated wells by a Field Research Water Quality Team from Dine’ College. The Nevada State Health Laboratory analyzed twenty-six samples, and of those, 12 wells showed uranium in exceedance of 13 μR/hr, the equivalent of 114 mrem per year, greater than the Nuclear Regulatory Commission’s exposure limit of 100 mrem per year. This project hypothesized that point locations of contaminated wells could be compared with US Geologic Survey National Uranium Resource Evaluation (NURE) measures of high uranium levels in soil to identify other possible areas of contamination. We used Cluster Analysis remote sensing methods from MultiSpec© with data acquired by Landsat 5-TM satellite to produce a false color composite band combination, (7 4 2/R G B). Overlaid with a geological map, the Landsat classification correlated sections of sediment with pixilated colored minerals in the NURE data. This map shows possible high levels of uranium in the soil in the watersheds below mine and mill locations. Ground truth studies are needed to confirm the presence of uranium at these suspected sites. The larger goal of this study is to help solve the uranium contamination problem for the Navajo Nation. Chaco was one of 21 TCU (Tribal Colleges and Universities) students who participated in the 2010 NASA/AIHEC (National Aeronautics and Space Administration/American Indian Higher Education Council) Summer Research Experience program. Robinson was his TCU faculty mentor, and Carlson and Rock were Summer Research Experience instructors.

Enhanced uranium immobilization and reduction by Geobacter sulfurreducens biofilms.

PubMed

Cologgi, Dena L; Speers, Allison M; Bullard, Blair A; Kelly, Shelly D; Reguera, Gemma

2014-11-01

Biofilms formed by dissimilatory metal reducers are of interest to develop permeable biobarriers for the immobilization of soluble contaminants such as uranium. Here we show that biofilms of the model uranium-reducing bacterium Geobacter sulfurreducens immobilized substantially more U(VI) than planktonic cells and did so for longer periods of time, reductively precipitating it to a mononuclear U(IV) phase involving carbon ligands. The biofilms also tolerated high and otherwise toxic concentrations (up to 5 mM) of uranium, consistent with a respiratory strategy that also protected the cells from uranium toxicity. The enhanced ability of the biofilms to immobilize uranium correlated only partially with the biofilm biomass and thickness and depended greatly on the area of the biofilm exposed to the soluble contaminant. In contrast, uranium reduction depended on the expression of Geobacter conductive pili and, to a lesser extent, on the presence of the c cytochrome OmcZ in the biofilm matrix. The results support a model in which the electroactive biofilm matrix immobilizes and reduces the uranium in the top stratum. This mechanism prevents the permeation and mineralization of uranium in the cell envelope, thereby preserving essential cellular functions and enhancing the catalytic capacity of Geobacter cells to reduce uranium. Hence, the biofilms provide cells with a physically and chemically protected environment for the sustained immobilization and reduction of uranium that is of interest for the development of improved strategies for the in situ bioremediation of environments impacted by uranium contamination. Copyright © 2014, American Society for Microbiology. All Rights Reserved.

Enhanced Uranium Immobilization and Reduction by Geobacter sulfurreducens Biofilms

PubMed Central

Cologgi, Dena L.; Speers, Allison M.; Bullard, Blair A.; Kelly, Shelly D.

2014-01-01

Biofilms formed by dissimilatory metal reducers are of interest to develop permeable biobarriers for the immobilization of soluble contaminants such as uranium. Here we show that biofilms of the model uranium-reducing bacterium Geobacter sulfurreducens immobilized substantially more U(VI) than planktonic cells and did so for longer periods of time, reductively precipitating it to a mononuclear U(IV) phase involving carbon ligands. The biofilms also tolerated high and otherwise toxic concentrations (up to 5 mM) of uranium, consistent with a respiratory strategy that also protected the cells from uranium toxicity. The enhanced ability of the biofilms to immobilize uranium correlated only partially with the biofilm biomass and thickness and depended greatly on the area of the biofilm exposed to the soluble contaminant. In contrast, uranium reduction depended on the expression of Geobacter conductive pili and, to a lesser extent, on the presence of the c cytochrome OmcZ in the biofilm matrix. The results support a model in which the electroactive biofilm matrix immobilizes and reduces the uranium in the top stratum. This mechanism prevents the permeation and mineralization of uranium in the cell envelope, thereby preserving essential cellular functions and enhancing the catalytic capacity of Geobacter cells to reduce uranium. Hence, the biofilms provide cells with a physically and chemically protected environment for the sustained immobilization and reduction of uranium that is of interest for the development of improved strategies for the in situ bioremediation of environments impacted by uranium contamination. PMID:25128347

Laser ablation inductively coupled plasma mass spectrometry measurement of isotope ratios in depleted uranium contaminated soils.

PubMed

Seltzer, Michael D

2003-09-01

Laser ablation of pressed soil pellets was examined as a means of direct sample introduction to enable inductively coupled plasma mass spectrometry (ICP-MS) screening of soils for residual depleted uranium (DU) contamination. Differentiation between depleted uranium, an anthropogenic contaminant, and naturally occurring uranium was accomplished on the basis of measured 235U/238U isotope ratios. The amount of sample preparation required for laser ablation is considerably less than that typically required for aqueous sample introduction. The amount of hazardous laboratory waste generated is diminished accordingly. During the present investigation, 235U/238U isotope ratios measured for field samples were in good agreement with those derived from gamma spectrometry measurements. However, substantial compensation was required to mitigate the effects of impaired pulse counting attributed to sample inhomogeneity and sporadic introduction of uranium analyte into the plasma.

Colorimetric detection of uranium in water

DOEpatents

DeVol, Timothy A [Clemson, SC; Hixon, Amy E [Piedmont, SC; DiPrete, David P [Evans, GA

2012-03-13

Disclosed are methods, materials and systems that can be used to determine qualitatively or quantitatively the level of uranium contamination in water samples. Beneficially, disclosed systems are relatively simple and cost-effective. For example, disclosed systems can be utilized by consumers having little or no training in chemical analysis techniques. Methods generally include a concentration step and a complexation step. Uranium concentration can be carried out according to an extraction chromatographic process and complexation can chemically bind uranium with a detectable substance such that the formed substance is visually detectable. Methods can detect uranium contamination down to levels even below the MCL as established by the EPA.

Uranium Sequestration During Biostimulated Reduction and In Response to the Return of Oxic Conditions In Shallow Aquifers

USGS Publications Warehouse

Fuller, Christopher C.; Johnson, Kelly J.; Akstin, Katherine; Singer, David M.; Yabusaki, Steven B.; Fang, Yilin; Fuhrmann, M.

2015-01-01

A proposed approach for groundwater remediation of uranium contamination is to generate reducing conditions by stimulating the growth of microbial populations through injection of electron donor compounds into the subsurface. Sufficiently reducing conditions will result in reduction of soluble hexavalent uranium, U(VI), and precipitation of the less soluble +4 oxidation state uranium, U(IV). This process is termed biostimulated reduction. A key issue in the remediation of uranium (U) contamination in aquifers by biostimulated reduction is the long term stability of the sequestered uranium. Three flow-through column experiments using aquifer sediment were used to evaluate the remobilization of bioreduced U sequestered under conditions in which biostimulation extended well into sulfate reduction to enhance precipitation of reduced sulfur phases such as iron sulfides. One column received added ferrous iron, Fe(II), increasing production of iron sulfides, to test their effect on remobilization of the sequestered uranium, either by serving as a redox buffer by competing for dissolved oxygen, or by armoring the reduced uranium. During biostimulation of the ambient microbial population with acetate, dissolved uranium was lowered by a factor of 2.5 or more with continued removal for over 110 days of biostimulation, well after the onset of sulfate reduction at ~30 days. Sequestered uranium was essentially all U(IV) resulting from the formation of nano-particulate uraninite that coated sediment grains to a thickness of a few 10’s of microns, sometimes in association with S and Fe. A multicomponent biogeochemical reactive transport model simulation of column effluents during biostimulation was generally able to describe the acetate oxidation, iron, sulfate, and uranium reduction for all three columns using parameters derived from simulations of field scale biostimulation experiments. Columns were eluted with artificial groundwater at equilibrium with atmospheric oxygen to simulate the upper limit of dissolved oxygen in recharge water. Overall about 9% of total uranium removed from solution during biostimulation was remobilized. Release of U during oxic elution was a continuous process over 140 days with dissolved uranium concentrations about 0.2 and 0.8 aM for columns with and without ferrous iron addition, respectively. Uranium remaining on the sediment was in the reduced form. The prolonged period of biostimulation and concomitant sulfate reduction appears to limit the rate of U(IV) oxidative remobilization in contrast to a large release observed for columns in previous studies that did not undergo sulfate reduction. Although continued sulfate reduction may cause decreased permeability from precipitation of iron sulfide, the greater apparent stability of the sequestered U(IV) provided by the sustained biostimulation should be considered in design of field scale remediation efforts. Remobilization of uranium following biostimulated reduction should be tested further at the field scale.

Cola soft drinks for evaluating the bioaccessibility of uranium in contaminated mine soils.

PubMed

Lottermoser, Bernd G; Schnug, Ewald; Haneklaus, Silvia

2011-08-15

There is a rising need for scientifically sound and quantitative as well as simple, rapid, cheap and readily available soil testing procedures. The purpose of this study was to explore selected soft drinks (Coca-Cola Classic®, Diet Coke®, Coke Zero®) as indicators of bioaccessible uranium and other trace elements (As, Ce, Cu, La, Mn, Ni, Pb, Th, Y, Zn) in contaminated soils of the Mary Kathleen uranium mine site, Australia. Data of single extraction tests using Coca-Cola Classic®, Diet Coke® and Coke Zero® demonstrate that extractable arsenic, copper, lanthanum, manganese, nickel, yttrium and zinc concentrations correlate significantly with DTPA- and CaCl₂-extractable metals. Moreover, the correlation between DTPA-extractable uranium and that extracted using Coca-Cola Classic® is close to unity (+0.98), with reduced correlations for Diet Coke® (+0.66) and Coke Zero® (+0.55). Also, Coca-Cola Classic® extracts uranium concentrations near identical to DTPA, whereas distinctly higher uranium fractions were extracted using Diet Coke® and Coke Zero®. Results of this study demonstrate that the use of Coca-Cola Classic® in single extraction tests provided an excellent indication of bioaccessible uranium in the analysed soils and of uranium uptake into leaves and stems of the Sodom apple (Calotropis procera). Moreover, the unconventional reagent is superior in terms of availability, costs, preparation and disposal compared to traditional chemicals. Contaminated site assessments and rehabilitation of uranium mine sites require a solid understanding of the chemical speciation of environmentally significant elements for estimating their translocation in soils and plant uptake. Therefore, Cola soft drinks have potential applications in single extraction tests of uranium contaminated soils and may be used for environmental impact assessments of uranium mine sites, nuclear fuel processing plants and waste storage and disposal facilities. Copyright © 2011 Elsevier B.V. All rights reserved.

ELUTION OF URANIUM FROM RESIN

DOEpatents

McLEan, D.C.

1959-03-10

A method is described for eluting uranium from anion exchange resins so as to decrease vanadium and iron contamination and permit recycle of the major portion of the eluats after recovery of the uranium. Diminution of vanadium and iron contamination of the major portion of the uranium is accomplished by treating the anion exchange resin, which is saturated with uranium complex by adsorption from a sulfuric acid leach liquor from an ore bearing uranium, vanadium and iron, with one column volume of eluant prepared by passing chlorine into ammonium hydroxide until the chloride content is about 1 N and the pH is about 1. The resin is then eluted with 8 to 9 column volumes of 0.9 N ammonium chloride--0.1 N hydrochloric acid solution. The eluants are collected separately and treated with ammonia to precipitate ammonium diuranate which is filtered therefrom. The uranium salt from the first eluant is contaminated with the major portion of ths vanadium and iron and is reworked, while the uranium recovered from the second eluant is relatively free of the undesirable vanadium and irons. The filtrate from the first eluant portion is discarded. The filtrate from the second eluant portion may be recycled after adding hydrochloric acid to increase the chloride ion concentration and adjust the pH to about 1.

Hydrologic and Temporal Influences of Evaporite Minerals on the Vertical Distribution, Storage, and Mobility of Uranium

NASA Astrophysics Data System (ADS)

Roycroft, S. J.; Noel, V.; Boye, K.; Besancon, C.; Weaver, K. L.; Johnson, R. H.; Dam, W. L.; Fendorf, S. E.; Bargar, J.

2016-12-01

Uranium contaminated groundwater in Riverton, Wyoming persists despite anticipated natural attenuation outside of a former uranium ore processing facility. The inability of natural flushing to dilute the uranium below the regulatory threshold indicates that sediments act as secondary sources likely (re)supplying uranium to groundwater. Throughout the contaminated floodplain, uranium rich-evaporites are readily abundant in the upper 2 m of sediments and are spatially coincident with the location of the plume, which suggests a likely link between evaporites and increased uranium levels. Knowledge of where and how uranium is stored within evaporite-associated sediments is required to understand processes controlling the mobility of uranium. We expect that flooding and seasonal changes in hydrologic conditions will affect U phase partitioning, and thus largely control U mobility. The primary questions we are addressing in this project are: What is the relative abundance of uranium incorporated in various mineral complexes throughout the evaporite sediments? How do the factors of depth, location, and seasonality influence the relative incorporation, mobility and speciation of uranium?We have systematically sampled from two soil columns over three dates in Riverton. The sampling dates span before and after a significant flooding event, providing insight into the flood's impact on local uranium mobility. Sequential chemical extractions are used to decipher the reactivity of uranium and approximate U operationally defined within reactants targeting carbonate, silicate, organic, and metal oxide bound or water and exchangeable phases. Extractions throughout the entirety of the sediment cores provide a high-resolution vertical profile of the distribution of uranium in various extracted phases. Throughout the profile, the majority (50-60%) of uranium is bound within carbonate-targeted extracts, a direct effect of the carbonate-rich evaporite sediments. The sum of our analyses provide a dynamic model of uranium incorporation within evaporite sediments holding implications for the fate of uranium throughout contaminated sites across the Colorado River Basin.

Ground-water contamination near a uranium tailings disposal site in Colorado

USGS Publications Warehouse

Goode, Daniel J.; Wilder, Russell J.

1987-01-01

Contaminants from uranium tailings disposed of at an active mill in Colorado have seeped into the shallow ground water onsite. This ground water discharges into the Arkansas River Valley through a superposed stream channel cut in the resistant sandstone ridge at the edge of a synclinal basin. In the river valley, seasonal surface-water irrigation has a significant impact on hydrodynamics. Water levels in residential wells fluctuate up to 20 ft and concentrations of uranium, molybdenum, and other contaminants also vary seasonally, with highest concentrations in the Spring, prior to irrigation, and lowest concentrations in the Fall. Results of a simple transient mixing cell model support the hypothesis that lateral ground-water inflow, and not irrigation recharge, is the source of ground-water contamination.

Exposure pathways and biological receptors: baseline data for the canyon uranium mine, Coconino County, Arizona

USGS Publications Warehouse

Hinck, Jo E.; Linder, Greg L.; Darrah, Abigail J.; Drost, Charles A.; Duniway, Michael C.; Johnson, Matthew J.; Méndez-Harclerode, Francisca M.; Nowak, Erika M.; Valdez, Ernest W.; van Riper, Charles; Wolff, S.W.

2014-01-01

Recent restrictions on uranium mining within the Grand Canyon watershed have drawn attention to scientific data gaps in evaluating the possible effects of ore extraction to human populations as well as wildlife communities in the area. Tissue contaminant concentrations, one of the most basic data requirements to determine exposure, are not available for biota from any historical or active uranium mines in the region. The Canyon Uranium Mine is under development, providing a unique opportunity to characterize concentrations of uranium and other trace elements, as well as radiation levels in biota, found in the vicinity of the mine before ore extraction begins. Our study objectives were to identify contaminants of potential concern and critical contaminant exposure pathways for ecological receptors; conduct biological surveys to understand the local food web and refine the list of target species (ecological receptors) for contaminant analysis; and collect target species for contaminant analysis prior to the initiation of active mining. Contaminants of potential concern were identified as arsenic, cadmium, chromium, copper, lead, mercury, nickel, selenium, thallium, uranium, and zinc for chemical toxicity and uranium and associated radionuclides for radiation. The conceptual exposure model identified ingestion, inhalation, absorption, and dietary transfer (bioaccumulation or bioconcentration) as critical contaminant exposure pathways. The biological survey of plants, invertebrates, amphibians, reptiles, birds, and small mammals is the first to document and provide ecological information on .200 species in and around the mine site; this study also provides critical baseline information about the local food web. Most of the species documented at the mine are common to ponderosa pine Pinus ponderosa and pinyon–juniper Pinus–Juniperus spp. forests in northern Arizona and are not considered to have special conservation status by state or federal agencies; exceptions are the locally endemic Tusayan flameflower Phemeranthus validulus, the long-legged bat Myotis volans, and the Arizona bat Myotis occultus. The most common vertebrate species identified at the mine site included the Mexican spadefoot toad Spea multiplicata, plateau fence lizard Sceloporus tristichus, violetgreen swallow Tachycineta thalassina, pygmy nuthatch Sitta pygmaea, purple martin Progne subis, western bluebird Sialia mexicana, deermouse Peromyscus maniculatus, valley pocket gopher Thomomys bottae, cliff chipmunk Tamias dorsalis, black-tailed jackrabbit Lepus californicus, mule deer Odocoileus hemionus, and elk Cervus canadensis. A limited number of the most common species were collected for contaminant analysis to establish baseline contaminant and radiological concentrations prior to ore extraction. These empirical baseline data will help validate contaminant exposure pathways and potential threats from contaminant exposures to ecological receptors. Resource managers will also be able to use these data to determine the extent to which local species are exposed to chemical and radiation contamination once the mine is operational and producing ore. More broadly, these data could inform resource management decisions on mitigating chemical and radiation exposure of biota at high-grade uranium breccia pipes throughout the Grand Canyon watershed.

Reactive transport modeling at uranium in situ recovery sites: uncertainties in uranium sorption on iron hydroxides

USGS Publications Warehouse

Johnson, Raymond H.; Tutu, Hlanganani; Brown, Adrian; Figueroa, Linda; Wolkersdorfer, Christian

2013-01-01

Geochemical changes that can occur down gradient from uranium in situ recovery (ISR) sites are important for various stakeholders to understand when evaluating potential effects on surrounding groundwater quality. If down gradient solid-phase material consists of sandstone with iron hydroxide coatings (no pyrite or organic carbon), sorption of uranium on iron hydroxides can control uranium mobility. Using one-dimensional reactive transport models with PHREEQC, two different geochemical databases, and various geochemical parameters, the uncertainties in uranium sorption on iron hydroxides are evaluated, because these oxidized zones create a greater risk for future uranium transport than fully reduced zones where uranium generally precipitates.

DOUBLE TRACKS Test Site interim corrective action plan

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

The DOUBLE TRACKS site is located on Range 71 north of the Nellis Air Force Range, northwest of the Nevada Test Site (NTS). DOUBLE TRACKS was the first of four experiments that constituted Operation ROLLER COASTER. On May 15, 1963, weapons-grade plutonium and depleted uranium were dispersed using 54 kilograms of trinitrotoluene (TNT) explosive. The explosion occurred in the open, 0.3 m above the steel plate. No fission yield was detected from the test, and the total amount of plutonium deposited on the ground surface was estimated to be between 980 and 1,600 grams. The test device was composed primarilymore » of uranium-238 and plutonium-239. The mass ratio of uranium to plutonium was 4.35. The objective of the corrective action is to reduce the potential risk to human health and the environment and to demonstrate technically viable and cost-effective excavation, transportation, and disposal. To achieve these objectives, Bechtel Nevada (BN) will remove soil with a total transuranic activity greater then 200 pCI/g, containerize the soil in ``supersacks,`` transport the filled ``supersacks`` to the NTS, and dispose of them in the Area 3 Radioactive Waste Management Site. During this interim corrective action, BN will also conduct a limited demonstration of an alternative method for excavation of radioactive near-surface soil contamination.« less

Uranium(IV) adsorption by natural organic matter in anoxic sediments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bone, Sharon E.; Dynes, James J.; Cliff, John

Uranium is an important carbon-free fuel source and environmental contaminant that accumulates in the tetravalent state, U(IV), in anoxic sediments, such as ore deposits, marine basins, and contaminated aquifers. However, little is known about the speciation of U(IV) in low-temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2+x) in anoxic sediments; however, studies now show that this is not often the case. Yet a model of U(IV) speciation in the absence of mineral formation under field-relevant conditions has not yetmore » been developed. Uranium(IV) speciation controls its reactivity, particularly its susceptibility to oxidative mobilization, impacting its distribution and toxicity. Here we show adsorption to organic carbon and organic carbon-coated clays dominate U(IV) speciation in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that U(IV) speciation is dictated by the mode of reduction (i.e., whether reduction is mediated by microbes or by inorganic reductants), our results demonstrate that mineral formation can be diminished in favor of adsorption, regardless of reduction pathway. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider U(IV) adsorption to organic matter within the sediment environment.« less

Uranium(IV) adsorption by natural organic matter in anoxic sediments

DOE PAGES

Bone, Sharon E.; Dynes, James J.; Cliff, John; ...

2017-01-09

Uranium is an important carbon-free fuel source and environmental contaminant that accumulates in the tetravalent state, U(IV), in anoxic sediments, such as ore deposits, marine basins, and contaminated aquifers. However, little is known about the speciation of U(IV) in low-temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2+x) in anoxic sediments; however, studies now show that this is not often the case. Yet a model of U(IV) speciation in the absence of mineral formation under field-relevant conditions has not yetmore » been developed. Uranium(IV) speciation controls its reactivity, particularly its susceptibility to oxidative mobilization, impacting its distribution and toxicity. Here we show adsorption to organic carbon and organic carbon-coated clays dominate U(IV) speciation in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that U(IV) speciation is dictated by the mode of reduction (i.e., whether reduction is mediated by microbes or by inorganic reductants), our results demonstrate that mineral formation can be diminished in favor of adsorption, regardless of reduction pathway. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider U(IV) adsorption to organic matter within the sediment environment.« less

System-Scale Model of Aquifer, Vadose Zone, and River Interactions for the Hanford 300 Area - Application to Uranium Reactive Transport

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rockhold, Mark L.; Bacon, Diana H.; Freedman, Vicky L.

2013-10-01

This report represents a synthesis and integration of basic and applied research into a system-scale model of the Hanford 300 Area groundwater uranium plume, supported by the U.S. Department of Energy’s Richland Operations (DOE-RL) office. The report integrates research findings and data from DOE Office of Science (DOE-SC), Office of Environmental Management (DOE-EM), and DOE-RL projects, and from the site remediation and closure contractor, Washington Closure Hanford, LLC (WCH). The three-dimensional, system-scale model addresses water flow and reactive transport of uranium for the coupled vadose zone, unconfined aquifer, and Columbia River shoreline of the Hanford 300 Area. The system-scale modelmore » of the 300 Area was developed to be a decision-support tool to evaluate processes of the total system affecting the groundwater uranium plume. The model can also be used to address “what if” questions regarding different remediation endpoints, and to assist in design and evaluation of field remediation efforts. For example, the proposed cleanup plan for the Hanford 300 Area includes removal, treatment, and disposal of contaminated sediments from known waste sites, enhanced attenuation of uranium hot spots in the vadose and periodically rewetted zone, and continued monitoring of groundwater with institutional controls. Illustrative simulations of polyphosphate infiltration were performed to demonstrate the ability of the system-scale model to address these types of questions. The use of this model in conjunction with continued field monitoring is expected to provide a rigorous basis for developing operational strategies for field remediation and for defining defensible remediation endpoints.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dam, William; Gil, Dr. April; Johnson, Raymond H.

The US Department of Energy Office of Legacy Management (LM) is responsible for maintaining protective public health and environmental conditions at former uranium mill tailings sites nationwide via long-term stewardship. One of these sites, a former uranium mill near Riverton, Wyoming, is within the boundary of the Wind River Indian Reservation and operated from 1958 to 1963. Tailings and contaminated material associated with mill operations were removed and transported to an offsite disposal cell in 1989. The remedial action was completed under Title I of the Uranium Mill Tailings Radiation Control Act of 1978. Milling operations, which included an unlinedmore » tailings impoundment and an unlined evaporation pond, contaminated the shallow groundwater, resulting in a downgradient groundwater plume that discharges to the Little Wind River. A natural flushing compliance strategy was implemented in 1998. This strategy allows contaminants of concern to naturally flush from the groundwater, provided that contaminants flush below US Environmental Protection Agency maximum concentration limits within 100 years. As part of the compliance strategy, LM has implemented a groundwater monitoring program along with institutional controls that include the installation of an alternate water supply, continued sampling of private wells, and restrictions on well drilling and gravel pit construction. LM works closely with local stakeholders and community members to ensure that these institutional controls are in place and maintained. The Riverton site provides an interesting case study where contaminant remobilization due to river flooding prompted a reevaluation of the conceptual site model to verify if the current compliance strategy would remain protective of human health and the environment. Concentrations of groundwater contaminants, which include sulfate, molybdenum, and uranium, were transiently elevated following flooding of the Little Wind River in 2010 and 2016. These flood events provided the impetus to investigate other aspects of the hydrologic system, including the unsaturated zone, naturally reduced (sulfidic) zones, and evaporite deposits. New site conceptual models, field and laboratory studies, and numerical models are being developed to explain how biogeochemical sediment–water interactions contribute to plume persistence and flood-related increases in groundwater concentrations. Updated human health and ecological risk assessments are progressing to evaluate the risk to human health and the environment based on current site conditions. Groundwater concentrations may remain above US Environmental Protection Agency maximum concentration limits beyond the 100-year natural flushing regulatory time frame. LM in its capacity as a long-term steward continues to monitor the site to ensure protectiveness is maintained and to determine the feasibility of alternative compliance and remediation strategies.« less

Meta-analysis of depleted uranium levels in the Balkan region.

PubMed

Besic, Larisa; Muhovic, Imer; Asic, Adna; Kurtovic-Kozaric, Amina

2017-06-01

In recent years, contradicting data has been published on the connection between the presence of depleted uranium and an increased cancer incidence among military personnel deployed in the Balkans during the 1992-1999 wars. This has led to numerous research articles investigating possible depleted uranium contamination of the afflicted regions of the Balkan Peninsula, namely Bosnia & Herzegovina, Serbia, Kosovo and Montenegro. The aim of this study was to collect data from previously published reports investigating the levels of depleted uranium in the Balkans and to present the data in the form of a meta-analysis. This would provide a clear image of the extent of depleted uranium contamination after the Balkan conflict. In addition, we tested the hypothesis that there is a correlation between the levels of depleted uranium and the assumed depleted uranium-related health effects. Our results suggest that the majority of the examined sites contain natural uranium, while the area of Kosovo appears to be most heavily afflicted by depleted uranium pollution, followed by Bosnia & Herzegovina. Furthermore, the results indicate that it is not possible to make a valid correlation between the health effects and depleted uranium-contaminated areas. We therefore suggest a structured collaborative plan of action where long-term monitoring of the residents of depleted uranium-afflicted areas would be performed. In conclusion, while the possibility of depleted uranium toxicity in post-conflict regions appears to exist, there currently exists no definitive proof of such effects, due to insufficient studies of potentially afflicted populations, in addition to the lack of a common epidemiological approach in the reviewed literature. Copyright © 2017 Elsevier Ltd. All rights reserved.

49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

Code of Federal Regulations, 2013 CFR

2013-10-01

... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in which the sole Class 7 (radioactive) material content is natural uranium, unirradiated depleted uranium...

49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

Code of Federal Regulations, 2014 CFR

2014-10-01

... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in which the sole Class 7 (radioactive) material content is natural uranium, unirradiated depleted uranium...

49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

Code of Federal Regulations, 2012 CFR

2012-10-01

... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in which the sole Class 7 (radioactive) material content is natural uranium, unirradiated depleted uranium...

Biosorption of heavy metals and uranium from dilute solutions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schneider, I.A.H.; Misra, M.; Smith, R.W.

1995-08-01

Eichhornia crassipes approaches being a scourge in many parts of the world, choking waterways and hindering transport upon them. At the same time it is known to readily abstract heavy metal ions from water and, thus, aids in the removal of heavy metals found in such waters. This paper considers the possibility of using specific parts of the plant as an inexpensive adsorbent for the removal of heavy metals from contaminated chemical and mining industry waste waters. In particular the root of the plant was found to be an excellent accumulator of heavy metal ions including uranium from solution. Itmore » is also suggested that dried roots of the plant might be placed in simple bags and used in a very low cost metal ion removal system.« less

Uranium contents in plants and mushrooms grown on a uranium-contaminated site near Ronneburg in Eastern Thuringia/Germany.

PubMed

Baumann, Nils; Arnold, Thuro; Haferburg, Götz

2014-01-01

Uranium concentrations in cultivated (sunflower, sunchoke, potato) and native plants, plant compartment specimens, and mushrooms, grown on a test site within a uranium-contaminated area in Eastern Thuringia, were analyzed and compared. This test site belongs to the Friedrich-Schiller University Jena and is situated on the ground of a former but now removed uranium mine waste leaching heap. For determination of the U concentrations in the biomaterials, the saps of the samples were squeezed out by using an ultracentrifuge, after that, the uranium concentrations in the saps and the remaining residue were measured, using ICP-MS. The study further showed that uranium concentrations observed in plant compartment and mushroom fruiting bodies sap samples were always higher than their associated solid residue sample. Also, it was found that the detected uranium concentration in the root samples were always higher than were observed in their associated above ground biomass, e.g., in shoots, leaves, blossoms etc. The highest uranium concentration was measured with almost 40 ppb U in a fruiting body of a mushroom and in roots of butterbur. However, the detected uranium concentrations in plants and mushrooms collected in this study were always lower than in the associated surface and soil water of the test site, indicating that under the encountered natural conditions, none of the studied plant and mushroom species turned out to be a hyperaccumulator for uranium, which could have extracted uranium in sufficient amounts out of the uranium-contaminated soil. In addition, it was found that the detected uranium concentrations in the sap samples, despite being above the sensitivity limit, proved to be too low-in combination with the presence of fluorescence quenching substances, e.g., iron and manganese ions, and/or organic quenchers-to extract a useful fluorescence signal, which could have helped to identify the uranium speciation in plants.

Uranium and its decay products in samples contaminated with uranium mine and mill waste

NASA Astrophysics Data System (ADS)

Benedik, L.; Klemencic, H.; Repinc, U.; Vrecek, P.

2003-05-01

The routine determination of the activity concentrations of uranium isotopes (^{238}U, ^{235}U and ^{234}U), thorium isotopes (^{212}Th, ^{230}TI, and ^{228}Th), ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in the environment is one of the most important tasks in uranium mining areas. Natural radionuclides contribute negligibly to the extemal radiation dose, but in the case of ingestion or inhalation can represent a very serious hazard. The objective of this study was to determine the activities of uranium and its decay products ^{230}Th, ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in sediments and water below sources of contamination (uranium mine, disposal sites and individual inflows) using gamma and alpha spectrometry, beta counting, the liquid scintillation technique and radiochemical neutron activation analysis.

Case Study of Urban Residential Remediation and Restoration in Port Hope, Canada - 13250

DOE Office of Scientific and Technical Information (OSTI.GOV)

Geddes, Brian; DeJong, John; Owen, Michael

2013-07-01

The Canadian Municipality of Port Hope, Ontario, is located some 100 km east of Toronto and has been the location of radium and/or uranium refining since the 1930's. Historically, these activities involved materials containing radium-226, uranium, arsenic and other contaminants generated by the refining process. In years past, properties and sites in Port Hope became contaminated from spillage during transportation, unrecorded, un-monitored or unauthorized diversion of contaminated fill and materials, wind and water erosion and spread from residue storage areas. Residential properties in Port Hope impacted by radioactive materials are being addressed by the Canadian federal government under programs administeredmore » by the Low-Level Radioactive Waste Management Office (LLRWMO) and the Port Hope Area Initiative Management Office (PHAIMO). Issues that currently arise at these properties are addressed by the LLRWMO's Interim Waste Management Program (IWM). In the future, these sites will be included in the PHAIMO's Small Scale Sites (SSS) remedial program. The LLRWMO has recently completed a remediation and restoration program at a residential property in Port Hope that has provided learnings that will be applicable to the PHAIMO's upcoming SSS remedial effort. The work scope at this property involved remediating contaminated refinery materials that had been re-used in the original construction of the residence. Following removal of the contaminated materials, the property was restored for continued residential use. This kind of property represents a relatively small, but potentially challenging subset of the portfolio of sites that will eventually be addressed by the SSS program. (authors)« less

Calixarene cleansing formulation for uranium skin contamination.

PubMed

Phan, Guillaume; Semili, Naïma; Bouvier-Capely, Céline; Landon, Géraldine; Mekhloufi, Ghozlene; Huang, Nicolas; Rebière, François; Agarande, Michelle; Fattal, Elias

2013-10-01

An oil-in-water cleansing emulsion containing calixarene molecule, an actinide specific chelating agent, was formulated in order to improve the decontamination of uranium from the skin. Commonly commercialized cosmetic ingredients such as surfactants, mineral oil, or viscosifying agents were used in preparing the calixarene emulsion. The formulation was characterized in terms of size and apparent viscosity measurements and then was tested for its ability to limit uranyl ion permeation through excoriated pig-ear skin explants in 24-h penetration studies. Calixarene emulsion effectiveness was compared with two other reference treatments consisting of DTPA and EHBP solutions. Application of calixarene emulsion induced the highest decontamination effect with an 87% decrease in uranium diffusion flux. By contrast, EHBP and DTPA solutions only allowed a 50% and 55% reduction of uranium permeation, respectively, and had the same effect as a simple dilution of the contamination by pure water. Uranium diffusion decrease was attributed to uranyl ion-specific chelation by calixarene within the formulation, since no significant effect was obtained after application of the same emulsion without calixarene. Thus, calixarene cleansing emulsion could be considered as a promising treatment in case of accidental contamination of the skin by highly diffusible uranium compounds.

Surface Cleaning Techniques: Ultra-Trace ICP-MS Sample Preparation and Assay of HDPE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Overman, Nicole R.; Hoppe, Eric W.; Addleman, Raymond S.

2013-06-01

The world’s most sensitive radiation detection and assay systems depend upon ultra-low background (ULB) materials to reduce unwanted radiological backgrounds. Herein, we evaluate methods to clean HDPE, a material of interest to ULB systems and the means to provide rapid assay of surface and bulk contamination. ULB level material and ultra-trace level detection of actinide elements is difficult to attain, due to the introduction of contamination from sample preparation equipment such as pipette tips, sample vials, forceps, etc. and airborne particulate. To date, literature available on the cleaning of such polymeric materials and equipment for ULB applications and ultra-trace analysesmore » is limited. For these reasons, a study has been performed to identify an effective way to remove surface contamination from polymers in an effort to provide improved instrumental detection limits. Inductively Coupled Plasma Mass Spectroscopy (ICP-MS) was utilized to assess the effectiveness of a variety of leachate solutions for removal of inorganic uranium and thorium surface contamination from polymers, specifically high density polyethylene (HDPE). HDPE leaching procedures were tested to optimize contaminant removal of thorium and uranium. Calibration curves for thorium and uranium ranged from 15 ppq (fg/mL) to 1 ppt (pg/mL). Detection limits were calculated at 6 ppq for uranium and 7 ppq for thorium. Results showed the most effective leaching reagent to be clean 6 M nitric acid for 72 hour exposures. Contamination levels for uranium and thorium found in the leachate solutions were significant for ultralow level radiation detection applications.« less

Release behavior of uranium in uranium mill tailings under environmental conditions.

PubMed

Liu, Bo; Peng, Tongjiang; Sun, Hongjuan; Yue, Huanjuan

2017-05-01

Uranium contamination is observed in sedimentary geochemical environments, but the geochemical and mineralogical processes that control uranium release from sediment are not fully appreciated. Identification of how sediments and water influence the release and migration of uranium is critical to improve the prevention of uranium contamination in soil and groundwater. To understand the process of uranium release and migration from uranium mill tailings under water chemistry conditions, uranium mill tailing samples from northwest China were investigated with batch leaching experiments. Results showed that water played an important role in uranium release from the tailing minerals. The uranium release was clearly influenced by contact time, liquid-solid ratio, particle size, and pH under water chemistry conditions. Longer contact time, higher liquid content, and extreme pH were all not conducive to the stabilization of uranium and accelerated the uranium release from the tailing mineral to the solution. The values of pH were found to significantly influence the extent and mechanisms of uranium release from minerals to water. Uranium release was monitored by a number of interactive processes, including dissolution of uranium-bearing minerals, uranium desorption from mineral surfaces, and formation of aqueous uranium complexes. Considering the impact of contact time, liquid-solid ratio, particle size, and pH on uranium release from uranium mill tailings, reducing the water content, decreasing the porosity of tailing dumps and controlling the pH of tailings were the key factors for prevention and management of environmental pollution in areas near uranium mines. Copyright © 2017 Elsevier Ltd. All rights reserved.

Injection of Emulsified Vegetable Oil for Long-Term Bioreduction of Uranium

NASA Astrophysics Data System (ADS)

Brooks, S. C.; Watson, D. B.; Schadt, C. W.; Jardine, P. M.; Gihring, T. M.; Zhang, G.; Mehlhorn, T.; Lowe, K.; Phillips, J.; Earles, J.; Wu, W.; Criddle, C. S.; Kemner, K. M.; Boyanov, M.

2011-12-01

In situ bioremediation of a uranium and nitrate-contaminated aquifer with the slow-release electron donor, emulsified vegetable oil (EVO), was tested at the US DOE Subsurface Biogeochemical Research Program (SBR) Integrated Field Research Challenge (IFRC) site, in Oak Ridge, TN. The EVO injection took place in Area 2 of the IFRC located about 300 m downgradient of the former S-3 disposal ponds. Liquid wastes, disposed in the ponds from 1951 to 1983, were primarily composed of nitric acid, plating wastes containing various metals (Cr, Ni) radionuclides (U, Tc), inorganics (nitrate, sulfate) and organic contaminants (tetrachloroethylene, acetone). Prior pond closure in 1987, large volumes of waste fluids migrated into the subsurface, down Bear Creek Valley and into Bear Creek. Contaminants detected at Area 2 were transported through a high permeability gravelly fill that is considered a preferred transport pathway for U to Bear Creek. Groundwater in the gravelly fill is contaminated with U (1-3 mg/L), sulfate (95-130 mg/L), and nitrate (20-40 mg/L) and 500 mg/kg or higher U has been detected on the solid phase of the fill material. The objective of this study is to investigate the feasibility and long-term sustainability of U(VI) reduction and immobilization, and nitrate degradation in the high permeability, high flow gravel fill using EVO as the electron donor. A one-time EVO injection was conducted over a 2 hour period in the highly permeable gravel (hydraulic conductivity 0.08 cm/sec) in the well instrumented IFRC Area 2 field plot. Extensive monitoring of geochemical parameters, dissolved gases and microbial populations were conducted during the test. A bromide tracer test was conducted prior to the injection of the EVO to assess transport pathways and rates. Geochemical analysis of site groundwater demonstrated the sequential bioreduction of oxygen, nitrate, Mn(IV), Fe(III) and sulfate. Transient accumulation of acetate was observed as an intermediate in the oil degradation. Reduction and removal of U and nitrate from groundwater was observed in all wells in hydraulic connection to the injection wells after 2-4 weeks. U concentrations in groundwater were reduced to below 30 ppb (US EPA drinking water standard) at some well locations and nitrate was reduced to below detectable levels. Rebound of U in groundwater was observed together with the rebound of sulfate concentrations as the EVO was consumed. The flux of U and nitrate contamination from groundwater to the surface water receptor (Bear Creek) was significantly reduced by the EVO injection over a one year period. Uranium (VI) reduction to U(IV) in the field tests was confirmed by X-ray absorption near-edge spectroscopy (XANES) analysis. The reduced U(IV) was determined by X-ray absorption fine structure (XAFS) to be in an Fe-U complex, not uraninite. The activities of major Fe(III)- and sulfate-reducing bacteria with U(VI)-reducing capability as well as methanogens was stimulated after injection of the oil.

Modeling of U-series Radionuclide Transport Through Soil at Pena Blanca, Chihuahua, Mexico

NASA Astrophysics Data System (ADS)

Pekar, K. E.; Goodell, P. C.; Walton, J. C.; Anthony, E. Y.; Ren, M.

2007-05-01

The Nopal I uranium deposit is located at Pena Blanca in Chihuahua, Mexico. Mining of high-grade uranium ore occurred in the early 1980s, with the ore stockpiled nearby. The stockpile was mostly cleared in the 1990s; however, some of the high-grade boulders have remained there, creating localized sources of radioactivity for a period of 25-30 years. This provides a unique opportunity to study radionuclide transport, because the study area did not have any uranium contamination predating the stockpile in the 1980s. One high-grade boulder was selected for study based upon its shape, location, and high activity. The presumed drip-line off of the boulder was marked, samples from the boulder surface were taken, and then the boulder was moved several feet away. Soil samples were taken from directly beneath the boulder, around the drip-line, and down slope. Eight of these samples were collected in a vertical profile directly beneath the boulder. Visible flakes of boulder material were removed from the surficial soil samples, because they would have higher concentrations of U-series radionuclides and cause the activities in the soil samples to be excessively high. The vertical sampling profile used 2-inch thicknesses for each sample. The soil samples were packaged into thin plastic containers to minimize the attenuation and to standardize sample geometry, and then they were analyzed by gamma-ray spectroscopy with a Ge(Li) detector for Th-234, Pa-234, U-234, Th-230, Ra-226, Pb-214, Bi-214, and Pb-210. The raw counts were corrected for self-attenuation and normalized using BL-5, a uranium standard from Beaverlodge, Saskatchewan. BL-5 allowed the counts obtained on the Ge(Li) to be referenced to a known concentration or activity, which was then applied to the soil unknowns for a reliable calculation of their concentrations. Gamma ray spectra of five soil samples from the vertical profile exhibit decreasing activities with increasing depth for the selected radionuclides. Independent multi-element analyses of three samples by ICP-MS show decreasing uranium concentration with depth as well. The transport of the radionuclides is evaluated using STANMOD, a Windows-based software package for evaluating solute transport in porous media using analytical solutions of the advection-dispersion solute transport equation. The package allows various one-dimensional, advection-dispersion parameters to be determined by fitting mathematical solutions of theoretical transport models to observed data. The results are promising for future work on the release rate of radionuclides from the boulder, the dominant mode of transport (e.g., particulate or dissolution), and the movement of radionuclides through porous media. The measured subsurface transport rates provide modelers with a model validation dataset.

Geology, geochemistry, and geophysics of the Fry Canyon uranium/copper project site, southeastern Utah - Indications of contaminant migration

USGS Publications Warehouse

Otton, James K.; Zielinski, Robert A.; Horton, Robert J.

2010-01-01

The Fry Canyon uranium/copper project site in San Juan County, southeastern Utah, was affected by the historical (1957-68) processing of uranium and copper-uranium ores. Relict uranium tailings and related ponds, and a large copper heap-leach pile at the site represent point sources of uranium and copper to local soils, surface water, and groundwater. This study was designed to establish the nature, extent, and pathways of contaminant dispersion. The methods used in this study are applicable at other sites of uranium mining, milling, or processing. The uranium tailings and associated ponds sit on a bench that is as much as 4.25 meters above the level of the adjacent modern channel of Fry Creek. The copper heap leach pile sits on bedrock just south of this bench. Contaminated groundwater from the ponds and other nearby sites moves downvalley and enters the modern alluvium of adjacent Fry Creek, its surface water, and also a broader, deeper paleochannel that underlies the modern creek channel and adjacent benches and stream terraces. The northern extent of contaminated groundwater is uncertain from geochemical data beyond an area of monitoring wells about 300 meters north of the site. Contaminated surface water extends to the State highway bridge. Some uranium-contaminated groundwater may also enter underlying bedrock of the Permian Cedar Mesa Sandstone along fracture zones. Four dc-resistivity surveys perpendicular to the valley trend were run across the channel and its adjacent stream terraces north of the heap-leach pile and ponds. Two surveys were done in a small field of monitoring wells and two in areas untested by borings to the north of the well field. Bedrock intercepts, salt distribution, and lithologic information from the wells and surface observations in the well field aided interpretation of the geophysical profiles there and allowed interpretation of the two profiles not tested by wells. The geophysical data for the two profiles to the north of the well field suggest that the paleochannel persists at least 900 m to the north of the heap leach and pond sites. Contamination of groundwater beneath the stream terraces may extend at least that far. Fry Creek surface water (six samples), seeps and springs (six samples), and wells (eight samples) were collected during a dry period of April 16-19, 2007. The most uranium-rich (18.7 milligrams per liter) well water on the site displays distinctive Ca-Mg-SO4-dominant chemistry indicating the legacy of heap leaching copper-uranium ores with sulfuric acid. This same water has strongly negative d34S of sulfate (-13.3 per mil) compared to most local waters of -2.4 to -5.4 per mil. Dissolved uranium species in all sampled waters are dominantly U(VI)-carbonate complexes. All waters are undersaturated with respect to U(VI) minerals. The average 234U/238U activity ratio (AR) in four well waters from the site (0.939 + or ? 0.011) is different from that of seven upstream waters (1.235 + or ? 0.069). This isotopic contrast permits quantitative estimates of mixing of site-derived uranium with natural uranium in waters collected downstream. At the time of sampling, uranium in downstream surface water was mostly (about 67 percent) site-derived and subject to further concentration by evaporation. Three monitoring wells located approximately 0.4 kilometer downstream contained dominantly (78-87 percent) site-derived uranium. Distinctive particles of chalcopyrite (CuFeS) and variably weathered pyrite (FeS2) are present in tailings at the stream edge on the site and are identified in stream sediments 1.3 kilometers downstream, based on inspection of polished grain mounts of magnetic mineral separates.

Structure and function of subsurface microbial communities affecting radionuclide transport and bioimmobilization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kostka, Joel E.; Prakash, Om; Green, Stefan J.

2012-05-01

Our objectives were to: 1) isolate and characterize novel anaerobic prokaryotes from subsurface environments exposed to high levels of mixed contaminants (U(VI), nitrate, sulfate), 2) elucidate the diversity and distribution of metabolically active metal- and nitrate-reducing prokaryotes in subsurface sediments, and 3) determine the biotic and abiotic mechanisms linking electron transport processes (nitrate, Fe(III), and sulfate reduction) to radionuclide reduction and immobilization. Mechanisms of electron transport and U(VI) transformation were examined under near in situ conditions in sediment microcosms and in field investigations. Field sampling was conducted at the Oak Ridge Field Research Center (ORFRC), in Oak Ridge, Tennessee. Themore » ORFRC subsurface is exposed to mixed contamination predominated by uranium and nitrate. In short, we effectively addressed all 3 stated objectives of the project. In particular, we isolated and characterized a large number of novel anaerobes with a high bioremediation potential that can be used as model organisms, and we are now able to quantify the function of subsurface sedimentary microbial communities in situ using state-of-the-art gene expression methods (molecular proxies).« less

Microbiological, Geochemical and Hydrologic Processes Controlling Uranium Mobility: An Integrated Field-Scale Subsurface Research Challenge Site at Rifle, Colorado, Quality Assurance Project Plan

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fix, N. J.

The U.S. Department of Energy (DOE) is cleaning up and/or monitoring large, dilute plumes contaminated by metals, such as uranium and chromium, whose mobility and solubility change with redox status. Field-scale experiments with acetate as the electron donor have stimulated metal-reducing bacteria to effectively remove uranium [U(VI)] from groundwater at the Uranium Mill Tailings Site in Rifle, Colorado. The Pacific Northwest National Laboratory and a multidisciplinary team of national laboratory and academic collaborators has embarked on a research proposed for the Rifle site, the object of which is to gain a comprehensive and mechanistic understanding of the microbial factors andmore » associated geochemistry controlling uranium mobility so that DOE can confidently remediate uranium plumes as well as support stewardship of uranium-contaminated sites. This Quality Assurance Project Plan provides the quality assurance requirements and processes that will be followed by the Rifle Integrated Field-Scale Subsurface Research Challenge Project.« less

Using 238U/235U ratios to understand the formation and oxidation of reduced uranium solids in naturally reduced zones

NASA Astrophysics Data System (ADS)

Jemison, N.; Johnson, T. M.; Druhan, J. L.; Davis, J. A.

2016-12-01

Uranium occurs in groundwater primarily as soluble and mobile U(VI), which can be reduced to immobile U(IV), often observed in sediments as uraninite. Numerous U(VI)-contaminated sites, such as the DOE field site in Rifle, CO, contain naturally reduced zones (NRZ's) that have relatively high concentrations of organic matter. Reduction of heavy metals occurs within NRZ's, producing elevated concentrations of iron sulfides and U(IV). Slow, natural oxidation of U(IV) from NRZ's may prolong U(VI) contamination of groundwater. The reduction of U(VI) produces U(IV) with a higher 238U/235U ratio. Samples from two NRZ sediment cores recovered from the Rifle site revealed that the outer fringes of the NRZ contain U(IV) with a high 238U/235U ratio, while lower values are observed in the center . We suggest that as aqueous U(VI) was reduced in the NRZ, it was driven to lower 238U/235U values, such that U(IV) formed in the core of the NRZ reflects a lower 238U/235U. Two oxidation experiments were conducted by injecting groundwater containing between 14.9 and 21.2 mg/L dissolved O2 as an oxidant into the NRZ. The oxidation of U(IV) from this NRZ increased aqueous U(VI) concentrations and caused a shift to higher 238U/235U in groundwater as U(IV) was oxidized primarily on the outer fringes of the NRZ. In total these observations suggest that the stability of solid phase uranium is governed by coupled reaction and transport processes. To better understand various reactive transport scenarios we developed a model for the formation and oxidation of NRZ's utilizing the reactive transport software CrunchTope. These simulations suggest that the development of isotopically heterogeneous U(IV) within NRZ's is largely controlled by permeability of the NRZ and the U(VI) reduction rate. Oxidation of U(IV) from the NRZ's is constrained by the oxidation rate of U(IV) as well as iron sulfides, which can prevent oxidation of U(IV) by scavenging dissolved oxygen.

Evolution of uranium distribution and speciation in mill tailings, COMINAK Mine, Niger.

PubMed

Déjeant, Adrien; Galoisy, Laurence; Roy, Régis; Calas, Georges; Boekhout, Flora; Phrommavanh, Vannapha; Descostes, Michael

2016-03-01

This study investigated the evolution of uranium distribution and speciation in mill tailings from the COMINAK mine (Niger), in production since 1978. A multi-scale approach was used, which combined high resolution remote sensing imagery, ICP-MS bulk rock analyses, powder X-ray diffraction, Scanning Electron Microscopy, Focused Ion Beam--Transmission Electron Microscopy and X-ray Absorption Near Edge Spectroscopy. Mineralogical analyses showed that some ore minerals, including residual uraninite and coffinite, undergo alteration and dissolution during tailings storage. The migration of uranium and other contaminants depends on (i) the chemical stability of secondary phases and sorbed species (dissolution and desorption processes), and (ii) the mechanical transport of fine particles bearing these elements. Uranium is stabilized after formation of secondary uranyl sulfates and phosphates, and adsorbed complexes on mineral surfaces (e.g. clay minerals). In particular, the stock of insoluble uranyl phosphates increases with time, thus contributing to the long-term stabilization of uranium. At the surface, a sulfate-cemented duricrust is formed after evaporation of pore water. This duricrust limits water infiltration and dust aerial dispersion, though it is enriched in uranium and many other elements, because of pore water rising from underlying levels by capillary action. Satellite images provided a detailed description of the tailings pile over time and allow monitoring of the chronology of successive tailings deposits. Satellite images suggest that uranium anomalies that occur at deep levels in the pile are most likely former surface duricrusts that have been buried under more recent tailings. Copyright © 2015 Elsevier B.V. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Szescody, James E.; Moore, Robert C.; Rigali, Mark J.

The Old Rifle Site is a former vanadium and uranium ore-processing facility located adjacent to the Colorado River and approximately 0.3 miles east of the city of Rifle, CO. The former processing facilities have been removed and the site uranium mill tailings are interned at a disposal cell north of the city of Rifle. However, some low level remnant uranium contamination still exists at the Old Rifle site. In 2002, the United States Nuclear Regulatory Commission (US NRC) concurred with United States Department of Energy (US DOE) on a groundwater compliance strategy of natural flushing with institutional controls to decreasemore » contaminant concentrations in the aquifer. In addition to active monitoring of contaminant concentrations, the site is also used for DOE Legacy Management (LM) and other DOE-funded small-scale field tests of remediation technologies. The purpose of this laboratory scale study was to evaluate the effectiveness of a hydroxyapatite (Ca 10(PO 4) 6(OH) 2) permeable reactive barrier and source area treatment in Old Rifle sediments. Phosphate treatment impact was evaluated by comparing uranium leaching and surface phase changes in untreated to PO 4-treated sediments. The impact of the amount of phosphate precipitation in the sediment on uranium mobility was evaluated with three different phosphate loadings. A range of flow velocity and uranium concentration conditions (i.e., uranium flux through the phosphate-treated sediment) was also evaluated to quantify the uranium uptake mass and rate by the phosphate precipitate.« less

Metals other than uranium affected microbial community composition in a historical uranium-mining site.

PubMed

Sitte, Jana; Löffler, Sylvia; Burkhardt, Eva-Maria; Goldfarb, Katherine C; Büchel, Georg; Hazen, Terry C; Küsel, Kirsten

2015-12-01

To understand the links between the long-term impact of uranium and other metals on microbial community composition, ground- and surface water-influenced soils varying greatly in uranium and metal concentrations were investigated at the former uranium-mining district in Ronneburg, Germany. A soil-based 16S PhyloChip approach revealed 2358 bacterial and 35 archaeal operational taxonomic units (OTU) within diverse phylogenetic groups with higher OTU numbers than at other uranium-contaminated sites, e.g., at Oak Ridge. Iron- and sulfate-reducing bacteria (FeRB and SRB), which have the potential to attenuate uranium and other metals by the enzymatic and/or abiotic reduction of metal ions, were found at all sites. Although soil concentrations of solid-phase uranium were high, ranging from 5 to 1569 μg·g (dry weight) soil(-1), redundancy analysis (RDA) and forward selection indicated that neither total nor bio-available uranium concentrations contributed significantly to the observed OTU distribution. Instead, microbial community composition appeared to be influenced more by redox potential. Bacterial communities were also influenced by bio-available manganese and total cobalt and cadmium concentrations. Bio-available cadmium impacted FeRB distribution while bio-available manganese and copper as well as solid-phase zinc concentrations in the soil affected SRB composition. Archaeal communities were influenced by the bio-available lead as well as total zinc and cobalt concentrations. These results suggest that (i) microbial richness was not impacted by heavy metals and radionuclides and that (ii) redox potential and secondary metal contaminants had the strongest effect on microbial community composition, as opposed to uranium, the primary source of contamination.

PROCESS FOR SEGREGATING URANIUM FROM PLUTONIUM AND FISSION-PRODUCT CONTAMINATION

DOEpatents

Ellison, C.V.; Runion, T.C.

1961-06-27

An aqueous nitric acid solution containing uranium, plutonium, and fission product values is contacted with an organic extractant comprised of a trialkyl phosphate and an organic diluent. The relative amounts of trialkyl phosphate and uranium values are controlled to achieve a concentration of uranium values in the organic extractant of at least 0.35 moles uranium per mole of trialkyl phosphate, thereby preferentially extracting uranium values into the organic extractant.

Radiochronological Age of a Uranium Metal Sample from an Abandoned Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meyers, L A; Williams, R W; Glover, S E

2012-03-16

A piece of scrap uranium metal bar buried in the dirt floor of an old, abandoned metal rolling mill was analyzed using multi-collector inductively coupled plasma mass spectroscopy (MC-ICP-MS). The mill rolled uranium rods in the 1940s and 1950s. Samples of the contaminated dirt in which the bar was buried were also analyzed. The isotopic composition of uranium in the bar and dirt samples were both the same as natural uranium, though a few samples of dirt also contained recycled uranium; likely a result of contamination with other material rolled at the mill. The time elapsed since the uranium metalmore » bar was last purified can be determined by the in-growth of the isotope {sup 230}Th from the decay of {sup 234}U, assuming that only uranium isotopes were present in the bar after purification. The age of the metal bar was determined to be 61 years at the time of this analysis and corresponds to a purification date of July 1950 {+-} 1.5 years.« less

New Technique for Speciation of Uranium in Sediments Following Acetate-Stimulated Bioremediation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

2011-06-22

Acetate-stimulated bioremediation is a promising new technique for sequestering toxic uranium contamination from groundwater. The speciation of uranium in sediments after such bioremediation attempts remains unknown as a result of low uranium concentration, and is important to analyzing the stability of sequestered uranium. A new technique was developed for investigating the oxidation state and local molecular structure of uranium from field site sediments using X-Ray Absorption Spectroscopy (XAS), and was implemented at the site of a former uranium mill in Rifle, CO. Glass columns filled with bioactive Rifle sediments were deployed in wells in the contaminated Rifle aquifer and amendedmore » with a hexavalent uranium (U(VI)) stock solution to increase uranium concentration while maintaining field conditions. This sediment was harvested and XAS was utilized to analyze the oxidation state and local molecular structure of the uranium in sediment samples. Extended X-Ray Absorption Fine Structure (EXAFS) data was collected and compared to known uranium spectra to determine the local molecular structure of the uranium in the sediment. Fitting was used to determine that the field site sediments did not contain uraninite (UO{sub 2}), indicating that models based on bioreduction using pure bacterial cultures are not accurate for bioremediation in the field. Stability tests on the monomeric tetravalent uranium (U(IV)) produced by bioremediation are needed in order to assess the efficacy of acetate-stimulation bioremediation.« less

Health effects of uranium: new research findings.

PubMed

Brugge, Doug; Buchner, Virginia

2011-01-01

Recent plans for a nuclear renaissance in both established and emerging economies have prompted increased interest in uranium mining. With the potential for more uranium mining worldwide and a growth in the literature on the toxicology and epidemiology of uranium and uranium mining, we found it timely to review the current state of knowledge. Here, we present a review of the health effects of uranium mining, with an emphasis on newer findings (2005-2011). Uranium mining can contaminate air, water, and soil. The chemical toxicity of the metal constitutes the primary environmental health hazard, with the radioactivity of uranium a secondary concern. The update of the toxicologic evidence on uranium adds to the established findings regarding nephrotoxicity, genotoxicity, and developmental defects. Additional novel toxicologic findings, including some at the molecular level, are now emerging that raise the biological plausibility of adverse effects on the brain, on reproduction, including estrogenic effects, on gene expression, and on uranium metabolism. Historically, most epidemiology on uranium mining has focused on mine workers and radon exposure. Although that situation is still overwhelmingly true, a smaller emerging literature has begun to form around environmental exposure in residential areas near uranium mining and processing facilities. We present and critique such studies. Clearly, more epidemiologic research is needed to contribute to causal inference. As much damage is irreversible, and possibly cumulative, present efforts must be vigorous to limit environmental uranium contamination and exposure.

Rhizofiltration using sunflower (Helianthus annuus L.) and bean (Phaseolus vulgaris L. var. vulgaris) to remediate uranium contaminated groundwater.

PubMed

Lee, Minhee; Yang, Minjune

2010-01-15

The uranium removal efficiencies of rhizofiltration in the remediation of groundwater were investigated in lab-scale experiments. Sunflower (Helianthus annuus L.) and bean (Phaseolus vulgaris L. var. vulgaris) were cultivated and an artificially uranium contaminated solution and three genuine groundwater samples were used in the experiments. More than 80% of the initial uranium in solution and genuine groundwater, respectively, was removed within 24h by using sunflower and the residual uranium concentration of the treated water was lower than 30 microg/L (USEPA drinking water limit). For bean, the uranium removal efficiency of the rhizofiltration was roughly 60-80%. The maximum uranium removal via rhizofiltration for the two plant cultivars occurred at pH 3-5 of solution and their uranium removal efficiencies exceeded 90%. The lab-scale continuous rhizofiltration clean-up system delivered over 99% uranium removal efficiency, and the results of SEM and EDS analyses indicated that most uranium accumulated in the roots of plants. The present results suggested that the uranium removal capacity of two plants evaluated in the clean-up system was about 25mg/kg of wet plant mass. Notably, the removal capacity of the root parts only was more than 500 mg/kg.

SOLVENT EXTRACTION PROCESS FOR URANIUM RECOVERY

DOEpatents

Clark, H.M.; Duffey, D.

1958-06-17

A process is described for extracting uranium from uranium ore, wherein the uranium is substantially free from molybdenum contamination. In a solvent extraction process for recovering uranium, uranium and molybdenum ions are extracted from the ore with ether under high acidity conditions. The ether phase is then stripped with water at a lower controiled acidity, resaturated with salting materials such as sodium nitrate, and reextracted with the separation of the molybdenum from the uranium without interference from other metals that have been previously extracted.

Microbial links between sulfate reduction and metal retention in uranium- and heavy metal-contaminated soil.

PubMed

Sitte, Jana; Akob, Denise M; Kaufmann, Christian; Finster, Kai; Banerjee, Dipanjan; Burkhardt, Eva-Maria; Kostka, Joel E; Scheinost, Andreas C; Büchel, Georg; Küsel, Kirsten

2010-05-01

Sulfate-reducing bacteria (SRB) can affect metal mobility either directly by reductive transformation of metal ions, e.g., uranium, into their insoluble forms or indirectly by formation of metal sulfides. This study evaluated in situ and biostimulated activity of SRB in groundwater-influenced soils from a creek bank contaminated with heavy metals and radionuclides within the former uranium mining district of Ronneburg, Germany. In situ activity of SRB, measured by the (35)SO(4)(2-) radiotracer method, was restricted to reduced soil horizons with rates of < or =142 +/- 20 nmol cm(-3) day(-1). Concentrations of heavy metals were enriched in the solid phase of the reduced horizons, whereas pore water concentrations were low. X-ray absorption near-edge structure (XANES) measurements demonstrated that approximately 80% of uranium was present as reduced uranium but appeared to occur as a sorbed complex. Soil-based dsrAB clone libraries were dominated by sequences affiliated with members of the Desulfobacterales but also the Desulfovibrionales, Syntrophobacteraceae, and Clostridiales. [(13)C]acetate- and [(13)C]lactate-biostimulated soil microcosms were dominated by sulfate and Fe(III) reduction. These processes were associated with enrichment of SRB and Geobacteraceae; enriched SRB were closely related to organisms detected in soils by using the dsrAB marker. Concentrations of soluble nickel, cobalt, and occasionally zinc declined < or =100% during anoxic soil incubations. In contrast to results in other studies, soluble uranium increased in carbon-amended treatments, reaching < or =1,407 nM in solution. Our results suggest that (i) ongoing sulfate reduction in contaminated soil resulted in in situ metal attenuation and (ii) the fate of uranium mobility is not predictable and may lead to downstream contamination of adjacent ecosystems.

Microbial Links between Sulfate Reduction and Metal Retention in Uranium- and Heavy Metal-Contaminated Soil▿

PubMed Central

Sitte, Jana; Akob, Denise M.; Kaufmann, Christian; Finster, Kai; Banerjee, Dipanjan; Burkhardt, Eva-Maria; Kostka, Joel E.; Scheinost, Andreas C.; Büchel, Georg; Küsel, Kirsten

2010-01-01

Sulfate-reducing bacteria (SRB) can affect metal mobility either directly by reductive transformation of metal ions, e.g., uranium, into their insoluble forms or indirectly by formation of metal sulfides. This study evaluated in situ and biostimulated activity of SRB in groundwater-influenced soils from a creek bank contaminated with heavy metals and radionuclides within the former uranium mining district of Ronneburg, Germany. In situ activity of SRB, measured by the 35SO42− radiotracer method, was restricted to reduced soil horizons with rates of ≤142 ± 20 nmol cm−3 day−1. Concentrations of heavy metals were enriched in the solid phase of the reduced horizons, whereas pore water concentrations were low. X-ray absorption near-edge structure (XANES) measurements demonstrated that ∼80% of uranium was present as reduced uranium but appeared to occur as a sorbed complex. Soil-based dsrAB clone libraries were dominated by sequences affiliated with members of the Desulfobacterales but also the Desulfovibrionales, Syntrophobacteraceae, and Clostridiales. [13C]acetate- and [13C]lactate-biostimulated soil microcosms were dominated by sulfate and Fe(III) reduction. These processes were associated with enrichment of SRB and Geobacteraceae; enriched SRB were closely related to organisms detected in soils by using the dsrAB marker. Concentrations of soluble nickel, cobalt, and occasionally zinc declined ≤100% during anoxic soil incubations. In contrast to results in other studies, soluble uranium increased in carbon-amended treatments, reaching ≤1,407 nM in solution. Our results suggest that (i) ongoing sulfate reduction in contaminated soil resulted in in situ metal attenuation and (ii) the fate of uranium mobility is not predictable and may lead to downstream contamination of adjacent ecosystems. PMID:20363796

Studying Legacy Uranium Contamination On Navajo, Laguna, and Isleta Lands In Collaboration With Native American Undergraduate Researchers

NASA Astrophysics Data System (ADS)

Cadol, D. D.; Frey, B.; Chee, C.

2017-12-01

Personally relevant research experiences at key points in a student's education are potentially powerful influences on their long-term career path. With this in mind, New Mexico EPSCoR created the STEM Advancement Program (STEMAP) to provide a summer research experience for students from the non-graduate-degree granting institutions in New Mexico. Recruitment focused on underrepresented minorities, primarily Native American and Hispanic students, who applied to work with one of six research components. Our research component focused on understanding the fate and transport of environmental uranium in the Four Corners region. The geosciences are especially amenable to providing meaningful research experiences, particularly for groups that have a strong cultural connection with the land. Uranium mining activities were extensive on several reservations in the 1950s to 1980s, and many of the sites have not been remediated. The impact of mining likely contributed to the high interest among Native American (especially Navajo) STEMAP applicants in this research topic. In four years of summer research we mentored four Native American students (two male and two female) and one white non-Hispanic female. Following their work in our research group, one student extended her research, three graduated, and one transferred to a research institution. This success likely reflects a combination of recruitment efforts, which built on community connections, as well as efforts to provide personal mentoring and to create an inclusive environment. The work of these students has advanced our understanding of fluvial transport of uranium from inactive mining districts, an important pathway given the role of these streams in providing water for agriculture and aggregate for construction. Findings demonstrate an affinity of uranium to sorb to fine-grained sediment, meaning standing water in stock ponds is of particular concern. The students also studied uranium-bearing dust generated from legacy sites, documenting dissolution of uranium in two contrasting simulated lung fluids. Student presentations in the affected communities closed the communication loop, presenting findings in an accessible format. Ideally these presentations also planted seeds of interest in the geosciences for younger community members.

Cholesterol 7alpha-hydroxylase (CYP7A1) activity is modified after chronic ingestion of depleted uranium in the rat.

PubMed

Racine, R; Grandcolas, L; Grison, S; Stefani, J; Delissen, O; Gourmelon, P; Veyssière, G; Souidi, M

2010-05-01

Depleted uranium (DU) is a radioactive heavy metal derived from the nuclear energy production. Its wide use in civilian and military items increases the risk of its environmental dissemination, and thus the risk of internal contamination of populations living in such contaminated territories. Previous studies have shown that vitamin D and cerebral cholesterol metabolisms were affected following chronic ingestion of DU. Even more than the brain, the liver is a crucial organ in cholesterol homeostasis since it regulates cholesterol distribution and elimination at body level. The aim of this work was to assess the impact of a low-level chronic ingestion of DU on hepatic cholesterol metabolism. Rats were contaminated with DU in their drinking water at a concentration of 40mg/l for 9 months. The major effect induced by DU was a decrease of CYP7A1 specific activity (-60%) correlated with a matching decrease of its product 7alpha-hydroxycholesterol in the plasma. Hepatic gene expression of transporters ABC A1, ABC G5, ABC G8 and of nuclear receptor RXR was increased, whereas that of catabolism enzyme CYP7B1 was decreased. Thus, after a chronic ingestion of DU, rats experience a modulation of cholesterol catabolism but overcome it, since their cholesterolemia is preserved and no pathology is declared.

49 CFR 173.420 - Uranium hexafluoride (fissile, fissile excepted and non-fissile).

Code of Federal Regulations, 2014 CFR

2014-10-01

... 49 Transportation 2 2014-10-01 2014-10-01 false Uranium hexafluoride (fissile, fissile excepted....420 Uranium hexafluoride (fissile, fissile excepted and non-fissile). (a) In addition to any other... non-fissile uranium hexafluoride must be offered for transportation as follows: (1) Before initial...

49 CFR 173.420 - Uranium hexafluoride (fissile, fissile excepted and non-fissile).

Code of Federal Regulations, 2011 CFR

2011-10-01

... 49 Transportation 2 2011-10-01 2011-10-01 false Uranium hexafluoride (fissile, fissile excepted....420 Uranium hexafluoride (fissile, fissile excepted and non-fissile). (a) In addition to any other... non-fissile uranium hexafluoride must be offered for transportation as follows: (1) Before initial...

49 CFR 173.420 - Uranium hexafluoride (fissile, fissile excepted and non-fissile).

Code of Federal Regulations, 2012 CFR

2012-10-01

... 49 Transportation 2 2012-10-01 2012-10-01 false Uranium hexafluoride (fissile, fissile excepted....420 Uranium hexafluoride (fissile, fissile excepted and non-fissile). (a) In addition to any other... non-fissile uranium hexafluoride must be offered for transportation as follows: (1) Before initial...

49 CFR 173.420 - Uranium hexafluoride (fissile, fissile excepted and non-fissile).

Code of Federal Regulations, 2013 CFR

2013-10-01

... 49 Transportation 2 2013-10-01 2013-10-01 false Uranium hexafluoride (fissile, fissile excepted....420 Uranium hexafluoride (fissile, fissile excepted and non-fissile). (a) In addition to any other... non-fissile uranium hexafluoride must be offered for transportation as follows: (1) Before initial...

49 CFR 173.420 - Uranium hexafluoride (fissile, fissile excepted and non-fissile).

Code of Federal Regulations, 2010 CFR

2010-10-01

... 49 Transportation 2 2010-10-01 2010-10-01 false Uranium hexafluoride (fissile, fissile excepted....420 Uranium hexafluoride (fissile, fissile excepted and non-fissile). (a) In addition to any other... non-fissile uranium hexafluoride must be offered for transportation as follows: (1) Before initial...

49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

Code of Federal Regulations, 2011 CFR

2011-10-01

... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U present...

49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

Code of Federal Regulations, 2010 CFR

2010-10-01

... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U present...

Subsurface Conditions Controlling Uranium Incorporation in Iron Oxides: A Redox Stable Sink

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fendorf, Scott

2016-04-05

Toxic metals and radionuclides throughout the U.S. Department of Energy Complex pose a serious threat to ecosystems and to human health. Of particular concern is the redox-sensitive radionuclide uranium, which is classified as a priority pollutant in soils and groundwaters at most DOE sites owing to its large inventory, its health risks, and its mobility with respect to primary waste sources. The goal of this research was to contribute to the long-term mission of the Subsurface Biogeochemistry Program by determining reactions of uranium with iron (hydr)oxides that lead to long-term stabilization of this pervasive contaminant. The research objectives of thismore » project were thus to (1) identify the (bio)geochemical conditions, including those of the solid-phase, promoting uranium incorporation in Fe (hydr)oxides, (2) determine the magnitude of uranium incorporation under a variety of relevant subsurface conditions in order to quantify the importance of this pathway when in competition with reduction or adsorption; (3) identify the mechanism(s) of U(VI/V) incorporation in Fe (hydr)oxides; and (4) determine the stability of these phases under different biogeochemical (inclusive of redox) conditions. Our research demonstrates that redox transformations are capable of achieving U incorporation into goethite at ambient temperatures, and that this transformation occurs within days at U and Fe(II) concentrations that are common in subsurface geochemical environments with natural ferrihydrites—inclusive of those with natural impurities. Increasing Fe(II) or U concentration, or initial pH, made U(VI) reduction to U(IV) a more competitive sequestration pathway in this system, presumably by increasing the relative rate of U reduction. Uranium concentrations commonly found in contaminated subsurface environments are often on the order of 1-10 μM, and groundwater Fe(II) concentrations can reach exceed 1 mM in reduced zones of the subsurface. The redox-driven U(V) incorporation mechanism may help to explain U retention in some geologic materials, improving our understanding of U-based geochronology and the redox status of ancient geochemical environments. Additionally, U(VI) may be incorporated within silicate minerals though encapsulation of U-bearing iron oxides, leading to a redox stable solid. Our research detailing previously unrecognized mechanism of U incorporation within sediment minerals may even lead to new approaches for in situ contamination remediation techniques, and will help refine models of U fate and transport in reduced subsurface zones.« less

40 CFR 192.10 - Applicability.

Code of Federal Regulations, 2013 CFR

2013-07-01

... AND ENVIRONMENTAL PROTECTION STANDARDS FOR URANIUM AND THORIUM MILL TAILINGS Standards for Cleanup of Land and Buildings Contaminated with Residual Radioactive Materials from Inactive Uranium Processing... radioactive materials at which all or substantially all of the uranium was produced for sale to any Federal...

40 CFR 192.10 - Applicability.

Code of Federal Regulations, 2014 CFR

2014-07-01

... AND ENVIRONMENTAL PROTECTION STANDARDS FOR URANIUM AND THORIUM MILL TAILINGS Standards for Cleanup of Land and Buildings Contaminated with Residual Radioactive Materials from Inactive Uranium Processing... radioactive materials at which all or substantially all of the uranium was produced for sale to any Federal...

Uranium Mines and Mills | RadTown USA | US EPA

EPA Pesticide Factsheets

2017-08-07

Uranium is used as nuclear fuel for electric power generation. U.S. mining industries can obtain uranium in two ways: mining or milling. Mining waste and mill tailings can contaminate water, soil and air if not disposed of properly.

Persistence of uranium groundwater plumes: contrasting mechanisms at two DOE sites in the groundwater-river interaction zone.

PubMed

Zachara, John M; Long, Philip E; Bargar, John; Davis, James A; Fox, Patricia; Fredrickson, Jim K; Freshley, Mark D; Konopka, Allan E; Liu, Chongxuan; McKinley, James P; Rockhold, Mark L; Williams, Kenneth H; Yabusaki, Steve B

2013-04-01

We examine subsurface uranium (U) plumes at two U.S. Department of Energy sites that are located near large river systems and are influenced by groundwater-river hydrologic interaction. Following surface excavation of contaminated materials, both sites were projected to naturally flush remnant uranium contamination to levels below regulatory limits (e.g., 30 μg/L or 0.126 μmol/L; U.S. EPA drinking water standard), with 10 years projected for the Hanford 300 Area (Columbia River) and 12 years for the Rifle site (Colorado River). The rate of observed uranium decrease was much lower than expected at both sites. While uncertainty remains, a comparison of current understanding suggests that the two sites have common, but also different mechanisms controlling plume persistence. At the Hanford 300 A, the persistent source is adsorbed U(VI) in the vadose zone that is released to the aquifer during spring water table excursions. The release of U(VI) from the vadose zone and its transport within the oxic, coarse-textured aquifer sediments is dominated by kinetically-limited surface complexation. Modeling implies that annual plume discharge volumes to the Columbia River are small (

Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater-river interaction zone

NASA Astrophysics Data System (ADS)

Zachara, John M.; Long, Philip E.; Bargar, John; Davis, James A.; Fox, Patricia; Fredrickson, Jim K.; Freshley, Mark D.; Konopka, Allan E.; Liu, Chongxuan; McKinley, James P.; Rockhold, Mark L.; Williams, Kenneth H.; Yabusaki, Steve B.

2013-04-01

We examine subsurface uranium (U) plumes at two U.S. Department of Energy sites that are located near large river systems and are influenced by groundwater-river hydrologic interaction. Following surface excavation of contaminated materials, both sites were projected to naturally flush remnant uranium contamination to levels below regulatory limits (e.g., 30 μg/L or 0.126 μmol/L; U.S. EPA drinking water standard), with 10 years projected for the Hanford 300 Area (Columbia River) and 12 years for the Rifle site (Colorado River). The rate of observed uranium decrease was much lower than expected at both sites. While uncertainty remains, a comparison of current understanding suggests that the two sites have common, but also different mechanisms controlling plume persistence. At the Hanford 300 A, the persistent source is adsorbed U(VI) in the vadose zone that is released to the aquifer during spring water table excursions. The release of U(VI) from the vadose zone and its transport within the oxic, coarse-textured aquifer sediments is dominated by kinetically-limited surface complexation. Modeling implies that annual plume discharge volumes to the Columbia River are small (< one pore volume). At the Rifle site, slow oxidation of naturally reduced, contaminant U(IV) in the saturated zone and a continuous influx of U(VI) from natural, up-gradient sources influence plume persistence. Rate-limited mass transfer and surface complexation also control U(VI) migration velocity in the sub-oxic Rifle groundwater. Flux of U(VI) from the vadose zone at the Rifle site may be locally important, but it is not the dominant process that sustains the plume. A wide range in microbiologic functional diversity exists at both sites. Strains of Geobacter and other metal reducing bacteria are present at low natural abundance that are capable of enzymatic U(VI) reduction in localized zones of accumulated detrital organic carbon or after organic carbon amendment. Major differences between the sites include the geochemical nature of residual, contaminant U; the rates of current kinetic processes (both biotic and abiotic) influencing U(VI) solid-liquid distribution; the presence of detrital organic matter and the resulting spatial heterogeneity in microbially-driven redox properties; and the magnitude of groundwater hydrologic dynamics controlled by river-stage fluctuations, geologic structures, and aquifer hydraulic properties. The comparative analysis of these sites provides important guidance to the characterization, understanding, modeling, and remediation of groundwater contaminant plumes influenced by surface water interaction that are common world-wide.

Hydrogeology, Water Chemistry, and Factors Affecting the Transport of Contaminants in the Zone of Contribution of a Public-Supply Well in Modesto, Eastern San Joaquin Valley, California

USGS Publications Warehouse

Jurgens, Bryant C.; Burow, Karen R.; Dalgish, Barbara A.; Shelton, Jennifer L.

2008-01-01

Ground-water chemistry in the zone of contribution of a public-supply well in Modesto, California, was studied by the U.S. Geological Survey National Water Quality Assessment (NAWQA) Program's topical team for Transport of Anthropogenic and Natural Contaminants (TANC) to supply wells. Twenty-three monitoring wells were installed in Modesto to record baseline hydraulic information and to collect water-quality samples. The monitoring wells were divided into four categories that represent the chemistry of different depths and volumes of the aquifer: (1) water-table wells were screened between 8.5 and 11.7 m (meter) (28 and 38.5 ft [foot]) below land surface (bls) and were within 5 m (16 ft) of the water table; (2) shallow wells were screened between 29 and 35 m (95 and 115 ft) bls; (3) intermediate wells were screened between 50.6 and 65.5 m (166 and 215 ft) bls; and (4) deep wells are screened between 100 to 106 m (328 and 348 ft) bls. Inorganic, organic, isotope, and age-dating tracers were used to characterize the geochemical conditions in the aquifer and understand the mechanisms of mobilization and movement of selected constituents from source areas to a public-supply well. The ground-water system within the study area has been significantly altered by human activities. Water levels in monitoring wells indicated that horizontal movement of ground water was generally from the agricultural areas in the northeast towards a regional water-level depression within the city in the southwest. However, intensive pumping and irrigation recharge in the study area has caused large quantities of ground water to move vertically downward within the regional and local flow systems. Analysis of age tracers indicated that ground-water age varied from recent recharge at the water table to more than 1,000 years in the deep part of the aquifer. The mean age of shallow ground water was determined to be between 30 and 40 years. Intermediate ground water was determined to be a mixture of modern (Post-1950) and old (Pre-1950) ground water. As a result, concentrations of age tracers were detectable but diluted by older ground water. Deep ground water generally represented water that was recharged under natural conditions and therefore had much older ages. Ground water reaching the public-supply well was a mixture of older intermediate and deep ground water and young shallow ground water that has been anthropogenically-influenced to a greater extent than intermediate ground water. Uranium and nitrate pose the most significant threat to the quality of water discharged from the public-supply well. Although pesticides and VOCs were present in ground water from the public-supply well and monitoring wells, currently concentrations of these contaminants are generally less than one-hundredth the concentration of drinking water standards. In contrast, both uranium and nitrate were above half the concentration of drinking water standards for public-supply well samples, and were above drinking water standards for several water-table and shallow monitoring wells. Shallow ground water contributes roughly 20 percent of the total flow to the public-supply well and was the entry point of most contaminants reaching the public-supply well. Naturally-occurring uranium, which is commonly adsorbed to aquifer sediments, was mobilized by oxygen-rich, high-alkalinity water, causing concentrations in some monitoring wells to be above the drinking-water standard of 30 ug/L (microgram per liter). Adsorption experiments, sediment extractions, and uranium isotopes indicated uranium in water-table and shallow ground water was leached from aquifer sediments. Uranium is strongly correlated to bicarbonate concentrations (as measured by alkalinity) in ground water. Bicarbonate can effectively limit uranium adsorption to sediments. As a result, continued downward movement of high-alkalinity, oxygen-rich ground water will likely lead to larger portions of the aquifer having

Hydrogeochemical and stream sediment reconnaissance basic data for Brownsville-McAllen NTMS Quadrangles, Texas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1980-09-30

Results of a reconnaissance geochemical survey of the Brownsville-McAllen Quadrangles, Texas are reported. Field and laboratory data are presented for 427 groundwater and 171 stream sediment samples. Statistical and areal distributions of uranium and possible uranium-related variables are displayed. Pertinent geologic factors which may be of significance in evaluating the potential for uranium mineralization are briefly discussed. Groundwater data indicate the most promising area for potential uranium mineralization occurs in the northwestern section of the quadrangles (Jim Hogg, Starr, and Zapata Counties), where waters are derived from the Catahoula Formation. These groundwaters have high concentrations of uranium, uranium associated elements,more » and low values for specific conductance. Another area with high uranium concentrations is in the southeastern portion of the survey area (Hidalgo, Cameron, and Willacy Counties). Shallow wells <10 m (30 ft) are numerous in this area and high specific conductance values may indicate contamination from extensive fertilization. Stream sediment data for the survey does not indicate an area favorable for uranium mineralization. Anomalous acid soluble uranium values in the southeastern area (Hidalgo, Cameron, and Willacy Counties) can be attributed to phosphate fertilizer contamination. Four samples in the western part of the area (western Starr County) have anomalously high total uranium values and low acid soluble uranium values, indicating the uranium may be contained in resistate minerals.« less

Geochemical investigation of UMTRAP designated site at Durango, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Markos, G.; Bush, K.J.

1983-09-01

This report is the result of a geochemical investigation of the former uranium mill and tailings site at Durango, Colorado. This is one in a series of site specific geochemical investigations performed on the inactive uranium mill tailings included in the UMTRA Project. The objectives of the investigation are to characterize the geochemistry, to determine the contaminant distribution resulting from the former milling activities and tailings, and to infer chemical pathways and transport mechanisms from the contaminant distribution. The results will be used to model contaminant migration and to develop criteria for long-term containment media such as a cover systemmore » which is impermeable to contaminant migration. This report assumes a familiarity with the hydrologic conditions of the site and the geochemical concepts underlying the investigation. The results reported are based on a one-time sampling of waters and solid material from the background, the area adjacent to the site, and the site. The solid samples are water extracted remove easily soluble salts and acids extracted to remove cabonates and hydroxides. The water extracts and solid samples were analyzed for the major and trace elements. A limited number of samples were analyzed for radiological components. The report includes the methods of sampling, sample processing, analysis, and data interpretation. Three major conclusions are: (1) carbonate salts and low TDS characterize the tailings; (2) the adjacent area and raffinate ponds contain contaminants deposited by a single event of fluid permeation of the soils; and (3) the Animas River adjacent to the site has elevated gross alpha activity attributed to /sup 226/Ra in the sediments derived from the tailings or milling activities.« less

PROCESS OF PURIFYING URANIUM

DOEpatents

Seaborg, G.T.; Orlemann, E.F.; Jensen, L.H.

1958-12-23

A method of obtaining substantially pure uranium from a uranium composition contaminated with light element impurities such as sodium, magnesium, beryllium, and the like is described. An acidic aqueous solution containing tetravalent uranium is treated with a soluble molybdate to form insoluble uranous molybdate which is removed. This material after washing is dissolved in concentrated nitric acid to obtaln a uranyl nitrate solution from which highly purified uranium is obtained by extraction with ether.

REMOVAL OF URANIUM FROM DRINKING WATER BY CONVENTIONAL TREATMENT METHODS

EPA Science Inventory

The USEPA currently does not regulate uranium in drinking water but will be revising the radionuclide regulations during 1989 and will propose a maximum contaminant level for uranium. The paper presents treatment technology information on the effectiveness of conventional method...

Metabolomics identifies a biological response to chronic low-dose natural uranium contamination in urine samples.

PubMed

Grison, Stéphane; Favé, Gaëlle; Maillot, Matthieu; Manens, Line; Delissen, Olivia; Blanchardon, Eric; Banzet, Nathalie; Defoort, Catherine; Bott, Romain; Dublineau, Isabelle; Aigueperse, Jocelyne; Gourmelon, Patrick; Martin, Jean-Charles; Souidi, Maâmar

2013-01-01

Because uranium is a natural element present in the earth's crust, the population may be chronically exposed to low doses of it through drinking water. Additionally, the military and civil uses of uranium can also lead to environmental dispersion that can result in high or low doses of acute or chronic exposure. Recent experimental data suggest this might lead to relatively innocuous biological reactions. The aim of this study was to assess the biological changes in rats caused by ingestion of natural uranium in drinking water with a mean daily intake of 2.7 mg/kg for 9 months and to identify potential biomarkers related to such a contamination. Subsequently, we observed no pathology and standard clinical tests were unable to distinguish between treated and untreated animals. Conversely, LC-MS metabolomics identified urine as an appropriate biofluid for discriminating the experimental groups. Of the 1,376 features detected in urine, the most discriminant were metabolites involved in tryptophan, nicotinate, and nicotinamide metabolic pathways. In particular, N -methylnicotinamide, which was found at a level seven times higher in untreated than in contaminated rats, had the greatest discriminating power. These novel results establish a proof of principle for using metabolomics to address chronic low-dose uranium contamination. They open interesting perspectives for understanding the underlying biological mechanisms and designing a diagnostic test of exposure.

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reinoso-Maset, Estela; Steefel, Carl I.; Um, Wooyong

Uranyl oxyhydroxide minerals are important weathering products in uranium-contaminated surface and subsurface environments that regulate dissolved uranium concentrations. However, dissolution rates for this class of minerals and associated dissolution mechanisms have not been previously reported for circumneutral pH conditions, particularly for the case of flow through porous media. In this paper, the dissolution rates of K- and Na-compreignacite (K 2(UO 2) 6O 4(OH) 6·8H 2O and Na 2(UO 2) 6O 4(OH) 6·8H 2O respectively) were measured using flow-through columns reacted with two simulated background porewater (BPW) solutions of low and high dissolved total carbonate content (ca. 0.2 and 2.8 mmolmore » L -1). Column materials were characterized before and after reaction with electron microscopy, bulk chemistry, and EXAFS to identify structural and chemical changes during dissolution and to obtain insight into molecular-scale processes. The reactive transport code CrunchFlow was used to calculate overall dissolution rates while accounting for fluid transport and changes in mineral volume and reactive surface area and results were compared to steady-state dissolution rate calculations. In low carbonate BPW systems, interlayer K and Na were initially leached from both minerals, and in Na-compreignacite, K and minor divalent cations from the input solution were incorporated into the mineral structure. Results of characterization analyses suggested that after reaction both K- and Na-compreignacite resembled a disordered K-compreignacite with altered surfaces. A 10-fold increase in dissolved carbonate concentration and corresponding increase in pH (from 6.65 to 8.40) resulted in a net removal of 58-87% of total uranium mass from the columns, compared to <1% net loss in low carbonate BPW systems. Steady-state release of dissolved uranium was not observed with high carbonate solutions and post-reaction characterizations indicated a lack of development of leached or altered surfaces. Dissolution rates (normalized to specific surface area) were about 2.5-3 orders-of-magnitude faster in high versus low carbonate BPW systems, with Na-compreignacite dissolving more rapidly than K-compreignacite under both BPW conditions, possibly due to greater ion exchange (1.57·10 -10 vs. 1.28·10 -13 mol m -2 s -1 [log R = -9.81 and -12.89] and 5.79·10 -10 vs. 3.71·10 -13 mol m -2 s -1 [log R = -9.24 and -12.43] for K- and Na-compreignacite respectively). Experimental and spectroscopic results suggest that the dissolution rate is controlled by bond breaking of a uranyl group and detachment from polyhedral layers of the mineral structure. With higher dissolved carbonate concentrations, this rate-determining step is accelerated by the formation of Ca-uranyl carbonate complexes (dominant species under these conditions), which resulted in an increase of the dissolution rates. Optimization of both dissolution rate and mineral volume fraction in the reactive transport model to account for uranium mass removal during dissolution more accurately reproduced effluent data in high carbonate systems, and resulted in faster overall rates compared with a steady-state dissolution assumption. Finally, this study highlights the importance of coupling reaction and transport processes during the quantification of mineral dissolution rates to accurately predict the fate of contaminants such as uranium in porous geomedia.« less

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

DOE PAGES

Reinoso-Maset, Estela; Steefel, Carl I.; Um, Wooyong; ...

2017-06-01

Uranyl oxyhydroxide minerals are important weathering products in uranium-contaminated surface and subsurface environments that regulate dissolved uranium concentrations. However, dissolution rates for this class of minerals and associated dissolution mechanisms have not been previously reported for circumneutral pH conditions, particularly for the case of flow through porous media. In this paper, the dissolution rates of K- and Na-compreignacite (K 2(UO 2) 6O 4(OH) 6·8H 2O and Na 2(UO 2) 6O 4(OH) 6·8H 2O respectively) were measured using flow-through columns reacted with two simulated background porewater (BPW) solutions of low and high dissolved total carbonate content (ca. 0.2 and 2.8 mmolmore » L -1). Column materials were characterized before and after reaction with electron microscopy, bulk chemistry, and EXAFS to identify structural and chemical changes during dissolution and to obtain insight into molecular-scale processes. The reactive transport code CrunchFlow was used to calculate overall dissolution rates while accounting for fluid transport and changes in mineral volume and reactive surface area and results were compared to steady-state dissolution rate calculations. In low carbonate BPW systems, interlayer K and Na were initially leached from both minerals, and in Na-compreignacite, K and minor divalent cations from the input solution were incorporated into the mineral structure. Results of characterization analyses suggested that after reaction both K- and Na-compreignacite resembled a disordered K-compreignacite with altered surfaces. A 10-fold increase in dissolved carbonate concentration and corresponding increase in pH (from 6.65 to 8.40) resulted in a net removal of 58-87% of total uranium mass from the columns, compared to <1% net loss in low carbonate BPW systems. Steady-state release of dissolved uranium was not observed with high carbonate solutions and post-reaction characterizations indicated a lack of development of leached or altered surfaces. Dissolution rates (normalized to specific surface area) were about 2.5-3 orders-of-magnitude faster in high versus low carbonate BPW systems, with Na-compreignacite dissolving more rapidly than K-compreignacite under both BPW conditions, possibly due to greater ion exchange (1.57·10 -10 vs. 1.28·10 -13 mol m -2 s -1 [log R = -9.81 and -12.89] and 5.79·10 -10 vs. 3.71·10 -13 mol m -2 s -1 [log R = -9.24 and -12.43] for K- and Na-compreignacite respectively). Experimental and spectroscopic results suggest that the dissolution rate is controlled by bond breaking of a uranyl group and detachment from polyhedral layers of the mineral structure. With higher dissolved carbonate concentrations, this rate-determining step is accelerated by the formation of Ca-uranyl carbonate complexes (dominant species under these conditions), which resulted in an increase of the dissolution rates. Optimization of both dissolution rate and mineral volume fraction in the reactive transport model to account for uranium mass removal during dissolution more accurately reproduced effluent data in high carbonate systems, and resulted in faster overall rates compared with a steady-state dissolution assumption. Finally, this study highlights the importance of coupling reaction and transport processes during the quantification of mineral dissolution rates to accurately predict the fate of contaminants such as uranium in porous geomedia.« less

Proteome changes in rat serum after a chronic ingestion of enriched uranium: Toward a biological signature of internal contamination and radiological effect.

PubMed

Petitot, F; Frelon, S; Chambon, C; Paquet, F; Guipaud, O

2016-08-22

The civilian and military use of uranium results in an increased risk of human exposure. The toxicity of uranium results from both its chemical and radiological properties that vary with isotopic composition. Validated biomarkers of health effects associated with exposure to uranium are neither sensitive nor specific to uranium radiotoxicity and/or radiological effect. This study aimed at investigating if serum proteins could be useful as biomarkers of both uranium exposure and radiological effect. Male Sprague-Dawley rats were chronically exposed through drinking water to low levels (40mg/L, corresponding to 1mg of uranium per animal per day) of either 4% (235)U-enriched uranium (EU) or 12% EU during 6 weeks. A proteomics approach based on two-dimensional electrophoresis (2D-DIGE) and mass spectrometry (MS) was used to establish protein expression profiles that could be relevant for discriminating between groups, and to identify some differentially expressed proteins following uranium ingestion. It demonstrated that the expressions of 174 protein spots over 1045 quantified spots were altered after uranium exposure (p<0.05). Using both inferential and non-supervised multivariate statistics, we show sets of spots features that lead to a clear discrimination between controls and EU exposed groups on the one hand (21 spots), and between 4% EU and 12% EU on the other hand (7 spots), showing that investigation of the serum proteome may possibly be of relevance to address both uranium contamination and radiological effect. Finally, using bioinformatics tools, pathway analyses of differentially expressed MS-identified proteins find that acute phase, inflammatory and immune responses as well as oxidative stress are likely involved in the response to contamination, suggesting a physiological perturbation, but that does not necessarily lead to a toxic effect. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

Evaluation of Using Caged Clams to Monitor Contaminated Groundwater Exposure in the Near-Shore Environment of the Hanford Site 300 Area

DOE Office of Scientific and Technical Information (OSTI.GOV)

Larson, Kyle B.; Poston, Ted M.; Tiller, Brett L.

2008-01-31

The Asiatic clam (Corbicula fluminea) has been identified as an indicator species for locating and monitoring contaminated groundwater in the Columbia River. Pacific Northwest National Laboratory conducted a field study to explore the use of caged Asiatic clams to monitor contaminated groundwater upwelling in the 300 Area near-shore environment and assess seasonal differences in uranium uptake in relation to seasonal flow regimes of the Columbia River. Additional objectives included examining the potential effects of uranium accumulation on growth, survival, and tissue condition of the clams. This report documents the field conditions and procedures, laboratory procedures, and statistical analyses used inmore » collecting samples and processing the data. Detailed results are presented and illustrated, followed by a discussion comparing uranium concentrations in Asiatic clams collected at the 300 Area and describing the relationship between river discharge, groundwater indicators, and uranium in clams. Growth and survival, histology, and other sources of environmental variation also are discussed.« less

Upscaling of U (VI) desorption and transport from decimeter‐scale heterogeneity to plume‐scale modeling

USGS Publications Warehouse

Curtis, Gary P.; Kohler, Matthias; Kannappan, Ramakrishnan; Briggs, Martin A.; Day-Lewis, Frederick D.

2015-01-01

Scientifically defensible predictions of field scale U(VI) transport in groundwater requires an understanding of key processes at multiple scales. These scales range from smaller than the sediment grain scale (less than 10 μm) to as large as the field scale which can extend over several kilometers. The key processes that need to be considered include both geochemical reactions in solution and at sediment surfaces as well as physical transport processes including advection, dispersion, and pore-scale diffusion. The research summarized in this report includes both experimental and modeling results in batch, column and tracer tests. The objectives of this research were to: (1) quantify the rates of U(VI) desorption from sediments acquired from a uranium contaminated aquifer in batch experiments;(2) quantify rates of U(VI) desorption in column experiments with variable chemical conditions, and(3) quantify nonreactive tracer and U(VI) transport in field tests.

Groundwater contamination from an inactive uranium mill tailings pile: 2. Application of a dynamic mixing model

NASA Astrophysics Data System (ADS)

Narasimhan, T. N.; White, A. F.; Tokunaga, T.

1986-12-01

At Riverton, Wyoming, low pH process waters from an abandoned uranium mill tailings pile have been infiltrating into and contaminating the shallow water table aquifer. The contamination process has been governed by transient infiltration rates, saturated-unsaturated flow, as well as transient chemical reactions between the many chemical species present in the mixing waters and the sediments. In the first part of this two-part series [White et al., 1984] we presented field data as well as an interpretation based on a static mixing model. As an upper bound, we estimated that 1.7% of the tailings water had mixed with the native groundwater. In the present work we present the results of numerical investigation of the dynamic mixing process. The model, DYNAMIX (DYNAmic MIXing), couples a chemical speciation algorithm, PHREEQE, with a modified form of the transport algorithm, TRUMP, specifically designed to handle the simultaneous migration of several chemical constituents. The overall problem of simulating the evolution and migration of the contaminant plume was divided into three sub problems that were solved in sequential stages. These were the infiltration problem, the reactive mixing problem, and the plume-migration problem. The results of the application agree reasonably with the detailed field data. The methodology developed in the present study demonstrates the feasibility of analyzing the evolution of natural hydrogeochemical systems through a coupled analysis of transient fluid flow as well as chemical reactions. It seems worthwhile to devote further effort toward improving the physicochemical capabilities of the model as well as to enhance its computational efficiency.

Groundwater contamination from an inactive uranium mill tailings pile. 2. Application of a dynamic mixing model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Narashimhan, T.N.; White, A.F.; Tokunaga, T.

1986-12-01

At Riverton, Wyoming, low pH process waters from an abandoned uranium mill tailings pile have been infiltrating into and contaminating the shallow water table aquifer. The contamination process has been governed by transient infiltration rates, saturated-unsaturated flow, as well as transient chemical reactions between the many chemical species present in the mixing waters and the sediments. In the first part of this two-part series the authors presented field data as well as an interpretation based on a static mixing models. As an upper bound, the authors estimated that 1.7% of the tailings water had mixed with the native groundwater. Inmore » the present work they present the results of numerical investigation of the dynamic mixing process. The model, DYNAMIX (DYNamic MIXing), couples a chemical speciation algorithm, PHREEQE, with a modified form of the transport algorithm, TRUMP, specifically designed to handle the simultaneous migration of several chemical constituents. The overall problem of simulating the evolution and migration of the contaminant plume was divided into three sub problems that were solved in sequential stages. These were the infiltration problem, the reactive mixing problem, and the plume-migration problem. The results of the application agree reasonably with the detailed field data. The methodology developed in the present study demonstrates the feasibility of analyzing the evolution of natural hydrogeochemical systems through a coupled analysis of transient fluid flow as well as chemical reactions. It seems worthwhile to devote further effort toward improving the physicochemical capabilities of the model as well as to enhance its computational efficiency.« less

Removal of uranium (VI) from aqueous systems by nanoscale zero-valent iron particles suspended in carboxy-methyl cellulose

NASA Astrophysics Data System (ADS)

Popescu (Hoştuc), Ioana-Carmen; Filip, Petru; Humelnicu, Doina; Humelnicu, Ionel; Scott, Thomas Bligh; Crane, Richard Andrew

2013-11-01

Carboxy-methyl-cellulose (CMC), a common "delivery vehicle" for the subsurface deployment of iron nanoparticles (INP) has been tested in the current work for the removal of aqueous uranium from synthetic water samples. A comparison of the removal of aqueous uranium from solutions using carboxy-methyl-cellulose with and without iron nanoparticles (CMC-INP and CMC, respectively) was tested over a 48 h reaction period. Analysis of liquid samples using spectrophotometry determined a maximum sorption capacity of uranium, Qmax, of 185.18 mg/g and 322.58 mg/g for CMC and CMC-INP respectively, providing strong evidence of an independent aqueous uranium removal ability exhibited by CMC. The results point out that CMC provides an additional capacity for aqueous uranium removal. Further tests are required to determine whether similar behaviour will be observed for other aqueous contaminant species and if the presence of CMC within a INP slurry inhibits or aids the reactivity, reductive capacity and affinity of INP for aqueous contaminant removal.

Identification of bacteria synthesizing ribosomal RNA in response to uranium addition during biostimulation at the Rifle, CO Integrated Field Research site

DOE PAGES

McGuinness, Lora R.; Wilkins, Michael J.; Williams, Kenneth H.; ...

2015-09-18

Understanding which organisms are capable of reducing uranium at historically contaminated sites provides crucial information needed to evaluate treatment options and outcomes. One approach is determination of the bacteria which directly respond to uranium addition. In this research, uranium amendments were made to groundwater samples from a site of ongoing biostimulation with acetate. The active microbes in the planktonic phase were deduced by monitoring ribosomes production via RT-PCR. The results indicated several microorganisms were synthesizing ribosomes in proportion with uranium amendment up to 2 μM. Concentrations of U (VI) >2 μM were generally found to inhibit ribosome synthesis. Two activemore » bacteria responding to uranium addition in the field were close relatives of Desulfobacter postgateii and Geobacter bemidjiensis. Since RNA content often increases with growth rate, our findings suggest it is possible to rapidly elucidate active bacteria responding to the addition of uranium in field samples and provides a more targeted approach to stimulate specific populations to enhance radionuclide reduction in contaminated sites.« less

Identification of Bacteria Synthesizing Ribosomal RNA in Response to Uranium Addition During Biostimulation at the Rifle, CO Integrated Field Research Site

PubMed Central

McGuinness, Lora R.; Wilkins, Michael J.; Williams, Kenneth H.; Long, Philip E.; Kerkhof, Lee J.

2015-01-01

Understanding which organisms are capable of reducing uranium at historically contaminated sites provides crucial information needed to evaluate treatment options and outcomes. One approach is determination of the bacteria which directly respond to uranium addition. In this study, uranium amendments were made to groundwater samples from a site of ongoing biostimulation with acetate. The active microbes in the planktonic phase were deduced by monitoring ribosomes production via RT-PCR. The results indicated several microorganisms were synthesizing ribosomes in proportion with uranium amendment up to 2 μM. Concentrations of U (VI) >2 μM were generally found to inhibit ribosome synthesis. Two active bacteria responding to uranium addition in the field were close relatives of Desulfobacter postgateii and Geobacter bemidjiensis. Since RNA content often increases with growth rate, our findings suggest it is possible to rapidly elucidate active bacteria responding to the addition of uranium in field samples and provides a more targeted approach to stimulate specific populations to enhance radionuclide reduction in contaminated sites. PMID:26382047

Polonium (²¹⁰Po), uranium (²³⁴U, ²³⁸U) isotopes and trace metals in mosses from Sobieszewo Island, northern Poland.

PubMed

Boryło, Alicja; Nowicki, Waldemar; Olszewski, Grzegorz; Skwarzec, Bogdan

2012-01-01

The activity of polonium (210)Po and uranium (234)U, (238)U radionuclides, as well as trace metals in mosses, collected from Sobieszewo Island area (northern Poland), were determined using the alpha spectrometry, AAS (atomic absorption spectrometry) and OES-ICP (atomic emission spectrometry with inductively coupled plasma). The concentrations of mercury (directly from the solid sample) were determined by the cold vapor technique of CV AAS. The obtained results revealed that the concentrations of (210)Po, (234)U, and (238)U in the two analyzed kinds of mosses: schrebers big red stem moss (Pleurozium schreberi) and broom moss (Dicranum scoparium) were similar. The higher polonium concentrations were found in broom moss (Dicranum scoparium), but uranium concentrations were relatively low for both species of analyzed mosses. Among the analyzed trace metals the highest concentration in mosses was recorded for iron, while the lowest for nickel, cadmium and mercury. The obtained studies showed that the sources of polonium and uranium isotopes, as well as trace metals in analyzed mosses are air city contaminations transported from Gdańsk and from existing in the vicinity the phosphogypsum waste heap in Wiślinka (near Gdańsk).

Influence of depleted uranium on hepatic cholesterol metabolism in apolipoprotein E-deficient mice.

PubMed

Souidi, M; Racine, R; Grandcolas, L; Grison, S; Stefani, J; Gourmelon, P; Lestaevel, P

2012-04-01

Depleted uranium (DU) is uranium with a lower content of the fissile isotope U-235 than natural uranium. It is a radioelement and a waste product from the enrichment process of natural uranium. Because of its very high density, it is used in the civil industry and for military purposes. DU exposure can affect many vital systems in the human body, because in addition to being weakly radioactive, uranium is a toxic metal. It should be emphasized that, to be exposed to radiation from DU, you have to eat, drink, or breathe it, or get it on your skin. This particular study is focusing on the health effects of DU for the cholesterol metabolism. Previous studies on the same issue have shown that the cholesterol metabolism was modulated at molecular level in the liver of laboratory rodents contaminated for nine months with DU. However, this modulation was not correlated with some effects at organs or body levels. It was therefore decided to use a "pathological model" such as hypercholesterolemic apolipoprotein E-deficient laboratory mice in order to try to clarify the situation. The purpose of the present study is to assess the effects of a chronic ingestion (during 3 months) of a low level DU-supplemented water (20 mg L(-1)) on the above mentioned mice in order to determine a possible contamination effect. Afterwards the cholesterol metabolism was studied in the liver especially focused on the gene expressions of cholesterol-catabolising enzymes (CYP7A1, CYP27A1 and CYP7B1), as well as those of associated nuclear receptors (LXRα, FXR, PPARα, and SREBP 2). In addition, mRNA levels of other enzymes of interest were measured (ACAT 2, as well as HMGCoA Reductase and HMGCoA Synthase). The gene expression study was completed with SRB1 and LDLr, apolipoproteins A1 and B and membrane transporters ABC A1, ABC G5. The major effect induced by a low level of DU contamination in apo-E deficient mice was a decrease in hepatic gene expression of the enzyme CYP7B1 (-23%) and nuclear receptors LXRα (-24%), RXR (-32%), HNF4α (-21%) when compared to unexposed ones. These modifications on cholesterol metabolism did not lead to increased disturbances that are specific for apolipoprotein E-deficient mice, suggesting that chronic DU exposure did not worsen the pathology in this experimental model. In conclusion, the results of this study indicate that even for a sensitive pathologic model the exposure to a low dose of DU has no relevant impact. The results confirm the results of our first study carried out on healthy laboratory rodents where a sub-chronic contamination with low dose DU did not affect in vivo the metabolism of cholesterol. Crown Copyright © 2012. Published by Elsevier Ltd. All rights reserved.

Actinide removal from spent salts

DOEpatents

Hsu, Peter C.; von Holtz, Erica H.; Hipple, David L.; Summers, Leslie J.; Adamson, Martyn G.

2002-01-01

A method for removing actinide contaminants (uranium and thorium) from the spent salt of a molten salt oxidation (MSO) reactor is described. Spent salt is removed from the reactor and analyzed to determine the contaminants present and the carbonate concentration. The salt is dissolved in water, and one or more reagents are added to precipitate the thorium as thorium oxide and/or the uranium as either uranium oxide or as a diuranate salt. The precipitated materials are filtered, dried and packaged for disposal as radioactive waste. About 90% of the thorium and/or uranium present is removed by filtration. After filtration, salt solutions having a carbonate concentration >20% can be dried and returned to the reactor for re-use. Salt solutions containing a carbonate concentration <20% require further clean-up using an ion exchange column, which yields salt solutions that contain less than 0.1 ppm of thorium or uranium.

Redox Roll-Front Mobilization of Geogenic Uranium by Nitrate Input into Aquifers: Risks for Groundwater Resources.

PubMed

van Berk, Wolfgang; Fu, Yunjiao

2017-01-03

Redox conditions are seen as the key to controlling aqueous uranium concentrations (cU (aq) ). Groundwater data collected by a state-wide groundwater quality monitoring study in Mecklenburg-Western Pomerania (Germany) reveal peak cU (aq) up to 75 μg L -1 but low background uranium concentrations (median cU (aq) < 0.5 μg L -1 ). To characterize the hydrogeochemical processes causing such groundwater contamination by peak cU (aq) , we reanalyzed measured redox potentials and total concentrations of aqueous uranium, nitrate, and sulfate species in groundwater together with their distribution across the aquifer depth and performed semigeneric 2D reactive mass transport modeling which is based on chemical thermodynamics. The combined interpretation of modeling results and measured data reveals that high cU (aq) and its depth-specific distribution depending on redox conditions is a result of a nitrate-triggered roll-front mobilization of geogenic uranium in the studied aquifers which are unaffected by nuclear activities. The modeling results show that groundwater recharge containing (fertilizer-derived) nitrate drives the redox shift from originally reducing toward oxidizing environments, when nitrate input has consumed the reducing capacity of the aquifers, which is present as pyrite, degradable organic carbon, and geogenic U(IV) minerals. This redox shift controls the uranium roll-front mobilization and results in high cU (aq) within the redoxcline. Moreover, the modeling results indicate that peak cU (aq) occurring at this redox front increase along with the temporal progress of such redox conversion within the aquifer.

Efficacy of Biostimulation for Uranium Sequestration: Coupled Effects Sediment/Groundwater Geochemistry and Microbiology

NASA Astrophysics Data System (ADS)

Xu, J.; Veeramani, H.; Qafoku, N. P.; Singh, G.; Pruden, A.; Kukkadapu, R. K.; Hochella, M. F., Jr.

2015-12-01

A systematic flow-through column study was conducted using sediments and groundwater from the subsurface at the U.S. Department of Energy's Integrated Field Research Challenge (IFRC) site in Rifle, Colorado, to better understand the efficacy of uranium removal from the groundwater with and without biostimulation in the form of acetate amendments. The interactive effects of acetate amendment, groundwater/sediment geochemistry, and intrinsic bacterial community composition were evaluated using four types of sediments, collected from different uranium-contaminated (D08, LQ107, CD) or non-contaminated (RABS) aquifers. Subtle variations in the sediments' geochemistry in terms of mineral compositions, particle sizes, redox conditions, and metal(loid) co-contaminants had a marked effect on the uranium removal efficiency, following a descending trend of D08 (~ 90 to 95%) >> RABS (~ 20 to 25) ≥ LQ107 (~ 15 to 20%) > CD (~ -10 to 0%). Overall, biostimulation of the sediments with acetate drove deeper anoxic conditions and observable shifts in bacterial population structures. The abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, were highest in the sediments that performed best in terms of uranium removal. By comparison, no obvious associations were found between the uranium removal efficiency and the abundance of typical iron-reducing microorganisms, e.g., Geobacter spp. In the sediments where bacterial biomass was relatively low and sulfate-reduction was not detected (i.e., CD), abiotic adsorption onto fine mineral surfaces such as phyllosilates likely played a dominant role in the attenuation of aqueous uranium. In these scenarios, however, acetate amendment induced significant remobilization of the sequestered uranium and other heavy metals (e.g., strontium), leading to zero or negative uranium removal efficiencies (i.e., CD). The results of this study suggest that reductive immobilization of uranium can be effectively achieved under predominantly sulfate-reducing conditions in sediment microenvironments when bioavailable iron (III) (oxyhydr)oxides are mostly depleted, and provide insight into the integrated roles of sediment geochemistry, mineralogy, and bacterial population dynamics.

Development of Modeling Methods and Tools for Predicting Coupled Reactive Transport Processes in Porous Media at Multiple Scales

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clement, T. Prabhakar; Barnett, Mark O.; Zheng, Chunmiao

DE-FG02-06ER64213: Development of Modeling Methods and Tools for Predicting Coupled Reactive Transport Processes in Porous Media at Multiple Scales Investigators: T. Prabhakar Clement (PD/PI) and Mark O. Barnett (Auburn), Chunmiao Zheng (Univ. of Alabama), and Norman L. Jones (BYU). The objective of this project was to develop scalable modeling approaches for predicting the reactive transport of metal contaminants. We studied two contaminants, a radioactive cation [U(VI)] and a metal(loid) oxyanion system [As(III/V)], and investigated their interactions with two types of subsurface materials, iron and manganese oxyhydroxides. We also developed modeling methods for describing the experimental results. Overall, the project supportedmore » 25 researchers at three universities. Produced 15 journal articles, 3 book chapters, 6 PhD dissertations and 6 MS theses. Three key journal articles are: 1) Jeppu et al., A scalable surface complexation modeling framework for predicting arsenate adsorption on goethite-coated sands, Environ. Eng. Sci., 27(2): 147-158, 2010. 2) Loganathan et al., Scaling of adsorption reactions: U(VI) experiments and modeling, Applied Geochemistry, 24 (11), 2051-2060, 2009. 3) Phillippi, et al., Theoretical solid/solution ratio effects on adsorption and transport: uranium (VI) and carbonate, Soil Sci. Soci. of America, 71:329-335, 2007« less

Diversity and Characterization of Sulfate-Reducing Bacteria in Groundwater at a Uranium Mill Tailings Site

PubMed Central

Chang, Yun-Juan; Peacock, Aaron D.; Long, Philip E.; Stephen, John R.; McKinley, James P.; Macnaughton, Sarah J.; Hussain, A. K. M. Anwar; Saxton, Arnold M.; White, David C.

2001-01-01

Microbially mediated reduction and immobilization of U(VI) to U(IV) plays a role in both natural attenuation and accelerated bioremediation of uranium-contaminated sites. To realize bioremediation potential and accurately predict natural attenuation, it is important to first understand the microbial diversity of such sites. In this paper, the distribution of sulfate-reducing bacteria (SRB) in contaminated groundwater associated with a uranium mill tailings disposal site at Shiprock, N.Mex., was investigated. Two culture-independent analyses were employed: sequencing of clone libraries of PCR-amplified dissimilatory sulfite reductase (DSR) gene fragments and phospholipid fatty acid (PLFA) biomarker analysis. A remarkable diversity among the DSR sequences was revealed, including sequences from δ-Proteobacteria, gram-positive organisms, and the Nitrospira division. PLFA analysis detected at least 52 different mid-chain-branched saturate PLFA and included a high proportion of 10me16:0. Desulfotomaculum and Desulfotomaculum-like sequences were the most dominant DSR genes detected. Those belonging to SRB within δ-Proteobacteria were mainly recovered from low-uranium (≤302 ppb) samples. One Desulfotomaculum-like sequence cluster overwhelmingly dominated high-U (>1,500 ppb) sites. Logistic regression showed a significant influence of uranium concentration over the dominance of this cluster of sequences (P = 0.0001). This strong association indicates that Desulfotomaculum has remarkable tolerance and adaptation to high levels of uranium and suggests the organism's possible involvement in natural attenuation of uranium. The in situ activity level of Desulfotomaculum in uranium-contaminated environments and its comparison to the activities of other SRB and other functional groups should be an important area for future research. PMID:11425735

Contribution of Uranium-Bearing Evaporites to Plume Persistence Issues at a Former Uranium Mill Site Riverton, Wyoming, USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Raymond; Dam, William; Campbell, Sam

2016-08-01

• Evaporites occur in an unsaturated silt layer, which is underlain by a sand and gravel aquifer. • These evaporites are rich in chloride across the site. • Uranium concentrations are higher in the evaporites that overlie the uranium contaminant plume. • Flooding can solubilize the evaporites in the silt layer and release chloride, sulfate (not shown), and uranium into the underlyingsand and gravel aquifer. • The uranium-rich evaporites can delay natural flushing, creating plume persistence near the Little Wind River.

Plutonium age dating reloaded

NASA Astrophysics Data System (ADS)

Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Mayer, Klaus; Prohaska, Thomas

2014-05-01

Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.

Complete genome sequence of Anaeromyxobacter sp. Fw109-5, an Anaerobic, Metal-Reducing Bacterium Isolated from a Contaminated Subsurface Environment

DOE PAGES

Hwang, C.; Copeland, A.; Lucas, Susan; ...

2015-01-22

We report the genome sequence of Anaeromyxobacter sp. Fw109-5, isolated from nitrate- and uranium-contaminated subsurface sediment of the Oak Ridge Integrated Field-Scale Subsurface Research Challenge (IFC) site, Oak Ridge Reservation, TN. The bacterium’s genome sequence will elucidate its physiological potential in subsurface sediments undergoing in situ uranium bioremediation and natural attenuation.

Groundwater transport of strontium 90 in a glacial outwash environment

USGS Publications Warehouse

Kipp, Kenneth L.; Stollenwerk, Kenneth G.; Grove, David B.

1986-01-01

As part of the investigation of groundwater contamination at a uranium-scrap recovery plant at Wood River Junction, Rhode Island, laboratory experiments led to the development of a model for predicting the transport of strontium 90 in glacial outwash sediments based on an approximate mechanism for ion exchange. The multicomponent system was simplified to two components by regarding all exchangeable cations other than strontium 90 as a single component. The binary ion-exchange parameter was a function of the variable, total ion concentration. A one-dimensional solute transport model was formulated to evaluate the time necessary for natural groundwater flow to remove the strontium 90 contamination plume from the groundwater system to the Pawcatuck River. The finite difference transport equations were solved sequentially for total ion concentrations, then strontium 90 concentrations. Clay-free quartz and feldspar sands at the study site have little potential for strontium 90 sorption, and high calcium, magnesium, and sodium concentrations compete for the few ion exchange sites. As the total ion concentration plume moves out of the system, ion exchange of strontium 90 increases, reducing the strontium 90 concentration in the groundwater. Cleanout times predicted using the binary ion exchange mechanism were about two thirds of those predicted using a constant distribution coefficient. It is suggested that this type of model can simulate solute transport more realistically in many groundwater systems where the total ion concentration is not constant.

Remediation of soils contaminated with particulate depleted uranium by multi stage chemical extraction.

PubMed

Crean, Daniel E; Livens, Francis R; Sajih, Mustafa; Stennett, Martin C; Grolimund, Daniel; Borca, Camelia N; Hyatt, Neil C

2013-12-15

Contamination of soils with depleted uranium (DU) from munitions firing occurs in conflict zones and at test firing sites. This study reports the development of a chemical extraction methodology for remediation of soils contaminated with particulate DU. Uranium phases in soils from two sites at a UK firing range, MOD Eskmeals, were characterised by electron microscopy and sequential extraction. Uranium rich particles with characteristic spherical morphologies were observed in soils, consistent with other instances of DU munitions contamination. Batch extraction efficiencies for aqueous ammonium bicarbonate (42-50% total DU extracted), citric acid (30-42% total DU) and sulphuric acid (13-19% total DU) were evaluated. Characterisation of residues from bicarbonate-treated soils by synchrotron microfocus X-ray diffraction and X-ray absorption spectroscopy revealed partially leached U(IV)-oxide particles and some secondary uranyl-carbonate phases. Based on these data, a multi-stage extraction scheme was developed utilising leaching in ammonium bicarbonate followed by citric acid to dissolve secondary carbonate species. Site specific U extraction was improved to 68-87% total U by the application of this methodology, potentially providing a route to efficient DU decontamination using low cost, environmentally compatible reagents. Copyright © 2013 The Authors. Published by Elsevier B.V. All rights reserved.

Imaging high stage river-water intrusion into a contaminated aquifer along a major river corridor using 2D time-lapse surface electrical resistivity tomography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wallin, Erin L.; Johnson, Timothy C.; Greenwood, William J.

2013-03-29

The Hanford 300 Area is located adjacent to the Columbia River in south-central Washington State, USA, and was a former site for nuclear fuel processing operations. Waste disposal practices resulted in persistent unsaturated zone and groundwater contamination, the primary contaminant of concern being uranium. Uranium behavior at the site is intimately linked with river stage driven groundwater-river water exchange such that understanding the nature of river water intrusion into the 300 Area is critical for predicting uranium desorption and transport. In this paper we use time-lapse electrical resistivity tomography (ERT) to image the inland intrusion of river during high stagemore » conditions. We demonstrate a modified time-lapse inversion approach, whereby the transient water table elevation is explicitly modeled by removing regularization constraints across the water table boundary. This implementation was critical for producing meaningful imaging results. We inverted approximately 1200 data sets (400 per line over 3 lines) using high performance computing resources to produce a time-lapse sequence of changes in bulk conductivity caused by river water intrusion during the 2011 spring runoff cycle over approximately 125 days. The resulting time series for each mesh element was then analyzed using common time series analysis to reveal the timing and location of river water intrusion beneath each line. The results reveal non-uniform flows characterized by preferred flow zones where river water enters and exits quickly with stage increase and decrease, and low permeability zones with broader bulk conductivity ‘break through’ curves and longer river water residence times. The time-lapse ERT inversion approach removes the deleterious effects of changing water table elevation and enables remote and spatial continuous groundwater-river water exchange monitoring using surface based ERT arrays under conditions where groundwater and river water conductivity are in contrast.« less

Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry.

PubMed

Janot, Noémie; Lezama Pacheco, Juan S; Pham, Don Q; O'Brien, Timothy M; Hausladen, Debra; Noël, Vincent; Lallier, Florent; Maher, Kate; Fendorf, Scott; Williams, Kenneth H; Long, Philip E; Bargar, John R

2016-01-05

The Rifle alluvial aquifer along the Colorado River in west central Colorado contains fine-grained, diffusion-limited sediment lenses that are substantially enriched in organic carbon and sulfides, as well as uranium, from previous milling operations. These naturally reduced zones (NRZs) coincide spatially with a persistent uranium groundwater plume. There is concern that uranium release from NRZs is contributing to plume persistence or will do so in the future. To better define the physical extent, heterogeneity and biogeochemistry of these NRZs, we investigated sediment cores from five neighboring wells. The main NRZ body exhibited uranium concentrations up to 100 mg/kg U as U(IV) and contains ca. 286 g of U in total. Uranium accumulated only in areas where organic carbon and reduced sulfur (as iron sulfides) were present, emphasizing the importance of sulfate-reducing conditions to uranium retention and the essential role of organic matter. NRZs further exhibited centimeter-scale variations in both redox status and particle size. Mackinawite, greigite, pyrite and sulfate coexist in the sediments, indicating that dynamic redox cycling occurs within NRZs and that their internal portions can be seasonally oxidized. We show that oxidative U(VI) release to the aquifer has the potential to sustain a groundwater contaminant plume for centuries. NRZs, known to exist in other uranium-contaminated aquifers, may be regionally important to uranium persistence.

Nevada Test and Training Range Depleted Uranium Target Disposal Environmental Assessment

DTIC Science & Technology

2005-03-01

to establish the probability and scope of such transport. Long-Term Fate of Depleted Uranium at Aberdeen and Yuma Proving Grounds Phase II: Human...1990. Long-Term Fate of Depleted Uranium at Aberdeen and Yuma Proving Grounds Final Report, Phase 1: Geochemical Transport and Modeling. Los...of Depleted Uranium at Aberdeen and Yuma Proving Grounds , Phase II: Human Health and Ecological Risk Assessments. Los Alamos National Laboratory

STRUCTURE AND FUNCTION OF SUBSURFACE MICROBIAL COMMUNITIES AFFECTING RADIONUCLIDE TRANSPORT AND BIOIMMOBILIZATION

DOE Office of Scientific and Technical Information (OSTI.GOV)

Joel E. Kostka; Lee Kerkhof; Kuk-Jeong Chin

2011-06-15

The objectives of this project were to: (1) isolate and characterize novel anaerobic prokaryotes from subsurface environments exposed to high levels of mixed contaminants (U(VI), nitrate, sulfate), (2) elucidate the diversity and distribution of metabolically active metal- and nitrate-reducing prokaryotes in subsurface sediments, and (3) determine the biotic and abiotic mechanisms linking electron transport processes (nitrate, Fe(III), and sulfate reduction) to radionuclide reduction and immobilization. Mechanisms of electron transport and U(VI) transformation were examined under near in situ conditions in sediment microcosms and in field investigations at the Oak Ridge Field Research Center (ORFRC), in Oak Ridge, Tennessee, where themore » subsurface is exposed to mixed contamination predominated by uranium and nitrate. A total of 20 publications (16 published or 'in press' and 4 in review), 10 invited talks, and 43 contributed seminars/ meeting presentations were completed during the past four years of the project. PI Kostka served on one proposal review panel each year for the U.S. DOE Office of Science during the four year project period. The PI leveraged funds from the state of Florida to purchase new instrumentation that aided the project. Support was also leveraged by the PI from the Joint Genome Institute in the form of two successful proposals for genome sequencing. Draft genomes are now available for two novel species isolated during our studies and 5 more genomes are in the pipeline. We effectively addressed each of the three project objectives and research highlights are provided. Task I - Isolation and characterization of novel anaerobes: (1) A wide range of pure cultures of metal-reducing bacteria, sulfate-reducing bacteria, and denitrifying bacteria (32 strains) were isolated from subsurface sediments of the Oak Ridge Field Research Center (ORFRC), where the subsurface is exposed to mixed contamination of uranium and nitrate. These isolates which are new to science all show high sequence identity to sequences retrieved from ORFRC subsurface. (2) Based on physiological and phylogenetic characterization, two new species of subsurface bacteria were described: the metal-reducer Geobacter daltonii, and the denitrifier Rhodanobacter denitrificans. (3) Strains isolated from the ORFRC show that Rhodanobacter species are well adapted to the contaminated subsurface. Strains 2APBS1 and 116-2 grow at high salt (3% NaCl), low pH (3.5) and tolerate high concentrations of nitrate (400mM) and nitrite (100mM). Strain 2APBS1 was demonstrated to grow at in situ acidic pHs down to 2.5. (4) R. denitrificans strain 2APBS1 is the first described Rhodanobacter species shown to denitrify. Nitrate is almost entirely converted to N2O, which may account for the large accumulation of N2O in the ORFRC subsurface. (5) G. daltonii, isolated from uranium- and hydrocarbon-contaminated subsurface sediments of the ORFRC, is the first organism from the subsurface clade of the genus Geobacter that is capable of growth on aromatic hydrocarbons. (6) High quality draft genome sequences and a complete eco-physiological description are completed for R. denitrificans strain 2APBS1 and G. daltonii strain FRC-32. (7) Given their demonstrated relevance to DOE remediation efforts and the availability of detailed genotypic/phenotypic characterization, Rhodanobacter denitrificans strain 2APBS1 and Geobacter daltonii strain FRC-32 represent ideal model organisms to provide a predictive understanding of subsurface microbial activity through metabolic modeling. Tasks II and III-Diversity and distribution of active anaerobes and Mechanisms linking electron transport and the fate of radionuclides: (1) Our study showed that members of genus Rhodanobacter and Geobacter are abundant and active in the uranium and nitrate contaminated subsurface. In the contaminant source zone of the Oak Ridge site, Rhodanobacter spp. are the predominant, active organisms detected (comprising 50% to 100% of rRNA detected). (2) We demonstrated for the first time that the function of microbial communities can be quantified in subsurface sediments using messenger RNA assays (molecular proxies) under in situ conditions. (3) Active Geobacteraceae were identified and phylogenetically characterized from the cDNA of messenger RNA extracted from ORFRC subsurface sediment cores. Multiple clone sequences were retrieved from G. uraniireducens, G. daltonii, and G. metallireducens. (4) Results show that Geobacter strain FRC-32 is capable of growth on benzoate, toluene and benzene as the electron donor, thereby providing evidence that this strain is physiologically distinct from other described members of the subsurface Geobacter clade. (5) Fe(III)-reducing bacteria transform structural Fe in clay minerals from their layer edges rather than from their basal surfaces.« less

Uranium(IV) adsorption by natural organic matter in anoxic sediments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bone, Sharon E.; Dynes, James J.; Cliff, John

2017-01-09

Uranium is an important fuel source and a global environmental contaminant. It accumulates in the tetravalent state, U(IV), in anoxic sediments, including ore deposits, marine basins, and contaminated aquifers. However, very little is known about the speciation of U(IV) in low temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2) in anoxic sediments; yet studies now show that UO 2 is not often dominant in these environments. However, a model of U(IV) speciation under environmentally relevant conditions has not yetmore » been developed. Here we show that complexes of U(IV) adsorb on organic carbon and organic carbon-coated clays in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that the U(IV) product depended on the reduction pathway, our results demonstrate that UO 2 formation can be inhibited simply by decreasing the U:solid ratio. Thus, it is the number and type of surface ligands that controls U(IV) speciation subsequent to U(VI) reduction. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider retention of U(IV) ions within the local sediment environment.« less

Advanced remediation of uranium-contaminated soil.

PubMed

Kim, S S; Han, G S; Kim, G N; Koo, D S; Kim, I G; Choi, J W

2016-11-01

The existing decontamination method using electrokinetic equipment after acidic washing for uranium-contaminated soil requires a long decontamination time and a significant amount of electric power. However, after soil washing, with a sulfuric acid solution and an oxidant at 65 °C, the removal of the muddy solution using a 100 mesh sieve can decrease the radioactivity of the remaining coarse soil to the clearance level. Therefore, only a small amount of fine soil collected from the muddy solution requires the electrokinetic process for its decontamination. Furthermore, it is found that the selective removal of uranium from the sulfuric washing solution is not obtained using an anion exchanger but rather using a cation exchanger, unexpectedly. More than 90% of the uranium in the soil washing solutions is adsorbed on the S-950 resin, and 87% of the uranium adsorbed on S-950 is desorbed by washing with a 0.5 M Na 2 CO 3 solution at 60 °C. Copyright © 2016 Elsevier Ltd. All rights reserved.

Fate of Noble Metals during the Pyroprocessing of Spent Nuclear Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

B.R. Westphal; D. Vaden; S.X. Li

During the pyroprocessing of spent nuclear fuel by electrochemical techniques, fission products are separated as the fuel is oxidized at the anode and refined uranium is deposited at the cathode. Those fission products that are oxidized into the molten salt electrolyte are considered active metals while those that do not react are considered noble metals. The primary noble metals encountered during pyroprocessing are molybdenum, zirconium, ruthenium, rhodium, palladium, and technetium. Pyroprocessing of spent fuel to date has involved two distinctly different electrorefiner designs, in particular the anode to cathode configuration. For one electrorefiner, the anode and cathode collector are horizontallymore » displaced such that uranium is transported across the electrolyte medium. As expected, the noble metal removal from the uranium during refining is very high, typically in excess of 99%. For the other electrorefiner, the anode and cathode collector are vertically collocated to maximize uranium throughput. This arrangement results in significantly less noble metals removal from the uranium during refining, typically no better than 20%. In addition to electrorefiner design, operating parameters can also influence the retention of noble metals, albeit at the cost of uranium recovery. Experiments performed to date have shown that as much as 100% of the noble metals can be retained by the cladding hulls while affecting the uranium recovery by only 6%. However, it is likely that commercial pyroprocessing of spent fuel will require the uranium recovery to be much closer to 100%. The above mentioned design and operational issues will likely be driven by the effects of noble metal contamination on fuel fabrication and performance. These effects will be presented in terms of thermal properties (expansion, conductivity, and fusion) and radioactivity considerations. Ultimately, the incorporation of minor amounts of noble metals from pyroprocessing into fast reactor metallic fuel will be shown to be of no consequence to reactor performance.« less

MICROSCALE METABOLIC, REDOX AND ABIOTIC REACTIONS IN HANFORD 300 AREA SUBSURFACE SEDIMENTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beyenal, Haluk; McLEan, Jeff; Majors, Paul

2013-11-14

The Hanford 300 Area is a unique site due to periodic hydrologic influence of river water resulting in changes in groundwater elevation and flow direction. This area is also highly subject to uranium remobilization, the source of which is currently believed to be the region at the base of the vadose zone that is subject to period saturation due to the changes in the water levels in the Columbia River. We found that microbial processes and redox and abiotic reactions which operate at the microscale were critical to understanding factors controlling the macroscopic fate and transport of contaminants in themore » subsurface. The combined laboratory and field research showed how microscale conditions control uranium mobility and how biotic, abiotic and redox reactions relate to each other. Our findings extended the current knowledge to examine U(VI) reduction and immobilization using natural 300 Area communities as well as selected model organisms on redox-sensitive and redox-insensitive minerals. Using innovative techniques developed specifically to probe biogeochemical processes at the microscale, our research expanded our current understanding of the roles played by mineral surfaces, bacterial competition, and local biotic, abiotic and redox reaction rates on the reduction and immobilization of uranium.« less

Oxidative dissolution of biogenic uraninite in groundwater at Old Rifle, CO

USGS Publications Warehouse

Campbell, Kate M.; Veeramani, Harish; Ulrich, Kai-Uwe; Blue, Lisa Y.; Giammar, Dianiel E.; Bernier-Latmani, Rizlan; Stubbs, Joanne E.; Suvorova, Elena; Yabusaki, Steve; Lezama-Pacheco, Juan S.; Mehta, Apurva; Long, Philip E.; Bargar, John R.

2011-01-01

Reductive bioremediation is currently being explored as a possible strategy for uranium-contaminated aquifers such as the Old Rifle site (Colorado). The stability of U(IV) phases under oxidizing conditions is key to the performance of this procedure. An in situ method was developed to study oxidative dissolution of biogenic uraninite (UO2), a desirable U(VI) bioreduction product, in the Old Rifle, CO, aquifer under different variable oxygen conditions. Overall uranium loss rates were 50–100 times slower than laboratory rates. After accounting for molecular diffusion through the sample holders, a reactive transport model using laboratory dissolution rates was able to predict overall uranium loss. The presence of biomass further retarded diffusion and oxidation rates. These results confirm the importance of diffusion in controlling in-aquifer U(IV) oxidation rates. Upon retrieval, uraninite was found to be free of U(VI), indicating dissolution occurred via oxidation and removal of surface atoms. Interaction of groundwater solutes such as Ca2+ or silicate with uraninite surfaces also may retard in-aquifer U loss rates. These results indicate that the prolonged stability of U(IV) species in aquifers is strongly influenced by permeability, the presence of bacterial cells and cell exudates, and groundwater geochemistry.

Uranium mobility across annual growth rings in three deciduous tree species

DOE Office of Scientific and Technical Information (OSTI.GOV)

McHugh, Kelly C.; Widom, Elisabeth; Spitz, Henry B.

Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is potentially dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236U) in growth rings of allmore » three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination.« less

Bioremediation of uranium-contaminated groundwater: a systems approach to subsurface biogeochemistry.

PubMed

Williams, Kenneth H; Bargar, John R; Lloyd, Jonathan R; Lovley, Derek R

2013-06-01

Adding organic electron donors to stimulate microbial reduction of highly soluble U(VI) to less soluble U(IV) is a promising strategy for immobilizing uranium in contaminated subsurface environments. Studies suggest that diagnosing the in situ physiological status of the subsurface community during uranium bioremediation with environmental transcriptomic and proteomic techniques can identify factors potentially limiting U(VI) reduction activity. Models which couple genome-scale in silico representations of the metabolism of key microbial populations with geochemical and hydrological models may be able to predict the outcome of bioremediation strategies and aid in the development of new approaches. Concerns remain about the long-term stability of sequestered U(IV) minerals and the release of co-contaminants associated with Fe(III) oxides, which might be overcome through targeted delivery of electrons to select microorganisms using in situ electrodes. Copyright © 2012 Elsevier Ltd. All rights reserved.

Uranium mobility across annual growth rings in three deciduous tree species.

PubMed

McHugh, Kelly C; Widom, Elisabeth; Spitz, Henry B; Wiles, Gregory C; Glover, Sam E

2018-02-01

Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236 U) in growth rings of all three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination. Copyright © 2017 Elsevier Ltd. All rights reserved.

Process for recovering uranium from waste hydrocarbon oils containing the same. [Uranium contaminated lubricating oils from gaseous diffusion compressors

DOEpatents

Conrad, M.C.; Getz, P.A.; Hickman, J.E.; Payne, L.D.

1982-06-29

The invention is a process for the recovery of uranium from uranium-bearing hydrocarbon oils containing carboxylic acid as a degradation product. In one aspect, the invention comprises providing an emulsion of water and the oil, heating the same to a temperature effecting conversion of the emulsion to an organic phase and to an acidic aqueous phase containing uranium carboxylate, and recovering the uranium from the aqueous phase. The process is effective, simple and comparatively inexpensive. It avoids the use of toxic reagents and the formation of undesirable intermediates.

Remedial action plan and site design for stabilization of the inactive Uranium Mill Tailing site Maybell, Colorado. Attachment 3, ground water hydrology report, Attachment 4, water resources protection strategy. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1994-06-01

The U.S. Environmental Protection Agency (EPA) has established health and environmental regulations to correct and prevent ground water contamination resulting from former uranium processing activities at inactive uranium processing sites (40 CFR Part 192 (1993)) (52 FR 36000 (1978)). According to the Uranium Mill Tailings Radiation Control Act (UMTRCA) of 1978 (42 USC {section} 7901 et seq.), the U.S. Department of Energy (DOE) is responsible for assessing the inactive uranium processing sites. The DOE has decided that each assessment will include information on hydrogeologic site characterization. The water resources protection strategy that describes the proposed action compliance with the EPAmore » ground water protection standards is presented in Attachment 4, Water Resources Protection Strategy. Site characterization activities discussed in this section include the following: (1) Definition of the hydrogeologic characteristics of the environment, including hydrostratigraphy, aquifer parameters, areas of aquifer recharge and discharge, potentiometric surfaces, and ground water velocities. (2) Definition of background ground water quality and comparison with proposed EPA ground water protection standards. (3) Evaluation of the physical and chemical characteristics of the contaminant source and/or residual radioactive materials. (4) Definition of existing ground water contamination by comparison with the EPA ground water protection standards. (5) Description of the geochemical processes that affect the migration of the source contaminants at the processing site. (6) Description of water resource use, including availability, current and future use and value, and alternate water supplies.« less

Plutonium release from the 903 pad at Rocky Flats.

PubMed

Mongan, T R; Ripple, S R; Winges, K D

1996-10-01

The Colorado Department of Public Health and Environment (CDH) sponsored a study to reconstruct contaminant doses to the public from operations at the Rocky Flats nuclear weapons plant. This analysis of the accidental release of plutonium from the area known as the 903 Pad is part of the CDH study. In the 1950's and 1960's, 55-gallon drums of waste oil contaminated with plutonium, and uranium were stored outdoors at the 903 Pad. The drums corroded, leaking contaminated oil onto soil subsequently carried off-site by the wind. The plutonium release is estimated using environmental data from the 1960's and 1970's and an atmospheric transport model for fugitive dust. The best estimate of total plutonium release to areas beyond plant-owned property is about 0.26 TBq (7 Ci). Off-site airborne concentrations and deposition of plutonium are estimated for dose calculation purposes. The best estimate of the highest predicted off-site effective dose is approximately 72 microSv (7.2 mrem).

Simplified behaviors from increased heterogeneity: II. 3-D uranium transport at the decimeter scale and intertank comparisons.

PubMed

Miller, Andrew W; Rodriguez, Derrick R; Honeyman, Bruce D

2013-05-01

Upscaling from bench scale systems to field scale systems incorporates physical and chemical heterogeneities from atomistic up to field scales. Heterogeneities of intermediate scale (~10(-1) m) are impossible to incorporate in a bench scale experiment. To transcend these scale discrepancies, this second in a pair of papers presents results from an intermediate scale, 3-D tank experiment completed using five different particle sizes of uranium contaminated sediment from a former uranium mill field site. The external dimensions of the tank were 2.44 m×0.61 m×0.61 m (L×H×W). The five particle sizes were packed in a heterogeneous manner using roughly 11 cm cubes. Small groundwater wells were installed for spatial characterization of chemical gradients and flow parameters. An approximately six month long bromide tracer test was used for flow field characterization. Within the flow domain, local uranium breakthrough curves exhibited a wide range of behaviors. However, the global effluent breakthrough curve was smooth, and not unlike breakthrough curves observed in column scale experiments. This paper concludes with an inter-tank comparison of all three experimental systems presented in this pair of papers. Although there is a wide range of chemical and physical variability between the three tanks, major chemical constituent behaviors are often quite similar or even identical. Copyright © 2013 Elsevier B.V. All rights reserved.

Scale-Up Information for Gas-Phase Ammonia Treatment of Uranium in the Vadose Zone at the Hanford Site Central Plateau

DOE Office of Scientific and Technical Information (OSTI.GOV)

Truex, Michael J.; Szecsody, James E.; Zhong, Lirong

Uranium is present in the vadose zone at the Hanford Central Plateau and is of concern for protection of groundwater. The Deep Vadose Zone Treatability Test Plan for the Hanford Central Plateau identified gas-phase treatment and geochemical manipulation as potentially effective treatment approaches for uranium and technetium in the Hanford Central Plateau vadose zone. Based on laboratory evaluation, use of ammonia vapor was selected as the most promising uranium treatment candidate for further development and field testing. While laboratory tests have shown that ammonia treatment effectively reduces the mobility of uranium, additional information is needed to enable deployment of thismore » technology for remediation. Of importance for field applications are aspects of the technology associated with effective distribution of ammonia to a targeted treatment zone, understanding the fate of injected ammonia and its impact on subsurface conditions, and identifying effective monitoring approaches. In addition, information is needed to select equipment and operational parameters for a field design. As part of development efforts for the ammonia technology for remediation of vadose zone uranium contamination, field scale-up issues were identified and have been addressed through a series of laboratory and modeling efforts. This report presents a conceptual description for field application of the ammonia treatment process, engineering calculations to support treatment design, ammonia transport information, field application monitoring approaches, and a discussion of processes affecting the fate of ammonia in the subsurface. The report compiles this information from previous publications and from recent research and development activities. The intent of this report is to provide technical information about these scale-up elements to support the design and operation of a field test for the ammonia treatment technology.« less

Uranium transport in the Walker River Basin, California and Nevada

USGS Publications Warehouse

Benson, L.V.; Leach, D.L.

1979-01-01

During the summer of 1976 waters from tributaries, rivers, springs and wells were sampled in the Walker River Basin. Snow and sediments from selected sites were also sampled. All samples were analyzed for uranium and other elements. The resulting data provide an understanding of the transport of uranium within a closed hydrologic basin as well as providing a basis for the design of geochemical reconnaissance studies for the Basin and Range Province of the Western United States. Spring and tributary data are useful in locating areas containing anomalous concentrations of uranium. However, agricultural practices obscure the presence of known uranium deposits and render impossible the detection of other known deposits. Uranium is extremely mobile in stream waters and does not appear to sorb or precipitate. Uranium has a long residence time (2500 years) in the open waters of Walker Lake; however, once it crosses the sediment-water interface, it is reduced to the U(IV) state and is lost from solution. Over the past two million years the amount of uranium transported to the terminal point of the Walker River system may have been on the order of 4 ?? 108 kg. This suggests that closed basin termini are sites for significant uranium accumulations and are, therefore, potential sites of uranium ore deposits. ?? 1979.

Characterization and Extraction of Uranium Contamination Perched within the Deep Vadose Zone at the Hanford Site, Washington State

NASA Astrophysics Data System (ADS)

Williams, B. A.; Rohay, V. J.; Benecke, M. W.; Chronister, G. B.; Doornbos, M. H.; Morse, J.

2012-12-01

A highly contaminated perched water zone has been discovered in the deep vadose zone above the unconfined aquifer during drilling of wells to characterize groundwater contamination within the 200 East Area of the U.S. Department of Energy's Hanford Site in southeast Washington. The perched water, which contains nitrate, uranium, and technetium-99 at concentrations that have exceeded 100,000 μg/L, 70,000 μg/L, and 45,000 pCi/L respectively, is providing contamination to the underlying unconfined aquifer. A perched zone extraction well has been installed and is successfully recovering the contaminated perched water as an early remedial measure to reduce impacts to the unconfined aquifer. The integration and interpretation of various borehole hydrogeologic, geochemical, and geophysical data sets obtained during drilling facilitated the delineation of the perching horizon and determination of the nature and extent of the perched contamination. Integration of the borehole geologic and geophysical logs defined the structural elevation and thickness of the perching low permeability silt interval. Borehole geophysical moisture logs, gamma logs, and sample data allowed detailed determination of the elevation and thickness of the oversaturated zone above the perching horizon, and the extent and magnitude of the radiological uranium contamination within the perching interval. Together, these data sets resolved the nature of the perching horizon and the location and extent of the contaminated perched water within the perching zone, allowing an estimation of remaining contaminant extent. The resulting conceptual model indicates that the contaminated perched water is contained within a localized sand lens deposited in a structural low on top of a semi-regional low-permeability silt layer. The top of the sand lens is approximately 72 m (235 ft) below ground surface; the maximum thickness of the sand lens is approximately 3 m (10 ft). The lateral and vertical extent of the perched water is limited to the presence of the sand lens and is approximately 4.6 m (15 ft) above the unconfined aquifer. Liquid wastes containing uranium and technetium-99 that were discharged decades ago to nearby engineered structures for subsurface infiltration and that leaked from single shell storage tanks have migrated vertically and laterally and are accumulating within this sand layer above the perching silt which forms a natural barrier that slows contaminant migration to the aquifer. Extraction of the contaminated perched water began in August 2011 using an automated pumping system installed in a well screened within the perched zone. As of August 1, 2012, approximately 52,000 gallons of perched water containing 115 kg of nitrate, 11.4 kg of uranium and 0.102 mg of technetium-99 have been removed from this zone.

Determination of uranium and thorium in materials associated with real time electronic solar neutrino detectors

NASA Astrophysics Data System (ADS)

Fassett, J. D.; Kelly, W. R.

1992-07-01

The application of isotope dilution thermal ionization mass spectrometry to the determination of both uranium and thorium in four different target materials used or proposed for electronic neutrino detectors is described. Isotope dilution analysis is done using highly enriched 233U and 230Th separated isotopes. Sensitivity of the technique is such that sub-picogram amounts of material are readily measured. The overall limit to measurement is caused by contamination of these elements during the measurement process. Uranium is more easily measured than thorium because both the instrumental sensitivity is higher and contamination is better controlled. The materials analyzed were light and heavy water, pseudocumene, and mineral oil.

Influence of season growth, soils and irrigation water composition on the concentration of uranium in two lettuce (Lactuca sativa L.) varieties. Field experiments

NASA Astrophysics Data System (ADS)

Abreu, M. M.; Neves, O.; Marcelino, M.

2012-04-01

Former uranium mines areas are frequently the sources of environmental radionuclides problems even many years after the closure of mining operations. A concern for inhabitants from mining areas is the use of contaminated land or irrigation water for agriculture, and the potential transfer of metals from soils to vegetables, and to humans through the food chain. The main aim of this study was to compare the uranium concentration in lettuce (Lactuca sativa L. varieties Marady and Romana) grown in different seasons (autumn and summer) and exposed to high and low uranium concentrations both in irrigation water and agricultural soil. The content of uranium in irrigation water, soil (total and available fraction) and in lettuce leaf samples was analyzed in a certified laboratory. In the field experiments, two agricultural soils were divided into two plots (four replicates each); one of them was irrigated with uranium contaminated water (0.94 to 1.14 mg/L) and the other with uncontaminated water (< 0.02 mg/L). Irrigation with contaminated water together with highest soil uranium available concentration (10 to 13 mg/kg) had negative effects on both studied lettuce varieties, namely yield reduction (up to 53% and 87% in autumn and summer experiments, respectively) and increase of uranium leaf concentration (up to 1.4 and 7 fold in autumn and summer, respectively). Effect on lettuce yield was mainly due to the high soil salinity (1.01 to 6.31 mS/cm) as a consequence of high irrigation water electrical conductivity (up to 1.82 mS/cm) and low lettuce soil salinity tolerance (1 to 3 mS/cm). The highest lettuce uranium concentration (dry weight) observed was 2.13 and 5.37 mg/kg for Marady and Romana variety, respectively. The highest uranium lettuce concentration in Romana variety was also the effect of its growing in summer season when it was subject to greatest frequency and amount of water irrigation. The consumption by an adult of the lettuce that concentrate more uranium, represents only 16.7% of the tolerable daily limit intake set by World Health Organisation for this element (0.6 mg/kg body weight daily), suggesting that lettuce uranium intake had a low contribution and do not represent a potential health risk for Cunha Baixa's residents.

Final report of the decontamination and decommissioning of Building 34 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-08-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7 acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the Grand Junction Projects Office Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, was also the remedialmore » action contractor. Building 34 was radiologically contaminated and the building was demolished in 1996. The soil area within the footprint of the building was analyzed and found to be not contaminated. The area can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual closeout report for each contaminated GJPO building.« less

Final report of the decontamination and decommissioning of Building 44 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-07-01

The U.S. Department of Energy (DOE) Junction Projects Office (GJPO) occupies a 61.7 acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the Grand Junction Projects Office Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, is also the remedial actionmore » contractor. Building 44 was radiologically contaminated and the building was demolished in 1994. The soil area within the footprint of the building was not contaminated; it complies with the identified standards and the area can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Final report of the decontamination and decommissioning of Building 18 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-08-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, also is the remedial action contractor. The soilmore » beneath Building 18 was found to be radiologically contaminated; the building was not contaminated. The soil was remediated in accordance with identified standards. Building 18 and the underlying soil can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Uranium Bio-accumulation and Cycling as revealed by Uranium Isotopes in Naturally Reduced Sediments from the Upper Colorado River Basin

NASA Astrophysics Data System (ADS)

Lefebvre, Pierre; Noël, Vincent; Jemison, Noah; Weaver, Karrie; Bargar, John; Maher, Kate

2016-04-01

Uranium (U) groundwater contamination following oxidized U(VI) releases from weathering of mine tailings is a major concern at numerous sites across the Upper Colorado River Basin (CRB), USA. Uranium(IV)-bearing solids accumulated within naturally reduced zones (NRZs) characterized by elevated organic carbon and iron sulfide compounds. Subsequent re-oxidation of U(IV)solid to U(VI)aqueous then controls the release to groundwater and surface water, resulting in plume persistence and raising public health concerns. Thus, understanding the extent of uranium oxidation and reduction within NRZs is critical for assessing the persistence of the groundwater contamination. In this study, we measured solid-phase uranium isotope fractionation (δ238/235U) of sedimentary core samples from four study sites (Shiprock, NM, Grand Junction, Rifle and Naturita, CO) using a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS). We observe a strong correlation between U accumulation and the extent of isotopic fractionation, with Δ238U up to +1.8 ‰ between uranium-enriched and low concentration zones. The enrichment in the heavy isotopes within the NRZs appears to be especially important in the vadose zone, which is subject to variations in water table depth. According to previous studies, this isotopic signature is consistent with biotic reduction processes associated with metal-reducing bacteria. Positive correlations between the amount of iron sulfides and the accumulation of reduced uranium underline the importance of sulfate-reducing conditions for U(IV) retention. Furthermore, the positive fractionation associated with U reduction observed across all sites despite some variations in magnitude due to site characteristics, shows a regional trend across the Colorado River Basin. The maximum extent of 238U enrichment observed in the NRZ proximal to the water table further suggests that the redox cycling of uranium, with net release of U(VI) to the groundwater by non-fractionating oxidation, is occurring within this zone. Thus, release of uranium from the NRZs may play a critical role in the persistence of groundwater contamination at these sites.

Laboratory column experiments and transport modeling to evaluate retardation of uranium in an aquifer downgradient of a uranium in-situ recovery site

DOE PAGES

Dangelmayr, Martin A.; Reimus, Paul W.; Wasserman, Naomi L.; ...

2017-05-01

The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47more » relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.« less

Laboratory column experiments and transport modeling to evaluate retardation of uranium in an aquifer downgradient of a uranium in-situ recovery site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dangelmayr, Martin A.; Reimus, Paul W.; Wasserman, Naomi L.

The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47more » relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.« less

Linking Specific Heterotrophic Bacterial Populations to Bioreduction of Uranium and Nitrate in Contaminated Subsurface Sediments by Using Stable Isotope Probing▿†

PubMed Central

Akob, Denise M.; Kerkhof, Lee; Küsel, Kirsten; Watson, David B.; Palumbo, Anthony V.; Kostka, Joel E.

2011-01-01

Shifts in terminal electron-accepting processes during biostimulation of uranium-contaminated sediments were linked to the composition of stimulated microbial populations using DNA-based stable isotope probing. Nitrate reduction preceded U(VI) and Fe(III) reduction in [13C]ethanol-amended microcosms. The predominant, active denitrifying microbial groups were identified as members of the Betaproteobacteria, whereas Actinobacteria dominated under metal-reducing conditions. PMID:21948831

High-Quality Draft Genome Sequence of Desulfovibrio carbinoliphilus FW-101-2B, an Organic Acid-Oxidizing Sulfate-Reducing Bacterium Isolated from Uranium(VI)-Contaminated Groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ramsay, Bradley D.; Hwang, Chiachi; Woo, Hannah L.

2015-03-12

Desulfovibrio carbinoliphilus subsp. oakridgensis FW-101-2B is an anaerobic, organic acid/alcohol-oxidizing, sulfate-reducing δ-proteobacterium. FW-101-2B was isolated from contaminated groundwater at The Field Research Center at Oak Ridge National Lab after in situ stimulation for heavy metal-reducing conditions. The genome will help elucidate the metabolic potential of sulfate-reducing bacteria during uranium reduction.

Upscaling of U(VI) Desorption and Transport from Decimeter-Scale Heterogeneity to Plume-Scale Modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Curtis, Gary P.; Kohler, Matthias; Kannappan, Ramakrishnan

2015-02-24

Scientifically defensible predictions of field scale U(VI) transport in groundwater requires an understanding of key processes at multiple scales. These scales range from smaller than the sediment grain scale (less than 10 μm) to as large as the field scale which can extend over several kilometers. The key processes that need to be considered include both geochemical reactions in solution and at sediment surfaces as well as physical transport processes including advection, dispersion, and pore-scale diffusion. The research summarized in this report includes both experimental and modeling results in batch, column and tracer tests. The objectives of this research weremore » to: (1) quantify the rates of U(VI) desorption from sediments acquired from a uranium contaminated aquifer in batch experiments;(2) quantify rates of U(VI) desorption in column experiments with variable chemical conditions, and(3) quantify nonreactive tracer and U(VI) transport in field tests.« less

Uranium Biominerals Precipitated by an Environmental Isolate of Serratia under Anaerobic Conditions.

PubMed

Newsome, Laura; Morris, Katherine; Lloyd, Jonathan R

2015-01-01

Stimulating the microbially-mediated precipitation of uranium biominerals may be used to treat groundwater contamination at nuclear sites. The majority of studies to date have focussed on the reductive precipitation of uranium as U(IV) by U(VI)- and Fe(III)-reducing bacteria such as Geobacter and Shewanella species, although other mechanisms of uranium removal from solution can occur, including the precipitation of uranyl phosphates via bacterial phosphatase activity. Here we present the results of uranium biomineralisation experiments using an isolate of Serratia obtained from a sediment sample representative of the Sellafield nuclear site, UK. When supplied with glycerol phosphate, this Serratia strain was able to precipitate 1 mM of soluble U(VI) as uranyl phosphate minerals from the autunite group, under anaerobic and fermentative conditions. Under phosphate-limited anaerobic conditions and with glycerol as the electron donor, non-growing Serratia cells could precipitate 0.5 mM of uranium supplied as soluble U(VI), via reduction to nano-crystalline U(IV) uraninite. Some evidence for the reduction of solid phase uranyl(VI) phosphate was also observed. This study highlights the potential for Serratia and related species to play a role in the bioremediation of uranium contamination, via a range of different metabolic pathways, dependent on culturing or in situ conditions.

Uranium Biominerals Precipitated by an Environmental Isolate of Serratia under Anaerobic Conditions

PubMed Central

Newsome, Laura; Morris, Katherine; Lloyd, Jonathan. R.

2015-01-01

Stimulating the microbially-mediated precipitation of uranium biominerals may be used to treat groundwater contamination at nuclear sites. The majority of studies to date have focussed on the reductive precipitation of uranium as U(IV) by U(VI)- and Fe(III)-reducing bacteria such as Geobacter and Shewanella species, although other mechanisms of uranium removal from solution can occur, including the precipitation of uranyl phosphates via bacterial phosphatase activity. Here we present the results of uranium biomineralisation experiments using an isolate of Serratia obtained from a sediment sample representative of the Sellafield nuclear site, UK. When supplied with glycerol phosphate, this Serratia strain was able to precipitate 1 mM of soluble U(VI) as uranyl phosphate minerals from the autunite group, under anaerobic and fermentative conditions. Under phosphate-limited anaerobic conditions and with glycerol as the electron donor, non-growing Serratia cells could precipitate 0.5 mM of uranium supplied as soluble U(VI), via reduction to nano-crystalline U(IV) uraninite. Some evidence for the reduction of solid phase uranyl(VI) phosphate was also observed. This study highlights the potential for Serratia and related species to play a role in the bioremediation of uranium contamination, via a range of different metabolic pathways, dependent on culturing or in situ conditions. PMID:26132209

PROCESS FOR PRODUCING URANIUM TETRAFLUORIDE

DOEpatents

Harvey, B.G.

1954-09-14

>This patent relates to improvements in the method for producing uranium tetrafluoride by treating an aqueous solutlon of a uranyl salt at an elevated temperature with a reducing agent effective in acld solutlon in the presence of hydrofluoric acid. Uranium tetrafluoride produced this way frequentiy contains impurities in the raw material serving as the source of uranium. Uranium tetrafluoride much less contaminated with impurities than when prepared by the above method can be prepared from materials containing such impurities by first adding a small proportion of reducing agent so as to cause a small fraction, for example 1 to 5% of the uranium tetrafluoride to be precipitated, rejecting such precipitate, and then precipitating and recovering the remainder of the uranium tetrafluoride.

Remedial Action Plan and site design for stabilization of the inactive uranium mill tailings site at Durango, Colorado: Attachment 3, Groundwater hydrology report. Revised final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1991-12-01

The US Environmental Protection Agency (EPA) has established health and environmental protection regulations to correct and prevent groundwater contamination resulting from processing activities at inactive uranium milling sites. According to the Uranium Mill Tailings Radiation Control Act of 1978, (UMTRCA) the US Department of Energy (DOE) is responsible for assessing the inactive uranium processing sites. The DOE has determined this assessment shall include information on hydrogeologic site characterization. The water resources protection strategy that describes how the proposed action will comply with the EPA groundwater protection standards is presented in Attachment 4. Site characterization activities discussed in this section include:more » Characterization of the hydrogeologic environment; characterization of existing groundwater quality; definition of physical and chemical characteristics of the potential contaminant source; and description of local water resources.« less

Carbon-free induction furnace

DOEpatents

Holcombe, Cressie E.; Masters, David R.; Pfeiler, William A.

1985-01-01

An induction furnace for melting and casting highly pure metals and alloys such as uranium and uranium alloys in such a manner as to minimize contamination of the melt by carbon derived from the materials and the environment within the furnace. The subject furnace is constructed of carbon free materials and is housed within a conventional vacuum chamber. The furnace comprises a ceramic oxide crucible for holding the charge of metal or alloy. The heating of the crucible is achieved by a plasma-sprayed tungsten susceptor surrounding the crucible which, in turn, is heated by an RF induction coil separated from the susceptor by a cylinder of inorganic insulation. The furnace of the present invention is capable of being rapidly cycled from ambient temperatures to about 1650.degree. C. for effectively melting uranium and uranium alloys without the attendant carbon contamination problems previously encountered when using carbon-bearing furnace materials.

Non-carbon induction furnace

DOEpatents

Holcombe, C.E.; Masters, D.R.; Pfeiler, W.A.

1984-01-06

The present invention is directed to an induction furnace for melting and casting highly pure metals and alloys such as uranium and uranium alloys in such a manner as to minimize contamination of the melt by carbon derived from the materials and the environment within the furnace. The subject furnace is constructed of non-carbon materials and is housed within a conventional vacuum chamber. The furnace comprises a ceramic oxide crucible for holding the charge of metal or alloys. The heating of the crucible is achieved by a plasma-sprayed tungsten susceptor surrounding the crucible which, in turn, is heated by an rf induction coil separated from the susceptor by a cylinder of inorganic insulation. The furnace of the present invention is capable of being rapidly cycled from ambient temperatures to about 1650/sup 0/C for effectively melting uranium and uranium alloys without the attendant carbon contamination problems previously encountered when using carbon-bearing furnace materials.

MULTIPLE CONTAMINANT ISSUES AND TECHNOLOGIES

EPA Science Inventory

The presentation provides information on the removal of arsenic with either nitrate, uranium, radium, radon and antimony as a co-contaminant. The technologies discussed as having the capability of removing arsenic and one of the other contaminants are reverse osmosis, anion and ...

Texturing formulations for uranium skin decontamination.

PubMed

Belhomme-Henry, Corinne; Phan, Guillaume; Huang, Nicolas; Bouvier, Céline; Rebière, François; Agarande, Michelle; Fattal, Elias

2014-09-01

Since no specific treatment exists in case of cutaneous contamination by radionuclides such as uranium, a nanoemulsion comprising calixarene molecules, known for their good chelation properties, was previously designed. However, this fluid topical form may be not suitable for optimal application on the skin or wounds. To develop a texturing pharmaceutical form for the treatment of wounded skins contaminated by uranium. The formulations consisted in oil-in-water (O/W) nanoemulsions, loaded with calixarene molecules. The external phase of the initial liquid nanoemulsion was modified with a combination of thermosensitive gelifying polymers: Poloxamer and HydroxyPropylMethylcellulose (HPMC) or methylcellulose (MC). These new formulations were characterized then tested by ex vivo experiments on Franz cells to prevent uranyl ions diffusion through excoriated pig ear skin explants. Despite strong changes in rheological properties, the physico-chemical characteristics of the new nanoemulsions, such as the size and the zeta potential as well as macroscopic aspect were preserved. In addition, on wounded skin, diffusion of uranyl ions, measured by ICP-MS, was limited to less than 5% for both HPMC and MC nanoemulsions. These results demonstrated that a hybrid formulation of nanoemulsion in hydrogel is efficient to treat uranium skin contamination.

Molybdenum Availability Is Key to Nitrate Removal in Contaminated Groundwater Environments

PubMed Central

Thorgersen, Michael P.; Lancaster, W. Andrew; Vaccaro, Brian J.; Poole, Farris L.; Rocha, Andrea M.; Mehlhorn, Tonia; Pettenato, Angelica; Ray, Jayashree; Waters, R. Jordan; Melnyk, Ryan A.; Chakraborty, Romy; Deutschbauer, Adam M.; Arkin, Adam P.

2015-01-01

The concentrations of molybdenum (Mo) and 25 other metals were measured in groundwater samples from 80 wells on the Oak Ridge Reservation (ORR) (Oak Ridge, TN), many of which are contaminated with nitrate, as well as uranium and various other metals. The concentrations of nitrate and uranium were in the ranges of 0.1 μM to 230 mM and <0.2 nM to 580 μM, respectively. Almost all metals examined had significantly greater median concentrations in a subset of wells that were highly contaminated with uranium (≥126 nM). They included cadmium, manganese, and cobalt, which were 1,300- to 2,700-fold higher. A notable exception, however, was Mo, which had a lower median concentration in the uranium-contaminated wells. This is significant, because Mo is essential in the dissimilatory nitrate reduction branch of the global nitrogen cycle. It is required at the catalytic site of nitrate reductase, the enzyme that reduces nitrate to nitrite. Moreover, more than 85% of the groundwater samples contained less than 10 nM Mo, whereas concentrations of 10 to 100 nM Mo were required for efficient growth by nitrate reduction for two Pseudomonas strains isolated from ORR wells and by a model denitrifier, Pseudomonas stutzeri RCH2. Higher concentrations of Mo tended to inhibit the growth of these strains due to the accumulation of toxic concentrations of nitrite, and this effect was exacerbated at high nitrate concentrations. The relevance of these results to a Mo-based nitrate removal strategy and the potential community-driving role that Mo plays in contaminated environments are discussed. PMID:25979890

Uptake and mobility of uranium in black oaks: implications for biomonitoring depleted uranium-contaminated groundwater.

PubMed

Edmands, J D; Brabander, D J; Coleman, D S

2001-08-01

In a preliminary study, the uptake and the mobility of uranium (U) by black oak trees (Quercus velutina) were assessed by measuring the isotopic composition of tree rings in two mature oak trees in a heavy metal contaminated bog in Concord, MA. The bog is adjacent to a nuclear industrial facility that has been processing depleted uranium (DU) since 1959. Over the past 40 years, DU has been leaking from an onsite holding basin and cooling pond down gradient to the bog where the oaks are located. Because DU has no source outside the nuclear industry, contamination from the industrial facility is readily discernable from uptake of natural U by measuring isotopic compositions. Isotope ratio analysis confirms the occurrence of DU in bark, sapwood and heartwood tree rings dating back to 1937, pre-dating the introduction of DU at the site by at least 20 years. Isotope dilution analysis indicates high concentrations of U (>3 ppb) in sapwood that drop rapidly to relatively constant concentrations (0.3-0.4 ppb) in heartwood. These data indicate that once incorporated into tree cells, U is mobile, possibly by diffusion through the tree wood. Concentrations of U in sapwood are approximately equal to average U concentrations in groundwater onsite over the past 10 years, suggesting that oak trees can be used as present-day bioindicators of U-contaminated groundwater. We suggest that regional sampling of oak bark and sapwood is a reasonable, inexpensive alternative to drilling wells to monitor shallow groundwater U contamination.

Extracellular reduction of uranium via Geobacter conductive pili as a protective cellular mechanism.

PubMed

Cologgi, Dena L; Lampa-Pastirk, Sanela; Speers, Allison M; Kelly, Shelly D; Reguera, Gemma

2011-09-13

The in situ stimulation of Fe(III) oxide reduction by Geobacter bacteria leads to the concomitant precipitation of hexavalent uranium [U(VI)] from groundwater. Despite its promise for the bioremediation of uranium contaminants, the biological mechanism behind this reaction remains elusive. Because Fe(III) oxide reduction requires the expression of Geobacter's conductive pili, we evaluated their contribution to uranium reduction in Geobacter sulfurreducens grown under pili-inducing or noninducing conditions. A pilin-deficient mutant and a genetically complemented strain with reduced outer membrane c-cytochrome content were used as controls. Pili expression significantly enhanced the rate and extent of uranium immobilization per cell and prevented periplasmic mineralization. As a result, pili expression also preserved the vital respiratory activities of the cell envelope and the cell's viability. Uranium preferentially precipitated along the pili and, to a lesser extent, on outer membrane redox-active foci. In contrast, the pilus-defective strains had different degrees of periplasmic mineralization matching well with their outer membrane c-cytochrome content. X-ray absorption spectroscopy analyses demonstrated the extracellular reduction of U(VI) by the pili to mononuclear tetravalent uranium U(IV) complexed by carbon-containing ligands, consistent with a biological reduction. In contrast, the U(IV) in the pilin-deficient mutant cells also required an additional phosphorous ligand, in agreement with the predominantly periplasmic mineralization of uranium observed in this strain. These findings demonstrate a previously unrecognized role for Geobacter conductive pili in the extracellular reduction of uranium, and highlight its essential function as a catalytic and protective cellular mechanism that is of interest for the bioremediation of uranium-contaminated groundwater.

Understanding controls on redox processes in floodplain sediments of the Upper Colorado River Basin

DOE PAGES

Noël, Vincent; Boye, Kristin; Kukkadapu, Ravi K.; ...

2017-12-15

Floodplains, heavily used for water supplies, housing, agriculture, mining, and industry, are important repositories of organic carbon, nutrients, and metal contaminants. The accumulation and release of these species is often mediated by redox processes. By understanding the physicochemical, hydrological, and biogeochemical controls on the distribution and variability of sediment redox conditions we can develop conceptual and numerical models of contaminant transport within floodplains. The Upper Colorado River Basin (UCRB) is impacted by former uranium and vanadium ore processing, resulting in contamination by V, Cr, Mn, As, Se, Mo and U. Previous authors have suggested that sediment redox activity occurring withinmore » organic carbon-enriched bodies located below the groundwater level may be regionally important to the maintenance and release of contaminant inventories, particularly uranium. To help assess this hypothesis, vertical distributions of Fe and S redox states and sulfide mineralogy were assessed in sediment cores from three floodplain sites spanning a 250 km transect of the central UCRB. Our results support the hypothesis that organic-enriched reduced sediments are important zones of biogeochemical activity within UCRB floodplains. Furthermore, we found that the presence of organic carbon, together with pore saturation, are the key requirements for maintaining reducing conditions, which were dominated by sulfate-reduction products. Sediment texture was found to be of secondary importance and to moderate the response of the system to external forcing, such as oxidant diffusion. Consequently, fine-grain sediments are relatively resistant to oxidation in comparison to coarser-grained sediments. Exposure to oxidants consumes precipitated sulfides, with a disproportionate loss of mackinawite (FeS) as compared to the more stable pyrite. The accompanying loss of redox buffering capacity creates the potential for release of sequestered radionuclides and metals. Because of their redox reactivity and stores of metals, C, and N, organic-enriched sediments are likely to be important to nutrient and contaminant mobility within UCRB floodplain aquifers.« less

Understanding controls on redox processes in floodplain sediments of the Upper Colorado River Basin

DOE Office of Scientific and Technical Information (OSTI.GOV)

Noël, Vincent; Boye, Kristin; Kukkadapu, Ravi K.

Floodplains, heavily used for water supplies, housing, agriculture, mining, and industry, are important repositories of organic carbon, nutrients, and metal contaminants. The accumulation and release of these species is often mediated by redox processes. By understanding the physicochemical, hydrological, and biogeochemical controls on the distribution and variability of sediment redox conditions we can develop conceptual and numerical models of contaminant transport within floodplains. The Upper Colorado River Basin (UCRB) is impacted by former uranium and vanadium ore processing, resulting in contamination by V, Cr, Mn, As, Se, Mo and U. Previous authors have suggested that sediment redox activity occurring withinmore » organic carbon-enriched bodies located below the groundwater level may be regionally important to the maintenance and release of contaminant inventories, particularly uranium. To help assess this hypothesis, vertical distributions of Fe and S redox states and sulfide mineralogy were assessed in sediment cores from three floodplain sites spanning a 250 km transect of the central UCRB. Our results support the hypothesis that organic-enriched reduced sediments are important zones of biogeochemical activity within UCRB floodplains. Furthermore, we found that the presence of organic carbon, together with pore saturation, are the key requirements for maintaining reducing conditions, which were dominated by sulfate-reduction products. Sediment texture was found to be of secondary importance and to moderate the response of the system to external forcing, such as oxidant diffusion. Consequently, fine-grain sediments are relatively resistant to oxidation in comparison to coarser-grained sediments. Exposure to oxidants consumes precipitated sulfides, with a disproportionate loss of mackinawite (FeS) as compared to the more stable pyrite. The accompanying loss of redox buffering capacity creates the potential for release of sequestered radionuclides and metals. Because of their redox reactivity and stores of metals, C, and N, organic-enriched sediments are likely to be important to nutrient and contaminant mobility within UCRB floodplain aquifers.« less

Removal of uranium from aqueous HF solutions

DOEpatents

Pulley, Howard; Seltzer, Steven F.

1980-01-01

This invention is a simple and effective method for removing uranium from aqueous HF solutions containing trace quantities of the same. The method comprises contacting the solution with particulate calcium fluoride to form uranium-bearing particulates, permitting the particulates to settle, and separting the solution from the settled particulates. The CaF.sub.2 is selected to have a nitrogen surface area in a selected range and is employed in an amount providing a calcium fluoride/uranium weight ratio in a selected range. As applied to dilute HF solutions containing 120 ppm uranium, the method removes at least 92% of the uranium, without introducing contaminants to the product solution.

40 CFR 142.65 - Variances and exemptions from the maximum contaminant levels for radionuclides.

Code of Federal Regulations, 2013 CFR

2013-07-01

... maximum contaminant levels for radionuclides. 142.65 Section 142.65 Protection of Environment... Available § 142.65 Variances and exemptions from the maximum contaminant levels for radionuclides. (a)(1) Variances and exemptions from the maximum contaminant levels for combined radium-226 and radium-228, uranium...

40 CFR 142.65 - Variances and exemptions from the maximum contaminant levels for radionuclides.

Code of Federal Regulations, 2012 CFR

2012-07-01

... maximum contaminant levels for radionuclides. 142.65 Section 142.65 Protection of Environment... Available § 142.65 Variances and exemptions from the maximum contaminant levels for radionuclides. (a)(1) Variances and exemptions from the maximum contaminant levels for combined radium-226 and radium-228, uranium...

40 CFR 142.65 - Variances and exemptions from the maximum contaminant levels for radionuclides.

Code of Federal Regulations, 2014 CFR

2014-07-01

... maximum contaminant levels for radionuclides. 142.65 Section 142.65 Protection of Environment... Available § 142.65 Variances and exemptions from the maximum contaminant levels for radionuclides. (a)(1) Variances and exemptions from the maximum contaminant levels for combined radium-226 and radium-228, uranium...

40 CFR 142.65 - Variances and exemptions from the maximum contaminant levels for radionuclides.

Code of Federal Regulations, 2011 CFR

2011-07-01

... maximum contaminant levels for radionuclides. 142.65 Section 142.65 Protection of Environment... Available § 142.65 Variances and exemptions from the maximum contaminant levels for radionuclides. (a)(1) Variances and exemptions from the maximum contaminant levels for combined radium-226 and radium-228, uranium...

Remediation of uranium in-situ leaching area at Straz Pod Ralskem, Czech Republic

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vokal, Vojtech; Muzak, Jiri; Ekert, Vladimir

2013-07-01

A large-scale development in exploration and production of uranium ores in the Czech Republic was done in the 2nd half of the 20. century. Many uranium deposits were discovered in the territory of the Czech Republic. One of the most considerable deposits in the Czech Republic is the site Hamr na Jezere - Straz pod Ralskem where both mining methods - the underground mining and the acidic in-situ leaching - were used. The extensive production of uranium led to widespread environmental impacts and contamination of ground waters. Over the period of 'chemical' leaching of uranium (ca. 32 years), a totalmore » of more than 4 million tons of sulphuric acid and other chemicals have been injected into the ground. Most of the products (approx. 99.5 %) of the acids reactions with the rocks are located in the Cenomanian aquifer. The contamination of Cenomanian aquifer covers the area larger then 27 km{sup 2}. The influenced volume of groundwater is more than 380 million m{sup 3}. The total amount of dissolved SO{sub 4}{sup 2-} is about 3.6 million tons. After 1990 a large-scale environmental program was established and the Czech government decided to liquidate the ISL Mine and start the remediation in 1996. The remediation consists of contaminated groundwater pumping, removing of the contaminants and discharging or reinjection of treated water. Nowadays four main remedial technological installations with sufficient capacity for reaching of the target values of remedial parameters in 2037 are used - the 'Station for Acid Solutions Liquidation No. One', the 'Mother liquor reprocessing' station, the 'Neutralization and Decontamination Station NDS 6' and the 'Neutralization and Decontamination Station NDS 10'. It is expected that the amount of withdrawn contaminants will vary from 80 000 to 120 000 tons per year. Total costs of all remediation activities are expected to be in excess of 2 billion EUR. (authors)« less

In Situ Monitoring of Groundwater Contamination Using the Kalman Filter For Sustainable Remediation

NASA Astrophysics Data System (ADS)

Schmidt, F.; Wainwright, H. M.; Faybishenko, B.; Denham, M. E.; Eddy-Dilek, C. A.

2017-12-01

Sustainable remediation - based on less intensive passive remediation and natural attenuation - has become a desirable remediation alternative at contaminated sites. Although it has a number of benefits, such as reduced waste and water/energy usage, it carries a significant burden of proof to verify plume stability and to ensure insignificant increase of risk to public health. Modeling of contaminant transport is still challenging despite recent advances in numerical methods. Long-term monitoring has, therefore, become a critical component in sustainable remediation. However, the current approach, which relies on sparse groundwater sampling, is problematic, since it could miss sudden significant changes in plume behavior. A new method is needed to combine existing knowledge about contaminant behavior and latest advances in in situ groundwater sensors. This study presents an example of the effective use of the Kalman filter approach to estimate contaminant concentrations, based on in situ measured water quality parameters (e.g. electrical conductivity and pH) along with the results of sparse groundwater sampling. The Kalman filter can effectively couple physical models and data correlations between the contaminant concentrations and in situ measured variables. We aim (1) to develop a framework capable of integrating different data types to provide accurate contaminant concentration estimates, (2) to demonstrate that these results remain reliable, even when the groundwater sampling frequency is reduced, and (3) to evaluate the future efficacy of this strategy using reactive transport simulations. This framework can also serve as an early warning system for detecting unexpected plume migration. We demonstrate our approach using historical and current groundwater data from the Savannah River Site (SRS) F-Area Seepage Basins to estimate uranium and tritium concentrations. The results show that the developed method can provide reliable estimates of contaminant concentrations. We also show that we can reduce the groundwater sampling frequency significantly, while capturing the dynamics of contaminant concentration changes. To our knowledge, this is the first study to apply data analytics to long-term groundwater monitoring extensively.

Conceptual Model of Uranium in the Vadose Zone for Acidic and Alkaline Wastes Discharged at the Hanford Site Central Plateau

DOE Office of Scientific and Technical Information (OSTI.GOV)

Truex, Michael J.; Szecsody, James E.; Qafoku, Nikolla

2014-09-01

Historically, uranium was disposed in waste solutions of varying waste chemistry at the Hanford Site Central Plateau. The character of how uranium was distributed in the vadose zone during disposal, how it has continued to migrate through the vadose zone, and the magnitude of potential impacts on groundwater are strongly influenced by geochemical reactions in the vadose zone. These geochemical reactions can be significantly influenced by the disposed-waste chemistry near the disposal location. This report provides conceptual models and supporting information to describe uranium fate and transport in the vadose zone for both acidic and alkaline wastes discharged at amore » substantial number of waste sites in the Hanford Site Central Plateau. The conceptual models include consideration of how co-disposed acidic or alkaline fluids influence uranium mobility in terms of induced dissolution/precipitation reactions and changes in uranium sorption with a focus on the conditions near the disposal site. This information, when combined with the extensive information describing uranium fate and transport at near background pH conditions, enables focused characterization to support effective fate and transport estimates for uranium in the subsurface.« less

Utilizing hydrologic, statistical, and geochemical tools to assess uranium mobility in surface and near-surface environments

NASA Astrophysics Data System (ADS)

Naftz, D. L.; Walton-Day, K. E.; Fuller, C.; Dam, W. L.; Briggs, M. A.; Snyder, T.

2015-12-01

Legacy uranium (U) mining and processing activities have resulted in soil and water contamination on Federal, state, and tribal lands in the western United States. Sites include legacy mill sites associated with U extraction now managed by the Department of Energy and thousands of waste dumps associated with U exploration, mining, and processing. Recently (2012), over 400,000 hectares of federally managed land in northern Arizona was withdrawn from consideration of mining for a 20-year period to protect the Grand Canyon watershed from potentially adverse effects of U mineral exploration and development. Ore from active and recently active U mines in the Colorado Plateau, the Henry Mountains Complex, and the Arizona Strip is transported to the only currently (2015) active conventional mill site in the western United States, located in Utah. Previous and ongoing U.S. Geological Survey assessments to examine U mobility at a variety of legacy and active sites associated with ore exploration, extraction, and processing will be presented as field-scale examples. Topics associated with site investigations will include: (1) offsite migration of radionuclides associated with the operation of the White Mesa U mill; (2) long-term contaminant transport from legacy U waste dumps on Bureau of Land Management regulated land in Utah; (3) application of incremental soil sampling techniques to determine pre- and post-mining radionuclide levels associated with planned and operating U mines in northern Arizona; (4) application of fiber optic digital temperature sensing equipment to identify areas where shallow groundwater containing elevated U levels may be discharging to a river adjacent to a reclaimed mill site in central Wyoming; and (5) field-scale manipulation of groundwater chemistry to limit U migration from a legacy upgrader site in southeastern Utah.

Exposure pathways and health effects associated with chemical and radiological toxicity of natural uranium: a review.

PubMed

Brugge, Doug; de Lemos, Jamie L; Oldmixon, Beth

2005-01-01

Natural uranium exposure derives from the mining, milling, and processing of uranium ore, as well as from ingestion of groundwater that is naturally contaminated with uranium. Ingestion and inhalation are the primary routes of entry into the body. Absorption of uranium from the lungs or digestive track is typically low but can vary depending on compound specific solubility. From the blood, two-thirds of the uranium is excreted in urine over the first 24 hours and up to 80% to 90% of uranium deposited in the bone leaves the body within 1.5 years. The primary health outcomes of concern documented with respect to uranium are renal, developmental, reproductive, diminished bone growth, and DNA damage. The reported health effects derive from experimental animal studies and human epidemiology. The Lowest Observed Adverse Effect Level (LOAEL) derived from animal studies is 50 microg/m3 for inhalation and 60 ug/kg body weight/day for ingestion. The current respiratory standard of the Occupational Safety and Health Administration (OSHA), 50 microg/m3, affords no margin of safety. Considering the safety factors for species and individual variation, the ingestion LOAEL corresponds to the daily consumption set by the World Health Organization Drinking Water Standard at 2 microg/L. Based on economic considerations, the United States Environmental Protection Agency maximum contaminant level is 30 microg/L. Further research is needed, with particular attention on the impact of uranium on indigenous populations, on routes of exposure in communities near uranium sites, on the combined exposures present at many uranium sites, on human developmental defects, and on health effects at or below established exposure standards.

PROGRESS WITH K BASINS SLUDGE RETRIEVAL STABILIZATION & PACKAGING AT THE HANFORD NUCLEAR SITE

DOE Office of Scientific and Technical Information (OSTI.GOV)

KNOLLMEYER, P.M.; PHILLIPS, C; TOWNSON, P.S.

This paper shows how Fluor Hanford and BNG America have combined nuclear plant skills from the U.S. and the U.K. to devise methods to retrieve and treat the sludge that has accumulated in K Basins at the Hanford Site over many years. Retrieving the sludge is the final stage in removing fuel and sludge from the basins to allow them to be decontaminated and decommissioned, so as to remove the threat of contamination of the Columbia River. A description is given of sludge retrieval using vacuum lances and specially developed nozzles and pumps into Consolidation Containers within the basins. Themore » special attention that had to be paid to the heat generation and potential criticality issues with the irradiated uranium-containing sludge is described. The processes developed to re-mobilize the sludge from the Consolidation Containers and pump it through flexible and transportable hose-in-hose piping to the treatment facility are explained with particular note made of dealing with the abrasive nature of the sludge. The treatment facility, housed in an existing Hanford building, is described, and the uranium-corrosion and grout packaging processes explained. The uranium corrosion process is a robust, tempered process very suitable for dealing with a range of differing sludge compositions. Optimization and simplification of the original sludge corrosion process design is described and the use of transportable and reusable equipment is indicated. The processes and techniques described in the paper are shown to have wide applicability to nuclear cleanup.« less

Reactive transport modeling of uranium 238 and radium 226 in groundwater of the Königstein uranium mine, Germany

NASA Astrophysics Data System (ADS)

Nitzsche, O.; Merkel, B.

Knowledge of the transport behavior of radionuclides in groundwater is needed for both groundwater protection and remediation of abandoned uranium mines and milling sites. Dispersion, diffusion, mixing, recharge to the aquifer, and chemical interactions, as well as radioactive decay, should be taken into account to obtain reliable predictions on transport of primordial nuclides in groundwater. This paper demonstrates the need for carrying out rehabilitation strategies before closure of the Königstein in-situ leaching uranium mine near Dresden, Germany. Column experiments on drilling cores with uranium-enriched tap water provided data about the exchange behavior of uranium. Uranium breakthrough was observed after more than 20 pore volumes. This strong retardation is due to the exchange of positively charged uranium ions. The code TReAC is a 1-D, 2-D, and 3-D reactive transport code that was modified to take into account the radioactive decay of uranium and the most important daughter nuclides, and to include double-porosity flow. TReAC satisfactorily simulated the breakthrough curves of the column experiments and provided a first approximation of exchange parameters. Groundwater flow in the region of the Königstein mine was simulated using the FLOWPATH code. Reactive transport behavior was simulated with TReAC in one dimension along a 6000-m path line. Results show that uranium migration is relatively slow, but that due to decay of uranium, the concentration of radium along the flow path increases. Results are highly sensitive to the influence of double-porosity flow. Résumé La protection des eaux souterraines et la restauration des sites miniers et de prétraitement d'uranium abandonnés nécessitent de connaître le comportement des radionucléides au cours de leur transport dans les eaux souterraines. La dispersion, la diffusion, le mélange, la recharge de l'aquifère et les interactions chimiques, de même que la décroissance radioactive, doivent être prises en compte pour obtenir des prédictions fiables concernant le transport des nucléides primaires dans les eaux souterraines. Ce papier montre la nécessité d'établir des stratégies de réhabilitation avant la fermeture de la mine d'uranium de Knigstein, près de Dresde (Allemagne). Des expériences de lessivage en colonne sur des carottes avec de l'eau enrichie en uranium fournissent des données sur le comportement de l'échange de l'uranium. La restitution de l'uranium a été observée après un lessivage par un volume supérieur à 20 fois celui des pores. Ce fort retard est dûà l'échange d'ions uranium positifs. Le code TReAC est un code de transport réactif en 1D, 2D et 3D, qui a été modifié pour prendre en compte la décroissance radioactive de l'uranium et les principaux nucléides descendants, et pour introduire l'écoulement dans un milieu à double porosité. TReAC a simulé de façon satisfaisante les courbes de restitution des expériences sur colonne et a fourni une première approche des paramètres de l'échange. L'écoulement souterrain dans la région de la mine de Knigstein a été simulé au moyen du code FLOWPATH. Le comportement du transport réactif a été simulé avec TReAC en une dimension, le long d'un axe d'écoulement long de 6000 m. Les résultats montrent que la migration de l'uranium est relativement lente ; mais du fait de la décroissance radioactive de l'uranium, la concentration en radium le long de cet axe augmente. Les résultats sont très sensibles à l'influence de l'écoulement en milieu à double porosité.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buck, E.C.; Dietz, N.L.; Bates, J.K.

Uranium contaminated soils from the Fernald Operation Site, Ohio, have been examined by a combination of optical microscopy, scanning electron microscopy with backscattered electron detection (SEM/BSE), and analytical electron microscopy (AEM). A method is described for preparing of transmission electron microscopy (TEM) thin sections by ultramicrotomy. By using these thin sections, SEM and TEM images can be compared directly. Uranium was found in iron oxides, silicates (soddyite), phosphates (autunites), and fluorite. Little uranium was associated with clays. The distribution of uranium phases was found to be inhomogeneous at the microscopic level.

Environmental assessment of remedial action at the Slick Rock uranium mill tailings sites, Slick Rock, Colorado. Revision 1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1994-09-01

The Uranium Mill Tailings Radiation Control Act of 1978 (42 USC {section}7901 et seq.), hereafter referred to as the UMTRCA, authorized the US Department of Energy (DOE) to clean up two uranium mill tailings processing sites near Slick Rock, Colorado, in San Miquel County. Contaminated materials cover an estimated 63 acres of the Union Carbide (UC) processing site and 15 ac of the North Continent (NC) processing site. The sites are within 1 mile of each other and are adjacent to the Dolores River. The sites contain concrete foundations of mill buildings, tailings piles, and areas contaminated by windblown andmore » waterborne radioactive tailings materials. The total estimated volume of contaminated materials is approximately 621,300 cubic yards (yd{sup 3}). In addition to the contamination in the two processing site areas, four VPs were found to contain contamination. As a result of the tailings being exposed to the environment, contamination associated with the UC and NC sites has leached into shallow ground water. Surface water has not been affected. The closest residence is approximately 0.3 air mi from either site. The proposed action is to remediate the UC and NC sites by removing all contaminated materials within the designing site boundaries or otherwise associated with the sites, and relocating them to, and stabilizing them at, a location approximately 5 road mi northeast of the sites on land administered by the Bureau of Land Management (BLM).« less

Proteogenomic insights into uranium tolerance of a Chernobyl's Microbacterium bacterial isolate.

PubMed

Gallois, Nicolas; Alpha-Bazin, Béatrice; Ortet, Philippe; Barakat, Mohamed; Piette, Laurie; Long, Justine; Berthomieu, Catherine; Armengaud, Jean; Chapon, Virginie

2018-04-15

Microbacterium oleivorans A9 is a uranium-tolerant actinobacteria isolated from the trench T22 located near the Chernobyl nuclear power plant. This site is contaminated with different radionuclides including uranium. To observe the molecular changes at the proteome level occurring in this strain upon uranyl exposure and understand molecular mechanisms explaining its uranium tolerance, we established its draft genome and used this raw information to perform an in-depth proteogenomics study. High-throughput proteomics were performed on cells exposed or not to 10μM uranyl nitrate sampled at three previously identified phases of uranyl tolerance. We experimentally detected and annotated 1532 proteins and highlighted a total of 591 proteins for which abundances were significantly differing between conditions. Notably, proteins involved in phosphate and iron metabolisms show high dynamics. A large ratio of proteins more abundant upon uranyl stress, are distant from functionally-annotated known proteins, highlighting the lack of fundamental knowledge regarding numerous key molecular players from soil bacteria. Microbacterium oleivorans A9 is an interesting environmental model to understand biological processes engaged in tolerance to radionuclides. Using an innovative proteogenomics approach, we explored its molecular mechanisms involved in uranium tolerance. We sequenced its genome, interpreted high-throughput proteomic data against a six-reading frame ORF database deduced from the draft genome, annotated the identified proteins and compared protein abundances from cells exposed or not to uranyl stress after a cascade search. These data show that a complex cellular response to uranium occurs in Microbacterium oleivorans A9, where one third of the experimental proteome is modified. In particular, the uranyl stress perturbed the phosphate and iron metabolic pathways. Furthermore, several transporters have been identified to be specifically associated to uranyl stress, paving the way to the development of biotechnological tools for uranium decontamination. Copyright © 2017. Published by Elsevier B.V.

SEPARATION OF URANIUM FROM OTHER METALS

DOEpatents

Hyman, H.H.

1959-07-01

The separation of uranium from other elements, such as ruthenium, zirconium, niobium, cerium, and other rare earth metals is described. According to the invention, this is accomplished by adding hydrazine to an acid aqueous solution containing salts of uranium, preferably hexavalent uranium, and then treating the mixture with a substantially water immiscible ketone, such as hexone. A reaction takes place between the ketone and the hydrazine whereby a complex, a ketazine, is formed; this complex has a greater power of extraction for uranium than the ketone by itself. When contaminating elements are present, they substantially remain in ihe aqueous solution.

Baseline risk assessment of ground water contamination at the uranium mill tailings site near Durango, Colorado. Revision 1

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1995-09-01

For the UMTRA Project site located near Durango, Colorado (the Durango site), the Surface Project cleanup occurred from 1986 to 1991. An evaluation was made to determine whether exposure to ground water contaminated by uranium processing could affect people`s health. Exposure could occur from drinking water pumped from a hypothetical well drilled in the contaminated ground water area. In addition, environmental risks may result if plants or animals are exposed to contaminated ground water, or surface water that has mixed with contaminated ground water. This risk assessment report is the first site-specific document prepared for the UMTRA Ground Water Projectmore » at the Durango site. The results of this report and further site characterization of the Durango site will be used to determine what is necessary to protect public health and the environment, and to comply with the EPA standards.« less

Spectroscopic studies of uranium species for environmental decontamination applications

NASA Astrophysics Data System (ADS)

Eng, Charlotte

After the Cold War, Department of Energy began to concentrate its efforts on cleanup of former nuclear material processing facilities, especially uranium-contaminated groundwater and soil. This research aims to study uranium association to both organic and inorganic compounds found in the contaminated environment in the hopes that the information gathered can be applied to the development and optimization of cost-effective remediation techniques. Spectroscopic and electrochemical methods will be employed to examine the behavior of uranium in given conditions to further our understanding of its impact on the environment. Uranium found in groundwater and soil bind with various ligands, especially organic ligands present in the environment due to natural sources (e.g. metabolic by-products or degradation of plants and animals) or man-made sources (e.g. chelating agents used in operating or cleanup of uranium processing facilities). We selected reasonable analogs of naturally occurring matter and studied their structure, chemical and electrochemical behavior and found that the structure of uranyl complexes depends heavily on the nature of the ligand and environmental factors such as pH. Association of uranium-organic complexes with anaerobic bacteria, Clostridium sp. was studied to establish if the bacteria can effectively bioreduce uranium while going through normal bacterial activity. It was found that the nature of the organic ligand affected the bioavailability and toxicity of the uranium on the bacteria. In addition, we have found that the type of iron corrosion products and uranyl species present on the surface of corroded steel depended on various environmental factors, which subsequently affected the removal rate of uranium by a citric acid/hydrogen peroxide/deionized water cleaning process. The method was found to remove uranium from only the topmost corrosion layers and residual uranium could be found (a) deeper in the corrosion layers where it is occluded by the steel corrosion products or (b) in areas where the dissolved uranium/iron species, the products generated by the dissolution power of citric acid, was not properly rinsed away.

Effect of saline waste solution infiltration rates on uranium retention and spatial distribution in Hanford sediments.

PubMed

Wan, Jiamin; Tokunaga, Tetsu K; Kim, Yongman; Wang, Zheming; Lanzirotti, Antonio; Saiz, Eduardo; Serne, R Jeffrey

2008-03-15

The accidental overfilling of waste liquid from tank BX-102 at the Hanford Site in 1951 put about 10 t of U(VI) into the vadose zone. In order to understand the dominant geochemical reactions and transport processes that occurred during the initial infiltration and to help understand current spatial distribution, we simulated the waste liquid spilling event in laboratory sediment columns using synthesized metal waste solution. We found that, as the plume propagated through sediments, pH decreased greatly (as much as 4 units) at the moving plume front. Infiltration flow rates strongly affect U behavior. Slower flow rates resulted in higher sediment-associated U concentrations, and higher flow rates (> or =5 cm/day) permitted practically unretarded U transport. Therefore, given the very high Ksat of most of Hanford formation, the low permeability zones within the sediment could have been most important in retaining high concentrations of U during initial release into the vadose zone. Massive amount of colloids, including U-colloids, formed at the plume fronts. Total U concentrations (aqueous and colloid) within plume fronts exceeded the source concentration by up to 5-fold. Uranium colloid formation and accumulation at the neutralized plume front could be one mechanism responsible for highly heterogeneous U distribution observed in the contaminated Hanford vadose zone.

Characterization of streamflow, water quality, and instantaneous dissolved solids, selenium, and uranium loads in selected reaches of the Arkansas River, southeastern Colorado, 2009-2010

USGS Publications Warehouse

Ivahnenko, Tamara; Ortiz, Roderick F.; Stogner, Sr., Robert W.

2013-01-01

As a result of continued water-quality concerns in the Arkansas River, including metal contamination from historical mining practices, potential effects associated with storage and movement of water, point- and nonpoint-source contamination, population growth, storm-water flows, and future changes in land and water use, the Arkansas River Basin Regional Resource Planning Group (RRPG) developed a strategy to address these issues. As such, a cooperative strategic approach to address the multiple water-quality concerns within selected reaches of the Arkansas River was developed to (1) identify stream reaches where stream-aquifer interactions have a pronounced effect on water quality and (or) where reactive transport, and physical and (or) chemical alteration of flow during conveyance, is occurring, (2) quantify loading from point sources, and (3) determine source areas and mass loading for selected constituents. (To see the complete abstract, open Report PDF.)

Monitoring of uranium concentrations in water samples collected near potentially hazardous objects in North-West Tajikistan.

PubMed

Zoriy, P; Schläger, M; Murtazaev, K; Pillath, J; Zoriy, M; Heuel-Fabianek, B

2018-01-01

The water contamination near ecologically problematic objects was investigated between 2009 and 2014 in North-West Tajikistan as a part of a joint project between Forschungszentrum Jülich and Khujand State University. The main part of this work was the determination of uranium in water samples collected near the Degmay tailings dump, the Taboshar pit lake and the Syr Darya river. More than 130 water samples were collected and analyzed to monitor the uranium concentration near the investigated areas. Two different mass spectrometers and an ion chromatograph were used for element concentration measurements. Based on the results obtained, the uranium influence of the Degmay tailings on the rivers Khoja-Bakyrgan-Say and Syr Darya and surrounding water was not found. The uranium concentration in water samples was monitored for a lengthy period at seven locations Great differences in the uranium concentration in waters collected in 2010, 2011, 2012, 2013 for each location were not observed. Drinking water samples from the region of North-West Tajikistan were analyzed and compared with the World Health Organization's guidelines. Seven out of nine drinking water samples near Taboshar exceeded the WHO guideline value for uranium concentrations (30 μg/L). The average uranium concentration of water samples from Syr Darya for the period from 2009 to 2014 was determined to be 20.1 (±5.2) μg/L. The uranium contamination of the Syr Darya was determined from the western border to the eastern border and the results are shown in this paper. Copyright © 2017 Elsevier Ltd. All rights reserved.

A study on possible use of Urtica dioica (common nettle) plants as uranium (234U, 238U) contamination bioindicator near phosphogypsum stockpile.

PubMed

Olszewski, Grzegorz; Boryło, Alicja; Skwarzec, Bogdan

The aim of this study was to determine uranium concentrations in common nettle ( Urtica dioica ) plants and corresponding soils samples which were collected from the area of phosphogypsum stockpile in Wiślinka (northern Poland). The uranium concentrations in roots depended on its concentrations in soils. Calculated BCF and TF values showed that soils characteristics and air deposition affect uranium absorption and that different uranium species have different affinities to U . dioica plants. The values of 234 U/ 238 U activity ratio indicate natural origin of these radioisotopes in analyzed plants. Uranium concentration in plants roots is negatively weakly correlated with distance from phosphogypsum stockpile.

From Nanowires to Biofilms: An Exploration of Novel Mechanisms of Uranium Transformation Mediated by Geobacter Bacteria

DOE Office of Scientific and Technical Information (OSTI.GOV)

REGUERA, GEMMA

2014-01-16

One promising strategy for the in situ bioremediation of radioactive groundwater contaminants that has been identified by the SBR Program is to stimulate the activity of dissimilatory metal-reducing microorganisms to reductively precipitate uranium and other soluble toxic metals. The reduction of U(VI) and other soluble contaminants by Geobacteraceae is directly dependent on the reduction of Fe(III) oxides, their natural electron acceptor, a process that requires the expression of Geobacter’s conductive pili (pilus nanowires). Expression of conductive pili by Geobacter cells leads to biofilm development on surfaces and to the formation of suspended biogranules, which may be physiological closer to biofilmsmore » than to planktonic cells. Biofilm development is often assumed in the subsurface, particularly at the matrix-well screen interface, but evidence of biofilms in the bulk aquifer matrix is scarce. Our preliminary results suggest, however, that biofilms develop in the subsurface and contribute to uranium transformations via sorption and reductive mechanisms. In this project we elucidated the mechanism(s) for uranium immobilization mediated by Geobacter biofilms and identified molecular markers to investigate if biofilm development is happening in the contaminated subsurface. The results provided novel insights needed in order to understand the metabolic potential and physiology of microorganisms with a known role in contaminant transformation in situ, thus having a significant positive impact in the SBR Program and providing novel concept to monitor, model, and predict biological behavior during in situ treatments.« less

Selective removal of uranium ions from contaminated waters using modified-X nanozeolite.

PubMed

Shakur, H R; Rezaee Ebrahim Saraee, Kh; Abdi, M R; Azimi, G

2016-12-01

In order to efficiently remove of uranium anionic species (which are the most dominant species of uranium in natural water at neutral pH) from contaminated waters, nano-NaX zeolite was synthesized and then modified using various divalent cations (Mg 2+ , Ca 2+ , Mn 2+ ) and ZnO nanoparticles (from 1.7 to 10.3wt%). Different characterization techniques of XRF, XRD, FE-SEM, TEM, FT-IR, and AAS were used to characterize the final synthesized absorbents. Sorption experiments by batch technique were done to study the effect of solid-liquid ratio, initial uranium concentration, contact time and temperature under neutral condition of pH and presence of all anions and cations which are available in the waters. Results showed that although nano-NaX zeolite due to its negative framework charge had a low sorption capacity for adsorption of uranium anionic species, but modification of parent nano-NaX zeolite with ZnO nanoparticles and various cations effectively improved its uranium adsorption capacity. Also, results showed that under optimum condition of pH=7.56, contact time of 60min at 27°C with solid-liquid ratio of 20g/L a maximum uranium removal efficiency of 99.7% can be obtained in the presence of all anions and cations which are available in the drinking waters by NaX/ZnO nanocomposite. Copyright © 2016 Elsevier Ltd. All rights reserved.

Groundwater remediation solutions at hanford

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gilmore, T.J.; Truex, M.J.; Williams, M.D.

2007-07-01

In 2006, Congress provided funding to the U. S. Department of Energy (DOE) to study new technologies that could be used to treat contamination from the Hanford Site that might impact the Columbia River. DOE identified three high priority sites that had groundwater contamination migrating towards the Columbia river for remediation. The contaminants included strontium-90, uranium and chromium. A natural systems approach was taken that uses a mass balance concept to frame the problem and determine the most appropriate remedial approach. This approach provides for a scientifically based remedial decision. The technologies selected to address these contaminants included an apatitemore » adsorption barrier coupled with a phyto-remediation to address the strontium-90 contamination, injection of polyphosphate into the subsurface to sequester uranium, and a bioremediation approach to reduce chromium contamination in the groundwater. The ability to provide scientifically based approaches to these sites was in large part due to work the Pacific Northwest National Laboratory developed under previous DOE Office of Science and Office of Environmental Management projects. (authors)« less

49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

Code of Federal Regulations, 2014 CFR

2014-10-01

... 49 Transportation 2 2014-10-01 2014-10-01 false Activity-mass relationships for uranium and....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U present...

49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

Code of Federal Regulations, 2012 CFR

2012-10-01

... 49 Transportation 2 2012-10-01 2012-10-01 false Activity-mass relationships for uranium and....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U present...

49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

Code of Federal Regulations, 2013 CFR

2013-10-01

... 49 Transportation 2 2013-10-01 2013-10-01 false Activity-mass relationships for uranium and....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U present...

Molybdenum Availability Is Key to Nitrate Removal in Contaminated Groundwater Environments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thorgersen, Michael P.; Lancaster, W. Andrew; Vaccaro, Brian J.

2015-05-15

The concentrations of molybdenum (Mo) and 25 other metals were measured in groundwater samples from 80 wells on the Oak Ridge Reservation (ORR) (Oak Ridge, TN), many of which are contaminated with nitrate, as well as uranium and various other metals. Moreover, the concentrations of nitrate and uranium were in the ranges of 0.1 μM to 230 mM and <0.2 nM to 580 μM, respectively. Most metals examined had significantly greater median concentrations in a subset of wells that were highly contaminated with uranium (≥126 nM). They included cadmium, manganese, and cobalt, which were 1,300- to 2,700-fold higher. A notablemore » exception, however, was Mo, which had a lower median concentration in the uranium-contaminated wells. This is significant, because Mo is essential in the dissimilatory nitrate reduction branch of the global nitrogen cycle. It is required at the catalytic site of nitrate reductase, the enzyme that reduces nitrate to nitrite. Furthermore, more than 85% of the groundwater samples contained less than 10 nM Mo, whereas concentrations of 10 to 100 nM Mo were required for efficient growth by nitrate reduction for twoPseudomonasstrains isolated from ORR wells and by a model denitrifier,Pseudomonas stutzeriRCH2. Higher concentrations of Mo tended to inhibit the growth of these strains due to the accumulation of toxic concentrations of nitrite, and this effect was exacerbated at high nitrate concentrations. The relevance of these results to a Mo-based nitrate removal strategy and the potential community-driving role that Mo plays in contaminated environments are discussed.« less

Uranium (U)-Tolerant Bacterial Diversity from U Ore Deposit of Domiasiat in North-East India and Its Prospective Utilisation in Bioremediation

PubMed Central

Kumar, Rakshak; Nongkhlaw, Macmillan; Acharya, Celin; Joshi, Santa Ram

2013-01-01

Uranium (U)-tolerant aerobic chemo-heterotrophic bacteria were isolated from the sub-surface soils of U-rich deposits in Domiasiat, North East India. The bacterial community explored at molecular level by amplified ribosomal DNA restriction analysis (ARDRA) resulted in 51 distinct phylotypes. Bacterial community assemblages at the U mining site with the concentration of U ranging from 20 to 100 ppm, were found to be most diverse. Representative bacteria analysed by 16S rRNA gene sequencing were affiliated to Firmicutes (51%), Gammaproteobacteria (26%), Actinobacteria (11%), Bacteroidetes (10%) and Betaproteobacteria (2%). Representative strains removed more than 90% and 53% of U from 100 μM and 2 mM uranyl nitrate solutions, respectively, at pH 3.5 within 10 min of exposure and the activity was retained until 24 h. Overall, 76% of characterized isolates possessed phosphatase enzyme and 53% had PIB-type ATPase genes. This study generated baseline information on the diverse indigenous U-tolerant bacteria which could serve as an indicator to estimate the environmental impact expected to be caused by mining in the future. Also, these natural isolates efficient in uranium binding and harbouring phosphatase enzyme and metal-transporting genes could possibly play a vital role in the bioremediation of metal-/radionuclide-contaminated environments. PMID:23080407

Oxidative Uranium Release from Anoxic Sediments under Diffusion-Limited Conditions.

PubMed

Bone, Sharon E; Cahill, Melanie R; Jones, Morris E; Fendorf, Scott; Davis, James; Williams, Kenneth H; Bargar, John R

2017-10-03

Uranium (U) contamination occurs as a result of mining and ore processing; often in alluvial aquifers that contain organic-rich, reduced sediments that accumulate tetravalent U, U(IV). Uranium(IV) is sparingly soluble, but may be mobilized upon exposure to nitrate (NO 3 - ) and oxygen (O 2 ), which become elevated in groundwater due to seasonal fluctuations in the water table. The extent to which oxidative U mobilization can occur depends upon the transport properties of the sediments, the rate of U(IV) oxidation, and the availability of inorganic reductants and organic electron donors that consume oxidants. We investigated the processes governing U release upon exposure of reduced sediments to artificial groundwater containing O 2 or NO 3 - under diffusion-limited conditions. Little U was mobilized during the 85-day reaction, despite rapid diffusion of groundwater within the sediments and the presence of nonuraninite U(IV) species. The production of ferrous iron and sulfide in conjunction with rapid oxidant consumption suggested that the sediments harbored large concentrations of bioavailable organic carbon that fueled anaerobic microbial respiration and stabilized U(IV). Our results suggest that seasonal influxes of O 2 and NO 3 - may cause only localized mobilization of U without leading to export of U from the reducing sediments when ample organic carbon is present.

Spatial Variation and Assessment of Heavy Metal and Radioactive Risk in Farmland around a Retired Uranium Mine

NASA Astrophysics Data System (ADS)

Liang, Jie; Shi, Chen-hao; Zeng, Guang-ming; Zhong, Min-zhou; Yuan, Yu-jie

2017-07-01

In recent years, heavy metal contamination in the environment has been attracted worldwide attention due to their toxicity, persistence,extensive sources and non-biodegradable properties. We herein investigate variation trend and risk of heavy metal and radiation distribution in the former mine stope, former mineral ore stockyard, and mine road with surface soils of a retired uranium mine in the mid-south of China. The mean concentrations (mg/kg) of Pb,Cd,Cu,Zn,As,Hg,Cr,Mn,Ni,U, and 232Th were analyzed according to the corresponding background values in Hunan, China. The Geo-accumulation index (Igeo ) were used for the assessment of pollution level of heavy metals and the radioactive elements of U and 232Th. Then, Pollution load index (PLI) and GIS techniquewere integrated to assess spatial distribution of heavy metal contamination and radioactive contamination. Results confirmed that three areas in the retired uranium mine was a primary source of pollution, which showed anthropogenic origin mainly from agricultural runoff, hydrometallurgy from chemical industries, radioactive tailings, and electroplating industriesfinally drained into Zishui River and Xiangjiang River. Based on the actual situation, some suggestions were put forward for the treatment of the retired uranium mine in conclusion.

Uranium reduction and microbial community development in response to stimulation with different electron donors.

PubMed

Barlett, Melissa; Moon, Hee Sun; Peacock, Aaron A; Hedrick, David B; Williams, Kenneth H; Long, Philip E; Lovley, Derek; Jaffe, Peter R

2012-07-01

Stimulating microbial reduction of soluble U(VI) to less soluble U(IV) shows promise as an in situ bioremediation strategy for uranium contaminated groundwater, but the optimal electron donors for promoting this process have yet to be identified. The purpose of this study was to better understand how the addition of various electron donors to uranium-contaminated subsurface sediments affected U(VI) reduction and the composition of the microbial community. The simple electron donors, acetate or lactate, or the more complex donors, hydrogen-release compound (HRC) or vegetable oil, were added to the sediments incubated in flow-through columns. The composition of the microbial communities was evaluated with quantitative PCR probing specific 16S rRNA genes and functional genes, phospholipid fatty acid analysis, and clone libraries. All the electron donors promoted U(VI) removal, even though the composition of the microbial communities was different with each donor. In general, the overall biomass, rather than the specific bacterial species, was the factor most related to U(VI) removal. Vegetable oil and HRC were more effective in stimulating U(VI) removal than acetate. These results suggest that the addition of more complex organic electron donors could be an excellent option for in situ bioremediation of uranium-contaminated groundwater.

2015 Advanced Site Investigation and Monitoring Report Riverton, Wyoming, Processing Site September 2016

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frazier, William; Campbell, Sam

The U.S. Department of Energy conducted initial groundwater characterization of the Riverton, Wyoming, Processing Site in the 1990s. The characterization culminated in a Site Observational Work Plan in 1998 that recommended a natural flushing compliance strategy. Results of verification monitoring indicated that natural flushing was generally progressing as expected until June 2010, when significant increases in contaminant concentrations were measured in several monitoring wells downgradient of the site after the area flooded. In response to the unexpected results following the flood, an enhanced characterization of the surficial aquifer was conducted in 2012, which included installation of 103 boreholes along ninemore » transects with a Geoprobe, collection of 103 water samples and 65 soil samples, laboratory tests on the soil samples, and additional groundwater modeling. This advanced site investigation report summarizes additional investigation in 2015 through the use of backhoe trenching, sonic drilling, multilevel monitoring wells, direct-push drilling, and temporary well points to collect soil and groundwater samples. Additional surface water measurements were made included the installation of a stilling well and the measurement of stream elevation along the Wind River to approximate upgradient groundwater heads. Groundwater sampling included the addition of geochemical constituents and isotopes that have not been sampled in the past to better understand post-flood conditions and the possibility of additional or ongoing contaminant sources. This sampling was performed to (1) better define the contaminant plumes, (2) verify the occurrence of persistent secondary contaminant sources, (3) better understand the reason for the contaminant spikes after a 2010 flood, and (4) assess contaminant plume stagnation near the Little Wind River. This report provides data analyses and interpretations for the 2015 site investigation that addresses these issues and provides recommendations for future efforts. Observations from trenches and sonic drilling indicate the general lithology of the shallow, unconsolidated sediments consists of a silt zone at the surface that ranges from 2.5 to 4.8 feet below ground surface, underlain by sand and gravel, underlain by the top of the weathered bedrock (Wind River Formation). Soil data from trenches and sonic drilling indicate (1) elevated concentrations of several constituents in the silt zone, likely due to the formation of evaporites, (2) uranium is the only measured element that appears to be concentrated in the silt over the groundwater contaminant plume, (3) in the former tailings impoundment area, there may be a thin unsaturated zone with elevated uranium in the native material just below the fill, (4) in the former tailings impoundment area, slightly higher uranium concentrations occur in the underlying saturated sand and gravel, and (5) several bedrock samples have a unique geochemical signature, generally related to a higher silt content. Assessment of groundwater flow included measuring river elevations along the Wind River and installing the temporary well points adjacent to the Little Wind River that provided additional data points to refine contours for water table elevations. These data confirm past interpretations of groundwater flow to the southeast across the site toward the Little Wind River. Hydraulic head elevations between paired surficial and semiconfined aquifer wells indicate variable vertical gradients across the site with the potential for upward and downward flow. Additional direct-push drilling and groundwater sampling confirmed the contaminant plume configuration, but it also revealed a low-sulfate-concentration zone at the edge of the former tailings impoundment. Temporary well points provided better definition of plume concentrations at the bank of the Little Wind River, and data from these wells indicate plume discharge to the river. Additional sampling in an area southwest of the plume that had elevated uranium groundwater concentrations in the past did not have any uranium concentrations above the U.S. Environmental Protection Agency maximum concentration limit for uranium. Results from multilevel monitoring wells indicate some geochemical differences with depth, but overall concentrations are similar to those in nearby conventional monitoring wells in the long-term monitoring program. Geochemistry data from these multilevel monitoring wells confirm the general increase in contaminant concentrations toward the river and toward the plume centerline for chloride, sulfate, and uranium but highlight geochemical controls on calcium. Iron data indicate slightly reducing conditions, especially near water table and bedrock surfaces, with more oxidizing conditions in the middle of the sand and gravel. Uranium activity ratios (234U/238U) confirm the uranium plume in the surficial aquifer as being mill related, and the area to the southwest outside the plume as natural, non-mill related. In the semiconfined aquifer, evidence of aquifer connection and impacts from the mill is inconclusive. Values of δD and δ 18O suggest water is derived from different sources and tritium data confirm that the semiconfined aquifer water is generally older than the surficial aquifer water. However, these data do indicate some groundwater communication from the surficial aquifer into the semiconfined aquifer, which resulted in δD and δ 18O and tritium values in the semiconfined aquifer that are more similar to those in the surficial aquifer. Values of δ 34S sulfate in the semiconfined aquifer combined with sulfate concentrations indicate the potential for some mill- related sulfate in the semiconfined aquifer, albeit limited to an area near and beneath the former tailings impoundment. Uranium and molybdenum concentrations in the semiconfined aquifer are below groundwater standards in all wells. However, the elevated molybdenum concentrations at one semiconfined aquifer well underneath the former tailings impoundment suggests a mill- derived source for the uranium and molybdenum in that well. It is possible that aquifer cross- communication occurred when the tailings impoundment was active and created a higher head. Current cross-communication appears unlikely given the large differences in tritium values and an upward hydraulic head at this location. Nine domestic wells are located within the institutional control boundary (eight in the confined aquifer and one in the semiconfined aquifer). Uranium and molybdenum concentrations in all samples collected from these wells were one or two orders of magnitude below the groundwater standards. Surface water flow in the Little Wind River in September 2015 was low compared to historical averages for that time of year. As a result, the uranium concentration measured in the Little Wind River was at a historical maximum at the sampling location upstream of the site. However, the impact of uranium discharge from the groundwater plume into the Little Wind River was not measureable. Elevated sulfate concentrations were observed in an outfall ditch related to an active sulfuric acid plant. Uranium concentrations in the oxbow lake remain at concentrations above the groundwater standard. Plume contaminant concentrations had returned to levels found prior to the 2010 flood by the end of 2015. However, these concentrations still exceed model predictions for natural flushing, and the current data indicate that natural flushing to achieve remediation goals within the 100-year time period is not likely, especially with the high potential for additional floods in the update to the conceptual site model (CSM), soil data indicate additional contaminant sources, specifically uranium, in evaporites within the silt layer over the uranium plume and in naturally reduced zones (NRZs). Additional zones of slightly elevated uranium concentration are in the native sediments just above the water table but below the fill layer in the former tailings impoundment area. This area also has slightly elevated uranium in the sand and gravel below the water table. Mass balance calculations indicate that small amounts of dissolution in any of these zones with increased uranium in the solid phase can produce groundwater uranium concentrations above the groundwater standard and could account for the post-flood uranium spike. The additional uranium near the former tailings impoundment provides a mechanism for a continuing source for the uranium plume that was not considered in earlier natural flushing models. In addition, uranium released from the silt layer or the NRZs seasonally and during flooding may add uranium to the groundwater plume near the Little Wind River. These mechanisms provide a possible explanation for plume persistence, along with spikes in concentrations during floods, that creates the current plume configuration. Additional updates to the CSM include (1) chloride flushes more rapidly than uranium beneath the former mill site, (2) chloride in the silt layer provides a scenario in which chloride cannot be used as a conservative tracer (especially in areas prone to flooding), (3) uranium concentrations with depth can be variable (especially below NRZs), and (4) calcite and gypsum solubility limits appear to provide important geochemical controls on groundwater geochemistry. The conclusion of this study provides several recommendations for additional work to refine the CSM and continue assessment of the natural flushing compliance strategy. Recommendations for additional work include targeted soil and groundwater sampling to assess geochemical conditions, distribution of contaminants, and groundwater/surface water interaction; additional column tests to provide data for geochemical modeling; and development of an updated groundwater flow model, which will be used in conjunction with a geochemical model to assess the viability of the natural flushing compliance strategy.« less

URANIUM RECOVERY AND PURIFICATION PROCESS AND PRODUCTION OF HIGH PURITY URANIUM TETRAFLUORIDE

DOEpatents

Bailes, R.H.; Long, R.S.; Grinstead, R.R.

1957-09-17

A process is described wherein an anionic exchange technique is employed to separate uramium from a large variety of impurities. Very efficient and economical purification of contamimated uranium can be achieved by treatment of the contaminated uranium to produce a solution containing a high concentration of chloride. Under these conditions the uranium exists as an aniomic chloride complex. Then the uranium chloride complex is adsorbed from the solution on an aniomic exchange resin, whereby a portion of the impurities remain in the solution and others are retained with the uramium by the resin. The adsorbed impurities are then removed by washing the resin with pure concentrated hydrochloric acid, after which operation the uranium is eluted with pure water yielding an acidic uranyl chloride solution of high purity.

Illicit Trafficking of Natural Radionuclides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Friedrich, Steinhaeusler; Lyudmila, Zaitseva

2008-08-07

Natural radionuclides have been subject to trafficking worldwide, involving natural uranium ore (U 238), processed uranium (yellow cake), low enriched uranium (<20% U 235) or highly enriched uranium (>20% U 235), radium (Ra 226), polonium (Po 210), and natural thorium ore (Th 232). An important prerequisite to successful illicit trafficking activities is access to a suitable logistical infrastructure enabling an undercover shipment of radioactive materials and, in case of trafficking natural uranium or thorium ore, capable of transporting large volumes of material. Covert en route diversion of an authorised uranium transport, together with covert diversion of uranium concentrate from anmore » operating or closed uranium mines or mills, are subject of case studies. Such cases, involving Israel, Iran, Pakistan and Libya, have been analyzed in terms of international actors involved and methods deployed. Using international incident data contained in the Database on Nuclear Smuggling, Theft and Orphan Radiation Sources (DSTO) and international experience gained from the fight against drug trafficking, a generic Trafficking Pathway Model (TPM) is developed for trafficking of natural radionuclides. The TPM covers the complete trafficking cycle, ranging from material diversion, covert material transport, material concealment, and all associated operational procedures. The model subdivides the trafficking cycle into five phases: (1) Material diversion by insider(s) or initiation by outsider(s); (2) Covert transport; (3) Material brokerage; (4) Material sale; (5) Material delivery. An Action Plan is recommended, addressing the strengthening of the national infrastructure for material protection and accounting, development of higher standards of good governance, and needs for improving the control system deployed by customs, border guards and security forces.« less

Illicit Trafficking of Natural Radionuclides

NASA Astrophysics Data System (ADS)

Friedrich, Steinhäusler; Lyudmila, Zaitseva

2008-08-01

Natural radionuclides have been subject to trafficking worldwide, involving natural uranium ore (U 238), processed uranium (yellow cake), low enriched uranium (<20% U 235) or highly enriched uranium (>20% U 235), radium (Ra 226), polonium (Po 210), and natural thorium ore (Th 232). An important prerequisite to successful illicit trafficking activities is access to a suitable logistical infrastructure enabling an undercover shipment of radioactive materials and, in case of trafficking natural uranium or thorium ore, capable of transporting large volumes of material. Covert en route diversion of an authorised uranium transport, together with covert diversion of uranium concentrate from an operating or closed uranium mines or mills, are subject of case studies. Such cases, involving Israel, Iran, Pakistan and Libya, have been analyzed in terms of international actors involved and methods deployed. Using international incident data contained in the Database on Nuclear Smuggling, Theft and Orphan Radiation Sources (DSTO) and international experience gained from the fight against drug trafficking, a generic Trafficking Pathway Model (TPM) is developed for trafficking of natural radionuclides. The TPM covers the complete trafficking cycle, ranging from material diversion, covert material transport, material concealment, and all associated operational procedures. The model subdivides the trafficking cycle into five phases: (1) Material diversion by insider(s) or initiation by outsider(s); (2) Covert transport; (3) Material brokerage; (4) Material sale; (5) Material delivery. An Action Plan is recommended, addressing the strengthening of the national infrastructure for material protection and accounting, development of higher standards of good governance, and needs for improving the control system deployed by customs, border guards and security forces.

The effects of phosphorus additions on the sedimentation of contaminants in a uranium mine pit-lake.

PubMed

Dessouki, Tarik C E; Hudson, Jeff J; Neal, Brian R; Bogard, Matthew J

2005-08-01

We investigated the usefulness of phytoplankton for the removal of surface water contaminants. Nine large mesocosms (92.2m(3)) were suspended in the flooded DJX uranium pit at Cluff Lake (Saskatchewan, Canada), and filled with highly contaminated mine water. Each mesocosm was fertilized with a different amount of phosphorus throughout the 35 day experiment to stimulate phytoplankton growth, and to create a range in phosphorus load (g) to examine how contaminants may be affected by different nutrient regimes. Algal growth was rapid in fertilized mesocosms (as demonstrated by chlorophyll a profiles). As phosphorus loads increased there were significant declines (p<0.05) in the surface water concentrations of As, Co, Cu, Mn, Ni, and Zn. This decline was near significant for uranium (p=0.065). The surface water concentrations of Ra-226, Mo, and Se showed no relationship to phosphorus load. Contaminant concentrations in sediment traps suspended at the bottom of each mesocosm generally showed the opposite trend to that observed in the surface water, with most contaminants (As, Co, Cu, Mn, Ni, Ra-226, U, and Zn) exhibiting a significant positive relationship (p<0.05) with phosphorus load. Selenium and Mo did not respond to nutrient treatments. Our results suggest that phytoremediation has the potential to lower many surface water contaminants through the sedimentation of phytoplankton. Based on our results, we estimate that the Saskatchewan Surface Water Quality Objectives (SSWQO) for DJX pit would be met in approximately 45 weeks for Co, 65 weeks for Ni, 15 weeks for U, and 5 weeks for Zn.

Blood-Brain Barrier Transport of Uranium

DTIC Science & Technology

2005-09-01

1.0) as well as an in vivo approach to delineate the pharmacokinetics of uranium transport across the BBB in rats embedded with DU fragments (Technical...observed for signs of morbidity. Surgical procedure: Animals were anesthetized with - xylazine and 80 mg/kg ketamine prior to- surger- gastrocnemius...2 ) in monkeys, dogs and rats (52, 53) . These researchers found that the lungs and tracheobronchial lymph nodes were the major sites of uranium

Biomineralization of U(VI) phosphate promoted by microbially-mediated phytate hydrolysis in contaminated soils

NASA Astrophysics Data System (ADS)

Salome, Kathleen R.; Beazley, Melanie J.; Webb, Samuel M.; Sobecky, Patricia A.; Taillefert, Martial

2017-01-01

The bioreduction of uranium may immobilize a significant fraction of this toxic contaminant in reduced environments at circumneutral pH. In oxic and low pH environments, however, the low solubility of U(VI)-phosphate minerals also makes them good candidates for the immobilization of U(VI) in the solid phase. As inorganic phosphate is generally scarce in soils, the biomineralization of U(VI)-phosphate minerals via microbially-mediated organophosphate hydrolysis may represent the main immobilization process of uranium in these environments. In this study, contaminated sediments were incubated aerobically in two pH conditions to examine whether phytate, a naturally-occurring and abundant organophosphate in soils, could represent a potential phosphorous source to promote U(VI)-phosphate biomineralization by natural microbial communities. While phytate hydrolysis was not evident at pH 7.0, nearly complete hydrolysis was observed both with and without electron donor at pH 5.5, suggesting indigenous microorganisms express acidic phytases in these sediments. While the rate of hydrolysis of phytate generally increased in the presence of uranium, the net rate of inorganic phosphate production in solution was decreased and inositol phosphate intermediates were generated in contrast to similar incubations conducted without uranium. These findings suggest uranium stress enhanced the phytate-metabolism of the microbial community, while simultaneously inhibiting phosphatase production and/or activity by the indigenous population. Finally, phytate hydrolysis drastically decreased uranium solubility, likely due to formation of ternary sorption complexes, U(VI)-phytate precipitates, and U(VI)-phosphate minerals. Overall, the results of this study provide evidence for the ability of natural microbial communities to liberate phosphate from phytate in acidic sediments, possibly as a detoxification mechanism, and demonstrate the potential utility of phytate-promoted uranium immobilization in subsurface environments. These processes should be investigated in more detail with pure cultures isolated from these sediments.

Hydrologic transport of depleted uranium associated with open air dynamic range testing at Los Alamos National Laboratory, New Mexico, and Eglin Air Force Base, Florida

DOE Office of Scientific and Technical Information (OSTI.GOV)

Becker, N.M.; Vanta, E.B.

Hydrologic investigations on depleted uranium fate and transport associated with dynamic testing activities were instituted in the 1980`s at Los Alamos National Laboratory and Eglin Air Force Base. At Los Alamos, extensive field watershed investigations of soil, sediment, and especially runoff water were conducted. Eglin conducted field investigations and runoff studies similar to those at Los Alamos at former and active test ranges. Laboratory experiments complemented the field investigations at both installations. Mass balance calculations were performed to quantify the mass of expended uranium which had transported away from firing sites. At Los Alamos, it is estimated that more thanmore » 90 percent of the uranium still remains in close proximity to firing sites, which has been corroborated by independent calculations. At Eglin, we estimate that 90 to 95 percent of the uranium remains at test ranges. These data demonstrate that uranium moves slowly via surface water, in both semi-arid (Los Alamos) and humid (Eglin) environments.« less

Refining the site conceptual model at a former uranium mill site in Riverton, Wyoming, USA

DOE PAGES

Dam, William; Campbell, Sam; Johnson, Ray; ...

2015-07-07

Milling activities at a former uranium mill site near Riverton, Wyoming, USA, contaminated the shallow groundwater beneath and downgradient of the site. Although the mill operated for <6 years (1958-1963), its impact remains an environmental liability. Groundwater modeling predicted that contaminant concentrations were declining steadily, which confirmed the conceptual site model (CSM). However, local flooding in 2010 mobilized contaminants that migrated downgradient from the Riverton site and resulted in a dramatic increase in groundwater contaminant concentrations. This observation indicated that the original CSM was inadequate to explain site conditions and needed to be refined. In response to the new observationsmore » after the flood, a collaborative investigation to better understand site conditions and processes commenced. This investigation included installing 103 boreholes to collect soil and groundwater samples, sampling and analysis of evaporite minerals along the bank of the Little Wind River, an analysis of evaportranspiration in the shallow aquifer, and sampling naturally organic-rich sediments near groundwater discharge areas. The enhanced characterization revealed that the existing CSM did not account for high uranium concentrations in groundwater remaining on the former mill site and groundwater plume stagnation near the Little Wind River. Observations from the flood and subsequent investigations indicate that additional characterization is still needed to continue refining the CSM and determine the viability of the natural flushing compliance strategy. Additional sampling, analysis, and testing of soil and groundwater are necessary to investigate secondary contaminant sources, mobilization of contaminants during floods, geochemical processes, contaminant plume stagnation, distribution of evaporite minerals and organic-rich sediments, and mechanisms and rates of contaminant transfer from soil to groundwater. Future data collection will be used to continually revise the CSM and evaluate the compliance strategy at the site.« less

Measuring and predicting the transport of actinides and fission product contaminants in unsaturated prairie soil

NASA Astrophysics Data System (ADS)

Sims, D. J.

Soil samples have been taken in 2001 from the area of a 1951 release from an underground storage tank of 6.7 L of an aqueous solution of irradiated uranium (360 GBq). A simulation of the dispersion of the actinides and fission products was conducted in the laboratory using irradiated natural uranium, non-irradiated natural uranium and metal standards dissolved in acidic aqueous solutions and added to soil columns containing uncontaminated prairie soil. The lab soil columns were allowed 12 to 14 months for contaminant transport. Soil samples were analyzed using gamma-ray spectroscopy, neutron activation analysis (NAA) and liquid scintillation counting (LSC) to determine the elemental concentrations of U, Cs and Sr. Diffusion coefficients from the 50 year soil samples and the lab soil samples were determined. The measured diffusion coefficients from the field samples were 3.0 x 10-4 cm2 s-1 (Cs-137), 1.8 x 10-5 cm2 s-1 (U-238) and 2.6 x 10-3 cm2 s-1 (Sr-90) and the values determined from lab simulation were 5 x 10-6 cm 2 s-1 (Cs-137), 3 x 10-5 cm2 s-1 (U-238) and 1.9 x 10-5 cm 2 s-1 (Sr-90). The differences between the sets of diffusion coefficients can be attributed to differences in retardation effects, weather effects and changes in the soil characteristics when transporting, such as porosity. The analytical work showed that Cs-137 content of soil can be determined effectively using gamma-ray spectroscopy; U-238 content can be measured using NAA; and Sr-90 content can be measured using LSC. For non- and low-radioactive species, it was shown that both flame atomic absorption spectrometry (FAAS) and inductively-coupled plasma-mass spectrometry (ICP-MS) gave comparable results for Sr, Cs and Sm, with the average values ranging from 0.5 to 4.5 ppm of each other. The U-238 content results from NAA and from ICP-MS showed general agreement with an average difference of 81.3 ppm on samples having concentrations up to 988.2 ppm. The difference may have been due to matrix interference. It was determined through finite element modeling that 250 years after the 1951 release, the soil concentration of the three contaminant of U-238, Sr-90 and Cs-137 will be less than their respective soil clearance level values and therefore will not pose a long term environmental hazard. The fastest nuclide to reach the water table, at a depth of 45 m below the surface, at Suffield Site 27 was calculated to be Sr-90 after a period of 15,000 years. Therefore, it is not necessary to remove the subsurface soil at Site 27 for site decontamination but it is recommended that a "no-digging" policy, except for scientific research, be enforced at this site.

Comparison of Grab, Air, and Surface Results for Radiation Site Characterization

NASA Astrophysics Data System (ADS)

Glassford, Eric Keith

2011-12-01

The use of proper sampling methods and sample types for evaluating sites believed to be contaminated with radioactive materials is necessary to avoid misrepresenting conditions at the site. This study was designed to investigate if the site characterization, based upon uranium contamination measured in different types of samples, is dependent upon the mass of the sample collected. A bulk sample of potentially contaminated interior dirt was collected from an abandoned metal processing mill that rolled uranium between 1948 and 1956. The original mill dates from 1910 and has a dirt floor. The bulk sample was a mixture of dirt, black and yellow particles of metal dust, and small fragments of natural debris. Small mass (approximately 0.75 grams (g)) and large mass (approximately 70g) grab samples were prepared from the bulk sample material to simulate collection of a "grab" type sample. Air sampling was performed by re-suspending a portion of the bulk sample material using a vibration table to simulate airborne contamination that might be present during site remediation. Additionally, samples of removable contaminated surface dust were collected on 47 mm diameter filter paper by wiping the surfaces of the exposure chamber used to resuspend the bulk material. Certified reference materials, one containing a precisely known quantity of U 3O8 and one containing a known quantity of natural uranium, were utilized to calibrate the gamma spectrometry measurement system. Non-destructive gamma spectrometry measurements were used to determine the content of uranium-235 (235U) at 185 keV and 143 keV, thorium-234 (234Th) at 63 keV, and protactinium-234m (234mPa) at 1001 keV in each sample. Measurement of natural uranium in small, 1 g samples is usually accomplished by radiochemical analysis in order to measure alpha particles emitted by 238U, 235U, and 234U. However, uranium in larger bulk samples can also be measured non-destructively using gamma spectrometry to detect the low energy photons from 234Th and 234mPa, the short-lived decay products of 238U, and 235U. Two sided t-tests and coefficient of variation were used to compare sampling types. The large grab samples had the lowest calculated coefficient of variation results for activity and atom percentage. The wipe samples had the highest calculated coefficient of variation of mean specific activity (dis/sec/g) for all three energies. The air filter samples had the highest coefficient of variation calculation for mean atom percentage, for both uranium isotopes examined. The data indicated that the large mass sample was the most effective at characterizing the rolling mill radioactive site conditions, since this would indicate which samples had the smallest variations compared to the mean. Additionally, measurement results of natural uranium in the samples indicate that the distribution of radioactive contamination at the sampling location is most likely non-homogeneous and that the size of the sample collected and analyzed must be sufficiently large to insure that the analytical results are truly representative of the activity present.

Environmental Education in Brazil: Preventive Measures to Avoid Contamination with U and Th

DOE Office of Scientific and Technical Information (OSTI.GOV)

Silva Pastura, Valeria Fonseca da; Wieland, Patricia

2008-08-07

Aiming at increasing awareness of radiation health effects, environmental issues and preventive measures, the Nuclear Energy National Commission (CNEN) launched in 2004 an education and public outreach programme for mine workers, students, teachers, governmental leaders, labor representatives and members of communities nearby small mining sites at the North and Northeast regions. Many Brazilian conventional mines present a significant risk of exposure to radiation due to Uranium and Thorium. CNEN inspects the mines but there are several small mining sites dedicated to open pit short term mineral extraction, called 'garimpagem', that are of difficult control. Therefore, information at large about preventivemore » measures to avoid contamination during exploration, transportation and storage is necessary. CNEN developed an educational campaign which includes a series of open seminars, talks, folders, booklets and posters. The objective of this paper is to present the Brazilian educational campaign to avoid contamination risks at those small mineral exploration sites and its results. This campaign is a joint task that receives collaboration of other organizations such as federal police, schools and universities.« less

Environmental Education in Brazil: Preventive Measures to Avoid Contamination with U and Th

NASA Astrophysics Data System (ADS)

da Silva Pastura, Valéria Fonseca; Wieland, Patricia

2008-08-01

Aiming at increasing awareness of radiation health effects, environmental issues and preventive measures, the Nuclear Energy National Commission (CNEN) launched in 2004 an education and public outreach programme for mine workers, students, teachers, governmental leaders, labor representatives and members of communities nearby small mining sites at the North and Northeast regions. Many Brazilian conventional mines present a significant risk of exposure to radiation due to Uranium and Thorium. CNEN inspects the mines but there are several small mining sites dedicated to open pit short term mineral extraction, called "garimpagem", that are of difficult control. Therefore, information at large about preventive measures to avoid contamination during exploration, transportation and storage is necessary. CNEN developed an educational campaign which includes a series of open seminars, talks, folders, booklets and posters. The objective of this paper is to present the Brazilian educational campaign to avoid contamination risks at those small mineral exploration sites and its results. This campaign is a joint task that receives collaboration of other organizations such as federal police, schools and universities.

Concentration and characteristics of depleted uranium in water, air and biological samples collected in Serbia and Montenegro.

PubMed

Jia, Guogang; Belli, Maria; Sansone, Umberto; Rosamilia, Silvia; Gaudino, Stefania

2005-09-01

During the Balkan conflicts, in 1995 and 1999, depleted uranium (DU) rounds were employed and were left in the battlefield. Health concern is related to the risk arising from contamination of the environment with DU penetrators and dust. In order to evaluate the impact of DU on the environment and population in Serbia and Montenegro, radiological surveys of DU in water, air and biological samples were carried out over the period 27 October-5 November 2001. The uranium isotopic concentrations in biological samples collected in Serbia and Montenegro, mainly lichens and barks, were found to be in the range of 0.67-704 Bqkg(-1) for (238)U, 0.48-93.9 Bqkg(-1) for (234)U and 0.02-12.2 Bqkg(-1) for (235)U, showing uranium levels to be higher than in the samples collected at the control sites. Moreover, (236)U was detectable in some of the samples. The isotopic ratios of (234)U/(238)U showed DU to be detectable in many biological samples at all examined sites, especially in Montenegro, indicating widespread ground-surface DU contamination, albeit at very low level. The uranium isotopic concentrations in air obtained from the air filter samples collected in Serbia and Montenegro were found to be in the range of 1.99-42.1 microBqm(-3) for (238)U, 0.96-38.0 microBqm(-3) for (234)U, and 0.05-1.83 microBqm(-3) for (235)U, being in the typical range of natural uranium values. Thus said, most of the air samples are DU positive, this fact agreeing well with the widespread DU contamination detected in the biological samples. The uranium concentrations in water samples collected in Serbia and Montenegro were found to be in the range of 0.40-21.9 mBql(-1) for (238)U, 0.27-28.1 mBql(-1) for (234)U, and 0.01-0.88 mBql(-1) for (235)U, these values being much lower than those in mineral water found in central Italy and below the WHO guideline for drinking water. From a radiotoxicological point of view, at this moment there is no significant radiological risk related to these investigated sites in terms of possible DU contamination of water, air and/or plants.

A coupled modelling effort to study the fate of contaminated sediments downstream of the Coles Hill deposit, Virginia, USA

NASA Astrophysics Data System (ADS)

Castro-Bolinaga, C. F.; Zavaleta, E. R.; Diplas, P.

2015-03-01

This paper presents the preliminary results of a coupled modelling effort to study the fate of tailings (radioactive waste-by product) downstream of the Coles Hill uranium deposit located in Virginia, USA. The implementation of the overall modelling process includes a one-dimensional hydraulic model to qualitatively characterize the sediment transport process under severe flooding conditions downstream of the potential mining site, a two-dimensional ANSYS Fluent model to simulate the release of tailings from a containment cell located partially above the local ground surface into the nearby streams, and a one-dimensional finite-volume sediment transport model to examine the propagation of a tailings sediment pulse in the river network located downstream. The findings of this investigation aim to assist in estimating the potential impacts that tailings would have if they were transported into rivers and reservoirs located downstream of the Coles Hill deposit that serve as municipal drinking water supplies.

quantifying and Predicting Reactive Transport

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peter C. Burns, Department of Civil Engineering and Geological Sciences, University of Notre Dame

2009-12-04

This project was led by Dr. Jiamin Wan at Lawrence Berkeley National Laboratory. Peter Burns provided expertise in uranium mineralogy and in identification of uranium minerals in test materials. Dr. Wan conducted column tests regarding uranium transport at LBNL, and samples of the resulting columns were sent to Dr. Burns for analysis. Samples were analyzed for uranium mineralogy by X-ray powder diffraction and by scanning electron microscopy, and results were provided to Dr. Wan for inclusion in the modeling effort. Full details of the project can be found in Dr. Wan's final reports for the associated effort at LBNL.

Grand Rounds: Nephrotoxicity in a Young Child Exposed to Uranium from Contaminated Well Water

PubMed Central

Magdo, H. Sonali; Forman, Joel; Graber, Nathan; Newman, Brooke; Klein, Kathryn; Satlin, Lisa; Amler, Robert W.; Winston, Jonathan A.; Landrigan, Philip J.

2007-01-01

Context Private wells that tap groundwater are largely exempt from federal drinking-water regulations, and in most states well water is not subject to much of the mandatory testing required of public water systems. Families that rely on private wells are thus at risk of exposure to a variety of unmeasured contaminants. Case Presentation A family of seven—two adults and five children—residing in rural northwestern Connecticut discovered elevated concentrations of uranium in their drinking water, with levels measured at 866 and 1,160 μg/L, values well above the U.S. Environmental Protection Agency maximum contaminant level for uranium in public water supplies of 30 μg/L. The uranium was of natural origin, and the source of exposure was found to be a 500-foot well that tapped groundwater from the Brookfield Gneiss, a geologic formation known to contain uranium. Other nearby wells also had elevated uranium, arsenic, and radon levels, though concentrations varied widely. At least one 24-hr urine uranium level was elevated (> 1 μg/24 hr) in six of seven family members (range, 1.1–2.5 μg/24 hr). To assess possible renal injury, we measured urinary beta-2-microglobulin. Levels were elevated (> 120 μg/L) in five of seven family members, but after correction for creatine excretion, the beta-2-microglobulin excretion rate remained elevated (> 40 μg/mmol creatinine) only in the youngest child, a 3-year-old with a corrected level of 90 μg/mmol creatinine. Three months after cessation of well water consumption, this child’s corrected beta-2-microglobulin level had fallen to 52 μg/mmol creatinine. Significance This case underscores the hazards of consuming groundwater from private wells. It documents the potential for significant residential exposure to naturally occurring uranium in well water. It highlights the special sensitivity of young children to residential environmental exposures, a reflection of the large amount of time they spend in their homes, the developmental immaturity of their kidneys and other organ systems, and the large volume of water they consume relative to body mass. PMID:17687453

Uptake of Uranium and Other Elements of Concern by Plants Growing on Uranium Mill Tailings Disposal Cells

NASA Astrophysics Data System (ADS)

Joseph, C. N.; Waugh, W.; Glenn, E.

2015-12-01

The U.S. Department of Energy (DOE) is responsible for long-term stewardship of disposal cells for uranium mill tailings throughout the United States. Rock-armored disposal cell covers create favorable habitat for deep-rooted plants by reducing soil evaporation, increasing soil water storage, and trapping windblown dust, thereby providing water and nutrients for plant germination and establishment. DOE is studying the tradeoffs of potential detrimental and beneficial effects of plants growing on disposal cell covers to develop a rational and consistent vegetation management policy. Plant roots often extend vertically through disposal cell covers into underlying tailings, therefore, uptake of tailings contaminants and dissemination through animals foraging on stems and leaves is a possible exposure pathway. The literature shows that plant uptake of contaminants in uranium mill tailings occurs, but levels can vary widely depending on plant species, tailings and soil chemistry, and cover soil hydrology. Our empirical field study measured concentrations of uranium, radium, thorium, molybdenum, selenium, manganese, lead, and arsenic in above ground tissues harvested from plants growing on disposal cells near Native American communities in western states that represent a range of climates, cover designs, cover soil types, and vegetation types. For risk screening, contaminant levels in above ground tissues harvested from plants on disposal cells were compared to Maximum Tolerance Levels (MTLs) set for livestock by the National Research Council, and to tissue levels in the same plant species growing in reference areas near disposal cells. Although tailings were covered with uncontaminated soils, for 14 of 46 comparisons, levels of uranium and other contaminants were higher in plants growing on disposal cells compared to reference area plants, indicating possible mobilization of these elements from the tailing into plant tissues. However, with one exception, all plant levels were well below MTLs. Selenium, the only element that exceeded its MTL, likely originated in local seleniferous soil found both at reference areas and in disposal cell covers, and not in the underlying tailings. Our screening risk assessment suggests that allowing plants to grow on disposal cells appears to be safe.

Investigating Freshwater Periphyton Community Response to Uranium with Phospholipid Fatty Acid and Denaturing Gradient Gel Electrophoresis Analyses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Small, Jack A.; Bunn, Amoret L.; McKinstry, Craig A.

2008-04-01

Periphyton communities can be used as monitors of ecosystem health and as indicators of contamination in lotic systems. Measures of biomass, community structure and genetic diversity were used to investigate impacts of uranium exposure on periphyton. Laboratory exposures of periphyton in river water amended with uranium were performed for 5 days, followed by 2 days of uranium depuration in unamended river water. Productivity as measured by biomass was not affected by concentrations up to 100 µg L-1 uranium. Phospholipid fatty acid (PLFA) profiles and denaturing gradient gel electrophoresis (DGGE) banding patterns found no changes in community or genetic structure relatedmore » to uranium exposure. We suggest that the periphyton community as a whole is not impacted by exposures of uranium up to a dose of 100 µg L-1. These findings have significance for the assessment and prediction of uranium impacts on aquatic ecosystems.« less

Applied technology for mine waste water decontamination in the uranium ores extraction from Romania

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bejenaru, C.; Filip, G.; Vacariu, V.T.

1996-12-31

The exploitation of uranium ores in Romania is carried out in underground mines. In all exploited uranium deposits, mine waste waters results and will still result after the closure of uranium ore extraction activity. The mine waters are radioactively contaminated with uranium and its decay products being a hazard both for underground waters as for the environment. This paper present the results of research work carried out by authors for uranium elimination from waste waters as the problems involved during the exploitation process of the existent equipment as its maintenance in good experimental conditions. The main waste water characteristics aremore » discussed: solids as suspension, uranium, radium, mineral salts, pH, etc. The moist suitable way to eliminate uranium from mine waste waters is the ion exchange process based on ion exchangers in fluidized bed. A flowsheet is given with main advantages resulted.« less

49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

Code of Federal Regulations, 2010 CFR

2010-10-01

... 49 Transportation 2 2010-10-01 2010-10-01 false Excepted packages for articles containing natural....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in which the sole Class 7 (radioactive) material content is natural uranium, unirradiated depleted uranium...

49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

Code of Federal Regulations, 2011 CFR

2011-10-01

... 49 Transportation 2 2011-10-01 2011-10-01 false Excepted packages for articles containing natural....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in which the sole Class 7 (radioactive) material content is natural uranium, unirradiated depleted uranium...

Innovative mathematical modeling in environmental remediation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yeh, Gour T.; National Central Univ.; Univ. of Central Florida

2013-05-01

There are two different ways to model reactive transport: ad hoc and innovative reaction-based approaches. The former, such as the Kd simplification of adsorption, has been widely employed by practitioners, while the latter has been mainly used in scientific communities for elucidating mechanisms of biogeochemical transport processes. It is believed that innovative mechanistic-based models could serve as protocols for environmental remediation as well. This paper reviews the development of a mechanistically coupled fluid flow, thermal transport, hydrologic transport, and reactive biogeochemical model and example-applications to environmental remediation problems. Theoretical bases are sufficiently described. Four example problems previously carried out aremore » used to demonstrate how numerical experimentation can be used to evaluate the feasibility of different remediation approaches. The first one involved the application of a 56-species uranium tailing problem to the Melton Branch Subwatershed at Oak Ridge National Laboratory (ORNL) using the parallel version of the model. Simulations were made to demonstrate the potential mobilization of uranium and other chelating agents in the proposed waste disposal site. The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium. The third example simulated laboratory experiments involving extremely high concentrations of uranium, technetium, aluminum, nitrate, and toxic metals (e.g.,Ni, Cr, Co).The fourth example modeled microbially-mediated immobilization of uranium in an unconfined aquifer using acetate amendment in a field-scale experiment. The purposes of these modeling studies were to simulate various mechanisms of mobilization and immobilization of radioactive wastes and to illustrate how to apply reactive transport models for environmental remediation.The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium.« less

Real-time 4D ERT monitoring of river water intrusion into a former nuclear disposal site using a transient warping-mesh water table boundary (Invited)

NASA Astrophysics Data System (ADS)

Johnson, T.; Hammond, G. E.; Versteeg, R. J.; Zachara, J. M.

2013-12-01

The Hanford 300 Area, located adjacent to the Columbia River in south-central Washington, USA, is the site of former research and uranium fuel rod fabrication facilities. Waste disposal practices at site included discharging between 33 and 59 metric tons of uranium over a 40 year period into shallow infiltration galleries, resulting in persistent uranium contamination within the vadose and saturated zones. Uranium transport from the vadose zone to the saturated zone is intimately linked with water table fluctuations and river water intrusion driven by upstream dam operations. As river stage increases, the water table rises into the vadose zone and mobilizes contaminated pore water. At the same time, river water moves inland into the aquifer, and river water chemistry facilitates further mobilization by enabling uranium desorption from contaminated sediments. As river stage decreases, flow moves toward the river, ultimately discharging contaminated water at the river bed. River water specific conductance at the 300 Area varies around 0.018 S/m whereas groundwater specific conductance varies around 0.043 S/m. This contrast provides the opportunity to monitor groundwater/river water interaction by imaging changes in bulk conductivity within the saturated zone using time-lapse electrical resistivity tomography. Previous efforts have demonstrated this capability, but have also shown that disconnecting regularization constraints at the water table is critical for obtaining meaningful time-lapse images. Because the water table moves with time, the regularization constraints must also be transient to accommodate the water table boundary. This was previously accomplished with 2D time-lapse ERT imaging by using a finely discretized computational mesh within the water table interval, enabling a relatively smooth water table to be defined without modifying the mesh. However, in 3D this approach requires a computational mesh with an untenable number of elements. In order to accommodate the water table boundary in 3D, we propose a time-lapse warping mesh inversion, whereby mesh elements that traverse the water table are modified to generate a smooth boundary at the known water table position, enabling regularization constraints to be accurately disconnected across the water table boundary at a given time. We demonstrate the approach using a surface ERT array installed adjacent to the Columbia River at the 300 Area, consisting of 352 electrodes and covering an area of approximately 350 m x 350 m. Using autonomous data collection, transmission, and filtering tools coupled with high performance computing resources, the 4D imaging process is automated and executed in real time. Each time lapse survey consists of approximately 40,000 measurements and 4 surveys are collected and processed per day from April 1st , 2013 to September 30th, 2013. The data are inverted on an unstructured tetrahedral mesh that honors LiDAR-based surface topography and is comprised of approximately 905,000 elements. Imaging results show the dynamic 4D extent of river water intrusion, and are validated with well-based fluid conductivity measurements at each monitoring well within the imaging domain.

Progress in understanding uranium(IV) speciation and dynamics in biologically reduced sediments: Research at molecular to centimeter scales by the SLAC SFA program

NASA Astrophysics Data System (ADS)

Bargar, J.; Williams, K. H.; Campbell, K. M.; Stubbs, J. E.; Suvorova, E.; Lezama-Pacheco, J. S.; Alessi, D.; Stylo, M.; Handley, K. M.; Bernier-Latmani, R.; Cerrato, J.; Davis, J. A.; Fox, P. M.; Giammar, D.; Long, P. E.

2011-12-01

The chemical and physical forms of U(IV) in reduced sediments, as well as the biogeochemical processes by which they form and transform, profoundly influence the stability of reduced U(IV) species and the behavior of uranium in biostimulated aquifers. Obtaining such information in field sediments is important because biogeochemical field conditions and their time dependence are difficult to replicate in the laboratory. The majority of contaminated aquifers in which bioremediation is of potential interest, including the Old Rifle, CO IFRC site, exhibit relatively low uranium sediment concentrations, i.e., < 10 ppm, presenting a formidable challenge to the use of spectroscopy and microscopy techniques that typically require 10-fold or higher uranium loadings. We have developed an in-situ column technique to study U(IV) species and evolving microbial communities in the Old Rifle aquifer and to correlate them with changes in trace and major ion groundwater composition during biostimulation treatments. Sediments were examined using x-ray and electron microscopy, x-ray absorption spectroscopy (XAS), and chemical extractions. XAS analysis showed that U(IV) occurred predominantly or exclusively as monomeric U(IV) complexes coordinated to oxo (or similar N/C) neighbors, and is associated with biomass or Fe sulfides. Even in the latter case, U(IV) was not coordinated directly to S neighbors. Sediment-hosted monomeric U(IV) complexes were found to partially transform into uraninite in the aquifer over a subsequent 12 month period. This work establishes the importance of monomeric U(IV) complexes in subsurface sediments at the Old Rifle site and provides a conceptual framework in which previously observed U(IV) reduction products can be related. These experiments also establish that U(IV) species are dynamic in aquifers and can undergo non-oxidative transformation reactions. These new results have important implications for uranium reactive transport models, long-term assessment of remediation technologies, and understanding natural uranium reduction in aquifers.

Final report of the decontamination and decommissioning of Building 6 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-07-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the domestic uranium procurement program funded by the U.S. Atomic Energy Commission. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, is also the remedial actionmore » contractor. Radiological contamination was identified in Building 6, and the building was demolished in 1992. The soil area within the footprint of the building has been remediated in accordance with the identified standards and the area can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Final report of the decontamination and decommissioning of Building 39 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-07-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, is also the remedial action contractor. The soilmore » beneath Building 39 was radiologically contaminated and the building was demolished in 1992. The soil area within the footprint of the building has been remediated in accordance with the identified standards and the area can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

US Department of Energy Grand Junction Projects Office Remedial Action Project, final report of the decontamination and decommissioning of Building 36 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-08-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, also is the remedial action contractor. Building 36more » was found to be radiologically contaminated and was demolished in 1996. The soil beneath the building was remediated in accordance with identified standards and can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Final report of the decontamination and decommissioning of Building 1 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1996-08-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, also is the remedial action contractor. Building 1more » was found to be radiologically contaminated and was demolished in 1996. The soil beneath and adjacent to the building was remediated in accordance with identified standards and can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Quantifying Contaminant Mass for the Feasibility Study of the DuPont Chambers Works FUSRAP Site - 13510

DOE Office of Scientific and Technical Information (OSTI.GOV)

Young, Carl; Rahman, Mahmudur; Johnson, Ann

2013-07-01

The U.S. Army Corps of Engineers (USACE) - Philadelphia District is conducting an environmental restoration at the DuPont Chambers Works in Deepwater, New Jersey under the Formerly Utilized Sites Remedial Action Program (FUSRAP). Discrete locations are contaminated with natural uranium, thorium-230 and radium-226. The USACE is proposing a preferred remedial alternative consisting of excavation and offsite disposal to address soil contamination followed by monitored natural attenuation to address residual groundwater contamination. Methods were developed to quantify the error associated with contaminant volume estimates and use mass balance calculations of the uranium plume to estimate the removal efficiency of the proposedmore » alternative. During the remedial investigation, the USACE collected approximately 500 soil samples at various depths. As the first step of contaminant mass estimation, soil analytical data was segmented into several depth intervals. Second, using contouring software, analytical data for each depth interval was contoured to determine lateral extent of contamination. Six different contouring algorithms were used to generate alternative interpretations of the lateral extent of the soil contamination. Finally, geographical information system software was used to produce a three dimensional model in order to present both lateral and vertical extent of the soil contamination and to estimate the volume of impacted soil for each depth interval. The average soil volume from all six contouring methods was used to determine the estimated volume of impacted soil. This method also allowed an estimate of a standard deviation of the waste volume estimate. It was determined that the margin of error for the method was plus or minus 17% of the waste volume, which is within the acceptable construction contingency for cost estimation. USACE collected approximately 190 groundwater samples from 40 monitor wells. It is expected that excavation and disposal of contaminated soil will remove the contaminant source zone and significantly reduce contaminant concentrations in groundwater. To test this assumption, a mass balance evaluation was performed to estimate the amount of dissolved uranium that would remain in the groundwater after completion of soil excavation. As part of this evaluation, average groundwater concentrations for the pre-excavation and post-excavation aquifer plume area were calculated to determine the percentage of plume removed during excavation activities. In addition, the volume of the plume removed during excavation dewatering was estimated. The results of the evaluation show that approximately 98% of the aqueous uranium would be removed during the excavation phase. The USACE expects that residual levels of contamination will remain in groundwater after excavation of soil but at levels well suited for the selection of excavation combined with monitored natural attenuation as a preferred alternative. (authors)« less

Mountain wetlands: efficient uranium filters - potential impacts

USGS Publications Warehouse

Owen, D.E.; Otton, J.K.

1995-01-01

Sediments in 67 of 145 Colorado wetlands sampled by the US Geological Survey contain moderate (20 ppm) or greater concentrations of uranium (some as high as 3000 ppm) based on dry weight. The proposed maximum contaminant level (MCL) for uranium in drinking water is 20 ??g/l or 20 ppb. By comparison, sediments in many of these wetlands contain 3 to 5 orders of magnitude more uranium than the proposed MCL. Wetlands near the workings of old mines may be trapping any number of additional metals/elements including Cu, Pb, Zn, As and Ag. Anthropogenic disturbances and natural changes may release uranium and other loosely bound metals presently contained in wetland sediments. -from Authors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, Mark B.; Rocha, Andrea M.; Smillie, Chris S.

Biological sensors can be engineered to measure a wide range of environmental conditions. Here we show that statistical analysis of DNA from natural microbial communities can be used to accurately identify environmental contaminants, including uranium and nitrate at a nuclear waste site. In addition to contamination, sequence data from the 16S rRNA gene alone can quantitatively predict a rich catalogue of 26 geochemical features collected from 93 wells with highly differing geochemistry characteristics. We extend this approach to identify sites contaminated with hydrocarbons from the Deepwater Horizon oil spill, finding that altered bacterial communities encode a memory of prior contamination,more » even after the contaminants themselves have been fully degraded. We show that the bacterial strains that are most useful for detecting oil and uranium are known to interact with these substrates, indicating that this statistical approach uncovers ecologically meaningful interactions consistent with previous experimental observations. Future efforts should focus on evaluating the geographical generalizability of these associations. Taken as a whole, these results indicate that ubiquitous, natural bacterial communities can be used as in situ environmental sensors that respond to and capture perturbations caused by human impacts. These in situ biosensors rely on environmental selection rather than directed engineering, and so this approach could be rapidly deployed and scaled as sequencing technology continues to become faster, simpler, and less expensive. Here we show that DNA from natural bacterial communities can be used as a quantitative biosensor to accurately distinguish unpolluted sites from those contaminated with uranium, nitrate, or oil. These results indicate that bacterial communities can be used as environmental sensors that respond to and capture perturbations caused by human impacts.« less

The Effect of Si and Al Concentration Ratios on the Removal of U(VI) under Hanford Site 200 Area Conditions-12115

DOE Office of Scientific and Technical Information (OSTI.GOV)

Katsenovich, Yelena; Gonzalez, Nathan; Moreno-Pastor, Carol

2012-07-01

Injection of reactive gases, such as NH{sub 3}, is an innovative technique to mitigate uranium contamination in soil for a vadose zone (VZ) contaminated with radionuclides. A series of experiments were conducted to examine the effect of the concentration ratio of silicon to aluminum in the presence of various bicarbonate concentrations on the coprecipitation process of U(VI). The concentration of Al in all tests remained unchanged at 2.8 mM. Experiments showed that the removal efficiency of uranium was not significantly affected by the different bicarbonate and U(VI) concentrations tested. For the lower Si:Al molar ratios of 2:1 and 18:1, themore » removal efficiency of uranium was relatively low (≤ 8%). For the Si:Al molar ratio of 35:1, the removal efficiency of uranium was increased to an average of ∼82% for all bicarbonate concentrations tested. At higher Si:Al molar ratios (53:1 and above), a relatively high removal efficiency of U(VI), approximately 85% and higher, was observed. These results demonstrate that the U(VI) removal efficiency is more affected by the Si:Al molar ratio than by the bicarbonate concentration in solution. The results of this experiment are promising for the potential implementation of NH{sub 3} gas injection for the remediation of U(VI) -contaminated VZ. (authors)« less

UMTRA project water sampling and analysis plan, Durango, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1994-01-01

Surface remedial action has been completed at the Uranium Mill Tailings Remedial Action Project in Durango, Colorado. Contaminated soil and debris have been removed from the former processing site and placed in the Bodo Canyon disposal cell. Ground water at the former uranium mill/tailings site and raffinate pond area has been contaminated by the former milling operations. The ground water at the disposal site was not impacted by the former milling operations at the time of the cell`s construction. Activities for fiscal 1994 involve ground water sampling and site characterization of the disposal site.

GEOPHYSICS AND SITE CHARACTERIZATION AT THE HANFORD SITE THE SUCCESSFUL USE OF ELECTRICAL RESISTIVITY TO POSITION BOREHOLES TO DEFINE DEEP VADOSE ZONE CONTAMINATION - 11509

DOE Office of Scientific and Technical Information (OSTI.GOV)

GANDER MJ; LEARY KD; LEVITT MT

2011-01-14

Historic boreholes confirmed the presence of nitrate and radionuclide contaminants at various intervals throughout a more than 60 m (200 ft) thick vadose zone, and a 2010 electrical resistivity survey mapped the known contamination and indicated areas of similar contaminants, both laterally and at depth; therefore, electrical resistivity mapping can be used to more accurately locate characterization boreholes. At the Hanford Nuclear Reservation in eastern Washington, production of uranium and plutonium resulted in the planned release of large quantities of contaminated wastewater to unlined excavations (cribs). From 1952 until 1960, the 216-U-8 Crib received approximately 379,000,000 L (100,000,000 gal) ofmore » wastewater containing 25,500 kg (56,218 lb) uranium; 1,029,000 kg (1,013 tons) of nitrate; 2.7 Ci of technetium-99; and other fission products including strontium-90 and cesium-137. The 216-U-8 Crib reportedly holds the largest inventory of waste uranium of any crib on the Hanford Site. Electrical resistivity is a geophysical technique capable of identifying contrasting physical properties; specifically, electrically conductive material, relative to resistive native soil, can be mapped in the subsurface. At the 216-U-8 Crib, high nitrate concentrations (from the release of nitric acid [HNO{sub 3}] and associated uranium and other fission products) were detected in 1994 and 2004 boreholes at various depths, such as at the base of the Crib at 9 m (30 ft) below ground surface (bgs) and sporadically to depths in excess of 60 m (200 ft) bgs. These contaminant concentrations were directly correlative with the presence of observed low electrical resistivity responses delineated during the summer 2010 geophysical survey. Based on this correlation and the recently completed mapping of the electrically conductive material, additional boreholes are planned for early 2011 to identify nitrate and radionuclide contamination: (a) throughout the entire vertical length of the vadose zone (i.e., 79 m [260 ft] bgs) within the footprint of the Crib, and (b) 15 to 30 m (50 to 100 ft) east of the Crib footprint, where contaminants are inferred to have migrated through relatively permeable soils. Confirmation of the presence of contamination in historic boreholes correlates well with mapping from the 2010 survey, and serves as a basis to site future characterization boreholes that will likely intersect contamination both laterally and at depth.« less

Determination of premining geochemical background and delineation of extent of sediment contamination in Blue Creek downstream from Midnite Mine, Stevens County, Washington

USGS Publications Warehouse

Church, Stan E.; Kirschner, Frederick E.; Choate, LaDonna M.; Lamothe, Paul J.; Budahn, James R.; Brown, Zoe Ann

2008-01-01

Geochemical and radionuclide studies of sediment recovered from eight core sites in the Blue Creek flood plain and Blue Creek delta downstream in Lake Roosevelt provided a stratigraphic geochemical record of the contamination from uranium mining at the Midnite Mine. Sediment recovered from cores in a wetland immediately downstream from the mine site as well as from sediment catchments in Blue Creek and from cores in the delta in Blue Creek cove provided sufficient data to determine the premining geochemical background for the Midnite Mine tributary drainage. These data provide a geochemical background that includes material eroded from the Midnite Mine site prior to mine development. Premining geochemical background for the Blue Creek basin has also been determined using stream-sediment samples from parts of the Blue Creek, Oyachen Creek, and Sand Creek drainage basins not immediately impacted by mining. Sediment geochemistry showed that premining uranium concentrations in the Midnite Mine tributary immediately downstream of the mine site were strongly elevated relative to the crustal abundance of uranium (2.3 ppm). Cesium-137 (137Cs) data and public records of production at the Midnite Mine site provided age control to document timelines in the sediment from the core immediately downstream from the mine site. Mining at the Midnite Mine site on the Spokane Indian Reservation between 1956 and 1981 resulted in production of more than 10 million pounds of U3O8. Contamination of the sediment by uranium during the mining period is documented from the Midnite Mine along a small tributary to the confluence of Blue Creek, in Blue Creek, and into the Blue Creek delta. During the period of active mining (1956?1981), enrichment of base metals in the sediment of Blue Creek delta was elevated by as much as 4 times the concentration of those same metals prior to mining. Cadmium concentrations were elevated by a factor of 10 and uranium by factors of 16 to 55 times premining geochemical background determined upstream of the mine site. Postmining metal concentrations in sediment are lower than during the mining period, but remain elevated relative to premining geochemical background. Furthermore, the sediment composition of surface sediment in the Blue Creek delta is contaminated. Base-metal contamination by arsenic, cadmium, lead, and zinc in sediment in the delta in Blue Creek cove is dominated by suspended sediment from the Coeur d?Alene mining district. Uranium contamination in surface sediment in the delta of Blue Creek cove extends at least 500 meters downstream from the mouth of Blue Creek as defined by the 1,290-ft elevation boundary between lands administered by the National Park Service and the Spokane Indian Tribe. Comparisons of the premining geochemical background to sediment sampled during the period the mine was in operation, and to the sediment data from the postmining period, are used to delineate the extent of contaminated sediment in Blue Creek cove along the thalweg of Blue Creek into Lake Roosevelt. The extent of contamination out into Lake Roosevelt by mining remains open.

Anaerobic bioremediation of hexavalent uranium in groundwater by reductive precipitation with methanogenic granular sludge.

PubMed

Tapia-Rodriguez, Aida; Luna-Velasco, Antonia; Field, Jim A; Sierra-Alvarez, Reyes

2010-04-01

Uranium has been responsible for extensive contamination of groundwater due to releases from mill tailings and other uranium processing waste. Past evidence has confirmed that certain bacteria can enzymatically reduce soluble hexavalent uranium (U(VI)) to insoluble tetravalent uranium (U(IV)) under anaerobic conditions in the presence of appropriate electron donors. This paper focuses on the evaluation of anaerobic granular sludge as a source of inoculum for the bioremediation of uranium in water. Batch experiments were performed with several methanogenic anaerobic granular sludge samples and different electron donors. Abiotic controls consisting of heat-killed inoculum and non-inoculated treatments confirmed the biological removal process. In this study, unadapted anaerobic granular sludge immediately reduced U(VI), suggesting an intrinsic capacity of the sludge to support this process. The high biodiversity of anaerobic granular sludge most likely accounts for the presence of specific microorganisms capable of reducing U(VI). Oxidation by O(2) was shown to resolubilize the uranium. This observation combined with X-ray diffraction evidence of uraninite confirmed that the removal during anaerobic treatment was due to reductive precipitation. The anaerobic removal activity could be sustained after several respikes of U(VI). The U(VI) removal was feasible without addition of electron donors, indicating that the decay of endogenous biomass substrates was contributing electron equivalents to the process. Addition of electron donors, such as H(2) stimulated the removal of U(VI) to varying degrees. The stimulation was greater in sludge samples with lower endogenous substrate levels. The present work reveals the potential application of anaerobic granular sludge for continuous bioremediation schemes to treat uranium-contaminated water. Copyright (c) 2009 Elsevier Ltd. All rights reserved.

In Situ Immobilization of Uranium in Structured Porous Media (Invited)

NASA Astrophysics Data System (ADS)

Brooks, S. C.; Gu, B.; Wu, W.; Spalding, B. P.; Watson, D. B.; Jardine, P.

2009-12-01

Defense related activities have resulted in broad areas of uranium contaminated groundwater across the U. S. Department of Energy complex. For example, past waste disposal practices at the DOE’s Y-12 site generated a plume of uranium and nitrate contamination in the underlying vadose and saturated zones which extends more than 120 meters deep and thousands of meters along geologic strike. Several DOE sponsored research programs have enabled the study of multiple biotic and abiotic methods of immobilizing uranium in situ at the site. These include biostimulation of metal reducing bacteria to promote reduction of the more soluble U(VI) to the sparingly soluble U(IV) and pH manipulation to immobilize U(VI) through its interactions (e.g., sorption, coprecipitation) with incipient aluminum oxyhydroxide minerals. The application of laboratory based results to the field site must also account for (i) the structured media which can impose incomplete mixing conditions and (ii) steep geochemical gradients or transition zones which differ significantly from the typically well mixed laboratory conditions. In this presentation results of several of these studies will be reviewed and lessons learned summarized.

Formation and Geological Sequestration of Uranium Nanoparticles in Deep Granitic Aquifer

PubMed Central

Suzuki, Yohey; Mukai, Hiroki; Ishimura, Toyoho; Yokoyama, Takaomi D.; Sakata, Shuhei; Hirata, Takafumi; Iwatsuki, Teruki; Mizuno, Takashi

2016-01-01

The stimulation of bacterial activities that convert hexavalent uranium, U(VI), to tetravalent uranium, U(IV), appears to be feasible for cost-effective remediation of contaminated aquifers. However, U(VI) reduction typically results in the precipitation of U(IV) particles less than 5 nanometers in diameter, except for environmental conditions enriched with iron. Because these tiny particles are mobile and susceptible to oxidative dissolution after the termination of nutrient injection, in situ bioremediation remains to be impractical. Here we show that U(IV) nanoparticles of coffinite (U(SiO4)1−x(OH)4x) formed in fracture-filling calcium carbonate in a granitic aquifer. In situ U-Pb isotope dating demonstrates that U(IV) nanoparticles have been sequestered in the calcium carbonate for at least 1 million years. As the microbiologically induced precipitation of calcium carbonate in aquifer systems worldwide is extremely common, we anticipate simultaneous stimulation of microbial activities for precipitation reactions of calcium carbonate and U(IV) nanoparticles, which leads to long-term sequestration of uranium and other radionuclides in contaminated aquifers and deep geological repositories. PMID:26948389

Formation and Geological Sequestration of Uranium Nanoparticles in Deep Granitic Aquifer.

PubMed

Suzuki, Yohey; Mukai, Hiroki; Ishimura, Toyoho; Yokoyama, Takaomi D; Sakata, Shuhei; Hirata, Takafumi; Iwatsuki, Teruki; Mizuno, Takashi

2016-03-07

The stimulation of bacterial activities that convert hexavalent uranium, U(VI), to tetravalent uranium, U(IV), appears to be feasible for cost-effective remediation of contaminated aquifers. However, U(VI) reduction typically results in the precipitation of U(IV) particles less than 5 nanometers in diameter, except for environmental conditions enriched with iron. Because these tiny particles are mobile and susceptible to oxidative dissolution after the termination of nutrient injection, in situ bioremediation remains to be impractical. Here we show that U(IV) nanoparticles of coffinite (U(SiO4)1-x(OH)4x) formed in fracture-filling calcium carbonate in a granitic aquifer. In situ U-Pb isotope dating demonstrates that U(IV) nanoparticles have been sequestered in the calcium carbonate for at least 1 million years. As the microbiologically induced precipitation of calcium carbonate in aquifer systems worldwide is extremely common, we anticipate simultaneous stimulation of microbial activities for precipitation reactions of calcium carbonate and U(IV) nanoparticles, which leads to long-term sequestration of uranium and other radionuclides in contaminated aquifers and deep geological repositories.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peterson, Dave; Miller, David; Kautsky, Mark

A uranium- and vanadium-ore-processing mill operated from 1954 to 1968 within the Navajo Nation near Shiprock, New Mexico. By September 1986, all tailings and structures on the former mill property were encapsulated in a disposal cell built on top of two existing tailings piles on the Shiprock site (the site) [1]. Local groundwater was contaminated by multiple inorganic constituents as a result of the milling operations. The U.S. Department of Energy (DOE) took over management of the site in 1978 as part of the Uranium Mill Tailings Remedial Action (UMTRA) Project. The DOE Office of Legacy Management currently manages ongoingmore » activities at the former mill facility, including groundwater remediation. Remediation activities are designed primarily to reduce the concentrations and total plume mass of the mill-related contaminants sulfate, uranium, and nitrate. In addition to contaminating groundwater in alluvial and bedrock sediments directly below the mill site, ore processing led to contamination of a nearby floodplain bordering the San Juan River. Groundwater in a shallow alluvial aquifer beneath the floodplain is strongly influenced by the morphology of the river channel as well as changing flows in the river, which provides drainage for regional runoff from the San Juan Mountains of Colorado. As part of a recent study of the floodplain hydrology, a revised conceptual model was developed for the alluvial aquifer along with an updated status of contaminant plumes that have been impacted by more than 10 years of groundwater pumping for site remediation purposes. Several findings from the recent study will be discussed here.« less

A Methodology for Characterizing Potential Uranium Transport in Deep Geological Disposal Sites

NASA Astrophysics Data System (ADS)

Dittrich, T. M.; Reimus, P. W.

2013-12-01

In order to make safe and reasonable decisions about radioactive waste disposal in deep geologic sites, it is important to understand the fate and potential transport of long half-life transuranic radionuclides over a wide range of time and distance scales. The objective of this study was to evaluate and demonstrate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured/weathered granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments involving uranium, as well as other actinides, have already been conducted. Working on this system provides a unique opportunity to compare lab experimental results with field-scale observations. Drilled rock cores and weathered fracture fill material (FFM) from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption/desorption and column breakthrough experiments. Uranium solutions were made by adding uranium to a synthetic Grimsel groundwater that matched the natural water chemistry found in the GTS groundwater. Batch and breakthrough experiments were conducted using solutions between pH 6.9 and 9.0. All column experiments were conducted using syringe pumps at low flow rate (<0.3 ml h-1) in small columns containing 5 g of material with pore volumes of 2-3 ml. These small columns allow rapid and economical evaluation of sorption/desorption behavior under flowing conditions (and in duplicate or triplicate). Solutions were switched to uranium-free synthetic Grimsel groundwater after equilibration in batch experiments or after near-steady uranium breakthrough occurred in column experiments. The measurement of uranium concentrations as a function of time under these conditions allowed interrogation of desorption rates which we believe control uranium fate and transport over long time and distance scales. Uranium transport was conservative and matched tritium breakthrough for pH 9.0; however, retardation increased when pH was reduced to 7.9 and 6.9. We are currently evaluating uranium adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, mineralogy, bentonite colloids and other actinides (e.g., Am). Figure 1. Uranium breakthrough results for (a) 6.5 μM U, (b) U-free solution, (c) flow rate increased from 0.3 to 0.6 mL h-1, (d) pH increased from 6.8 to 7.2, and (e) pH increased from 7.2 to 8.8.

Potential Aquifer Vulnerability in Regions Down-Gradient from ...

EPA Pesticide Factsheets

Sandstone-hosted roll-front uranium ore deposits originate when U(VI) dissolved in groundwater is reduced and precipitated as insoluble U(IV) minerals. Groundwater redox geochemistry, aqueous complexation, and solute migration are instrumental in leaching uranium from source rocks and transporting it in low concentrations to a chemical redox interface where it is deposited in an ore zone typically containing the uranium minerals uraninite, pitchblende, and/or coffinite; various iron sulfides; native selenium; clays; and calcite. In situ recovery (ISR) of these uranium ores is a process of contacting the uranium mineral deposit with leaching (lixiviant) fluids via injection of the lixiviant into wells drilled into the subsurface aquifer that hosts uranium ore, while other extraction wells pump the dissolved uranium after dissolution of the uranium minerals. Environmental concerns during and after ISR include water quality impacts from: 1) potential excursions of leaching solutions away from the injection zone into down-dip, underlying, or overlying aquifers; 2) potential migration of uranium and its decay products (e.g., Ra, Rn, Pb); and, 3) potential migration of redox-sensitive trace metals (e.g., Fe, Mn, Mo, Se, V), metalloids (e.g., As), and anions (e.g., sulfate). This review describes the geochemical processes that control roll-front uranium transport and fate in groundwater systems, identifies potential aquifer vulnerabilities to ISR operations, identifies

Rapid Dissolution of Soluble Uranyl Phases in Arid, Mine-Impacted Catchments Near Church Rock, NM

DOE Office of Scientific and Technical Information (OSTI.GOV)

deLemos, J.L.; Bostick, B.C.; Quicksall, A.N.

2009-05-14

We tested the hypothesis that runoff of uranium-bearing particles from mining waste disposal areas was a significant mechanism for redistribution of uranium in the northeastern part of the Upper Puerco River watershed (New Mexico). However, our results were not consistent with this hypothesis. Analysis of >100 sediment and suspended sediment samples collected adjacent to and downstream from uranium source areas indicated that uranium levels in the majority of the samples were not elevated above background. Samples collected within 50 m of a known waste disposal site were subjected to detailed geochemical characterization. Uranium in these samples was found to bemore » highly soluble; treatment with synthetic pore water for 24 h caused dissolution of 10-50% of total uranium in the samples. Equilibrium uranium concentrations in pore water were >4.0 mg/L and were sustained in repeated wetting events, effectively depleting soluble uranium from the solid phase. The dissolution rate of uranium appeared to be controlled by solid-phase diffusion of uranium from within uranium-bearing mineral particles. X-ray adsorption spectroscopy indicated the presence of a soluble uranyl silicate, and possibly a uranyl phosphate. These phases were exhausted in transported sediment suggesting that uranium was readily mobilized from sediments in the Upper Puerco watershed and transported in the dissolved load. These results could have significance for uranium risk assessment as well as mining waste management and cleanup efforts.« less

Rapid Dissolution of Soluble Uranyl Phases in Arid, Mine-Impacted Catchments near Church Rock, NM

PubMed Central

DELEMOS, JAMIE L.; BOSTICK, BENJAMIN C.; QUICKSALL, ANDREW N.; LANDIS, JOSHUA D.; GEORGE, CHRISTINE C.; SLAGOWSKI, NAOMI L.; ROCK, TOMMY; BRUGGE, DOUG; LEWIS, JOHNNYE; DURANT, JOHN L.

2008-01-01

We tested the hypothesis that runoff of uranium-bearing particles from mining waste disposal areas was a significant mechanism for redistribution of uranium in the northeastern part of the Upper Puerco River watershed (New Mexico). However, our results were not consistent with this hypothesis. Analysis of >100 sediment and suspended sediment samples collected adjacent to and downstream from uranium source areas indicated that uranium levels in the majority of the samples were not elevated above background. Samples collected within 50 m of a known waste disposal site were subjected to detailed geochemical characterization. Uranium in these samples was found to be highly soluble; treatment with synthetic pore water for 24 h caused dissolution of 10–50% of total uranium in the samples. Equilibrium uranium concentrations in pore water were >4.0 mg/L and were sustained in repeated wetting events, effectively depleting soluble uranium from the solid phase. The dissolution rate of uranium appeared to be controlled by solid-phase diffusion of uranium from within uranium-bearing mineral particles. X-ray adsorption spectroscopy indicated the presence of a soluble uranyl silicate, and possibly a uranyl phosphate. These phases were exhausted in transported sediment suggesting that uranium was readily mobilized from sediments in the Upper Puerco watershed and transported in the dissolved load. These results could have significance for uranium risk assessment as well as mining waste management and cleanup efforts. PMID:18589950

Radio-Ecological Conditions of Groundwater in the Area of Uranium Mining and Milling Facility - 13525

DOE Office of Scientific and Technical Information (OSTI.GOV)

Titov, A.V.; Semenova, M.P.; Seregin, V.A.

2013-07-01

Manmade chemical and radioactive contamination of groundwater is one of damaging effects of the uranium mining and milling facilities. Groundwater contamination is of special importance for the area of Priargun Production Mining and Chemical Association, JSC 'PPMCA', because groundwater is the only source of drinking water. The paper describes natural conditions of the site, provides information on changes of near-surface area since the beginning of the company, illustrates the main trends of contaminators migration and assesses manmade impact on the quality and mode of near-surface and ground waters. The paper also provides the results of chemical and radioactive measurements inmore » groundwater at various distances from the sources of manmade contamination to the drinking water supply areas. We show that development of deposits, mine water discharge, leakages from tailing dams and cinder storage facility changed general hydro-chemical balance of the area, contributed to new (overlaid) aureoles and flows of scattering paragenetic uranium elements, which are much smaller in comparison with natural ones. However, increasing flow of groundwater stream at the mouth of Sukhoi Urulyungui due to technological water infiltration, mixing of natural water with filtration streams from industrial reservoirs and sites, containing elevated (relative to natural background) levels of sulfate-, hydro-carbonate and carbonate- ions, led to the development and moving of the uranium contamination aureole from the undeveloped field 'Polevoye' to the water inlet area. The aureole front crossed the southern border of water inlet of drinking purpose. The qualitative composition of groundwater, especially in the southern part of water inlet, steadily changes for the worse. The current Russian intervention levels of gross alpha activity and of some natural radionuclides including {sup 222}Rn are in excess in drinking water; regulations for fluorine and manganese concentrations are also in excess. Possible ways to improve the situation are considered. (authors)« less

Influence of Reactive Transport on the Reduction of U(VI) in the Presence of Fe(III) and Nitrate: Implications for U(VI) Immobilization by Bioremediation / Biobarriers- Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

B.D. Wood

2007-01-01

Subsurface contamination by metals and radionuclides represent some of the most challenging remediation problems confronting the Department of Energy (DOE) complex. In situ remediation of these contaminants by dissimilatory metal reducing bacteria (DMRB) has been proposed as a potential cost effective remediation strategy. The primary focus of this research is to determine the mechanisms by which the fluxes of electron acceptors, electron donors, and other species can be controlled to maximize the transfer of reductive equivalents to the aqueous and solid phases. The proposed research is unique in the NABIR portfolio in that it focuses on (i) the role ofmore » flow and transport in the initiation of biostimulation and the successful sequestration of metals and radionuclides [specifically U(VI)], (ii) the subsequent reductive capacity and stability of the reduced sediments produced by the biostimulation process, and (iii) the potential for altering the growth of biomass in the subsurface by the addition of specific metabolic uncoupling compounds. A scientifically-based understanding of these phenomena are critical to the ability to design successful bioremediation schemes. The laboratory research will employ Shewanella putrefaciens (CN32), a facultative DMRB that can use Fe(III) oxides as a terminal electron acceptor. Sediment-packed columns will be inoculated with this organism, and the reduction of U(VI) by the DMRB will be stimulated by the addition of a carbon and energy source in the presence of Fe(III). Separate column experiments will be conducted to independently examine: (1) the importance of the abiotic reduction of U(VI) by biogenic Fe(II); (2) the influence of the transport process on Fe(III) reduction and U(VI) immobilization, with emphasis on methods for controlling the fluxes of aqueous species to maximize uranium reduction; (3) the reductive capacity of biologically-reduced sediments (with respect to re-oxidation by convective fluxes of O2 and NO3-) and the long-term stability of immobilized uranium mineral phases after bioremediation processes are complete, and (4) the ability for metabolic uncoupling compounds to maintain microbial growth while limiting biomass production. The results of the laboratory experiments will be used to develop mathematical descriptive models for the coupled transport and reduction processes.« less

Transportability Class of Americium in K Basin Sludge under Ambient and Hydrothermal Processing Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.

2006-08-01

This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to themore » Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization data is derived spent nuclear fuel corroded within the K Basins at 10-15?C. The STP process will place water-laden sludges from the K Basin in process vessels at {approx}150-180 C. Therefore, published studies with other irradiated (uranium oxide) fuel were examined. From these studies, the affinity of plutonium and americium for uranium in irradiated UO2 also was demonstrated at hydrothermal conditions (150 C anoxic liquid water) approaching those proposed for the STP process and even for hydrothermal conditions outside of the STP operating envelope (e.g., 150 C oxic and 100 C oxic and anoxic liquid water). In summary, by demonstrating that the chemical and physical behavior of 241Am in the sludge matrix is similar to that of the predominant species (uranium and for the plutonium from which it originates), a technical basis is provided for using the slow uptake transportability factor for 241Am that is currently used for plutonium and uranium oxides. The change from moderate to slow uptake for 241Am could reduce the overall analyzed dose consequences for the STP by more than 30%.« less

Contaminant Leach Testing of Hanford Tank 241-C-104 Residual Waste

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cantrell, Kirk J.; Snyder, Michelle M.V.; Wang, Guohui

2015-07-01

Leach testing of Tank C-104 residual waste was completed using batch and column experiments. Tank C-104 residual waste contains exceptionally high concentrations of uranium (i.e., as high as 115 mg/g or 11.5 wt.%). This study was conducted to provide data to develop contaminant release models for Tank C-104 residual waste and Tank C-104 residual waste that has been treated with lime to transform uranium in the waste to a highly insoluble calcium uranate (CaUO4) or similar phase. Three column leaching cases were investigated. In the first case, C-104 residual waste was leached with deionized water. In the second case, crushedmore » grout was added to the column so that deionized water contacted the grout prior to contacting the waste. In the third case, lime was mixed in with the grout. Results of the column experiments demonstrate that addition of lime dramatically reduces the leachability of uranium from Tank C-104 residual waste. Initial indications suggest that CaUO4 or a similar highly insoluble calcium rich uranium phase forms as a result of the lime addition. Additional work is needed to definitively identify the uranium phases that occur in the as received waste and the waste after the lime treatment.« less

Reduction of uranium by cytochrome c3 of Desulfovibrio vulgaris

USGS Publications Warehouse

Lovley, D.R.; Widman, P.K.; Woodward, J.C.; Phillips, E.J.P.

1993-01-01

The mechanism for U(VI) reduction by Desulfovibrio vulgaris (Hildenborough) was investigated. The H2-dependent U(VI) reductase activity in the soluble fraction of the cells was lost when the soluble fraction was passed over a cationic exchange column which extracted cytochrome c3. Addition of cytochrome c3 back to the soluble fraction that had been passed over the cationic exchange column restored the U(VI)-reducing capacity. Reduced cytochrome c3 was oxidized by U(VI), as was a c-type cytochrome(s) in whole-cell suspensions. When cytochrome c3 was combined with hydrogenase, its physiological electron donor, U(VI) was reduced in the presence of H2. Hydrogenase alone could not reduce U(VI). Rapid U(VI) reduction was followed by a subsequent slow precipitation of the U(IV) mineral uraninite. Cytochrome c3 reduced U(VI) in a uranium-contaminated surface water and groundwater. Cytochrome c3 provides the first enzyme model for the reduction and biomineralization of uranium in sedimentary environments. Furthermore, the finding that cytochrome c3 can catalyze the reductive precipitation of uranium may aid in the development of fixed-enzyme reactors and/or organisms with enhanced U(VI)-reducing capacity for the bioremediation of uranium- contaminated waters and waste streams.

Metabolomics reveals dose effects of low-dose chronic exposure to uranium in rats: identification of candidate biomarkers in urine samples.

PubMed

Grison, Stéphane; Favé, Gaëlle; Maillot, Matthieu; Manens, Line; Delissen, Olivia; Blanchardon, Éric; Dublineau, Isabelle; Aigueperse, Jocelyne; Bohand, Sandra; Martin, Jean-Charles; Souidi, Maâmar

2016-01-01

Data are sparse about the potential health risks of chronic low-dose contamination of humans by uranium (natural or anthropogenic) in drinking water. Previous studies report some molecular imbalances but no clinical signs due to uranium intake. In a proof-of-principle study, we reported that metabolomics is an appropriate method for addressing this chronic low-dose exposure in a rat model (uranium dose: 40 mg L -1 ; duration: 9 months, n = 10). In the present study, our aim was to investigate the dose-effect pattern and identify additional potential biomarkers in urine samples. Compared to our previous protocol, we doubled the number of rats per group (n = 20), added additional sampling time points (3 and 6 months) and included several lower doses of natural uranium (doses used: 40, 1.5, 0.15 and 0.015 mg L -1 ). LC-MS metabolomics was performed on urine samples and statistical analyses were made with SIMCA-P+ and R packages. The data confirmed our previous results and showed that discrimination was both dose and time related. Uranium exposure was revealed in rats contaminated for 9 months at a dose as low as 0.15 mg L -1 . Eleven features, including the confidently identified N1-methylnicotinamide, N1-methyl-2-pyridone-5-carboxamide and 4-hydroxyphenylacetylglycine, discriminated control from contaminated rats with a specificity and a sensitivity ranging from 83 to 96 %, when combined into a composite score. These findings show promise for the elucidation of underlying radiotoxicologic mechanisms and the design of a diagnostic test to assess exposure in urine, in a dose range experimentally estimated to be above a threshold between 0.015 and 0.15 mg L -1 .

Evaluation of alternatives for best available technology treatment and retreatment of uranium-contaminated wastewater at the Paducah Gaseous Diffusion Plant C-400 Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Del Cul, G.D.; Osborne, P.E.; Beck, D.E.

1991-01-01

The Paducah Gaseous Diffusion Plant (PGDP) C-400 Decontamination Facility generates aqueous solutions that originate in drum washing, machine parts and equipment cleaning, and other decontamination processes. The chemical composition of the waste depends on the particular operation involved. In general, the waste contains uranyl, fluoride, carbonate, and nitrate ions, plus soaps, detergents, secondary contaminants, and particulate matter. The uranium content is rather variable ranging between 0.5 and 30 g/l. The main contaminants are fluoride, technetium, uranium, and other heavy metals. The plan included (1) a literature search to support best available technology (BAT) evaluation of treatment alternatives, (2) a qualitymore » assurance/quality control plan, (3) suggestion of alternative treatment options, (4) bench-scale tests studies of the proposed treatment alternatives, and (5) establishment of the final recommendation. The following report records the evaluation of items (1) to (3) of the action plan for the BAT evaluation of alternatives for the treatment and retreatment of uranium-contaminated wastewater at the PGDP C-400 treatment facility. After a thorough literature search, five major technologies were considered: (1) precipitation/coprecipitation, (2) reverse osmosis, (3) ultrafiltration, (4) supported liquid membranes, and (5) ion exchange. Biosorption was also considered, but as it is a fairly new technology with few demonstrations of its capabilities, it is mentioned only briefly in the report. Based on C-400's requirements and facilities, the precipitation/coprecipitation process appears to be the best suited for use at the plant. Four different treatment options using the precipitation/coprecipitation technology are proposed. Bench-scale studies of the four options are suggested. 37 refs.« less

Uranium decay daughters from isolated mines: Accumulation and sources.

PubMed

Cuvier, A; Panza, F; Pourcelot, L; Foissard, B; Cagnat, X; Prunier, J; van Beek, P; Souhaut, M; Le Roux, G

2015-11-01

This study combines in situ gamma spectrometry performed at different scales, in order to accurately locate the contamination pools, to identify the concerned radionuclides and to determine the distribution of the contaminants from soil to bearing phase scale. The potential mobility of several radionuclides is also evaluated using sequential extraction. Using this procedure, an accumulation area located downstream of a former French uranium mine and concentrating a significant fraction of radioactivity is highlighted. We report disequilibria in the U-decay chains, which are likely related to the processes implemented on the mining area. Coupling of mineralogical analyzes with sequential extraction allow us to highlight the presence of barium sulfate, which may be the carrier of the Ra-226 activities found in the residual phase (Ba(Ra)SO4). In contrast, uranium is essentially in the reducible fraction and potentially trapped in clay-iron coatings located on the surface of minerals. Copyright © 2015 Elsevier Ltd. All rights reserved.

Assessment of the quality of groundwater and the Little Wind River in the area of a former uranium processing facility on the Wind River Reservation, Wyoming, 1987 through 2010

USGS Publications Warehouse

Ranalli, Anthony J.; Naftz, David L.

2014-01-01

In 2010, the U.S Geological Survey (USGS), in cooperation with the Wind River Environmental Quality Commission (WREQC), began an assessment of the effectiveness of the existing monitoring network at the Riverton, Wyoming, Uranium Mill Tailings Remedial Action (UMTRA) site. The USGS used existing data supplied by the U.S. Department of Energy (DOE). The study was to determine (1) seasonal variations in the direction of groundwater flow in the area of the former uranium processing facility toward the Little Wind River, (2) the extent of contaminated groundwater among the aquifers and between the aquifers and the Little Wind River, (3) whether current monitoring is adequate to establish the effectiveness of natural attenuation for the contaminants of concern, and (4) the influence of groundwater discharged from the sulfuric-acid plant on water quality in the Little Wind River.

Combining particle-tracking and geochemical data to assess public supply well vulnerability to arsenic and uranium

USGS Publications Warehouse

Hinkle, S.R.; Kauffman, L.J.; Thomas, M.A.; Brown, C.J.; McCarthy, K.A.; Eberts, S.M.; Rosen, Michael R.; Katz, B.G.

2009-01-01

Flow-model particle-tracking results and geochemical data from seven study areas across the United States were analyzed using three statistical methods to test the hypothesis that these variables can successfully be used to assess public supply well vulnerability to arsenic and uranium. Principal components analysis indicated that arsenic and uranium concentrations were associated with particle-tracking variables that simulate time of travel and water fluxes through aquifer systems and also through specific redox and pH zones within aquifers. Time-of-travel variables are important because many geochemical reactions are kinetically limited, and geochemical zonation can account for different modes of mobilization and fate. Spearman correlation analysis established statistical significance for correlations of arsenic and uranium concentrations with variables derived using the particle-tracking routines. Correlations between uranium concentrations and particle-tracking variables were generally strongest for variables computed for distinct redox zones. Classification tree analysis on arsenic concentrations yielded a quantitative categorical model using time-of-travel variables and solid-phase-arsenic concentrations. The classification tree model accuracy on the learning data subset was 70%, and on the testing data subset, 79%, demonstrating one application in which particle-tracking variables can be used predictively in a quantitative screening-level assessment of public supply well vulnerability. Ground-water management actions that are based on avoidance of young ground water, reflecting the premise that young ground water is more vulnerable to anthropogenic contaminants than is old ground water, may inadvertently lead to increased vulnerability to natural contaminants due to the tendency for concentrations of many natural contaminants to increase with increasing ground-water residence time.

Recovery of uranium from an irradiated solid target after removal of molybdenum-99 produced from the irradiated target

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reilly, Sean Douglas; May, Iain; Copping, Roy

A process for minimizing waste and maximizing utilization of uranium involves recovering uranium from an irradiated solid target after separating the medical isotope product, molybdenum-99, produced from the irradiated target. The process includes irradiating a solid target comprising uranium to produce fission products comprising molybdenum-99, and thereafter dissolving the target and conditioning the solution to prepare an aqueous nitric acid solution containing irradiated uranium. The acidic solution is then contacted with a solid sorbent whereby molybdenum-99 remains adsorbed to the sorbent for subsequent recovery. The uranium passes through the sorbent. The concentrations of acid and uranium are then adjusted tomore » concentrations suitable for crystallization of uranyl nitrate hydrates. After inducing the crystallization, the uranyl nitrate hydrates are separated from a supernatant. The process results in the purification of uranyl nitrate hydrates from fission products and other contaminants. The uranium is therefore available for reuse, storage, or disposal.« less

Bioengineered Chimeric Spider Silk-Uranium Binding Proteins

PubMed Central

Krishnaji, Sreevidhya Tarakkad; Kaplan, David L.

2014-01-01

Heavy metals constitute a source of environmental pollution. Here, novel functional hybrid biomaterials for specific interactions with heavy metals are designed by bioengineering consensus sequence repeats from spider silk of Nephila clavipes with repeats of a uranium peptide recognition motif from a mutated 33-residue of calmodulin protein from Paramecium tetraurelia. The self-assembly features of the silk to control nanoscale organic/inorganic material interfaces provides new biomaterials for uranium recovery. With subsequent enzymatic digestion of the silk to concentrate the sequestered metals, options can be envisaged to use these new chimeric protein systems in environmental engineering, including to remediate environments contaminated by uranium. PMID:23212989

Spatially variable stage-driven groundwater-surface water interaction inferred from time-frequency analysis of distributed temperature sensing data

USGS Publications Warehouse

Mwakanyamale, Kisa; Slater, Lee; Day-Lewis, Frederick D.; Elwaseif, Mehrez; Johnson, Carole D.

2012-01-01

Characterization of groundwater-surface water exchange is essential for improving understanding of contaminant transport between aquifers and rivers. Fiber-optic distributed temperature sensing (FODTS) provides rich spatiotemporal datasets for quantitative and qualitative analysis of groundwater-surface water exchange. We demonstrate how time-frequency analysis of FODTS and synchronous river stage time series from the Columbia River adjacent to the Hanford 300-Area, Richland, Washington, provides spatial information on the strength of stage-driven exchange of uranium contaminated groundwater in response to subsurface heterogeneity. Although used in previous studies, the stage-temperature correlation coefficient proved an unreliable indicator of the stage-driven forcing on groundwater discharge in the presence of other factors influencing river water temperature. In contrast, S-transform analysis of the stage and FODTS data definitively identifies the spatial distribution of discharge zones and provided information on the dominant forcing periods (≥2 d) of the complex dam operations driving stage fluctuations and hence groundwater-surface water exchange at the 300-Area.

Groundwater quality and the relation between pH values and occurrence of trace elements and radionuclides in water samples collected from private wells in part of the Kickapoo Tribe of Oklahoma Jurisdictional Area, central Oklahoma, 2011

USGS Publications Warehouse

Becker, Carol J.

2013-01-01

From 1999 to 2007, the Indian Health Service reported that gross alpha-particle activities and concentrations of uranium exceeded the Maximum Contaminant Levels for public drinking-water supplies in water samples from six private wells and two test wells in a rural residential neighborhood in the Kickapoo Tribe of Oklahoma Jurisdictional Area, in central Oklahoma. Residents in this rural area use groundwater from Quaternary-aged terrace deposits and the Permian-aged Garber-Wellington aquifer for domestic purposes. Uranium and other trace elements, specifically arsenic, chromium, and selenium, occur naturally in rocks composing the Garber-Wellington aquifer and in low concentrations in groundwater throughout its extent. Previous studies have shown that pH values above 8.0 from cation-exchange processes in the aquifer cause selected metals such as arsenic, chromium, selenium, and uranium to desorb (if present) from mineral surfaces and become mobile in water. On the basis of this information, the U.S. Geological Survey, in cooperation with the Kickapoo Tribe of Oklahoma, conducted a study in 2011 to describe the occurrence of selected trace elements and radionuclides in groundwater and to determine if pH could be used as a surrogate for laboratory analysis to quickly and inexpensively identify wells that might contain high concentrations of uranium and other trace elements. The pH and specific conductance of groundwater from 59 private wells were measured in the field in an area of about 18 square miles in Lincoln and Pottawatomie Counties. Twenty of the 59 wells also were sampled for dissolved concentrations of major ions, trace elements, gross alpha-particle and gross beta-particle activities, uranium, radium-226, radium-228, and radon-222 gas. Arsenic concentrations exceeded the Maximum Contaminant Level of 10 micrograms per liter in one sample having a concentration of 24.7 micrograms per liter. Selenium concentrations exceeded the Maximum Contaminant Level of 50 micrograms per liter in one sample having a concentration of 147 micrograms per liter. Both samples had alkaline pH values, 8.0 and 8.4, respectively. Uranium concentrations ranged from 0.02 to 383 micrograms per liter with 5 of 20 samples exceeding the Maximum Contaminant Level of 30 micrograms per liter; the five wells with uranium concentrations exceeding 30 micrograms per liter had pH values ranging from 8.0 to 8.5. Concentrations of uranium and radon-222 and gross alpha-particle activity showed a positive relation to pH, with the highest concentrations and activity in samples having pH values of 8.0 or above. The groundwater samples contained dissolved oxygen and high concentrations of bicarbonate; these characteristics are also factors in increasing uranium solubility. Concentrations of radium-226 and radium-228 (combined) ranged from 0.03 to 1.7 picocuries per liter, with a median concentration of 0.45 picocuries per liter for all samples. Radon-222 concentrations ranged from 95 to 3,600 picocuries per liter with a median concentration of 261 picocuries per liter. Eight samples having pH values ranging from 8.0 to 8.7 exceeded the proposed Maximum Contaminant Level of 300 picocuries per liter for radon-222. Eight samples exceeded the 15 picocuries per liter Maximum Contaminant Level for gross alpha-particle activity at 72 hours (after sample collection) and at 30 days (after the initial count); those samples had pH values ranging from 8.0 to 8.5. Gross beta-particle activity increased in 15 of 21 samples during the interval from 72 hours to 30 days. The increase in gross beta-particle activity over time probably was caused by the ingrowth and decay of uranium daughter products that emit beta particles. Water-quality data collected for this study indicate that pH values above 8.0 are associated with potentially high concentrations of uranium and radon-222 and high gross alpha-particle activity in the study area. High pH values also are associated with potentially high concentrations of arsenic, chromium, and selenium in groundwater when these elements occur in the aquifer matrix along groundwater-flow paths.

Innovative mathematical modeling in environmental remediation.

PubMed

Yeh, Gour-Tsyh; Gwo, Jin-Ping; Siegel, Malcolm D; Li, Ming-Hsu; Fang, Yilin; Zhang, Fan; Luo, Wensui; Yabusaki, Steve B

2013-05-01

There are two different ways to model reactive transport: ad hoc and innovative reaction-based approaches. The former, such as the Kd simplification of adsorption, has been widely employed by practitioners, while the latter has been mainly used in scientific communities for elucidating mechanisms of biogeochemical transport processes. It is believed that innovative mechanistic-based models could serve as protocols for environmental remediation as well. This paper reviews the development of a mechanistically coupled fluid flow, thermal transport, hydrologic transport, and reactive biogeochemical model and example-applications to environmental remediation problems. Theoretical bases are sufficiently described. Four example problems previously carried out are used to demonstrate how numerical experimentation can be used to evaluate the feasibility of different remediation approaches. The first one involved the application of a 56-species uranium tailing problem to the Melton Branch Subwatershed at Oak Ridge National Laboratory (ORNL) using the parallel version of the model. Simulations were made to demonstrate the potential mobilization of uranium and other chelating agents in the proposed waste disposal site. The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium. The third example simulated laboratory experiments involving extremely high concentrations of uranium, technetium, aluminum, nitrate, and toxic metals (e.g., Ni, Cr, Co). The fourth example modeled microbially-mediated immobilization of uranium in an unconfined aquifer using acetate amendment in a field-scale experiment. The purposes of these modeling studies were to simulate various mechanisms of mobilization and immobilization of radioactive wastes and to illustrate how to apply reactive transport models for environmental remediation. Copyright © 2011 Elsevier Ltd. All rights reserved.

BIO-MONITORING FOR URANIUM USING STREAM-SIDE TERRESTRIAL PLANTS AND MACROPHYTES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Caldwell, E.; Duff, M.; Hicks, T.

2012-01-12

This study evaluated the abilities of various plant species to act as bio-monitors for environmental uranium (U) contamination. Vegetation and soil samples were collected from a U processing facility. The water-way fed from facility storm and processing effluents was the focal sample site as it represented a primary U transport mechanism. Soils and sediments from areas exposed to contamination possessed U concentrations that averaged 630 mg U kg{sup -1}. Aquatic mosses proved to be exceptional accumulators of U with dry weight (dw) concentrations measuring as high as 12500 mg U kg{sup -1} (approximately 1% of the dw mass was attributablemore » to U). The macrophytes (Phragmites communis, Scripus fontinalis and Sagittaria latifolia) were also effective accumulators of U. In general, plant roots possessed higher concentrations of U than associated upper portions of plants. For terrestrial plants, the roots of Impatiens capensis had the highest observed levels of U accumulation (1030 mg kg{sup -1}), followed by the roots of Cyperus esculentus and Solidago speciosa. The concentration ratio (CR) characterized dry weight (dw) vegetative U levels relative to that in associated dw soil. The plant species that accumulated U at levels in excess of that found in the soil were: P. communis root (CR, 17.4), I. capensis root (CR, 3.1) and S. fontinalis whole plant (CR, 1.4). Seven of the highest ten CR values were found in the roots. Correlations with concentrations of other metals with U were performed, which revealed that U concentrations in the plant were strongly correlated with nickel (Ni) concentrations (correlation: 0.992; r-squared: 0.984). Uranium in plant tissue was also strongly correlated with strontium (Sr) (correlation: 0.948; r-squared: 0.899). Strontium is chemically and physically similar to calcium (Ca) and magnesium (Mg), which were also positively-correlated with U. The correlation with U and these plant nutrient minerals, including iron (Fe), suggests that active uptake mechanisms may influence plant U accumulation.« less

49 CFR 173.477 - Approval of packagings containing greater than 0.1 kg of non-fissile or fissile-excepted uranium...

Code of Federal Regulations, 2014 CFR

2014-10-01

... kg of non-fissile or fissile-excepted uranium hexafluoride. 173.477 Section 173.477 Transportation... non-fissile or fissile-excepted uranium hexafluoride. (a) Each offeror of a package containing more than 0.1 kg of uranium hexafluoride must maintain on file for at least two years after the offeror's...

49 CFR 173.477 - Approval of packagings containing greater than 0.1 kg of non-fissile or fissile-excepted uranium...

Code of Federal Regulations, 2011 CFR

2011-10-01

... kg of non-fissile or fissile-excepted uranium hexafluoride. 173.477 Section 173.477 Transportation... non-fissile or fissile-excepted uranium hexafluoride. (a) Each offeror of a package containing more than 0.1 kg of uranium hexafluoride must maintain on file for at least one year after the latest...

49 CFR 173.477 - Approval of packagings containing greater than 0.1 kg of non-fissile or fissile-excepted uranium...

Code of Federal Regulations, 2012 CFR

2012-10-01

... kg of non-fissile or fissile-excepted uranium hexafluoride. 173.477 Section 173.477 Transportation... non-fissile or fissile-excepted uranium hexafluoride. (a) Each offeror of a package containing more than 0.1 kg of uranium hexafluoride must maintain on file for at least one year after the latest...

49 CFR 173.477 - Approval of packagings containing greater than 0.1 kg of non-fissile or fissile-excepted uranium...

Code of Federal Regulations, 2013 CFR

2013-10-01

... kg of non-fissile or fissile-excepted uranium hexafluoride. 173.477 Section 173.477 Transportation... non-fissile or fissile-excepted uranium hexafluoride. (a) Each offeror of a package containing more than 0.1 kg of uranium hexafluoride must maintain on file for at least one year after the latest...

49 CFR 173.477 - Approval of packagings containing greater than 0.1 kg of non-fissile or fissile-excepted uranium...

Code of Federal Regulations, 2010 CFR

2010-10-01

... kg of non-fissile or fissile-excepted uranium hexafluoride. 173.477 Section 173.477 Transportation... non-fissile or fissile-excepted uranium hexafluoride. (a) Each offeror of a package containing more than 0.1 kg of uranium hexafluoride must maintain on file for at least one year after the latest...

Bioaccessibility of U, Th and Pb in particulate matter from an abandoned uranium mine

NASA Astrophysics Data System (ADS)

Millward, Geoffrey; Foulkes, Michael; Henderson, Sam; Blake, William

2016-04-01

Currently, there are approximately 150 uranium mines in Europe at various stages of either operation, development, decommissioning, restoration or abandonment (wise-uranium.com). The particulate matter comprising the mounds of waste rock and mill tailings poses a risk to human health through the inadvertent ingestion of particles contaminated with uranium and thorium, and their decay products, which exposes recipients to the dual toxicity of heavy elements and their radioactive emissions. We investigated the bioaccessibility of 238U, 232Th and 206,214,210Pb in particulate samples taken from a contaminated, abandoned uranium mine in South West England. Sampling included a mine shaft, dressing floor and waste heap, as well as soils from a field used for grazing. The contaminants were extracted using the in-vitro Unified Bioaccessibility Research Group of Europe Method (UBM) in order to mimic the digestion processes in the human stomach (STOM) and the combined stomach and gastrointestinal tract (STOM+INT). Analyses of concentrations of U, Th and Pb in the extracts were by ICP-MS and the activity concentrations of radionuclides were determined on the same particles, before and after extraction, using gamma spectroscopy. 'Total' concentrations of U, Th and Pb for all samples were in the range 57 to 16,200, 0.28 to 3.8 and 69 to 4750 mg kg-1, respectively. For U and Pb the concentrations in the STOM fraction were lower than the total and STOM+INT fractions were even lower. However, for Th the STOM+INT fractions were higher than the STOM due to the presence of Th carbonate species within the gastrointestinal fluid. Activity concentrations for 214Pb and 210Pb, including total, STOM and STOM+INT, were in the range 180 to <1 Bq g-1 for the dressing floor and waste heap and 18 to <1 Bq g-1 for the grazing land. Estimates of the bioaccessible fractions (BAFs) of 238U in the most contaminated samples were 39% and 8% in the STOM and STOM+INT, respectively, whereas the respective BAFs for 232Th were 3% and 9%. For stable 206Pb the STOM and STOM+INT BAFs were 16% and 3% for the most contaminated samples, whereas those from the field had 44% in the STOM fraction and 17% in the STOM+INT fraction. The BAFs for 214Pb and 210Pb were the same as 206Pb. Dose estimates were made for the contaminants together with radioactive doses in order to assess potential risk to human health.

REGENERATION OF FISSION-PRODUCT-CONTAINING MAGNESIUM-THORIUM ALLOYS

DOEpatents

Chiotti, P.

1964-02-01

A process of regenerating a magnesium-thorium alloy contaminated with fission products, protactinium, and uranium is presented. A molten mixture of KCl--LiCl-MgCl/sub 2/ is added to the molten alloy whereby the alkali, alkaline parth, and rare earth fission products (including yttrium) and some of the thorium and uranium are chlorinated and

Evidence of Geobacter-associated phage in a uranium-contaminated aquifer

PubMed Central

Holmes, Dawn E; Giloteaux, Ludovic; Chaurasia, Akhilesh K; Williams, Kenneth H; Luef, Birgit; Wilkins, Michael J; Wrighton, Kelly C; Thompson, Courtney A; Comolli, Luis R; Lovley, Derek R

2015-01-01

Geobacter species may be important agents in the bioremediation of organic and metal contaminants in the subsurface, but as yet unknown factors limit the in situ growth of subsurface Geobacter well below rates predicted by analysis of gene expression or in silico metabolic modeling. Analysis of the genomes of five different Geobacter species recovered from contaminated subsurface sites indicated that each of the isolates had been infected with phage. Geobacter-associated phage sequences were also detected by metagenomic and proteomic analysis of samples from a uranium-contaminated aquifer undergoing in situ bioremediation, and phage particles were detected by microscopic analysis in groundwater collected from sediment enrichment cultures. Transcript abundance for genes from the Geobacter-associated phage structural proteins, tail tube Gp19 and baseplate J, increased in the groundwater in response to the growth of Geobacter species when acetate was added, and then declined as the number of Geobacter decreased. Western blot analysis of a Geobacter-associated tail tube protein Gp19 in the groundwater demonstrated that its abundance tracked with the abundance of Geobacter species. These results suggest that the enhanced growth of Geobacter species in the subsurface associated with in situ uranium bioremediation increased the abundance and activity of Geobacter-associated phage and show that future studies should focus on how these phages might be influencing the ecology of this site. PMID:25083935

BLENDING LOW ENRICHED URANIUM WITH DEPLETED URANIUM TO CREATE A SOURCE MATERIAL ORE THAT CAN BE PROCESSED FOR THE RECOVERY OF YELLOWCAKE AT A CONVENTIONAL URANIUM MILL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schutt, Stephen M.; Hochstein, Ron F.; Frydenlund, David C.

2003-02-27

Throughout the United States Department of Energy (DOE) complex, there are a number of streams of low enriched uranium (LEU) that contain various trace contaminants. These surplus nuclear materials require processing in order to meet commercial fuel cycle specifications. To date, they have not been designated as waste for disposal at the DOE's Nevada Test Site (NTS). Currently, with no commercial outlet available, the DOE is evaluating treatment and disposal as the ultimate disposition path for these materials. This paper will describe an innovative program that will provide a solution to DOE that will allow disposition of these materials atmore » a cost that will be competitive with treatment and disposal at the NTS, while at the same time recycling the material to recover a valuable energy resource (yellowcake) for reintroduction into the commercial nuclear fuel cycle. International Uranium (USA) Corporation (IUSA) and Nuclear Fuel Services, Inc. (NFS) have entered into a commercial relationship to pursue the development of this program. The program involves the design of a process and construction of a plant at NFS' site in Erwin, Tennessee, for the blending of contaminated LEU with depleted uranium (DU) to produce a uranium source material ore (USM Ore{trademark}). The USM Ore{trademark} will then be further processed at IUC's White Mesa Mill, located near Blanding, Utah, to produce conventional yellowcake, which can be delivered to conversion facilities, in the same manner as yellowcake that is produced from natural ores or other alternate feed materials. The primary source of feed for the business will be the significant sources of trace contaminated materials within the DOE complex. NFS has developed a dry blending process (DRYSM Process) to blend the surplus LEU material with DU at its Part 70 licensed facility, to produce USM Ore{trademark} with a U235 content within the range of U235 concentrations for source material. By reducing the U235 content to source material levels in this manner, the material will be suitable for processing at a conventional uranium mill under its existing Part 40 license to remove contaminants and enable the product to re-enter the commercial fuel cycle. The tailings from processing the USM Ore{trademark} at the mill will be permanently disposed of in the mill's tailings impoundment as 11e.(2) byproduct material. Blending LEU with DU to make a uranium source material ore that can be returned to the nuclear fuel cycle for processing to produce yellowcake, has never been accomplished before. This program will allow DOE to disposition its surplus LEU and DU in a cost effective manner, and at the same time provide for the recovery of valuable energy resources that would be lost through processing and disposal of the materials. This paper will discuss the nature of the surplus LEU and DU materials, the manner in which the LEU will be blended with DU to form a uranium source material ore, and the legal means by which this blending can be accomplished at a facility licensed under 10 CFR Part 70 to produce ore that can be processed at a conventional uranium mill licensed under 10 CFR Part 40.« less

Natural bacterial communities serve as quantitative geochemical biosensors.

PubMed

Smith, Mark B; Rocha, Andrea M; Smillie, Chris S; Olesen, Scott W; Paradis, Charles; Wu, Liyou; Campbell, James H; Fortney, Julian L; Mehlhorn, Tonia L; Lowe, Kenneth A; Earles, Jennifer E; Phillips, Jana; Techtmann, Steve M; Joyner, Dominique C; Elias, Dwayne A; Bailey, Kathryn L; Hurt, Richard A; Preheim, Sarah P; Sanders, Matthew C; Yang, Joy; Mueller, Marcella A; Brooks, Scott; Watson, David B; Zhang, Ping; He, Zhili; Dubinsky, Eric A; Adams, Paul D; Arkin, Adam P; Fields, Matthew W; Zhou, Jizhong; Alm, Eric J; Hazen, Terry C

2015-05-12

Biological sensors can be engineered to measure a wide range of environmental conditions. Here we show that statistical analysis of DNA from natural microbial communities can be used to accurately identify environmental contaminants, including uranium and nitrate at a nuclear waste site. In addition to contamination, sequence data from the 16S rRNA gene alone can quantitatively predict a rich catalogue of 26 geochemical features collected from 93 wells with highly differing geochemistry characteristics. We extend this approach to identify sites contaminated with hydrocarbons from the Deepwater Horizon oil spill, finding that altered bacterial communities encode a memory of prior contamination, even after the contaminants themselves have been fully degraded. We show that the bacterial strains that are most useful for detecting oil and uranium are known to interact with these substrates, indicating that this statistical approach uncovers ecologically meaningful interactions consistent with previous experimental observations. Future efforts should focus on evaluating the geographical generalizability of these associations. Taken as a whole, these results indicate that ubiquitous, natural bacterial communities can be used as in situ environmental sensors that respond to and capture perturbations caused by human impacts. These in situ biosensors rely on environmental selection rather than directed engineering, and so this approach could be rapidly deployed and scaled as sequencing technology continues to become faster, simpler, and less expensive. Here we show that DNA from natural bacterial communities can be used as a quantitative biosensor to accurately distinguish unpolluted sites from those contaminated with uranium, nitrate, or oil. These results indicate that bacterial communities can be used as environmental sensors that respond to and capture perturbations caused by human impacts. Copyright © 2015 Smith et al.

Natural bacterial communities serve as quantitative geochemical biosensors

DOE PAGES

Smith, Mark B.; Rocha, Andrea M.; Smillie, Chris S.; ...

2015-05-12

Biological sensors can be engineered to measure a wide range of environmental conditions. Here we show that statistical analysis of DNA from natural microbial communities can be used to accurately identify environmental contaminants, including uranium and nitrate at a nuclear waste site. In addition to contamination, sequence data from the 16S rRNA gene alone can quantitatively predict a rich catalogue of 26 geochemical features collected from 93 wells with highly differing geochemistry characteristics. We extend this approach to identify sites contaminated with hydrocarbons from the Deepwater Horizon oil spill, finding that altered bacterial communities encode a memory of prior contamination,more » even after the contaminants themselves have been fully degraded. We show that the bacterial strains that are most useful for detecting oil and uranium are known to interact with these substrates, indicating that this statistical approach uncovers ecologically meaningful interactions consistent with previous experimental observations. Future efforts should focus on evaluating the geographical generalizability of these associations. Taken as a whole, these results indicate that ubiquitous, natural bacterial communities can be used as in situ environmental sensors that respond to and capture perturbations caused by human impacts. These in situ biosensors rely on environmental selection rather than directed engineering, and so this approach could be rapidly deployed and scaled as sequencing technology continues to become faster, simpler, and less expensive. Here we show that DNA from natural bacterial communities can be used as a quantitative biosensor to accurately distinguish unpolluted sites from those contaminated with uranium, nitrate, or oil. These results indicate that bacterial communities can be used as environmental sensors that respond to and capture perturbations caused by human impacts.« less

Hydrogeophysical Cyberinfrastructure For Real-Time Interactive Browser Controlled Monitoring Of Near Surface Hydrology: Results Of A 13 Month Monitoring Effort At The Hanford 300 Area

NASA Astrophysics Data System (ADS)

Versteeg, R. J.; Johnson, T.; Henrie, A.; Johnson, D.

2013-12-01

The Hanford 300 Area, located adjacent to the Columbia River in south-central Washington, USA, is the site of former research and uranium fuel rod fabrication facilities. Waste disposal practices at the site included discharging between 33 and 59 metric tons of uranium over a 40 year period into shallow infiltration galleries, resulting in persistent uranium contamination within the vadose and saturated zones. Uranium transport from the vadose zone to the saturated zone is intimately linked with water table fluctuations and river water driven by upstream dam operations. Different remedial efforts have occurred at the site to address uranium contamination. Numerous investigations are occurring at the site, both to investigate remedial performance and to increase the understanding of uranium dynamics. Several of these studies include acquisition of large hydrological and time lapse electrical geophysical data sets. Such datasets contain large amounts of information on hydrological processes. There are substantial challenges in how to effectively deal with the data volumes of such datasets, how to process such datasets and how to provide users with the ability to effectively access and synergize the hydrological information contained in raw and processed data. These challenges motivated the development of a cloud based cyberinfrastructure for dealing with large electrical hydrogeophysical datasets. This cyberinfrastructure is modular and extensible and includes datamanagement, data processing, visualization and result mining capabilities. Specifically, it provides for data transmission to a central server, data parsing in a relational database and processing of the data using a PNNL developed parallel inversion code on either dedicated or commodity compute clusters. Access to results is done through a browser with interactive tools allowing for generation of on demand visualization of the inversion results as well as interactive data mining and statistical calculation. This infrastructure was used for the acquisition and processing of an electrical geophysical timelapse survey which was collected over a highly instrumented field site in the Hanford 300 Area. Over a 13 month period between November 2011 and December 2012 1823 timelapse datasets were collected (roughly 5 datasets a day for a total of 23 million individual measurements) on three parallel resistivity lines of 30 m each with 0.5 meter electrode spacing. In addition, hydrological and environmental data were collected from dedicated and general purpose sensors. This dataset contains rich information on near surface processes on a range of different spatial and temporal scales (ranging from hourly to seasonal). We will show how this cyberinfrastructure was used to manage and process this dataset and how the cyberinfrastructure can be used to access, mine and visualize the resulting data and information.

US Department of Energy Grand Junction Projects Office Remedial Action Project. Final report of the decontamination and decommissioning of Building 52 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krabacher, J.E.

1996-08-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the U.S. Atomic Energy Commission`s domestic uranium procurement program. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, also was the remedial action contractor. Building 52more » was found to be radiologically contaminated and was demolished in 1994. The soil area within the footprint of the building has been remediated in accordance with the identified standards and the area can be released for unlimited exposure and unrestricted use. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Final report of the decontamination and decommission of Building 31 at the Grand Junction Projects Office Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krabacher, J.E.

1996-07-01

The U.S. Department of Energy (DOE) Grand Junction Projects Office (GJPO) occupies a 61.7-acre facility along the Gunnison River near Grand Junction, Colorado. This site was contaminated with uranium ore and mill tailings during uranium refining activities of the Manhattan Engineer District and during pilot milling experiments conducted for the domestic uranium procurement program funded by the U.S. Atomic Energy Commission. The DOE Defense Decontamination and Decommissioning Program established the GJPO Remedial Action Project to clean up and restore the facility lands, improvements, and the underlying aquifer. The site contractor for the facility, Rust Geotech, also was the remedial actionmore » contractor. Radiological contamination was identified in Building 31 and the building was demolished in 1992. The soil area within the footprint of the building has been remediated in accordance with the identified standards and the area can be released for unlimited exposure and unrestricted use. This area was addressed in the summary final report of the remediation of the exterior areas of the GJPO facility. This document was prepared in response to a DOE request for an individual final report for each contaminated GJPO building.« less

Anaerobic U(IV) Bio-oxidation and the Resultant Remobilization of Uranium in Contaminated Sediments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Coates, John D.

2005-06-01

A proposed strategy for the remediation of uranium (U) contaminated sites is based on immobilizing U by reducing the oxidized soluble U, U(VI), to form a reduced insoluble end product, U(IV). Due to the use of nitric acid in the processing of nuclear fuels, nitrate is often a co-contaminant found in many of the environments contaminated with uranium. Recent studies indicate that nitrate inhibits U(VI) reduction in sediment slurries. However, the mechanism responsible for the apparent inhibition of U(VI) reduction is unknown, i.e. preferential utilization of nitrate as an electron acceptor, direct biological oxidation of U(IV) coupled to nitrate reduction,more » and/or abiotic oxidation by intermediates of nitrate reduction. Recent studies indicates that direct biological oxidation of U(IV) coupled to nitrate reduction may exist in situ, however, to date no organisms have been identified that can grow by this metabolism. In an effort to evaluate the potential for nitrate-dependent bio-oxidation of U(IV) in anaerobic sedimentary environments, we have initiated the enumeration of nitrate-dependent U(IV) oxidizing bacteria. Sediments, soils, and groundwater from uranium (U) contaminated sites, including subsurface sediments from the NABIR Field Research Center (FRC), as well as uncontaminated sites, including subsurface sediments from the NABIR FRC and Longhorn Army Ammunition Plant, Texas, lake sediments, and agricultural field soil, sites served as the inoculum source. Enumeration of the nitrate-dependent U(IV) oxidizing microbial population in sedimentary environments by most probable number technique have revealed sedimentary microbial populations ranging from 9.3 x 101 - 2.4 x 103 cells (g sediment)-1 in both contaminated and uncontaminated sites. Interestingly uncontaminated subsurface sediments (NABIR FRC Background core FB618 and Longhorn Texas Core BH2-18) both harbored the most numerous nitrate-dependent U(IV) oxidizing population 2.4 x 103 cells (g sediment)-1. The nitrate-dependent U(IV) oxidizing microbial population in groundwaters is less numerous ranging from 0 cells mL-1 (Well FW300, Uncontaminated Background NABIR FRC) to 4.3 x 102 cells mL-1 (Well TPB16, Contaminated Area 2 NABIR FRC). The presence of nitrate-dependent U(IV) oxidizing bacteria supports our hypothesis that bacteria capable of anaerobic U(IV) oxidation are ubiquitous and indigenous to sedimentary and groundwater environments.« less

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2013 CFR

2013-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2012 CFR

2012-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2014 CFR

2014-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

Iron Mineralogy and Uranium-Binding Environment in the Rhizosphere of a Wetland Soil

EPA Science Inventory

Wetlands mitigate the migration of groundwater contaminants through a series of biogeochemical gradients that enhance multiple contaminant-binding processes. The hypothesis of this study was that wetland plant roots contribute organic carbon and release O₂ within the ...

Potential aquifer vulnerability in regions down-gradient from uranium in situ recovery (ISR) sites.

PubMed

Saunders, James A; Pivetz, Bruce E; Voorhies, Nathan; Wilkin, Richard T

2016-12-01

Sandstone-hosted roll-front uranium ore deposits originate when U(VI) dissolved in groundwater is reduced and precipitated as insoluble U(IV) minerals. Groundwater redox geochemistry, aqueous complexation, and solute migration are important in leaching uranium from source rocks and transporting it in low concentrations to a chemical redox interface where it is deposited in an ore zone typically containing the uranium minerals uraninite, pitchblende, and/or coffinite; various iron sulfides; native selenium; clays; and calcite. In situ recovery (ISR) of uranium ores is a process of contacting the uranium mineral deposit with leaching and oxidizing (lixiviant) fluids via injection of the lixiviant into wells drilled into the subsurface aquifer that hosts uranium ore, while other extraction wells pump the dissolved uranium after dissolution of the uranium minerals. Environmental concerns during and after ISR include water quality degradation from: 1) potential excursions of leaching solutions away from the injection zone into down-gradient, underlying, or overlying aquifers; 2) potential migration of uranium and its decay products (e.g., Ra, Rn, Pb); and, 3) potential mobilization and migration of redox-sensitive trace metals (e.g., Fe, Mn, Mo, Se, V), metalloids (e.g., As), and anions (e.g., sulfate). This review describes the geochemical processes that control roll-front uranium transport and fate in groundwater systems, identifies potential aquifer vulnerabilities to ISR operations, identifies data gaps in mitigating these vulnerabilities, and discusses the hydrogeological characterization involved in developing a monitoring program. Published by Elsevier Ltd.

Uranium and other contaminants in hair from the parents of children with congenital anomalies in Fallujah, Iraq

PubMed Central

2011-01-01

Background Recent reports have drawn attention to increases in congenital birth anomalies and cancer in Fallujah Iraq blamed on teratogenic, genetic and genomic stress thought to result from depleted Uranium contamination following the battles in the town in 2004. Contamination of the parents of the children and of the environment by Uranium and other elements was investigated using Inductively Coupled Plasma Mass Spectrometry. Hair samples from 25 fathers and mothers of children diagnosed with congenital anomalies were analysed for Uranium and 51 other elements. Mean ages of the parents was: fathers 29.6 (SD 6.2); mothers: 27.3 (SD 6.8). For a sub-group of 6 women, long locks of hair were analysed for Uranium along the length of the hair to obtain information about historic exposures. Samples of soil and water were also analysed and Uranium isotope ratios determined. Results Levels of Ca, Mg, Co, Fe, Mn, V, Zn, Sr, Al, Ba, Bi, Ga, Pb, Hg, Pd and U (for mothers only) were significantly higher than published mean levels in an uncontaminated population in Sweden. In high excess were Ca, Mg, Sr, Al, Bi and Hg. Of these only Hg can be considered as a possible cause of congenital anomaly. Mean levels for Uranium were 0.16 ppm (SD: 0.11) range 0.02 to 0.4, higher in mothers (0.18 ppm SD 0.09) than fathers (0.11 ppm; SD 0.13). The highly unusual non-normal Fallujah distribution mean was significantly higher than literature results for a control population Southern Israel (0.062 ppm) and a non-parametric test (Mann Whitney-Wilcoxon) gave p = 0.016 for this comparison of the distribution. Mean levels in Fallujah were also much higher than the mean of measurements reported from Japan, Brazil, Sweden and Slovenia (0.04 ppm SD 0.02). Soil samples show low concentrations with a mean of 0.76 ppm (SD 0.42) and range 0.1-1.5 ppm; (N = 18). However it may be consistent with levels in drinking water (2.28 μgL-1) which had similar levels to water from wells (2.72 μgL-1) and the river Euphrates (2.24 μgL-1). In a separate study of a sub group of mothers with long hair to investigate historic Uranium excretion the results suggested that levels were much higher in the past. Uranium traces detected in the soil samples and the hair showed slightly enriched isotopic signatures for hair U238/U235 = (135.16 SD 1.45) compared with the natural ratio of 137.88. Soil sample Uranium isotope ratios were determined after extraction and concentration of the Uranium by ion exchange. Results showed statistically significant presence of enriched Uranium with a mean of 129 with SD5.9 (for this determination, the natural Uranium 95% CI was 132.1 < Ratio < 144.1). Conclusions Whilst caution must be exercised about ruling out other possibilities, because none of the elements found in excess are reported to cause congenital diseases and cancer except Uranium, these findings suggest the enriched Uranium exposure is either a primary cause or related to the cause of the congenital anomaly and cancer increases. Questions are thus raised about the characteristics and composition of weapons now being deployed in modern battlefields PMID:21888647

Compositions and methods for removing arsenic in water

DOEpatents

Gadgil, Ashok Jagannth [El Cerrito, CA

2011-02-22

Compositions and methods and for contaminants from water are provided. The compositions comprise ferric hydroxide and ferric oxyhydride coated substrates for use in removing the contaminant from the water. Contacting water bearing the contaminant with the substrates can substantially reduce contaminant levels therein. Methods of oxidizing the contaminants in water to facilitate their removal by the ferric hydroxide and ferric oxyhydride coated substrates are also provided. The contaminants include, but are not limited to, arsenic, selenium, uranium, lead, cadmium, nickel, copper, zinc, chromium and vanadium, their oxides and soluble salts thereof.

Characterization of Archaeal Community in Contaminated and Uncontaminated Surface Stream Sediments

PubMed Central

Porat, Iris; Vishnivetskaya, Tatiana A.; Mosher, Jennifer J.; Brandt, Craig C.; Yang, Zamin K.; Brooks, Scott C.; Liang, Liyuan; Drake, Meghan M.; Podar, Mircea; Brown, Steven D.

2010-01-01

Archaeal communities from mercury and uranium-contaminated freshwater stream sediments were characterized and compared to archaeal communities present in an uncontaminated stream located in the vicinity of Oak Ridge, TN, USA. The distribution of the Archaea was determined by pyrosequencing analysis of the V4 region of 16S rRNA amplified from 12 streambed surface sediments. Crenarchaeota comprised 76% of the 1,670 archaeal sequences and the remaining 24% were from Euryarchaeota. Phylogenetic analysis further classified the Crenarchaeota as a Freshwater Group, Miscellaneous Crenarchaeota group, Group I3, Rice Cluster VI and IV, Marine Group I and Marine Benthic Group B; and the Euryarchaeota into Methanomicrobiales, Methanosarcinales, Methanobacteriales, Rice Cluster III, Marine Benthic Group D, Deep Sea Hydrothermal Vent Euryarchaeota 1 and Eury 5. All groups were previously described. Both hydrogen- and acetate-dependent methanogens were found in all samples. Most of the groups (with 60% of the sequences) described in this study were not similar to any cultivated isolates, making it difficult to discern their function in the freshwater microbial community. A significant decrease in the number of sequences, as well as in the diversity of archaeal communities was found in the contaminated sites. The Marine Group I, including the ammonia oxidizer Nitrosopumilus maritimus, was the dominant group in both mercury and uranium/nitrate-contaminated sites. The uranium-contaminated site also contained a high concentration of nitrate, thus Marine Group I may play a role in nitrogen cycle. Electronic supplementary material The online version of this article (doi:10.1007/s00248-010-9734-2) contains supplementary material, which is available to authorized users. PMID:20725722

Uranium in bone: metabolic and autoradiographic studies in the rat.

PubMed

Priest, N D; Howells, G R; Green, D; Haines, J W

1982-03-01

The distribution and retention of intravenously injected hexavalent uranium-233 in the skeleton of the female rat has been investigated using a variety of autoradiographic and radiochemical techniques. These showed that approximately one third of the injected uranium is deposited in the skeleton where it is retained with an initial biological half-time of approximately 40 days. The studies also showed that: 1 Uranium is initially deposited onto all types of bone surface, but preferentially onto those that are accreting. 2 Uranium is deposited in the calcifying zones of skeletal cartilage. 3 Bone accretion results in the burial of surface deposits of uranium. 4 Bone resorption causes the removal of uranium from surfaces. 5 Resorbed uranium is not retained by osteoclasts and macrophages in the bone marrow. 6 Uranium removed from bone surfaces enters the bloodstream where most is either redeposited in bone or excreted via the kidneys. 7 The recycling of resorbed uranium within the skeleton tends to produce a uniform level of uranium contamination throughout mineralized bone. These results are taken to indicate that uranium deposition in bone shares characteristics in common with both the 'volume-seeking radionuclides' typified by the alkaline earth elements and with the 'bone surface-seeking radionuclides' typified by plutonium.

The effect of Si and Al concentrations on the removal of U(VI) in the alkaline conditions created by NH3 gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Katsenovich, Yelena P.; Cardona, Claudia; Lapierre, Robert

2016-10-01

Remediation of uranium in the deep unsaturated zone is a challenging task, especially in the presence of oxygenated, high-carbonate alkalinity soil and pore water composition typical for arid and semi-arid environments of the western regions of the U.S. This study evaluates the effect of various pore water constituencies on changes of uranium concentrations in alkaline conditions, created in the presence of reactive gases such as NH3 to effectively mitigate uranium contamination in the vadose zone sediments. This contaminant is a potential source for groundwater pollution through slow infiltration of soluble and highly mobile uranium species towards the water table. Themore » objective of this research was to evaluate uranium sequestration efficiencies in the alkaline synthetic pore water solutions prepared in a broad range of Si, Al, and bicarbonate concentrations typically present in field systems of the western U.S. regions and identify solid uranium-bearing phases that result from ammonia gas treatment. In previous studies (Szecsody et al. 2012; Zhong et al. 2015), although uranium mobility was greatly decreased, solid phases could not be identified at the low uranium concentrations in field-contaminated sediments. The chemical composition of the synthetic pore water used in the experiments varied for silica (5–250 mM), Al3+ (2.8 or 5 mM), HCO3- (0–100 mM) and U(VI) (0.0021–0.0084 mM) in the solution mixture. Experiment results suggested that solutions with Si concentrations higher than 50 mM exhibited greater removal efficiencies of U(VI). Solutions with higher concentrations of bicarbonate also exhibited greater removal efficiencies for Si, Al, and U(VI). Overall, the silica polymerization reaction leading to the formation of Si gel correlated with the removal of U(VI), Si, and Al from the solution. If no Si polymerization was observed, there was no U removal from the supernatant solution. Speciation modeling indicated that the dominant uranium species in the presence of bicarbonate were anionic uranyl carbonate complexes (UO2(CO3)2-2 and UO2(CO3)3-4) and in the absence of bicarbonate in the solution, U(VI) major species appeared as uranyl-hydroxide (UO2(OH)3- and UO2(OH)4-2) species. The model also predicted the formation of uranium solid phases. Uranyl carbonates as rutherfordine [UO2CO3], cejkaite [Na4(UO2)(CO3)3] and hydrated uranyl silicate phases as Na-boltwoodite [Na(UO2)(SiO4)·1.5H2O] were anticipated for most of the synthetic pore water compositions amended from medium (2.9 mM) to high (100 mM) bicarbonate concentrations.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kanel, S. R.; Clement, T. P.; Barnett, M. O.

Synthetic nano-scale hydroxyapatite (NHA) was prepared and characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM) methods. The XRD data confirmed that the crystalline structure and chemical composition of NHA correspond to Ca 5 OH(PO 4 ) 3 . The SEM data confirmed the size of NHA to be less than 50 nm. A two-dimensional physical model packed with saturated porous media was used to study the transport characteristics of NHA under constant flow conditions. The data show that the transport patterns of NHA were almost identical to tracer transport patterns. This result indicates that the NHA material can movemore » with water like a tracer, and its movement was neither retarded nor influenced by any physicochemical interactions and/or density effects. We have also tested the reactivity of NHA with 1 mg/L hexavalent uranium (U(VI)) and found that complete removal of U(VI) is possible using 0.5 g/L NHA at pH 5 to 6. Our results demonstrate that NHA has the potential to be injected as a dilute slurry for in situ treatment of U(VI)-contaminated groundwater systems.« less

Linearity assumption in soil-to-plant transfer factors of natural uranium and radium in Helianthus annuus L.

PubMed

Rodríguez, P Blanco; Tomé, F Vera; Fernández, M Pérez; Lozano, J C

2006-05-15

The linearity assumption of the validation of soil-to-plant transfer factors of natural uranium and (226)Ra was tested using Helianthus annuus L. (sunflower) grown in a hydroponic medium. Transfer of natural uranium and (226)Ra was tested in both the aerial fraction of plants and in the overall seedlings (roots and shoots). The results show that the linearity assumption can be considered valid in the hydroponic growth of sunflowers for the radionuclides studied. The ability of sunflowers to translocate uranium and (226)Ra was also investigated, as well as the feasibility of using sunflower plants to remove uranium and radium from contaminated water, and by extension, their potential for phytoextraction. In this sense, the removal percentages obtained for natural uranium and (226)Ra were 24% and 42%, respectively. Practically all the uranium is accumulated in the roots. However, 86% of the (226)Ra activity concentration in roots was translocated to the aerial part.

Chemical aspects of uranium behavior in soils: A review

NASA Astrophysics Data System (ADS)

Vodyanitskii, Yu. N.

2011-08-01

Uranium has varying degrees of oxidation (+4 and +6) and is responsive to changes in the redox potential of the environment. It is deposited at the reduction barrier with the participation of biota and at the sorption barrier under oxidative conditions. Iron (hydr)oxides are the strongest sorbents of uranium. Uranium, being an element of medium biological absorption, can accumulate (relative to thorium) in the humus horizons of some soils. The high content of uranium in uncontaminated soils is most frequently inherited from the parent rocks in the regions of positive U anomalies: in the soils developed on oil shales and in the marginal zone of bogs at the reduction barrier. The development of nuclear and coal-fired power engineering resulted in the environmental contamination with uranium. The immobilization of anthropogenic uranium at artificial geochemical barriers is based on two preconditions: the stimulation of on-site metal-reducing bacteria or the introduction of strong mineral reducers, e.g., Fe at low degrees of oxidation.

Dose-response relationships between internally-deposited uranium and select health outcomes in gaseous diffusion plant workers, 1948-2011.

PubMed

Yiin, James H; Anderson, Jeri L; Bertke, Stephen J; Tollerud, David J

2018-05-09

To examine dose-response relationships between internal uranium exposures and select outcomes among a cohort of uranium enrichment workers. Cox regression was conducted to examine associations between selected health outcomes and cumulative internal uranium with consideration for external ionizing radiation, work-related medical X-rays and contaminant radionuclides technetium ( 99 Tc) and plutonium ( 239 Pu) as potential confounders. Elevated and monotonically increasing mortality risks were observed for kidney cancer, chronic renal diseases, and multiple myeloma, and the association with internal uranium absorbed organ dose was statistically significant for multiple myeloma. Adjustment for potential confounders had minimal impact on the risk estimates. Kidney cancer, chronic renal disease, and multiple myeloma mortality risks were elevated with increasing internal uranium absorbed organ dose. The findings add to evidence of an association between internal exposure to uranium and cancer. Future investigation includes a study of cancer incidence in this cohort. © 2018 Wiley Periodicals, Inc.

Vacuum ultraviolet spectra of uranium hexafluoride/argon mixtures

NASA Technical Reports Server (NTRS)

Krascella, N. L.

1976-01-01

The transmission properties of room temperature helium at pressures up to 20 atmospheres were determined in the wavelength range from 80 to 300 nm. Similarly, the transmission properties of uranium hexafluoride at 393 K (pressures less than 1.0 mm) were determined in the wavelength range from 80 to about 120 nm. The results show that high pressure helium is sufficiently transparent in the vacuum ultraviolet region (provided trace contaminants are removed) to be utilized as a transparent purge gas in future fissioning gaseous uranium plasma reactor experiments. Absorption cross sections for uranium hexafluoride were calculated from the data between 80 and 120 nm and were of the order of 10 to the -17 power sq cm.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rabin, S.A.; Lotts, A.L.; Hammond, J.P.

Uranium --molybdenum alloy rods containing from 10 to 15 wt% Mo and 1/16- in. in diameter were successfully fabricated by hot rotary swaging, followed by machining to remove the protective sheathing (Inconel with molybdenum barrier). Structurally strong rods with densities greater than 95% of theoretical were produced from both calciumreduced uranium mixed with hydrogen-reduced molybdenum and acid-cleaned, prealloyed shot when reduced in area about 55% at 1050 or 1100 deg C. Alloy homogeneity was good with prealloyed powders; however, traces of molybdenum -rich, gamma phase persisted in the elemental uranium -molybdenum material after swaging at 1100 deg C. Swagings embodyingmore » hydride uranium or oxide- contaminated prealloyed shot were unsatisfactory because of insufficient consolidation or poor interparticle bonding. (auth)« less

Removal of Trace Elements by Cupric Oxide Nanoparticles from Uranium In Situ Recovery Bleed Water and Its Effect on Cell Viability

PubMed Central

Schilz, Jodi R.; Reddy, K. J.; Nair, Sreejayan; Johnson, Thomas E.; Tjalkens, Ronald B.; Krueger, Kem P.; Clark, Suzanne

2015-01-01

In situ recovery (ISR) is the predominant method of uranium extraction in the United States. During ISR, uranium is leached from an ore body and extracted through ion exchange. The resultant production bleed water (PBW) contains contaminants such as arsenic and other heavy metals. Samples of PBW from an active ISR uranium facility were treated with cupric oxide nanoparticles (CuO-NPs). CuO-NP treatment of PBW reduced priority contaminants, including arsenic, selenium, uranium, and vanadium. Untreated and CuO-NP treated PBW was used as the liquid component of the cell growth media and changes in viability were determined by the MTT (3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide) assay in human embryonic kidney (HEK 293) and human hepatocellular carcinoma (Hep G2) cells. CuO-NP treatment was associated with improved HEK and HEP cell viability. Limitations of this method include dilution of the PBW by growth media components and during osmolality adjustment as well as necessary pH adjustment. This method is limited in its wider context due to dilution effects and changes in the pH of the PBW which is traditionally slightly acidic however; this method could have a broader use assessing CuO-NP treatment in more neutral waters. PMID:26132311

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium

PubMed Central

Thorgersen, Michael P.; Lancaster, W. Andrew; Rajeev, Lara; Ge, Xiaoxuan; Vaccaro, Brian J.; Poole, Farris L.; Arkin, Adam P.; Mukhopadhyay, Aindrila

2016-01-01

ABSTRACT Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC had an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. IMPORTANCE Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Herein, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. While other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments. PMID:27913415

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thorgersen, Michael P.; Lancaster, W. Andrew; Rajeev, Lara

Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC hadmore » an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Here in this paper, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. Finally, while other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments.« less

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium.

PubMed

Thorgersen, Michael P; Lancaster, W Andrew; Rajeev, Lara; Ge, Xiaoxuan; Vaccaro, Brian J; Poole, Farris L; Arkin, Adam P; Mukhopadhyay, Aindrila; Adams, Michael W W

2017-02-15

Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC had an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Herein, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. While other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments. Copyright © 2017 American Society for Microbiology.

The importance of colloids and mires for the transport of uranium isotopes through the Kalix River watershed and Baltic Sea

DOE Office of Scientific and Technical Information (OSTI.GOV)

Porcelli, D.; Wasserburg, G.J.; Andersson, P.S.

The importance of colloids and organic deposits for the transport of uranium isotopes from continental source regions and through the estuarine environment was investigated in the mire-rich Kalix River drainage basin in northern Sweden and the Baltic Sea. Ultrafiltration techniques were used to separate uranium and other elements associated with colloids > 10 kD and >3 kD from {open_quotes}solute{close_quotes} uranium and provided consistent results and high recovery rates for uranium as well as for other elements from large volume samples. Uranium concentrations in 0.45 {mu}m-filtered Kalix River water samples increased by a factor of 3 from near the headwaters inmore » the Caledonides to the river mouth while major cation concentrations were relatively constant. {sup 234}U {sup 238}U ratios were high ({delta}{sup 234}U = 770-1500) throughout the basin, without showing any simple pattern, and required a supply of {sup 234}U-rich water. Throughout the Kalix River, a large fraction (30-90%) of the uranium is carried by >10 kD colloids, which is compatible with uranium complexation with humic acids. No isotopic differences were found between colloid-associated and solute uranium. Within the Baltic Sea, about half of the uranium is removed at low salinities. The proportion that is lost is equivalent to that of river-derived colloid-bound uranium, suggesting that while solute uranium behaves conservatively during estuarine mixing, colloid-bound uranium is lost due to rapid flocculation of colloidal material. The association of uranium with colloids therefore may be an important parameter in determining uranium estuarine behavior. Mire peats in the Kalix River highly concentrate uranium and are potentially a significant source of recoil {sup 234}U to the mirewaters and river waters. However, mirewater data clearly demonstrate that only small {sup 234}U/{sup 238}U shifts are generated relative to inflowing groundwater. 63 refs., 8 figs., 3 tabs.« less

The use of unmanned aerial systems for the mapping of legacy uranium mines.

PubMed

Martin, P G; Payton, O D; Fardoulis, J S; Richards, D A; Scott, T B

2015-05-01

Historical mining of uranium mineral veins within Cornwall, England, has resulted in a significant amount of legacy radiological contamination spread across numerous long disused mining sites. Factors including the poorly documented and aged condition of these sites as well as the highly localised nature of radioactivity limit the success of traditional survey methods. A newly developed terrain-independent unmanned aerial system [UAS] carrying an integrated gamma radiation mapping unit was used for the radiological characterisation of a single legacy mining site. Using this instrument to produce high-spatial-resolution maps, it was possible to determine the radiologically contaminated land areas and to rapidly identify and quantify the degree of contamination and its isotopic nature. The instrument was demonstrated to be a viable tool for the characterisation of similar sites worldwide. Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.

Radioactivity of the soil in Vojvodina (northern province of Serbia and Montenegro).

PubMed

Bikit, I; Slivka, J; Conkić, Lj; Krmar, M; Vesković, M; Zikić-Todorović, N; Varga, E; Curcić, S; Mrdja, D

2005-01-01

The widespread public belief that during the bombardment of Vojvodina (Yugoslavia) this region was contaminated by depleted uranium has recently raised public concern with respect to the potential contamination of agricultural products due to soil radioactivity. Based on the gamma-spectrometric analysis of 50 soil samples taken from the region of Vojvodina we concluded that there is no increase of radioactivity that could endanger the food production. Taking into account the transfer factors of 137Cs to plants, the measured activity concentrations of this isotope should not endanger the health safety of the produced food. No traces of depleted uranium have been found. The natural radioactivity levels are compared with the results form other countries.

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Sutton, J.B.

1958-02-18

This patent relates to an improved method for the decontamination of plutonium. The process consists broadly in an improvement in a method for recovering plutonium from radioactive uranium fission products in aqueous solutions by decontamination steps including byproduct carrier precipitation comprising the step of introducing a preformed aqueous slurry of a hydroxide of a metal of group IV B into any aqueous acidic solution which contains the plutonium in the hexavalent state, radioactive uranium fission products contaminant and a by-product carrier precipitate and separating the metal hydroxide and by-product precipitate from the solution. The process of this invention is especially useful in the separation of plutonium from radioactive zirconium and columbium fission products.

Nuclear facility decommissioning and site remedial actions: A selected bibliography, Volume 18. Part 1B: Citations with abstracts, sections 10 through 16

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1997-09-01

This bibliography contains 3,638 citations with abstracts of documents relevant to environmental restoration, nuclear facility decontamination and decommissioning (D and D), uranium mill tailings management, and site remedial actions. The bibliography contains scientific, technical, financial, and regulatory information that pertains to DOE environmental restoration programs. The citations are separated by topic into 16 sections, including (1) DOE Environmental Restoration Program; (2) DOE D and D Program; (3) Nuclear Facilities Decommissioning; (4) DOE Formerly Utilized sites Remedial Action Program; (5) NORM-Contaminated Site Restoration; (6) DOE Uranium Mill Tailings Remedial Action Project; (7) Uranium Mill Tailings Management; (8) DOE Site-Wide Remedial Actions;more » (9) DOE Onsite Remedial Action Projects; (10) Contaminated Site Remedial Actions; (11) DOE Underground Storage Tank Remediation; (12) DOE Technology Development, Demonstration, and Evaluation; (13) Soil Remediation; (14) Groundwater Remediation; (15) Environmental Measurements, Analysis, and Decision-Making; and (16) Environmental Management Issues.« less

Determining the isotopic compositions of uranium and fission products in radioactive environmental microsamples using laser ablation ICP-MS with multiple ion counters.

PubMed

Boulyga, Sergei F; Prohaska, Thomas

2008-01-01

This paper presents the application of a multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS)--a Nu Plasma HR--equipped with three ion-counting multipliers and coupled to a laser ablation system (LA) for the rapid and sensitive determination of the 235U/238U, 236U/238U, 145Nd/143Nd, 146Nd/143Nd, 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios in microsamples collected in the vicinity of Chernobyl. Microsamples with dimensions ranging from a hundred mum to about 1 mm and with surface alpha activities of 3-38 mBq were first identified using nuclear track radiography. U, Nd and Ru isotope systems were then measured sequentially for the same microsample by LA-MC-ICP-MS. The application of a zoom ion optic for aligning the ion beams into the ion counters allows fast switching between different isotope systems, which enables all of the abovementioned isotope ratios to be measured for the same microsample within a total analysis time of 15-20 min (excluding MC-ICP-MS optimization and calibration). The 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios were measured for four microsamples and were found to be significantly lower than the natural ratios, indicating that the microsamples were contaminated with the corresponding fission products (Ru and Tc). A slight depletion in 146Nd of about 3-5% was observed in the contaminated samples, but the Nd isotopic ratios measured in the contaminated samples coincided with natural isotopic composition within the measurement uncertainty, as most of the Nd in the analyzed samples originates from the natural soil load of this element. The 235U/238U and 236U/238U isotope ratios were the most sensitive indicators of irradiated uranium. The present work yielded a significant variation in uranium isotope ratios in microsamples, in contrast with previously published results from the bulk analysis of contaminated samples originating from the vicinity of Chernobyl. Thus, the 235U/238U ratios measured in ten microsamples varied in the range from 0.0073 (corresponding to the natural uranium isotopic composition) to 0.023 (corresponding to initial 235U enrichment in reactor fuel). An inverse correlation was observed between the 236U/238U and 235U/238U isotope ratios, except in the case of one sample with natural uranium. The heterogeneity of the uranium isotope composition is attributed to the different burn-up grades of uranium in the fuel rods from which the microsamples originated.

Final Scientific/Technical Report – DE-FG02-06ER64172 – Reaction-Based Reactive Transport Modeling of Iron Reduction and Uranium Immobilization at Area 2 of the NABIR Field Research Center – Subproject to Co-PI Eric E. Roden

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eric E. Roden

2009-03-17

This report summarizes research conducted in conjunction with a project entitled “Reaction-Based Reactive Transport Modeling of Iron Reduction and Uranium Immobilization at Area 2 of the NABIR Field Research Center”, which was funded through the Integrative Studies Element of the former NABIR Program (now the Environmental Remediation Sciences Program) within the Office of Biological and Environmental Research. Dr. William Burgos (The Pennsylvania State University) was the overall PI/PD for the project, which included Brian Dempsey (Penn State), Gour-Tsyh (George) Yeh (Central Florida University), and Eric Roden (formerly at The University of Alabama, now at the University of Wisconsin) as separately-fundedmore » co-PIs. The project focused on development of a mechanistic understanding and quantitative models of coupled Fe(III)/U(VI) reduction in FRC Area 2 sediments. The work builds on our previous studies of microbial Fe(III) and U(VI) reduction, and was directly aligned with the Scheibe et al. ORNL FRC Field Project at Area 2. Area 2 is a shallow pathway for migration of contaminated groundwater to seeps in the upper reach of Bear Creek at ORNL, mainly through a ca. 1 m thick layer of gravel located 4-5 m below the ground surface. The gravel layer is sandwiched between an overlying layer of disturbed fill material, and 2-3 m of undisturbed shale saprolite derived from the underlying Nolichucky Shale bedrock. The fill was put in place when contaminated soils were excavated and replaced by native saprolite from an uncontaminated area within Bear Creek Valley; the gravel layer was presumably installed prior to addition of the fill in order to provide a stable surface for the operation of heavy machinery. The undisturbed saprolite is highly weathered bedrock that has unconsolidated character but retains much of the bedding and fracture structure of the parent rock (shale with interbedded limestone). Hydrological tracer studies conducted during the Scheibe et al. field project indicate that the gravel layer receives input of uranium from both upstream sources and from diffusive mass transfer out of highly contaminated fill and saprolite materials above and below the gravel layer. This research sought to examine biogeochemical processes likely to take place in the less conductive materials above and below the gravel during the in situ ethanol biostimulation experiment conducted at Area 2 during 2005-2006. The in situ experiment in turn examined the hypothesis that injection of electron donor into this layer would induce formation of a redox barrier in the less conductive materials, resulting in decreased mass transfer of uranium out these materials and attendant declines in groundwater U(VI) concentration. Our research was directed toward the following three major objectives relevant to formation of this redox barrier: (1) elucidate the kinetics and mechanisms of reduction of solid-phase Fe(III) and U(VI) in Area 2 sediments; (2) evaluate the potential for long-term sustained U(IV) reductive immobilization in Area 2 sediments; (3) numerically simulate the suite of hydrobiogeochemical processes occurring in experimental systems so as to facilitate modeling of in situ U(IV) immobilization at the field-scale.« less

Phytoremediation of a nitrogen-contaminated desert soil by native shrubs and microbial processes

DOE PAGES

Glenn, Edward P.; Jordan, Fiona; Waugh, W. Joseph

2016-02-24

Here, we combined phytoremediation and soil microbial nitrification and denitrification cycles to reduce nitrate and ammonium levels at a former uranium mill site near Monument Valley, Arizona. Ammonia used in uranium extraction was present throughout the soil profile. Sulfate,applied as sulfuric acid to solubilize uranium, was also present in the soil. These contaminants were leaching from a denuded area where a tailings pile had been removed and were migrating away from the site in groundwater. We planted the source area with two deep-rooted native shrubs, Atriplex cansescens and Sarcobatus vermiculatus, and irrigated transplants for 11 years at 20% the ratemore » of potential evapotranspiration to stimulate growth, then discontinued irrigation for 4 years. Over 15 years, total nitrogen levels dropped 82%, from 347 to 64 mg kg –1. Analysis of δ 15N supported our hypothesis that coupled microbial nitrification and denitrification processes were responsible for the loss of N. Soil sulfate levels changed little; however, evapotranspiration reduced sulfate leaching into the aquifer. For arid sites where traditional pump-and-treat methods are problematic, the Monument Valley data suggest that alternatives that incorporate native plants and rely on vadose zone biogeochemistry and hydrology could be a sustainable remediation for nitrogen contaminated soil.« less

Phytoremediation of a nitrogen-contaminated desert soil by native shrubs and microbial processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glenn, Edward P.; Jordan, Fiona; Waugh, W. Joseph

Here, we combined phytoremediation and soil microbial nitrification and denitrification cycles to reduce nitrate and ammonium levels at a former uranium mill site near Monument Valley, Arizona. Ammonia used in uranium extraction was present throughout the soil profile. Sulfate,applied as sulfuric acid to solubilize uranium, was also present in the soil. These contaminants were leaching from a denuded area where a tailings pile had been removed and were migrating away from the site in groundwater. We planted the source area with two deep-rooted native shrubs, Atriplex cansescens and Sarcobatus vermiculatus, and irrigated transplants for 11 years at 20% the ratemore » of potential evapotranspiration to stimulate growth, then discontinued irrigation for 4 years. Over 15 years, total nitrogen levels dropped 82%, from 347 to 64 mg kg –1. Analysis of δ 15N supported our hypothesis that coupled microbial nitrification and denitrification processes were responsible for the loss of N. Soil sulfate levels changed little; however, evapotranspiration reduced sulfate leaching into the aquifer. For arid sites where traditional pump-and-treat methods are problematic, the Monument Valley data suggest that alternatives that incorporate native plants and rely on vadose zone biogeochemistry and hydrology could be a sustainable remediation for nitrogen contaminated soil.« less

Uranium(VI) interactions with mackinawite in the presence and absence of bicarbonate and oxygen.

PubMed

Gallegos, Tanya J; Fuller, Christopher C; Webb, Samuel M; Betterton, William

2013-07-02

Mackinawite, Fe(II)S, samples loaded with uranium (10(-5), 10(-4), and 10(-3) mol U/g FeS) at pH 5, 7, and 9, were characterized using X-ray absorption spectroscopy and X-ray diffraction to determine the effects of pH, bicarbonate, and oxidation on uptake. Under anoxic conditions, a 5 g/L suspension of mackinawite lowered 5 × 10(-5) M uranium(VI) to below 30 ppb (1.26 × 10(-7) M) U. Between 82 and 88% of the uranium removed from solution by mackinawite was U(IV) and was nearly completely reduced to U(IV) when 0.012 M bicarbonate was added. Near-neighbor coordination consisting of uranium-oxygen and uranium-uranium distances indicates the formation of uraninite in the presence and absence of bicarbonate, suggesting reductive precipitation as the dominant removal mechanism. Following equilibration in air, mackinawite was oxidized to mainly goethite and sulfur and about 76% of U(IV) was reoxidized to U(VI) with coordination of uranium to axial and equatorial oxygen, similar to uranyl. Additionally, uranium-iron distances, typical of coprecipitation of uranium with iron oxides, and uranium-sulfur distances indicating bidentate coordination of U(VI) to sulfate were evident. The affinity of mackinawite and its oxidation products for U(VI) provides impetus for further study of mackinawite as a potential reactive medium for remediation of uranium-contaminated water.

Highly Efficient Interception and Precipitation of Uranium(VI) from Aqueous Solution by Iron-Electrocoagulation Combined with Cooperative Chelation by Organic Ligands.

PubMed

Li, Peng; Zhun, Bao; Wang, Xuegang; Liao, PingPing; Wang, Guanghui; Wang, Lizhang; Guo, Yadan; Zhang, Weimin

2017-12-19

A new strategy combining iron-electrocoagulation and organic ligands (OGLs) cooperative chelation was proposed to screen and precipitate low concentrations (0-18.52 μmol/L) of uranium contaminant in aqueous solution. We hypothesized that OGLs with amino, hydroxyl, and carboxyl groups hydrophobically/hydrophilically would realize precuring of uranyl ion at pH < 3.0, and the following iron-electrocoagulation would achieve faster and more efficient uranium precipitation. Experimentally, the strategy demonstrated highly efficient uranium(VI) precipitation efficiency, especially with hydrophilic macromolecular OGLs. The uranium removal efficiency at optimized experimental condition reached 99.65%. The decrease of zeta potential and the lattice enwrapping between U-OGLs chelates and flocculation precursor were ascribed to the enhanced uranium precipitation activity. Uranium was precipitated as oxides of U(VI) or higher valences that were easily captured in aggregated micelles under low operation current potential. The actual uranium tailing wastewater was treated, and a satisfied uranium removal efficiency of 99.02% was discovered. After elution of the precipitated flocs, a concentrated uranium solution (up to 106.52 μmol/L) with very few other metallic impurities was obtained. Therefore, the proposed strategy could remove uranium and concentrate it concurrently. This work could provide new insights into the purification and recovery of uranium from aqueous solutions in a cost-effective and environmentally friendly process.

Seasonal Hydrologic Controls on Uranium and Iron Biogeochemistry in a Riparian Aquifer

NASA Astrophysics Data System (ADS)

Wilkins, M.; Williams, K. H.; Danczak, R. E.; Yabusaki, S.; Fang, Y.; Hobson, C.

2015-12-01

The maintenance of geochemically reducing conditions is generally optimal for the formation and preservation of reduced metals and mineral phases that can limit contaminant fate and transport. At a riparian aquifer near Rifle, CO, we tracked over six months the biogeochemical response within the aquifer to an annual pulse of dissolved oxygen (DO) that results from snowmelt-driven changes in Colorado River stage. In reduced portions of the aquifer (naturally reduced zones; NRZs) the re-oxidation of abundant iron sulfide minerals was the dominant oxygen-consuming process, and resulted in little DO intrusion into the deeper aquifer. In less reduced areas, DO intruded through the entire vertical profile of the aquifer. Across both regions, these perturbations resulted in changes to the microbial community structure, and aqueous metal pools. Two potentially different mechanisms of uranium mobilization were observed; (1) re-oxidation of reduced U(IV) phases in response to DO intrusion, and (2) mobilization of U(VI) from the vadose zone during water table rise. This high-resolution, long-term monitoring of aquifer biogeochemistry at the Rifle site has revealed dynamic microbial and geochemical responses to predictable, annual hydrologic perturbations, and offers an opportunity to further refine modeling approaches for such regions.

Determination of the origin of elevated uranium at a Former Air Force Landfill using non-parametric statistics analysis and uranium isotope ratio analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weismann, J.; Young, C.; Masciulli, S.

2007-07-01

Lowry Air Force Base (Lowry) was closed in September 1994 as part of the Base Realignment and Closure (BRAC) program and the base was transferred to the Lowry Redevelopment Authority in 1995. As part of the due diligence activities conducted by the Air Force, a series of remedial investigations were conducted across the base. A closed waste landfill, designated Operable Unit 2 (OU 2), was initially assessed in a 1990 Remedial Investigation (RI; [1]). A Supplemental Remedial Investigation was conducted in 1995 [2] and additional studies were conducted in a 1998 Focused Feasibility Study. [3] The three studies indicated thatmore » gross alpha, gross beta, and uranium concentrations were consistently above regulatory standards and that there were detections of low concentrations other radionuclides. Results from previous investigations at OU 2 have shown elevated gross alpha, gross beta, and uranium concentrations in groundwater, surface water, and sediments. The US Air Force has sought to understand the provenance of these radionuclides in order to determine if they could be due to leachates from buried radioactive materials within the landfill or whether they are naturally-occurring. The Air Force and regulators agreed to use a one-year monitoring and sampling program to seek to explain the origins of the radionuclides. Over the course of the one-year program, dissolved uranium levels greater than the 30 {mu}g/L Maximum Contaminant Level (MCL) were consistently found in both up-gradient and down-gradient wells at OU 2. Elevated Gross Alpha and Gross Beta measurements that were observed during prior investigations and confirmed during the LTM were found to correlate with high dissolved uranium content in groundwater. If Gross Alpha values are corrected to exclude uranium and radon contributions in accordance with US EPA guidance, then the 15 pCi/L gross alpha level is not exceeded. The large dataset also allowed development of gross alpha to total uranium correlation factors so that gross alpha action levels can be applied to future long-term landfill monitoring to track radiological conditions at lower cost. Ratios of isotopic uranium results were calculated to test whether the elevated uranium displayed signatures indicative of military use. Results of all ratio testing strongly supports the conclusion that the uranium found in groundwater, surface water, and sediment at OU 2 is naturally-occurring and has not undergone anthropogenic enrichment or processing. U-234:U-238 ratios also show that a disequilibrium state, i.e., ratio greater than 1, exists throughout OU 2 which is indicative of long-term aqueous transport in aged aquifers. These results all support the conclusion that the elevated uranium observed at OU 2 is due to the high concentrations in the regional watershed. Based on the results of this monitoring program, we concluded that the elevated uranium concentrations measured in OU 2 groundwater, surface water, and sediment are due to the naturally-occurring uranium content of the regional watershed and are not the result of waste burials in the former landfill. Several lines of evidence indicate that natural uranium has been naturally concentrated beneath OU 2 in the geologic past and the higher of uranium concentrations in down-gradient wells is the result of geochemical processes and not the result of a uranium ore disposal. These results therefore provide the data necessary to support radiological closure of OU 2. (authors)« less

Remediation of the Highland Drive South Ravine, Port Hope, Ontario: Contaminated Groundwater Discharge Management Using Permeable Reactive Barriers and Contaminated Sediment Removal - 13447

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smyth, David; Roos, Gillian; Ferguson Jones, Andrea

2013-07-01

The Highland Drive South Ravine (HDSR) is the discharge area for groundwater originating from the Highland Drive Landfill, the Pine Street North Extension (PSNE) roadbed parts of the Highland Drive roadbed and the PSNE Consolidation Site that contain historical low-level radioactive waste (LLRW). The contaminant plume from these LLRW sites contains elevated concentrations of uranium and arsenic and discharges with groundwater to shallow soils in a wet discharge area within the ravine, and directly to Hunt's Pond and Highland Drive South Creek, which are immediately to the south of the wet discharge area. Remediation and environmental management plans for HDSRmore » have been developed within the framework of the Port Hope Project and the Port Hope Area Initiative. The LLRW sites will be fully remediated by excavation and relocation to a new Long-Term Waste Management Facility (LTWMF) as part of the Port Hope Project. It is projected, however, that the groundwater contaminant plume between the remediated LLRW sites and HDSR will persist for several hundreds of years. At the HDSR, sediment remediation within Hunt's Ponds and Highland Drive South Creek, excavation of the existing and placement of clean fill will be undertaken to remove current accumulations of solid-phase uranium and arsenic associated with the upper 0.75 m of soil in the wet discharge area, and permeable reactive barriers (PRBs) will be used for in situ treatment of contaminated groundwater to prevent the ongoing discharge of uranium and arsenic to the area in HDSR where shallow soil excavation and replacement has been undertaken. Bench-scale testing using groundwater from HDSR has confirmed excellent treatment characteristics for both uranium and arsenic using permeable reactive mixtures containing granular zero-valent iron (ZVI). A sequence of three PRBs containing ZVI and sand in backfilled trenches has been designed to intercept the groundwater flow system prior to its discharge to the ground surface and the creek and ponds in the HDSR. The first of the PRBs will be installed immediately up-gradient of the wet discharge area approximately 50 m from the creek, the other two will be installed across the area of shallow soil replacement, and all will extend from ground surface to the base of the water table aquifer through which the impacted groundwater flows. The PRBs have been designed to provide the removal of uranium and arsenic for decades, although the capacity of the treatment mixture for contaminant removal suggests that a longer period of treatment may be feasible. The environmental management plan includes an allowance for on-going monitoring, and replacement of a PRB(s) as might be required. (authors)« less

Capacity of Lemna gibba L. (duckweed) for uranium and arsenic phytoremediation in mine tailing waters.

PubMed

Mkandawire, Martin; Taubert, Barbara; Dudel, E Gert

2004-01-01

The potential of Lemna gibba L. to clean uranium and arsenic contamination from mine surface waters was investigated in wetlands of two former uranium mines in eastern Germany and in laboratory hydroponic culture. Water and plants were sampled and L gibba growth and yield were monitored in tailing ponds from the field study sites. Contaminant accumulation, growth and yield experiments were conducted in the laboratory using synthetic tailing water. Mean background concentrations of the surface waters were 186.0+/-81.2 microg l(-1) uranium and 47.0+/-21.3 microg l(-1) arsenic in Site one and 293.7+/-121.3 microg l(-1) uranium and 41.37+/-24.7 microg l(-1) arsenic in Site two. The initial concentration of both uranium and arsenic in the culture solutions was 100 microg l(-1). The plant samples were either not leached, leached with deionized H2O or ethylenediaminetetracetic (EDTA). The results revealed high bioaccumulation coefficients for both uranium and arsenic. Uranium and arsenic content of L gibba dry biomass of the field samples were as follows: nonleached samples > deionized H2O leached (insignificant ANOVA p = 0.05) > EDTA leached. The difference in both arsenic and uranium enrichment were significantly high between the nonleached and the other two lead samples tested at ANOVA p > 0.001. Estimated mean L gibba density in surface water was 85,344.8+/-1843.4 fronds m(-2) (approximately 1319.7 g m(-2)). The maximum specific growth rate was 0.47+/-0.2 d(-1), which exceeded reported specific growth rates for L gibba in the literature. Average yield was estimated at 20.2+/-6.7 g m(-2) d(-1), giving approximately 73.6+/-21.4 t ha(-1) y(-1) as the annual yield. The highest accumulations observed were 896.9+/-203.8 mg kg(-1) uranium and 1021.7+/-250.8 mg kg(-1) arsenic dry biomass for a 21-d test period in the laboratory steady-state experiments. The potential extractions from surface waters with L gibba L. were estimated to be 662.7 kg uranium ha(-1) yr(-1) and 751.9 kg arsenic ha(-1) yr(-1) under the above conditions.

Influence of microorganisms on the oxidation state distribution of multivalent actinides under anoxic conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean - Francois

2010-12-10

The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity.more » Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paton, Ian

The Rocky Flats Environmental Technology Site (RFETS) is a Department of Energy facility located approximately 16 miles northwest of Denver, Colorado. Processing and fabrication of nuclear weapons components occurred at Rocky Flats from 1952 through 1989. Operations at the Site included the use of several radionuclides, including plutonium-239/240 (Pu), americium-241 (Am), and various uranium (U) isotopes, as well as several types of chlorinated solvents. The historic operations resulted in legacy contamination, including contaminated facilities, process waste lines, buried wastes and surface soil contamination. Decontamination and removal of buildings at the site was completed in late 2005, culminating more than tenmore » years of active environmental remediation work. The Corrective Action Decision/Record of Decision was subsequently approved in 2006, signifying regulatory approval and closure of the site. The use of RFETS as a National Wildlife Refuge is scheduled to be in full operation by 2012. To develop a plan for remediating different types of radionuclide contaminants present in the RFETS environment required understanding the different environmental transport pathways for the various actinides. Developing this understanding was the primary objective of the Actinide Migration Evaluation (AME) project. Findings from the AME studies were used in the development of RFETS remediation strategies. The AME project focused on issues of actinide behavior and mobility in surface water, groundwater, air, soil and biota at RFETS. For the purposes of the AME studies, actinide elements addressed included Pu, Am, and U. The AME program, funded by DOE, brought together personnel with a broad range of relevant expertise in technical investigations. The AME advisory panel identified research investigations and approaches that could be used to solve issues related to actinide migration at the Site. An initial step of the AME was to develop a conceptual model to provide a qualitative description of the relationships among potential actinide sources and transport pathways at RFETS. One conceptual model was developed specifically for plutonium and americium, because of their similar geochemical and transport properties. A separate model was developed for uranium because of its different properties and mobility in the environment. These conceptual models were guidelines for quantitative analyses described in the RFETS Pathway Analysis Report, which used existing data from the literature as well as site-specific analyses, including field, laboratory and modeling studies to provide quantitative estimates of actinide migration in the RFETS environment. For pathways where more than one method was used to estimate offsite loads for a specific pathway, the method yielding the highest estimated off-site was used for comparison purposes. For all actinides studied, for pre-remediation conditions, air and surface water were identified to be the dominant transport mechanisms. The estimated annual airborne plutonium-239/240 load transported off site exceeded the surface water load by roughly a factor of 40. However, despite being the largest transport pathway, airborne radionuclide concentrations at the monitoring location with the highest measurements during the period studied were less than two percent of the allowable 10 milli-rem standard governing DOE facilities. Estimated actinide loads for other pathways were much less. Shallow groundwater was approximately two orders of magnitude lower, or 1/100 of the load conveyed in surface water. The estimated biological pathway load for plutonium was approximately five orders of magnitude less, or 1/100,000, of the load estimated for surface-water. The pathway analysis results were taken into consideration during subsequent remediation activities that occurred at the site. For example, when the 903 Pad area was remediated to address elevated concentrations of Pu and Am in the surface soil, portable tent structures were constructed to prevent wind and water erosion from occurring while remediation activities took place. Following remediation of the 903 Pad and surrounding area, coconut erosion blankets were installed to mitigate erosion effects while vegetation was reestablished [2]. These measures were effective tools to address the primary transport mechanisms identified, coupling the scientific understanding of the site with the remediation strategy.« less

Cleaning of uranium vs machine coolant formulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cristy, S.S.; Byrd, V.R.; Simandl, R.F.

1984-10-01

This study compares methods for cleaning uranium chips and the residues left on chips from alternate machine coolants based on propylene glycol-water mixtures with either borax, ammonium tetraborate, or triethanolamine tetraborate added as a nuclear poison. Residues left on uranium surfaces machined with perchloroethylene-mineral oil coolant and on surfaces machined with the borax-containing alternate coolant were also compared. In comparing machined surfaces, greater chlorine contamination was found on the surface of the perchloroethylene-mineral oil machined surfaces, but slightly greater oxidation was found on the surfaces machined with the alternate borax-containing coolant. Overall, the differences were small and a change tomore » the alternate coolant does not appear to constitute a significant threat to the integrity of machined uranium parts.« less

Uranium in groundwater--Fertilizers versus geogenic sources.

PubMed

Liesch, Tanja; Hinrichsen, Sören; Goldscheider, Nico

2015-12-01

Due to its radiological and toxicological properties even at low concentration levels, uranium is increasingly recognized as relevant contaminant in drinking water from aquifers. Uranium originates from different sources, including natural or geogenic, mining and industrial activities, and fertilizers in agriculture. The goal of this study was to obtain insights into the origin of uranium in groundwater while differentiating between geogenic sources and fertilizers. A literature review concerning the sources and geochemical processes affecting the occurrence and distribution of uranium in the lithosphere, pedosphere and hydrosphere provided the background for the evaluation of data on uranium in groundwater at regional scale. The state of Baden-Württemberg, Germany, was selected for this study, because of its hydrogeological and land-use diversity, and for reasons of data availability. Uranium and other parameters from N=1935 groundwater monitoring sites were analyzed statistically and geospatially. Results show that (i) 1.6% of all water samples exceed the German legal limit for drinking water (10 μg/L); (ii) The range and spatial distribution of uranium and occasional peak values seem to be related to geogenic sources; (iii) There is a clear relation between agricultural land-use and low-level uranium concentrations, indicating that fertilizers generate a measurable but low background of uranium in groundwater. Copyright © 2015 Elsevier B.V. All rights reserved.

Caulobacter crescentus as a Whole-Cell Uranium Biosensor▿ †

PubMed Central

Hillson, Nathan J.; Hu, Ping; Andersen, Gary L.; Shapiro, Lucy

2007-01-01

We engineered a strain of the bacterium Caulobacter crescentus to fluoresce in the presence of micromolar levels of uranium at ambient temperatures when it is exposed to a hand-held UV lamp. Previous microarray experiments revealed that several Caulobacter genes are significantly upregulated in response to uranium but not in response to other heavy metals. We designated one of these genes urcA (for uranium response in caulobacter). We constructed a reporter that utilizes the urcA promoter to produce a UV-excitable green fluorescent protein in the presence of the uranyl cation, a soluble form of uranium. This reporter is specific for uranium and has little cross specificity for nitrate (<400 μM), lead (<150 μM), cadmium (<48 μM), or chromium (<41.6 μM). The uranium reporter construct was effective for discriminating contaminated groundwater samples (4.2 μM uranium) from uncontaminated groundwater samples (<0.1 μM uranium) collected at the Oak Ridge Field Research Center. In contrast to other uranium detection methodologies, the Caulobacter reporter strain can provide on-demand usability in the field; it requires minimal sample processing and no equipment other than a hand-held UV lamp, and it may be sprayed directly on soil, groundwater, or industrial surfaces. PMID:17905881

Uranium and radon in ground water in the lower Illinois River basin

USGS Publications Warehouse

Morrow, William S.

2001-01-01

Uranium and radon are present in ground water throughout the United States, along with other naturally occurring radionuclides. The occurrence and distribution of uranium and radon are of concern because these radionuclides are carcinogens that can be ingested through drinking water. As part of the U.S. Geological Survey (USGS) National Water-Quality Assessment (NAWQA) program, water samples were collected and analyzed for uranium and radon from 117 wells in four aquifers in the lower Illinois River Basin (LIRB) from 1996 to 1997. The aquifers were the shallow glacial drift deposits of the Bloomington Ridged Plain (BRP) not overlying a buried bedrock valley (BRP N/O BV), shallow glacial drift deposits of the BRP overlying the Mahomet Buried Bedrock Valley (BRP O/L MBBV), shallow glacial drift deposits of the Galesburg/Springfield Plain not overlying a buried bedrock valley (GSP N/O BV), and the deep glacial drift deposits of the Mahomet Buried Bedrock Valley (MBBV). Uranium was detected in water samples from all aquifers except the MBBV and ranged in concentration from less than 1 microgram per liter ( ? g/L) to 17 ? g/L. Uranium concentrations did not exceed 20 ? g/L, the proposed U.S. Environmental Protection Agency (USEPA) Maximum Contaminant Level (MCL) at the time of sampling (1996?97). The current (2001) promulgated MCL is 30 ? g/L (U.S. Environmental Protection Agency, 2000). The highest median uranium concentration (2.0 ? g/L) among the four aquifers was in the BRP N/O BV. Uranium most often occurred in oxidizing and sulfate-rich water. Radon was detected in water samples from all aquifers in the LIRB. Radon concentrations in all aquifers ranged from less than 80 picocuries per liter (pCi/L) to 1,300 pCi/L. Of 117 samples, radon concentrations exceeded 300 pCi/L (the proposed USEPA MCL) in 34 percent of the samples. Radon concentrations exceeded 300 pCi/L in more than one-half of the samples from the GSP N/O BV and the BRP O/L MBBV. No sample exceeded the proposed Alternative Maximum Contaminant Level (AMCL) of 4,000 pCi/L. Concentrations of uranium and radon were not correlated.

Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

PubMed

Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

2010-03-01

Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are <2 x 10(-14), and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

GROUNDWATER REMEDIATION SOLUTIONS AT HANFORD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gilmore, Tyler J.; Truex, Michael J.; Williams, Mark D.

2007-02-26

In 2006, Congress provided funding to the U. S. Department of Energy (DOE) to study new technologies that could be used to treat contamination from the Hanford Site that might impact the Columbia River. The contaminants of concern are primarily metals and radionuclides, which are byproducts of Hanford’s cold war mission to produce plutonium for atomic weapons. The DOE asked Pacific Northwest National Laboratory (PNNL) to consider this problem and develop approaches to address the contamination that threatens the river. DOE identified three high priority sites that had groundwater contamination migrating towards the Columbia river for remediation. The contaminants includedmore » strontium-90, uranium and chromium. Remediation techniques for metals and radionuclides focus primarily on altering the oxidation state of the contaminant chemically or biologically, isolating the contaminants from the environment through adsorption or encapsulation or concentrating the contaminants for removal. A natural systems approach was taken that uses a mass balance concept to frame the problem and determine the most appropriate remedial approach. This approach provides for a scientifically based remedial decision. The technologies selected to address these contaminants included an apatite adsorption barrier coupled with a phytoremediation to address the strontium-90 contamination, injection of polyphosphate into the subsurface to sequester uranium, and a bioremediation approach to reduce chromium contamination in the groundwater. The ability to provide scientifically based approaches is in large part due to work developed under previous DOE Office of Science and Office of Environmental Management projects. For example, the polyphosphate and the bioremediation techniques, were developed by PNNL under the EMSP and NABIR programs. Contaminated groundwater under the Hanford Site poses a potential risk to humans and the Columbia River. These new technologies holds great promise for effectively remediating the residual waste that threatens the environment.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kamboj, Sunita; Durham, Lisa A.

A post-remediation radiological dose assessment was conducted for the Formerly Utilized Sites Remedial Action Program (FUSRAP) Linde Site by using the measured residual concentrations of the radionuclides of concern following the completion of the soils remedial action. The site’s FUSRAP-related contaminants of concern (COCs) are radionuclides associated with uranium processing activities conducted by the Manhattan Engineer District (MED) in support of the Nation’s early atomic energy and weapons program and include radium-226 (Ra-226), thorium-230 (Th-230), and total uranium (Utotal). Remedial actions to address Linde Site soils and structures were conducted in accordance with the Record of Decision for the Lindemore » Site, Tonawanda, New York (ROD) (USACE 2000a). In the ROD, the U.S. Army Corps of Engineers (USACE) determined that the cleanup standards found in Title 40, Part 192 of the Code of Federal Regulations (40 CFR Part 192), the standards for cleanup of uranium mill sites designated under the Uranium Mill Tailings Radiation Control Act (UMTRCA), and the Nuclear Regulatory Commission (NRC) standards for decommissioning of licensed uranium and thorium mills, found in 10 CFR Part 40, Appendix A, Criterion 6(6), are Applicable or Relevant and Appropriate Requirements (ARARs) for cleanup of MED-related contamination at the Linde Site. The major elements of this remedy will involve excavation of the soils with COCs above soil cleanup levels and placement of clean materials to meet the other criteria of 40 CFR Part 192.« less

Comparison of heavy metals and uranium removal using adsorbent in soil

NASA Astrophysics Data System (ADS)

Choi, Jaeyoung; Yun, Hunsik

2017-04-01

This study investigates heavy metals (As, Ni, Zn, Cd, and Pb) and uranium removal onto geomaterials (limestone, black shale, and concrete) and biosorbents (Pseudomonas putida and starfish) from waste in soil. Geomaterials or biosorbents with a high capacity for heavy metals and uranium can be obtained and employed of with little cost. For investigating the neutralization capacity, the change in pH, Eh, and EC as a function of time was quantified. The adsorption of heavy metals and uranium by the samples was influenced by pH, and increased with increasing heavy metals and uranium concentrations. Dead cells adsorbed the largest quantity of all heavy metals than lother sorbents. The adsorption capacity followed the order: U(VI) > Pb > Cd > Ni. The results also suggest that bacterial membrane cells can be used successfully in the treatment of high strength metal-contaminated soil.

Uranium(VI) interactions with mackinawite in the presence and absence of bicarbonate and oxygen

USGS Publications Warehouse

Gallegos, Tanya J.; Fuller, Christopher C.; Webb, Samuel M.; Betterton, William J.

2013-01-01

Mackinawite, Fe(II)S, samples loaded with uranium (10-5, 10-4, and 10-3 mol U/g FeS) at pH 5, 7, and 9, were characterized using X-ray absorption spectroscopy and X-ray diffraction to determine the effects of pH, bicarbonate, and oxidation on uptake. Under anoxic conditions, a 5 g/L suspension of mackinawite lowered 5 × 10-5 M uranium(VI) to below 30 ppb (1.26 × 10-7 M) U. Between 82 and 88% of the uranium removed from solution by mackinawite was U(IV) and was nearly completely reduced to U(IV) when 0.012 M bicarbonate was added. Near-neighbor coordination consisting of uranium–oxygen and uranium-uranium distances indicates the formation of uraninite in the presence and absence of bicarbonate, suggesting reductive precipitation as the dominant removal mechanism. Following equilibration in air, mackinawite was oxidized to mainly goethite and sulfur and about 76% of U(IV) was reoxidized to U(VI) with coordination of uranium to axial and equatorial oxygen, similar to uranyl. Additionally, uranium-iron distances, typical of coprecipitation of uranium with iron oxides, and uranium-sulfur distances indicating bidentate coordination of U(VI) to sulfate were evident. The affinity of mackinawite and its oxidation products for U(VI) provides impetus for further study of mackinawite as a potential reactive medium for remediation of uranium-contaminated water.

Uranium interaction with soil minerals in the presence of co-contaminants: Case Study- subsurface sediments at or below the water table

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gartman, Brandy N.; Qafoku, Nikolla

2016-03-09

Uranium (U) contaminated subsurface systems are common on a global scale mainly because of its essential role in the production of plutonium for nuclear weapons and other nuclear energy and research activities. Studying the behavior and fate of U in these systems is challenging because of heterogeneities of different types (i.e., physical, chemical and mineralogical) and a complex network of often time-dependent hydrological, biological and chemical reactions and processes that occur sequentially or simultaneously, affecting and/or controlling U mobility. A U contaminated site, i.e., the Integrated Field Research Challenge site in Rifle, CO, USA (a former U mill site) ismore » the focus of this discussion. The overall objectives of this chapter are to 1) provide an overview of the contamination levels (U and other co-contaminants) at this field site; 2) review and discuss different aspects of mineral-U contaminant interactions in reduced and oxidized environments, and in the presence of co-contaminants; 3) present results from a systematic macroscopic, microscopic, and spectroscopic study as an example of the current research efforts and the state-of-knowledge in this important research area; and 4) offer insightful conclusive remarks and future research needs about reactions and processes that control U and other contaminants’ fate and behavior under hydraulically saturated conditions. The implications and applications presented in this chapter are valid for U contaminated sites across the world.« less

Environmental proteomics reveals early microbial community responses to biostimulation at a uranium- and nitrate-contaminated site.

PubMed

Chourey, Karuna; Nissen, Silke; Vishnivetskaya, Tatiana; Shah, Manesh; Pfiffner, Susan; Hettich, Robert L; Löffler, Frank E

2013-10-01

High-performance MS instrumentation coupled with improved protein extraction techniques enables metaproteomics to identify active members of soil and groundwater microbial communities. Metaproteomics workflows were applied to study the initial responses (i.e. 4 days post treatment) of the indigenous aquifer microbiota to biostimulation with emulsified vegetable oil (EVO) at a uranium-contaminated site. Members of the Betaproteobacteria (i.e. Dechloromonas, Ralstonia, Rhodoferax, Polaromonas, Delftia, Chromobacterium) and the Firmicutes dominated the biostimulated aquifer community. Proteome characterization revealed distinct differences between the microbial biomass collected from groundwater influenced by biostimulation and groundwater collected upgradient of the EVO injection points. In particular, proteins involved in ammonium assimilation, EVO degradation, and polyhydroxybutyrate granule formation were prominent following biostimulation. Interestingly, the atypical NosZ of Dechloromonas spp. was highly abundant, suggesting active nitrous oxide (N2 O) respiration. c-Type cytochromes were barely detected, as was citrate synthase, a biomarker for hexavalent uranium reduction activity, suggesting that uranium reduction has not commenced 4 days post EVO amendment. Environmental metaproteomics identified microbial community responses to biostimulation and elucidated active pathways demonstrating the value of this technique as a monitoring tool and for complementing nucleic acid-based approaches. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Reclamation with Recovery of Radionuclides and Toxic Metals from Contaminated Materials, Soils, and Wastes

NASA Technical Reports Server (NTRS)

Francis, A. J.; Dodge, C. J.

1993-01-01

A process has been developed at Brookhaven National Laboratory (BNL) for the removal of metals and radionuclides from contaminated materials, soils, and waste sites. In this process, citric acid, a naturally occurring organic complexing agent, is used to extract metals such as Ba, Cd, Cr, Ni, Zn, and radionuclides Co, Sr, Th, and U from solid wastes by formation of water soluble, metal-citrate complexes. Citric acid forms different types of complexes with the transition metals and actinides, and may involve formation of a bidentate, tridentate, binuclear, or polynuclear complex species. The extract containing radionuclide/metal complex is then subjected to microbiological degradation followed by photochemical degradation under aerobic conditions. Several metal citrate complexes are biodegraded, and the metals are recovered in a concentrated form with the bacterial biomass. Uranium forms binuclear complex with citric acid and is not biodegraded. The supernatant containing uranium citrate complex is separated and upon exposure to light, undergoes rapid degradation resulting in the formation of an insoluble, stable polymeric form of uranium. Uranium is recovered as a precipitate (polyuranate) in a concentrated form for recycling or for appropriate disposal. This treatment process, unlike others which use caustic reagents, does not create additional hazardous wastes for disposal and causes little damage to soil which can then be returned to normal use.

Final report of the decontamination and decommissioning of the exterior land areas at the Grand Junction Projects Office facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widdop, M.R.

1995-09-01

The US Department of Energy (DOE) Grand Junction Projects Office (GJPO) facility occupies approximately 56.4 acres (22.8 hectares) along the Gunnison River near Grand Junction, Colorado. The site was contaminated with uranium ore and mill tailings during uranium-refining activities conducted by the Manhattan Engineer District and during pilot-milling experiments conducted for the US Atomic Energy Commission`s (AEC`s) domestic uranium procurement program. The GJPO facility was the collection and assay point for AEC uranium and vanadium oxide purchases until the early 1970s. The DOE Decontamination and Decommissioning Program sponsored the Grand Junction Projects Office Remedial Action Project (GJPORAP) to remediate themore » facility lands, site improvements, and the underlying aquifer. The site contractor, Rust Geotech, was the Remedial Action Contractor for GJPORAP. The exterior land areas of the facility assessed as contaminated have been remediated in accordance with identified standards and can be released for unrestricted use. Restoration of the aquifer will be accomplished through the natural flushing action of the aquifer during the next 50 to 80 years. The remediation of the DOE-GJPO facility buildings is ongoing and will be described in a separate report.« less

Evapotranspiration And Geochemical Controls On Groundwater Plumes At Arid Sites: Toward Innovative Alternate End-States For Uranium Processing And Tailings Facilities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Looney, Brian B.; Denham, Miles E.; Eddy-Dilek, Carol A.

2014-01-08

Management of legacy tailings/waste and groundwater contamination are ongoing at the former uranium milling site in Tuba City AZ. The tailings have been consolidated and effectively isolated using an engineered cover system. For the existing groundwater plume, a system of recovery wells extracts contaminated groundwater for treatment using an advanced distillation process. The ten years of pump and treat (P&T) operations have had minimal impact on the contaminant plume – primarily due to geochemical and hydrological limits. A flow net analysis demonstrates that groundwater contamination beneath the former processing site flows in the uppermost portion of the aquifer and exitsmore » the groundwater as the plume transits into and beneath a lower terrace in the landscape. The evaluation indicates that contaminated water will not reach Moenkopi Wash, a locally important stream. Instead, shallow groundwater in arid settings such as Tuba City is transferred into the vadose zone and atmosphere via evaporation, transpiration and diffuse seepage. The dissolved constituents are projected to precipitate and accumulate as minerals such as calcite and gypsum in the deep vadose zone (near the capillary fringe), around the roots of phreatophyte plants, and near seeps. The natural hydrologic and geochemical controls common in arid environments such as Tuba City work together to limit the size of the groundwater plume, to naturally attenuate and detoxify groundwater contaminants, and to reduce risks to humans, livestock and the environment. The technical evaluation supports an alternative beneficial reuse (“brownfield”) scenario for Tuba City. This alternative approach would have low risks, similar to the current P&T scenario, but would eliminate the energy and expense associated with the active treatment and convert the former uranium processing site into a resource for future employment of local citizens and ongoing benefit to the Native American Nations.« less

Microbial Community Responses to Organophosphate Substrate Additions in Contaminated Subsurface Sediments

PubMed Central

Martinez, Robert J.; Wu, Cindy H.; Beazley, Melanie J.; Andersen, Gary L.; Conrad, Mark E.; Hazen, Terry C.; Taillefert, Martial; Sobecky, Patricia A.

2014-01-01

Background Radionuclide- and heavy metal-contaminated subsurface sediments remain a legacy of Cold War nuclear weapons research and recent nuclear power plant failures. Within such contaminated sediments, remediation activities are necessary to mitigate groundwater contamination. A promising approach makes use of extant microbial communities capable of hydrolyzing organophosphate substrates to promote mineralization of soluble contaminants within deep subsurface environments. Methodology/Principal Findings Uranium-contaminated sediments from the U.S. Department of Energy Oak Ridge Field Research Center (ORFRC) Area 2 site were used in slurry experiments to identify microbial communities involved in hydrolysis of 10 mM organophosphate amendments [i.e., glycerol-2-phosphate (G2P) or glycerol-3-phosphate (G3P)] in synthetic groundwater at pH 5.5 and pH 6.8. Following 36 day (G2P) and 20 day (G3P) amended treatments, maximum phosphate (PO4 3−) concentrations of 4.8 mM and 8.9 mM were measured, respectively. Use of the PhyloChip 16S rRNA microarray identified 2,120 archaeal and bacterial taxa representing 46 phyla, 66 classes, 110 orders, and 186 families among all treatments. Measures of archaeal and bacterial richness were lowest under G2P (pH 5.5) treatments and greatest with G3P (pH 6.8) treatments. Members of the phyla Crenarchaeota, Euryarchaeota, Bacteroidetes, and Proteobacteria demonstrated the greatest enrichment in response to organophosphate amendments and the OTUs that increased in relative abundance by 2-fold or greater accounted for 9%–50% and 3%–17% of total detected Archaea and Bacteria, respectively. Conclusions/Significance This work provided a characterization of the distinct ORFRC subsurface microbial communities that contributed to increased concentrations of extracellular phosphate via hydrolysis of organophosphate substrate amendments. Within subsurface environments that are not ideal for reductive precipitation of uranium, strategies that harness microbial phosphate metabolism to promote uranium phosphate precipitation could offer an alternative approach for in situ sequestration. PMID:24950228

Raoultella sp. SM1, a novel iron-reducing and uranium-precipitating strain.

PubMed

Sklodowska, Aleksandra; Mielnicki, Sebastian; Drewniak, Lukasz

2018-03-01

The main aim of this study was the characterisation of novel Raoutella isolate, an iron-reducing and uranium-precipitating strain, originating from microbial mats occurring in the sediments of a closed down uranium mine in Kowary (SW Poland). Characterisation was done in the context of its potential role in the functioning of these mats and the possibility to use them in uranium removal/recovery processes. In our experiment, we observed the biological precipitation of iron and uranium's secondary minerals containing oxygen, potassium, sodium and phosphor, which were identified as ningyoite-like minerals. The isolated strain, Raoultella sp. SM1, was also able to dissimilatory reduce iron (III) and uranium (VI) in the presence of citrate as an electron donor. Our studies allowed us to characterise a new strain which may be used as a model microorganism in the study of Fe and U respiratory processes and which may be useful in the bioremediation of uranium-contaminated waters and sediments. During this process, uranium may be immobilised in ningyoite-like minerals and can then be recovered in nano/micro-particle form, which may be easily transformed to uraninite. Copyright © 2017 Elsevier Ltd. All rights reserved.

Depleted uranium instead of lead in munitions: the lesser evil.

PubMed

Jargin, Sergei V

2014-03-01

Uranium has many similarities to lead in its exposure mechanisms, metabolism and target organs. However, lead is more toxic, which is reflected in the threshold limit values. The main potential hazard associated with depleted uranium is inhalation of the aerosols created when a projectile hits an armoured target. A person can be exposed to lead in similar ways. Accidental dangerous exposures can result from contact with both substances. Encountering uranium fragments is of minor significance because of the low penetration depth of alpha particles emitted by uranium: they are unable to penetrate even the superficial keratin layer of human skin. An additional cancer risk attributable to the uranium exposure might be significant only in case of prolonged contact of the contaminant with susceptible tissues. Lead intoxication can be observed in the wounded, in workers manufacturing munitions etc; moreover, lead has been documented to have a negative impact on the intellectual function of children at very low blood concentrations. It is concluded on the basis of the literature overview that replacement of lead by depleted uranium in munitions would be environmentally beneficial or largely insignificant because both lead and uranium are present in the environment.

Uranium mining wastes: The use of the Fish Embryo Acute Toxicity Test (FET) test to evaluate toxicity and risk of environmental discharge.

PubMed

Lourenço, J; Marques, S; Carvalho, F P; Oliveira, J; Malta, M; Santos, M; Gonçalves, F; Pereira, R; Mendo, S

2017-12-15

Active and abandoned uranium mining sites often create environmentally problematic situations, since they cause the contamination of all environmental matrices (air, soil and water) with stable metals and radionuclides. Due to their cytotoxic, genotoxic and teratogenic properties, the exposure to these contaminants may cause several harmful effects in living organisms. The Fish Embryo Acute Toxicity Test (FET) test was employed to evaluate the genotoxic and teratogenic potential of mine liquid effluents and sludge elutriates from a deactivated uranium mine. The aims were: a) to determine the risk of discharge of such wastes in the environment; b) the effectiveness of the chemical treatment applied to the uranium mine water, which is a standard procedure generally applied to liquid effluents from uranium mines and mills, to reduce its toxicological potential; c) the suitability of the FET test for the evaluation the toxicity of such wastes and the added value of including the evaluation of genotoxicity. Results showed that through the FET test it was possible to determine that both elutriates and effluents are genotoxic and also that the mine effluent is teratogenic at low concentrations. Additionally, liquid effluents and sludge elutriates affect other parameters namely, growth and hatching and that water pH alone played an important role in the hatching process. The inclusion of genotoxicity evaluation in the FET test was crucial to prevent the underestimation of the risks posed by some of the tested effluents/elutriates. Finally, it was possible to conclude that care should be taken when using benchmark values calculated for specific stressors to evaluate the risk posed by uranium mining wastes to freshwater ecosystems, due to their chemical complexity. Copyright © 2017 Elsevier B.V. All rights reserved.

Validation of MCNP6 Version 1.0 with the ENDF/B-VII.1 Cross Section Library for Uranium Metal, Oxide, and Solution Systems on the High Performance Computing Platform Moonlight

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chapman, Bryan Scott; MacQuigg, Michael Robert; Wysong, Andrew Russell

In this document, the code MCNP is validated with ENDF/B-VII.1 cross section data under the purview of ANSI/ANS-8.24-2007, for use with uranium systems. MCNP is a computer code based on Monte Carlo transport methods. While MCNP has wide reading capability in nuclear transport simulation, this validation is limited to the functionality related to neutron transport and calculation of criticality parameters such as k eff.

Investigation of the radiological impact on the coastal environment surrounding a fertilizer plant.

PubMed

El Samad, O; Aoun, M; Nsouli, B; Khalaf, G; Hamze, M

2014-07-01

This investigation was carried out in order to assess the marine environmental radioactive pollution and the radiological impact caused by a large production plant of phosphate fertilizer, located in the Lebanese coastal zone. Natural radionuclides ((238)U, (235)U, (232)Th, (226)Ra, (210)Po, (210)Pb, (40)K) and anthropogenic (137)Cs were measured by alpha and gamma spectrometry in seawater, sediment, biota and coastal soil samples collected from the area impacted by this industry. The limited environmental monitoring program within 2 km of the plant indicates localized contamination with radionuclides of the uranium decay chain mainly due to the transport, the storage of raw materials and the free release of phosphogypsum waste. Copyright © 2013 Elsevier Ltd. All rights reserved.

Detection of depleted uranium in urine of veterans from the 1991 Gulf War.

PubMed

Gwiazda, R H; Squibb, K; McDiarmid, M; Smith, D

2004-01-01

American soldiers involved in "friendly fire" accidents during the 1991 Gulf War were injured with depleted-uranium-containing fragments or possibly exposed to depleted uranium via other routes such as inhalation, ingestion, and/or wound contamination. To evaluate the presence of depleted uranium in these soldiers eight years later, the uranium concentration and depleted uranium content of urine samples were determined by inductively coupled plasma mass spectrometry in (a) depleted uranium exposed soldiers with embedded shrapnel, (b) depleted uranium exposed soldiers with no shrapnel, and (c) a reference group of deployed soldiers not involved in the friendly fire incidents. Uranium isotopic ratios measured in many urine samples injected directly into the inductively coupled plasma mass spectrometer and analyzed at a mass resolution m/delta m of 300 appeared enriched in 235U with respect to natural abundance (0.72%) due to the presence of an interference of a polyatomic molecule of mass 234.81 amu that was resolved at a mass resolution m/delta m of 4,000. The 235U abundance measured on uranium separated from these urines by anion exchange chromatography was clearly natural or depleted. Urine uranium concentrations of soldiers with shrapnel were higher than those of the two other groups, and 16 out of 17 soldiers with shrapnel had detectable depleted uranium in their urine. In depleted uranium exposed soldiers with no shrapnel, depleted uranium was detected in urine samples of 10 out of 28 soldiers. The median uranium concentration of urines with depleted uranium from soldiers without shrapnel was significantly higher than in urines with no depleted uranium, though substantial overlap in urine uranium concentrations existed between the two groups. Accordingly, assessment of depleted uranium exposure using urine must rely on uranium isotopic analyses, since urine uranium concentration is not an unequivocal indicator of depleted uranium presence in soldiers with no embedded shrapnel.

Final environmental assessment for the U.S. Department of Energy, Oak Ridge Operations receipt and storage of uranium materials from the Fernald Environmental Management Project site

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

Through a series of material transfers and sales agreements over the past 6 to 8 years, the Fernald Environmental Management Project (FEMP) has reduced its nuclear material inventory from 14,500 to approximately 6,800 metric tons of uranium (MTU). This effort is part of the US Department of energy`s (DOE`s) decision to change the mission of the FEMP site; it is currently shut down and the site is being remediated. This EA focuses on the receipt and storage of uranium materials at various DOE-ORO sites. The packaging and transportation of FEMP uranium material has been evaluated in previous NEPA and othermore » environmental evaluations. A summary of these evaluation efforts is included as Appendix A. The material would be packaged in US Department of Transportation-approved shipping containers and removed from the FEMP site and transported to another site for storage. The Ohio Field Office will assume responsibility for environmental analyses and documentation for packaging and transport of the material as part of the remediation of the site, and ORO is preparing this EA for receipt and storage at one or more sites.« less

Effect of Reaction Pathway on the Extent and Mechanism of Uranium(VI) Immobilization with Calcium and Phosphate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming

Phosphate addition to subsurface environments contaminated with uranium can be used as an in situ remediation approach. Batch experiments were conducted to evaluate the dependence of the extent and mechanism of uranium uptake on the pathway for reaction with calcium phosphates. At pH 4.0 and 6.0 uranium uptake occurred via autunite (Ca(UO2)(PO4)3) precipitation irrespective of the starting forms of calcium and phosphate. At pH 7.5, the uptake mechanism depended on the nature of the calcium and phosphate. When dissolved uranium, calcium, and phosphate were added simultaneously, uranium was structurally incorporated into a newly formed amorphous calcium phosphate solid. Adsorption wasmore » the dominant removal mechanism for uranium contacted with pre-formed amorphous calcium phosphate solids,. When U(VI) was added to a suspension containing amorphous calcium phosphate solids as well as dissolved calcium and phosphate, then removal occurred through precipitation (57±4 %) of autunite and adsorption (43±4 %) onto calcium phosphate. The solid phase speciation of the uranium was determined using X-ray absorption spectroscopy and laser induced fluorescence spectroscopy. Dissolved uranium, calcium, and phosphate concentrations with saturation index calculations helped identify removal mechanisms and determine thermodynamically favorable solid phases.« less

Environmental and taxonomic bacterial diversity of anaerobic uranium(IV) bio-oxidation.

PubMed

Weber, Karrie A; Thrash, J Cameron; Van Trump, J Ian; Achenbach, Laurie A; Coates, John D

2011-07-01

Microorganisms in diverse terrestrial surface and subsurface environments can anaerobically catalyze the oxidative dissolution of uraninite. While a limited quantity (∼5 to 12 μmol liter(-1)) of uranium is oxidatively dissolved in pure culture studies, the metabolism is coupled to electron transport, providing the potential of uraninite to support indigenous microbial populations and to solubilize uranium.

Quantification of kinetic rate law parameters for the dissolution of natural autunite in the presence of aqueous bicarbonate ions at high concentrations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn

Uranium is a key contaminant of concern in the groundwater at 91 waste sites at 18 U.S. Department of Energy (DOE) facilities within the United States and is a potential source of groundwater contamination and a risk to human health and the environment through discharges to surface water. Dissolved inorganic carbon (bicarbonate/carbonate) has a high affinity for complexing with uranium that is present as sorbed or unique uranium-bearing mineral phases within the sedimentary matrix. This process can result in the formation of soluble uranyl carbonate aqueous species, which are mobile under circumneutral pH conditions. This study was conducted to quantifymore » the rate of release of uranium from the autunite mineral, (Ca[(UO 2)(PO 4)] 2∙3H 2O), that was formed during polyphosphate injection to remediate uranium; the dissolution of uranium was studied as a function of the aqueous bicarbonate concentration, ranging from 25 to 100 mM. Experiments were carried out in the pH range from 7 to 11 in the temperature range of 23-90°C via single-pass flow-through testing. Consistent with the results of previous studies (Gudavalli et al., 2013 a, b), the rate of uranium release from autunite exhibited minimal dependency on temperature, but was strongly dependent on pH and increasing concentrations of bicarbonate in the solution. Data obtained during these experiments were compared with results of previous experiments conducted using a low-concentration range of bicarbonate solutions (0.5-3.0 mM). An 8- to 30 fold increase in the rate of uranium release was observed in the presence of high bicarbonate concentrations at pH 7-8 compared to low bicarbonate values, while at pH 9-11, there was only a 5-fold increase in uranium rate of release with an increase in bicarbonate concentrations. The rate of uranium release was calculated to be between 5.18 x 10 -8 and 1.69 x 10 -7 mol m -2 s -1. The activation energy values at high and low bicarbonate concentrations were similar, with ratio values in the range of 0.6-1.0.« less

Quantification of kinetic rate law parameters for the dissolution of natural autunite in the presence of aqueous bicarbonate ions at high concentrations.

PubMed

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn

2018-05-02

Uranium is a key contaminant of concern in the groundwater at U.S. Department of Energy (DOE) facilities within the United States and is a potential source of groundwater contamination and a risk to human health and the environment through discharges to surface water. Dissolved inorganic carbon (bicarbonate/carbonate) has a high affinity for complexing with uranium that is present as sorbed or unique uranium-bearing mineral phases within the sedimentary matrix. This process can result in the formation of soluble uranyl carbonate aqueous species, which are mobile under circumneutral pH conditions. This study was conducted to quantify the rate of release of uranium from the autunite mineral, (Ca[(UO 2 )(PO 4 )] 2 •3H 2 O), that was formed during polyphosphate injection to remediate uranium; the dissolution of uranium was studied as a function of the aqueous bicarbonate concentration, ranging from 25 to 100 mM. Experiments were carried out in the pH range from 7 to 11 in the temperature range of 23-90 °C via single-pass flow-through testing. Consistent with the results of previous studies (Gudavalli et al., 2013a, 2013b), the rate of uranium release from autunite exhibited minimal dependency on temperature, but was strongly dependent on pH and increasing concentrations of bicarbonate in the solution. Data obtained during these experiments were compared with results of previous experiments conducted using a low-concentration range of bicarbonate solutions (0.5-3.0 mM). An 8- to 30-fold increase in the rate of uranium release was observed in the presence of high bicarbonate concentrations at pH 7-8 compared to low bicarbonate values, while at pH 9-11, there was only a 5-fold increase in uranium rate of release with an increase in bicarbonate concentrations. The rate of uranium release was calculated to be between 5.18 × 10 -8 and 1.69 × 10 -7  mol m -2 s -1 . The activation energy values at high and low bicarbonate concentrations were similar, with ratio values in the range of 0.6-1.0. Copyright © 2018 Elsevier Ltd. All rights reserved.

[Uranium exposure and cancer risk: a review of epidemiological studies].

PubMed

Tirmarche, M; Baysson, H; Telle-Lamberton, M

2004-02-01

At the end of 2000, certain diseases including leukemia were reported among soldiers who participated in the Balkan and in the Gulf wars. Depleted uranium used during these conflicts was considered as a possible cause. Its radiotoxicity is close to that of natural uranium. This paper reviews the epidemiological knowledge of uranium, the means of exposure and the associated risk of cancer. The only available epidemiological data concerns nuclear workers exposed to uranium. A review of the international literature is proposed by distinguishing between uranium miners and other workers of the nuclear industry. French studies are described in details. In ionizing radiation epidemiology, contamination by uranium is often cited as a risk factor, but the dose-effect relationship is rarely studied. Retrospective assessment of individual exposure is generally insufficient. Moreover, it is difficult to distinguish between uranium radiotoxicity, its chemical toxicity and the radiotoxicity of its progeny. A causal relation between lung cancer and radon exposure, a gas derived from the decay of uranium, has been demonstrated in epidemiological studies of miners. Among other nuclear workers exposed to uranium, there is a mortality deficit from all causes (healthy worker effect). No cancer site appears systematically in excess compared to the national population; very few studies describe a dose-response relationship. Only studies with a precise reconstruction of doses and sufficient numbers of workers will allow a better assessment of risks associated with uranium exposure at levels encountered in industry or during conflicts using depleted uranium weapons.

Method for providing uranium with a protective copper coating

DOEpatents

Waldrop, Forrest B.; Jones, Edward

1981-01-01

The present invention is directed to a method for providing uranium metal with a protective coating of copper. Uranium metal is subjected to a conventional cleaning operation wherein oxides and other surface contaminants are removed, followed by etching and pickling operations. The copper coating is provided by first electrodepositing a thin and relatively porous flash layer of copper on the uranium in a copper cyanide bath. The resulting copper-layered article is then heated in an air or inert atmosphere to volatilize and drive off the volatile material underlying the copper flash layer. After the heating step an adherent and essentially non-porous layer of copper is electro-deposited on the flash layer of copper to provide an adherent, multi-layer copper coating which is essentially impervious to corrosion by most gases.

Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction

DOE PAGES

Belli, Keaton M.; DiChristina, Thomas J.; Van Cappellen, Philippe; ...

2015-02-16

The ability to predict the success of the microbial reduction of soluble U(VI) to highly insoluble U(IV) as an in situ bioremediation strategy is complicated by the wide range of geochemical conditions at contaminated sites and the strong influence of aqueous uranyl speciation on the bioavailability and toxicity of U(VI) to metal-reducing bacteria. In order to determine the effects of aqueous uranyl speciation on uranium bioreduction kinetics, incubations and viability assays with Shewanella putrefaciens strain 200 were conducted over a range of pH and dissolved inorganic carbon (DIC), Ca 2+, and Mg 2+ concentrations. A speciation-dependent kinetic model was developedmore » to reproduce the observed time series of total dissolved uranium concentration over the range of geochemical conditions tested. The kinetic model yielded the highest rate constant for the reduction of uranyl non-carbonate species (i.e., the ‘free’ hydrated uranyl ion, uranyl hydroxides, and other minor uranyl complexes), indicating that they represent the most readily reducible fraction of U(VI) despite being the least abundant uranyl species in solution. In the presence of DIC, Ca 2+, and Mg 2+ is suppressed during the formation of more bioavailable uranyl non-carbonate species and resulted in slower bioreduction rates. At high concentrations of bioavailable U(VI), however, uranium toxicity to S. putrefaciens inhibited bioreduction, and viability assays confirmed that the concentration of non-carbonate uranyl species best predicts the degree of toxicity. The effect of uranium toxicity was accounted for by incorporating the free ion activity model of metal toxicity into the bioreduction rate law. These results demonstrate that, in the absence of competing terminal electron acceptors, uranium bioreduction kinetics can be predicted over a wide range of geochemical conditions based on the bioavailability and toxicity imparted on U(VI) by solution composition. Finally, these findings also imply that the concentration of uranyl non-carbonate species, despite being extremely low, is a determining factor controlling uranium bioreduction at contaminated sites.« less

Lessons from Natural Analog Studies for Geologic Disposal of High-Level Nuclear Waste (Invited)

NASA Astrophysics Data System (ADS)

Murphy, W. M.

2009-12-01

For over fifty years natural analog studies have provided lessons addressing scientific, technical, and social problems concerning geologic disposal of high-level nuclear waste. Idealized concepts for permanent disposal environments evolved from an understanding of the geological, geochemical and hydrological characteristics of analogous rocks including natural salt deposits (as advocated by the US National Academy of Sciences in 1957), ancient cratonic rocks (as investigated at Lac du Bonnet, Canada, Aspö, Sweden, and Vienne, France), and marine sedimentary rock formations (as studied at Mol, Belgium, and Bure, France). Additional multidisciplinary studies have been conducted at natural sites that bear characteristics analogous to potential repository systems, notably at natural uranium (and thorium) deposits including Poços de Caldas, Brazil, Alligator Rivers, Australia, Peña Blanca, Mexico, and Oklo, Gabon. Researchers of natural analogs for geologic disposal have addressed technical uncertainties regarding processes that have transpired over large time and space scales, which are generally inaccessible to laboratory studies. Principal questions for nuclear waste disposal include the geochemical stability and alteration rates of radionuclide bearing minerals and the mechanisms and rates of transport of radionuclides in groundwater. In their most direct applications, natural analogs studies have been devoted to testing specific models for repository performance and the experimental data that support those models. Parameters used in predictive performance assessment modeling have been compared to natural system data, including mineral solubilities, sorption coefficients, diffusion rates, and colloid transport properties. For example, the rate of uraninite oxidation and the natural paragenesis of uranium mineral alteration at Peña Blanca have been compared favorably to results of experimental studies of spent fuel alteration related to the proposed repository at Yucca Mountain, Nevada, USA. These results generally bracket repository conditions between natural and experimental systems providing confidence in the understanding of expected processes. Also, the conceptual bases and numerical techniques for modeling unsaturated zone contaminant transport over periods of thousands of years at Yucca Mountain were tested by modeling the observable record of metal transport from archaeological artifacts buried in Holocene tuff at Akrotiri, Greece. Geologically episodic mineral alteration and contaminant transport have been documented using radioisotope data in numerous analog systems providing insights for the interpretation and validity of predictive models for long term repository performance. The applicability and value of natural analog studies to understanding geologic disposal systems is a persistent question. As proposed disposal sites become increasingly well defined by site characterization and engineering design, the strengths and weaknesses of analogies can be assessed. Confidence in predictive models for complex geologic and engineered phenomena can be enhanced through multiple lines of investigation including studies of natural analog systems.

Electrorefining process and apparatus for recovery of uranium and a mixture of uranium and plutonium from spent fuels

DOEpatents

Ackerman, John P.; Miller, William E.

1989-01-01

An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuel using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuel, and two cathodes, the first cathode composed of either a solid alloy or molten cadmium and the second cathode composed of molten cadmium. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then substantially pure uranium is electrolytically transported and deposited on the first alloy or molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on the second molten cadmium cathode.

Electrorefining process and apparatus for recovery of uranium and a mixture of uranium and plutonium from spent fuels

DOEpatents

Ackerman, J.P.; Miller, W.E.

1987-11-05

An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuels is disclosed using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuels, two cathodes and electrical power means connected to the anode basket, cathodes and lower molten cadmium pool for providing electrical power to the cell. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then purified uranium is electrolytically transported and deposited on a first molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on a second cathode. 3 figs.

Four methods for determining the composition of trace radioactive surface contamination of low-radioactivity metal

NASA Astrophysics Data System (ADS)

O'Keeffe, H. M.; Burritt, T. H.; Cleveland, B. T.; Doucas, G.; Gagnon, N.; Jelley, N. A.; Kraus, C.; Lawson, I. T.; Majerus, S.; McGee, S. R.; Myers, A. W.; Poon, A. W. P.; Rielage, K.; Robertson, R. G. H.; Rosten, R. C.; Stonehill, L. C.; VanDevender, B. A.; Van Wechel, T. D.

2011-12-01

Four methods for determining the composition of low-level uranium- and thorium-chain surface contamination are presented. One method is the observation of Cherenkov light production in water. In two additional methods a position-sensitive proportional counter surrounding the surface is used to make both a measurement of the energy spectrum of alpha particle emissions and also coincidence measurements to derive the thorium-chain content based on the presence of short-lived isotopes in that decay chain. The fourth method is a radiochemical technique in which the surface is eluted with a weak acid, the eluate is concentrated, added to liquid scintillator and assayed by recording beta-alpha coincidences. These methods were used to characterize two 'hotspots' on the outer surface of one of the 3He proportional counters in the Neutral Current Detection array of the Sudbury Neutrino Observatory experiment. The methods have similar sensitivities, of order tens of ng, to both thorium- and uranium-chain contamination.

BetaScint{trademark} fiber-optic sensor for detecting strontium-90 and uranium-238 in soil. Innovative technology summary report

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1998-12-01

Accurate measurements of radioactivity in soils contaminated with Strontium-90 (Sr-90) or Uranium-238 (U-238) are essential for many DOE site remediation programs. These crucial measurements determine if excavation and soil removal is necessary, where remediation efforts should be focused, and/or if a site has reached closure. Measuring soil contamination by standard EPA laboratory methods typically takes a week (accelerated analytical test turnaround) or a month (standard analytical test turnaround). The time delay extends to operations involving heavy excavation equipment and associated personnel which are the main costs of remediation. This report describes an application of the BetaScint{trademark} fiber-optic sensor that measuresmore » Sr-90 or U-238 contamination in soil samples on site in about 20 minutes, at a much lower cost than time-consuming laboratory methods, to greatly facilitate remediation. This report describes the technology, its performance, its uses, cost, regulatory and policy issues, and lessons learned.« less

Microanalytical X-ray imaging of depleted uranium speciation in environmentally aged munitions residues.

PubMed

Crean, Daniel E; Livens, Francis R; Stennett, Martin C; Grolimund, Daniel; Borca, Camelia N; Hyatt, Neil C

2014-01-01

Use of depleted uranium (DU) munitions has resulted in contamination of the near-surface environment with penetrator residues. Uncertainty in the long-term environmental fate of particles produced by impact of DU penetrators with hard targets is a specific concern. In this study DU particles produced in this way and exposed to the surface terrestrial environment for longer than 30 years at a U.K. firing range were characterized using synchrotron X-ray chemical imaging. Two sites were sampled: a surface soil and a disposal area for DU-contaminated wood, and the U speciation was different between the two areas. Surface soil particles showed little extent of alteration, with U speciated as oxides U3O7 and U3O8. Uranium oxidation state and crystalline phase mapping revealed these oxides occur as separate particles, reflecting heterogeneous formation conditions. Particles recovered from the disposal area were substantially weathered, and U(VI) phosphate phases such as meta-ankoleite (K(UO2)(PO4) · 3H2O) were dominant. Chemical imaging revealed domains of contrasting U oxidation state linked to the presence of both U3O7 and meta-ankoleite, indicating growth of a particle alteration layer. This study demonstrates that substantial alteration of DU residues can occur, which directly influences the health and environmental hazards posed by this contamination.

Depleted uranium contamination by inhalation exposure and its detection after approximately 20 years: implications for human health assessment.

PubMed

Parrish, Randall R; Horstwood, Matthew; Arnason, John G; Chenery, Simon; Brewer, Tim; Lloyd, Nicholas S; Carpenter, David O

2008-02-01

Inhaled depleted uranium (DU) aerosols are recognised as a distinct human health hazard and DU has been suggested to be responsible in part for illness in both military and civilian populations that may have been exposed. This study aimed to develop and use a testing procedure capable of detecting an individual's historic milligram-quantity aerosol exposure to DU up to 20 years after the event. This method was applied to individuals associated with or living proximal to a DU munitions plant in Colonie New York that were likely to have had a significant DU aerosol inhalation exposure, in order to improve DU-exposure screening reliability and gain insight into the residence time of DU in humans. We show using sensitive mass spectrometric techniques that when exposure to aerosol has been unambiguous and in sufficient quantity, urinary excretion of DU can be detected more than 20 years after primary DU inhalation contamination ceased, even when DU constitutes only approximately 1% of the total excreted uranium. It seems reasonable to conclude that a chronically DU-exposed population exists within the contamination 'footprint' of the munitions plant in Colonie, New York. The method allows even a modest DU exposure to be identified where other less sensitive methods would have failed entirely. This should allow better assessment of historical exposure incidence than currently exists.

The application of zero-valent iron nanoparticles for the remediation of a uranium-contaminated waste effluent.

PubMed

Dickinson, Michelle; Scott, Thomas B

2010-06-15

Zero-valent iron nanoparticles (INP) were investigated as a remediation strategy for a uranium-contaminated waste effluent from AWE, Aldermaston. Nanoparticles were introduced to the effluent, under both oxic and anoxic conditions, and allowed to react for a 28-d period during which the liquid and nanoparticle solids were periodically sampled. Analysis of the solution indicated that under both conditions U was removed to <1.5% of its initial concentration within 1h of introduction and remained at similar concentrations until approximately 48 h. A rapid release of Fe into solution was also recorded during this initial period; attributed to the limited partial dissolution of the INP. XPS analyses of the reacted nanoparticulate solids between 1 and 48 h showed an increased Fe(III):Fe(II) ratio, consistent with the detection of iron oxidation products (akaganeite and magnetite) by XRD and FIB. XPS analysis also recorded uranium on the recovered particulates indicating the chemical reduction of U(VI) to U(IV) within 1h. Following the initial retention period U-dissolution of U was recorded from 48 h, and attributed to reoxidation. The efficient uptake and retention of U on the INP for periods up to 48 h provide proof that INP may be effectively used for the remediation of complex U-contaminated effluents. Copyright 2010 Elsevier B.V. All rights reserved.

Aqueous biphasic extraction of uranium and thorium from contaminated soils. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chaiko, D.J.; Gartelmann, J.; Henriksen, J.L.

1995-07-01

The aqueous biphasic extraction (ABE) process for soil decontamination involves the selective partitioning of solutes and fine particulates between two immiscible aqueous phases. The biphase system is generated by the appropriate combination of a water-soluble polymer (e.g., polyethlene glycol) with an inorganic salt (e.g., sodium carbonate). Selective partitioning results in 99 to 99.5% of the soil being recovered in the cleaned-soil fraction, while only 0.5 to 1% is recovered in the contaminant concentrate. The ABE process is best suited to the recovery of ultrafine, refractory material from the silt and clay fractions of soils. During continuous countercurrent extraction tests withmore » soil samples from the Fernald Environmental Management Project site (Fernald, OH), particulate thorium was extracted and concentrated between 6- and 16-fold, while the uranium concentration was reduced from about 500 mg/kg to about 77 mg/kg. Carbonate leaching alone was able to reduce the uranium concentration only to 146 mg/kg. Preliminary estimates for treatment costs are approximately $160 per ton of dry soil. A detailed flowsheet of the ABE process is provided.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goins, L.F.; Webb, J.R.; Cravens, C.D.

This publication contains 1035 abstracted references on environmental restoration, nuclear facility decommissioning, uranium mill tailings management, and site remedial actions. These citations constitute the thirteenth in a series of reports prepared annually for the US Department of Energy (DOE) Environmental Restoration programs. Citations to foreign and domestic literature of all types. There are 13 major sections of the publication, including: (1) DOE Decontamination and Decommissioning Program; (2) Nuclear Facilities Decommissioning; (3) DOE Formerly Utilized Sites Remedial Action Program; (4) DOE Uranium Mill Tailings Remedial Action Project; (5) Uranium Mill Tailings Management; (6) DOE Environmental Restoration Program; (7) DOE Site-Specific Remedialmore » Actions; (8) Contaminated Site Restoration; (9) Remediation of Contaminated Soil and Groundwater; (10) Environmental Data Measurements, Management, and Evaluation; (11) Remedial Action Assessment and Decision-Making; (12) Technology Development and Evaluation; and (13) Environmental and Waste Management Issues. Bibliographic references are arranged in nine subject categories by geographic location and then alphabetically by first author, corporate affiliation, or publication title. Indexes are provided for author, corporate affiliation, title word, publication description, geographic location, subject category, and key word.« less

Cleanup protocol for 226Ra-contaminated cobbly soil at UMTRA Project sites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gonzales, D.E.; Millard, J.B.; Miller, M.L.

The nonuniform distribution of 226Ra and other radiological contamination of cobbly soil encountered on several Uranium Mill Tailings Remedial Action Project sites is presented and discussed, and the concomitant challenges to the intent and implementation of the U.S. Environmental Protection Agency's soil cleanup standards are noted. In response to technical assessments and information presented to the U.S. Nuclear Regulatory Commission by the U.S. Department of Energy, the Nuclear Regulatory Commission has recently resolved the dilemma by concluding that compliance with Environmental Protection Agency soil cleanup standards for cobby soil at Uranium Mill Tailings Remedial Action Project sites would be adequatelymore » attained using bulk radionuclide concentrations, instead of requiring that the radionuclide concentration of the finer soil fraction passing a No. 4 mesh sieve met the standards. A Nuclear Regulatory Commission-approved procedure developed for cobbly soil remediation is outlined and discussed. The site-specific implementation of this procedure at Uranium Mill Tailings Remedial Action Project sites containing cobbly soil is estimated to save millions of dollars.« less

Literature review: Phytoaccumulation of chromium, uranium, and plutonium in plant systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hossner, L.R.; Loeppert, R.H.; Newton, R.J.

1998-05-01

Phytoremediation is an integrated multidisciplinary approach to the cleanup of contaminated soils, which combines the disciplines of plant physiology, soil chemistry, and soil microbiology. Metal hyperaccumulator plants are attracting increasing attention because of their potential application in decontamination of metal-polluted soils. Traditional engineering technologies may be too expensive for the remediation of most sites. Removal of metals from these soils using accumulator plants is the goal of phytoremediation. The emphasis of this review has been placed on chromium (Cr), plutonium (Pu), and uranium (U). With the exception of Cr, these metals and their decay products exhibit two problems, specifically, radiationmore » dose hazards and their chemical toxicity. The radiation hazard introduces the need for special precautions in reclamation beyond that associated with non-radioactive metals. The uptake of beneficial metals by plants occurs predominantly by way of channels, pores, and transporters in the root plasma membrane. Plants characteristically exhibit a remarkable capacity to absorb what they need and exclude what they don`t need. But most vascular plants absorb toxic and heavy metals through their roots to some extent, though to varying degrees, from negligible to substantial. Sometimes absorption occurs because of the chemical similarity between beneficial and toxic metals. Some plants utilize exclusion mechanisms, where there is a reduced uptake by the roots or a restricted transport of the metal from root to shoot. At the other extreme, hyperaccumulator plants absorb and concentrate metals in both roots and shoots. Some plant species endemic to metalliferous soils accumulate metals in percent concentrations in the leaf dry matter.« less

Remediation of a uranium-contamination in ground water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Woerner, Joerg; Margraf, Sonja; Hackel, Walter

2007-07-01

The former production site of NUKEM where nuclear fuel-elements were developed and handled from 1958 to 1988 was situated in the centre of an industrial park for various activities of the chemical and metallurgical industry. The size of the industrially used part is about 300.000 m{sup 2}. Regulatory routine controls showed elevated CHC (Chlorinated Hydro-Carbons) values of the ground water at the beginning of the 1990's in an area which represented about 80.000 m{sup 2} down-gradient of locations where CHC compounds were stored and handled. Further investigations until 1998 proved that former activities on the NUKEM site, like the UF{submore » 6} conversion process, were of certain relevance. The fact that several measured values were above the threshold values made the remediation of the ground water mandatory. This was addressed in the permission given by the Ministry for Nuclear Installations and Environment of Hesse according to chap. 7 of the German atomic law in October 2000. Ground water samples taken in an area of about 5.000 m{sup 2} showed elevated values of total Uranium activity up to between 50 and 75 Bq/l in 2002. Furthermore in an area of another 20.000 m{sup 2} the samples were above threshold value. In this paper results of the remediation are presented. The actual alpha-activities of the ground waters of the remediation wells show values of 3 to 9 Bq/l which are dominated by 80 to 90 % U-234 activity. The mass-share of total Uranium for this nuclide amounts to 0,05% on average. The authority responsible for conventional water utilisation defined target values for remediation: 20 {mu}g/l for dissolved Uranium and 10 {mu}g/l for CHC. Both values have not yet been reached for an area of about 10.000 m{sup 2}. The remediation process by extracting water from four remediation wells has proved its efficiency by reduction of the starting concentrations by a factor of 3 to 6. Further pumping will be necessary especially in that area of the site where the contaminations were found later during soil remediation activities. Only two wells have been in operation since July 2002 when the remediation technique was installed and an apparatus for direct gamma-spectroscopic measurement of the accumulated activities on the adsorbers was qualified. Two further remediation wells have been in operation since August 2006, when the installed remediation technique was about to be doubled from a throughput of 5 m{sup 3}/h to 10 m{sup 3}/h. About 20.000 m{sup 3} of ground water have been extracted since from these two wells and the decrease of their Uranium concentrations behaves similar to that of the two other wells being extracted since the beginning of remediation. Both, total Uranium-concentrations and the weight-share of the nuclides U-234, U-235 and U-238 are measured by ICP-MS (Inductively Coupled Plasma - Mass Spectrometry) besides measurements of Uranium-Alpha-Activities in addition to the measurement of CHC components of which PCE (Per-chlor-Ethene) is dominant in the contaminated area. CHC compounds are measured by GC (Gas Chromatography). Down-gradient naturally attenuated products are detected in various compositions. Overall 183.000 m{sup 3} of ground water have been extracted. Using a pump and treat method 11 kg Uranium have been collected on an ion-exchange material based on cellulose, containing almost 100 MBq U-235 activity, and almost 15 kg of CHC, essentially PCE, were collected on GAC (Granules of Activated Carbon). Less than 3% of the extracted Uranium have passed the adsorber-system of the remediation plant and were adsorbed by the sewage sludge of the industrial site's waste water treatment. The monthly monitoring of 19 monitoring wells shows that an efficient artificial barrier was built up by the water extraction. The Uranium contamination of two ground water plumes has drastically been reduced by the used technique dependent on the amounts of extracted water. The concentration of the CHC contamination has changed depending on the location of temporal pumping. Thereby maximum availability of this contaminant for the remediation process is ensured. If locations with unchanged water quality are detected electrochemical parameters of the water or hydro-geologic data of the aquifer have to be taken into further consideration to improve the process of remediation. (authors)« less

Molecular Simulations of the Diffusion of Uranyl Carbonate Species in Nanosized Mineral Fractures

NASA Astrophysics Data System (ADS)

Kerisit, S.; Liu, C.

2010-12-01

Uranium is a major groundwater contaminant at uranium processing and mining sites as a result of intentional and accidental discharges of uranium-containing waste products into subsurface environments. Recent characterization has shown that uranium preferentially associates with intragrain and intra-aggregate domains in some of the uranium-contaminated sediments collected from the US Department of Energy Hanford Site [1, 2]. In these sediments, uranium existed as precipitated and/or adsorbed phases in grain micropores with nano- to microscale sizes. Desorption and diffusion characterization studies and continuum-scale modeling indicated that ion diffusion in the microfractures is a major mechanism that led to preferential uranium concentration in the microfracture regions and will control the future mobility of uranium in the subsurface sediments [1, 3-4]. However, the diffusion properties of uranyl species in the intragrain regions, especially at the solid-liquid interface, are still poorly understood. Therefore, a general aim of this work is to provide atomic-level insights into the contribution of microscopic surface effects to the slow diffusion process of uranyl species in porous media with nano- to microsized fractures. In this presentation, we will first present molecular dynamics (MD) simulations of feldspar-water interfaces to investigate their interfacial structure and dynamics and establish a theoretical framework for subsequent simulations of water and ion diffusion at these interfaces [5]. We will then report on MD simulations carried out to probe the effects of confinement and of the presence of the mineral surface on the diffusion of water and electrolyte ions in nanosized feldspar fractures [6]. Several properties of the mineral-water interface were varied, such as the fracture width, the ionic strength of the contacting solution, and the surface charge. Our calculations reveal a 2.0-2.5 nm interfacial region within which the diffusion properties of water and that of the electrolyte ions differ significantly from those in bulk aqueous solutions. We will then present MD simulations of the diffusion of a series of alkaline-earth uranyl carbonate species in aqueous solutions [7]. The MD simulations show that the alkaline-earth uranyl carbonate complexes have distinct water exchange dynamics, which could lead to different reactivities. Finally, we will present recent results on the diffusion and adsorption of uranyl carbonate species in intragrain micropores, modeled with the feldspar-water interfaces mentioned in the above, to help interpret the diffusion behavior of uranium in contaminated sediments. [1] Liu C. et al. Geochim. Cosmochim. Acta 68 4519 (2004) [2] McKinley J. P. et al. Geochim. Cosmochim. Acta 70 1873 (2006) [3] Liu C. et al. Water Resour. Res. 42 W12420 (2006) [4] Ilton E. S. et al. Environ. Sci. Technol. 42 1565 (2009) [5] Kerisit S. et al. Geochim. Cosmochim. Acta 72 1481 (2008) [6] Kerisit S. and Liu C. Environ. Sci. Technol. 43 777 (2009) [7] Kerisit S. and Liu C. Geochim. Cosmochim. Acta 74 4937 (2010)

Field Testing of Downgradient Uranium Mobility at an In-Situ Recovery Uranium Mine

NASA Astrophysics Data System (ADS)

Reimus, P. W.; Clay, J. T.; Rearick, M.; Perkins, G.; Brown, S. T.; Basu, A.; Chamberlain, K.

2015-12-01

In-situ recovery (ISR) mining of uranium involves the injection of O2 and CO2 (or NaHCO3) into saturated roll-front deposits to oxidize and solubilize the uranium, which is then removed by ion exchange at the surface and processed into U3O8. While ISR is economical and environmentally-friendly relative to conventional mining, one of the challenges of extracting uranium by this process is that it leaves behind a geochemically-altered aquifer that is exceedingly difficult to restore to pre-mining geochemical conditions, a regulatory objective. In this research, we evaluated the ability of the aquifer downgradient of an ISR mining area to attenuate the transport of uranium and other problem constituents that are mobilized by the mining process. Such an evaluation can help inform both regulators and the mining industry as to how much restoration of the mined ore zone is necessary to achieve regulatory compliance at various distances downgradient of the mining zone even if complete restoration of the ore zone proves to be difficult or impossible. Three single-well push-pull tests and one cross-well test were conducted in which water from an unrestored, previously-mined ore zone was injected into an unmined ore zone that served as a geochemical proxy for the downgradient aquifer. In all tests, non-reactive tracers were injected with the previously-mined ore zone water to allow the transport of uranium and other constituents to be compared to that of the nonreactive species. In the single-well tests, it was shown that the recovery of uranium relative to the nonreactive tracers ranged from 12-25%, suggesting significant attenuation capacity of the aquifer. In the cross-well test, selenate, molybdate and metavanadate were injected with the unrestored water to provide information on the transport of these potentially-problematic anionic constituents. In addition to the species-specific transport information, this test provided valuable constraints on redox conditions within the system, as redox couples involving these species collectively bracket the predicted transition redox potential for the U(VI)/U(IV) couple. Reduction should provide much longer-lasting immobilization of constituents than adsorption, especially given the inherent reducing characteristics of roll-front systems.

Bioreduction of U(VI)-Phthalate to a Polymeric U(IV)-Phthalate Colloid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vazquez, G.; Dodge, C; Francis, A

2009-01-01

Phthalic acid, a ubiquitous organic ligand, formed soluble mono- and biligand complexes with a uranyl ion that was then reduced to a U(IV)-phthalate by a Clostridium species under anaerobic conditions. We confirmed the reduction of the hexavalent uranium to the tetravalent oxidation state by UV-vis absorption and X-ray absorption near edge structure spectroscopy. Sequential micro- and ultrafiltration of the solution revealed that the bioreduced uranium was present as a colloid with particles between 0.03 and 0.45 {mu}m. Analysis with extended X-ray absorption fine structure revealed the association of the reduced uranium with the phthalic acid as a repeating biligand 1:2more » U(IV):phthalic acid polymer. This is the first report of the formation of a U(IV) complexed to two phthalic acid molecules in the form of a polymeric colloid. Although it was proposed that the bioreduction and the precipitation of uranium might be an invaluable strategy to immobilize uranium in contaminated environments, our results suggest that the organic ligands present there might hinder the precipitation of the bioreduced uranium under anaerobic conditions and, thereby, enhance its environmental mobility as uranium organic complexes or colloids.« less

Continuous process electrorefiner

DOEpatents

Herceg, Joseph E [Naperville, IL; Saiveau, James G [Hickory Hills, IL; Krajtl, Lubomir [Woodridge, IL

2006-08-29

A new device is provided for the electrorefining of uranium in spent metallic nuclear fuels by the separation of unreacted zirconium, noble metal fission products, transuranic elements, and uranium from spent fuel rods. The process comprises an electrorefiner cell. The cell includes a drum-shaped cathode horizontally immersed about half-way into an electrolyte salt bath. A conveyor belt comprising segmented perforated metal plates transports spent fuel into the salt bath. The anode comprises the conveyor belt, the containment vessel, and the spent fuel. Uranium and transuranic elements such as plutonium (Pu) are oxidized at the anode, and, subsequently, the uranium is reduced to uranium metal at the cathode. A mechanical cutter above the surface of the salt bath removes the deposited uranium metal from the cathode.

Influence of acidic and alkaline waste solution properties on uranium migration in subsurface sediments.

PubMed

Szecsody, Jim E; Truex, Mike J; Qafoku, Nikolla P; Wellman, Dawn M; Resch, Tom; Zhong, Lirong

2013-08-01

This study shows that acidic and alkaline wastes co-disposed with uranium into subsurface sediments have significant impact on changes in uranium retardation, concentration, and mass during downward migration. For uranium co-disposal with acidic wastes, significant rapid (i.e., hours) carbonate and slow (i.e., 100 s of hours) clay dissolution resulted, releasing significant sediment-associated uranium, but the extent of uranium release and mobility change was controlled by the acid mass added relative to the sediment proton adsorption capacity. Mineral dissolution in acidic solutions (pH2) resulted in a rapid (<10 h) increase in aqueous carbonate (with Ca(2+), Mg(2+)) and phosphate and a slow (100 s of hours) increase in silica, Al(3+), and K(+), likely from 2:1 clay dissolution. Infiltration of uranium with a strong acid resulted in significant shallow uranium mineral dissolution and deeper uranium precipitation (likely as phosphates and carbonates) with downward uranium migration of three times greater mass at a faster velocity relative to uranium infiltration in pH neutral groundwater. In contrast, mineral dissolution in an alkaline environment (pH13) resulted in a rapid (<10h) increase in carbonate, followed by a slow (10 s to 100 s of hours) increase in silica concentration, likely from montmorillonite, muscovite, and kaolinite dissolution. Infiltration of uranium with a strong base resulted in not only uranium-silicate precipitation (presumed Na-boltwoodite) but also desorption of natural uranium on the sediment due to the high ionic strength solution, or 60% greater mass with greater retardation compared with groundwater. Overall, these results show that acidic or alkaline co-contaminant disposal with uranium can result in complex depth- and time-dependent changes in uranium dissolution/precipitation reactions and uranium sorption, which alter the uranium migration mass, concentration, and velocity. Copyright © 2013 Elsevier B.V. All rights reserved.

Agriculture in an area impacted by past uranium mining activities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carvalho, F. P.; Oliveira, J. M.; Neves, O.

2007-07-01

The shallow aquifer near the old Cunha Baixa uranium mine (Viseu, Portugal) was contaminated by acid mine drainage. Concentration of radionuclides in water from irrigation wells and in the topsoil layer of the agriculture fields nearby display enhanced concentrations of uranium, radium and polonium. Two types of agriculture land in this area were selected, one with enhanced and another with low uranium concentrations, for controlled growth of lettuce and potatoes. Plants were grown in replicate portions of land (two plots) in each soil type and were periodically irrigated with water from wells. In each soil, one plot was irrigated withmore » water containing low concentration of dissolved uranium and the other plot with water containing enhanced concentration of dissolved uranium. At the end of the growth season, plants were harvested and analysed, along with soil and irrigation water samples. Results show the accumulation of radionuclides in edible parts of plants, specially in the field plots with higher radionuclide concentrations in soil. Radionuclides in irrigation water contributed less to the radioactivity accumulated in plants than radionuclides from soils. (authors)« less

Biosorption and biomineralization of uranium(VI) by Saccharomyces cerevisiae-Crystal formation of chernikovite.

PubMed

Zheng, Xin-Yan; Wang, Xiao-Yu; Shen, Yang-Hao; Lu, Xia; Wang, Tie-Shan

2017-05-01

Biosorption of heavy metal elements including radionuclides by microorganisms is a promising and effective method for the remediation of the contaminated places. The responses of live Saccharomyces cerevisiae in the toxic uranium solutions during the biosorption process and the mechanism of uranium biomineralization by cells were investigated in the present study. A novel experimental phenomenon that uranium concentrations have negative correlation with pH values and positive correlation with phosphate concentrations in the supernatant was observed, indicating that hydrogen ions, phosphate ions and uranyl ions were involved in the chernikovite precipitation actively. During the biosorption process, live cells desorb deposited uranium within the equilibrium state of biosorption system was reached and the phosphorus concentration increased gradually in the supernatant. These metabolic detoxification behaviours could significantly alleviate uranium toxicity and protect the survival of the cells better in the environment. The results of microscopic and spectroscopic analysis demonstrated that the precipitate on the cell surface was a type of uranium-phosphate compound in the form of a scale-like substance, and S. cerevisiae could transform the uranium precipitate into crystalline state-tetragonal chernikovite [H 2 (UO 2 ) 2 (PO 4 ) 2 ·8H 2 O]. Copyright © 2017 Elsevier Ltd. All rights reserved.

A survey of uranium levels in urine and hair of people living in a coal mining area in Yili, Xinjiang, China.

PubMed

Wufuer, Rehemanjiang; Song, Wenjuan; Zhang, Daoyong; Pan, Xiangliang; Gadd, Geoffrey Michael

2018-09-01

Recent reports have drawn attention to the uranium contamination arising from coal mining activities in the Yili region of Xinjiang, China due to the mixed distribution of uranium and coal mines, and some of the coal mines being associated with a high uranium content. In this study, we have collected water samples, solid samples such as soil, mud, coal, and coal ash, and hair and urine samples from local populations in order to evaluate the uranium level in this environment and its implications for humans in this high uranium coal mining area. Our results showed that uranium concentrations were 8.71-10.91 μg L -1 in underground water, whereas lower levels of uranium occurred in river water. Among the solid samples, coal ash contained fairly high concentrations of uranium (33.1 μg g -1 ) due to enrichment from coal burning. In addition, uranium levels in the other solid samples were around 2.8 μg g -1 (the Earth's average background value). Uranium concentrations in hair and urine samples were 22.2-634.5 ng g -1 (mean: 156.2 ng g -1 ) and 8.44-761.6 ng L -1 (mean: 202.6 ng L -1 ), respectively, which are significantly higher than reference values reported for unexposed subjects in other areas. Therefore, these results indicate that people living in this coal mining area have been subjected to uranium exposure for long periods of time. Copyright © 2018. Published by Elsevier Ltd.

Annual INTEC Groundwater Monitoring Report for Group 5 - Snake River Plain Aquifer (2001)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roddy, Michael Scott

2002-02-01

This report describes the monitoring activities conducted and presents the results of groundwater sampling and water-level measurements from October 2000 to September 2001. Groundwater samples were initially collected from 41 wells from the Idaho Nuclear Technology and Engineering Center and the Central Facilities Area and analyzed for iodine-129, strontium-90, tritium, gross alpha, gross beta, technetium-99, uranium isotopes, plutonium isotopes, neptunium-237, americium-241, gamma spectrometry, and mercury. Samples from 41 wells were collected in April and May 2001. Additional sampling was conducted in August 2001 and included the two CFA production wells, the CFA point of compliance for the production wells, onemore » well that was previously sampled and five additional monitoring wells. Iodine-129 and strontium-90 were the only analytes above their respective maximum contaminant levels. Iodine-129 was detected just above its maximum contaminant level of 1 pCi/L at two of the Central Facilities Area landfill wells. Iodine-129 was detected in the CFA production wells at 0.35±0.083 pCi/L in CFA-1, but was below detectable activity in CFA-2. Strontium-90 was above its maximum contaminant level of 8 pCi/L in several wells near the Idaho Nuclear Technology and Engineering Center but was below its maximum contaminant level in the downgradient wells at the Central Facilities Area landfills. Sr-90 was not detected in the CFA production wells. Gross beta results generally mirrored the results for strontium-90 and technetium-99. Plutonium isotopes and neptunium-237 were not detected. Uranium-233/234 and uranium-238 isotopes were detected in all samples. Concentrations of background and site wells were similar and are within background limits for total uranium determined by the USGS, suggesting that the concentrations are background. Uranium-235/236 was detected in 11 samples, but all the detected concentrations were similar and near the minimum detectable activity. Americium-241 was detected at three locations near the minimum detectable activity of approximately 0.07 pCi/L. The gamma spectrometry results detected cesium-137 in three samples, potassium-40 at eight locations, and radium-226 at one location. Mercury was below its maximum contaminant level of 2 µg/L in all samples. Gamma spectrometry results for the CFA production wells did not detect any analytes. Water-level measurements were taken from wells in the Idaho Nuclear Technology and Engineering Center, Central Facilities Area, and the area south of Central Facilities Area to evaluate groundwater flow directions. Water-level measurements indicated groundwater flow to the south-southwest from the Idaho Nuclear Technology and Engineering Center.« less

77 FR 26149 - Access Authorization Fees

Federal Register 2010, 2011, 2012, 2013, 2014

2012-05-03

... Regulatory Affairs of OMB. List of Subjects 10 CFR Part 11 Hazardous materials--transportation... licensees for work performed under the Material Access Authorization Program (MAAP) and the Information... assigned duties which require access to special nuclear material (plutonium, uranium-233, and uranium...

Uranium Biomineralization By Natural Microbial Phosphatase Activities in the Subsurface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taillefert, Martial

This project investigated the geochemical and microbial processes associated with the biomineralization of radionuclides in subsurface soils. During this study, it was determined that microbial communities from the Oak Ridge Field Research subsurface are able to express phosphatase activities that hydrolyze exogenous organophosphate compounds and result in the non-reductive bioimmobilization of U(VI) phosphate minerals in both aerobic and anaerobic conditions. The changes of the microbial community structure associated with the biomineralization of U(VI) was determined to identify the main organisms involved in the biomineralization process, and the complete genome of two isolates was sequenced. In addition, it was determined thatmore » both phytate, the main source of natural organophosphate compounds in natural environments, and polyphosphate accumulated in cells could also be hydrolyzed by native microbial population to liberate enough orthophosphate and precipitate uranium phosphate minerals. Finally, the minerals produced during this process are stable in low pH conditions or environments where the production of dissolved inorganic carbon is moderate. These findings suggest that the biomineralization of U(VI) phosphate minerals is an attractive bioremediation strategy to uranium bioreduction in low pH uranium-contaminated environments. These efforts support the goals of the SBR long-term performance measure by providing key information on "biological processes influencing the form and mobility of DOE contaminants in the subsurface".« less

Competing retention pathways of uranium upon reaction with Fe(II)

NASA Astrophysics Data System (ADS)

Massey, Michael S.; Lezama-Pacheco, Juan S.; Jones, Morris E.; Ilton, Eugene S.; Cerrato, José M.; Bargar, John R.; Fendorf, Scott

2014-10-01

Biogeochemical retention processes, including adsorption, reductive precipitation, and incorporation into host minerals, are important in contaminant transport, remediation, and geologic deposition of uranium. Recent work has shown that U can become incorporated into iron (hydr)oxide minerals, with a key pathway arising from Fe(II)-induced transformation of ferrihydrite, (Fe(OH)3·nH2O) to goethite (α-FeO(OH)); this is a possible U retention mechanism in soils and sediments. Several key questions, however, remain unanswered regarding U incorporation into iron (hydr)oxides and this pathway's contribution to U retention, including: (i) the competitiveness of U incorporation versus reduction to U(IV) and subsequent precipitation of UO2; (ii) the oxidation state of incorporated U; (iii) the effects of uranyl aqueous speciation on U incorporation; and, (iv) the mechanism of U incorporation. Here we use a series of batch reactions conducted at pH ∼7, [U(VI)] from 1 to 170 μM, [Fe(II)] from 0 to 3 mM, and [Ca] at 0 or 4 mM coupled with spectroscopic examination of reaction products of Fe(II)-induced ferrihydrite transformation to address these outstanding questions. Uranium retention pathways were identified and quantified using extended X-ray absorption fine structure (EXAFS) spectroscopy, X-ray powder diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy. Analysis of EXAFS spectra showed that 14-89% of total U was incorporated into goethite, upon reaction with Fe(II) and ferrihydrite. Uranium incorporation was a particularly dominant retention pathway at U concentrations ⩽50 μM when either uranyl-carbonato or calcium-uranyl-carbonato complexes were dominant, accounting for 64-89% of total U. With increasing U(VI) and Fe(II) concentrations, U(VI) reduction to U(IV) became more prevalent, but U incorporation remained a functioning retention pathway. These findings highlight the potential importance of U(V) incorporation within iron oxides as a retention process of U across a wide range of biogeochemical environments and the sensitivity of uranium retention processes to operative (bio)geochemical conditions.

Competing retention pathways of uranium upon reaction with Fe(II)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Massey, Michael S.; Lezama Pacheco, Juan S.; Jones, Morris

Biogeochemical retention processes, including adsorption, reductive precipitation, and incorporation into host minerals, are important in contaminant transport, remediation, and geologic deposition of uranium. Recent work has shown that U can become incorporated into iron (hydr)oxide minerals, with a key pathway arising from Fe(II)-induced transformation of ferrihydrite, (Fe(OH)3•nH2O) to goethite (α-FeO(OH)); this is a possible U retention mechanism in soils and sediments. Several key questions, however, remain unanswered regarding U incorporation into iron (hydr)oxides and this pathway’s contribution to U retention, including: (i) the competitiveness of U incorporation versus reduction to U(IV) and subsequent precipitation of UO2; (ii) the oxidation statemore » of incorporated U; (iii) the effects of uranyl aqueous speciation on U incorporation; and, (iv) the mechanism of U incorporation. Here we use a series of batch reactions conducted at pH ~7, [U(VI)] from 1 to 170 μM, [Fe(II)] from 0 to 3 mM, and [Ca] at 0 or 4 mM) coupled with spectroscopic examination of reaction products of Fe(II)-induced ferrihydrite transformation to address these outstanding questions. Uranium retention pathways were identified and quantified using extended x-ray absorption fine structure (EXAFS) spectroscopy, x-ray powder diffraction, x-ray photoelectron spectroscopy, and transmission electron microscopy. Analysis of EXAFS spectra showed that 14 to 89% of total U was incorporated into goethite, upon reaction with Fe(II) and ferrihydrite. Uranium incorporation was a particularly dominant retention pathway at U concentrations ≤ 50 μM when either uranyl-carbonato or calcium-uranyl-carbonato complexes were dominant, accounting for 64 to 89% of total U. With increasing U(VI) and Fe(II) concentrations, U(VI) reduction to U(IV) became more prevalent, but U incorporation remained a functioning retention pathway. These findings highlight the potential importance of U(V) incorporation within iron oxides as a retention process of U across a wide range of biogeochemical environments and the sensitivity of uranium retention processes to operative (bio)geochemical conditions.« less

Comparison of solvent extraction and extraction chromatography resin techniques for uranium isotopic characterization in high-level radioactive waste and barrier materials.

PubMed

Hurtado-Bermúdez, Santiago; Villa-Alfageme, María; Mas, José Luis; Alba, María Dolores

2018-07-01

The development of Deep Geological Repositories (DGP) to the storage of high-level radioactive waste (HLRW) is mainly focused in systems of multiple barriers based on the use of clays, and particularly bentonites, as natural and engineered barriers in nuclear waste isolation due to their remarkable properties. Due to the fact that uranium is the major component of HLRW, it is required to go in depth in the analysis of the chemistry of the reaction of this element within bentonites. The determination of uranium under the conditions of HLRW, including the analysis of silicate matrices before and after the uranium-bentonite reaction, was investigated. The performances of a state-of-the-art and widespread radiochemical method based on chromatographic UTEVA resins, and a well-known and traditional method based on solvent extraction with tri-n-butyl phosphate (TBP), for the analysis of uranium and thorium isotopes in solid matrices with high concentrations of uranium were analysed in detail. In the development of this comparison, both radiochemical approaches have an overall excellent performance in order to analyse uranium concentration in HLRW samples. However, due to the high uranium concentration in the samples, the chromatographic resin is not able to avoid completely the uranium contamination in the thorium fraction. Copyright © 2018 Elsevier Ltd. All rights reserved.

THE BEHAVIOR OF STRONTIUM-90 IN SOILS AND PLANTS AND AGRICULTURAL PRECAUTIONS FOR LESSENING THE STRONTIUM-90 CONTAMINATION OF FOOD (in German)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Scheffer, F.; Ludwieg, F.

The development of dirty atom bombs (hydrogen bombs with a uranium mantle) and the resultant high radioactive fall-out have made the strontium-90 contamination of foodstuffs a serious problem for humanity. The literature of recent years is used to survey the behavior of strontium-90 in plants and soil, and to discuss agricultural measures which could be taken to lessen the contamination of foodstuffs in case of atomic warfare. (auth)

Characterization of uranium surfaces machined with aqueous propylene glycol-borax or perchloroethylene-mineral oil coolants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cristy, S.S.; Bennett, R.K. Jr.; Dillon, J.J.

1986-12-31

The use of perchloroethylene (perc) as an ingredient in coolants for machining enriched uranium at the Oak Ridge Y-12 Plant has been discontinued because of environmental concerns. A new coolant was substituted in December 1985, which consists of an aqueous solution of propylene glycol with borax (sodium tetraborate) added as a nuclear poison and with a nitrite added as a corrosion inhibitor. Uranium surfaces machined using the two coolants were compared with respects to residual contamination, corrosion or corrosion potential, and with the aqueous propylene glycol-borax coolant was found to be better than that of enriched uranium machined with themore » perc-mineral oil coolant. The boron residues on the final-finished parts machined with the borax-containing coolant were not sufficient to cause problems in further processing. All evidence indicated that the enriched uranium surfaces machined with the borax-containing coolant will be as satisfactory as those machined with the perc coolant.« less

Breccia-pipe uranium mining in northern Arizona; estimate of resources and assessment of historical effects

USGS Publications Warehouse

Bills, Donald J.; Brown, Kristin M.; Alpine, Andrea E.; Otton, James K.; Van Gosen, Bradley S.; Hinck, Jo Ellen; Tillman, Fred D.

2011-01-01

About 1 million acres of Federal land in the Grand Canyon region of Arizona were temporarily withdrawn from new mining claims in July 2009 by the Secretary of the Interior because of concern that increased uranium mining could have negative impacts on the land, water, people, and wildlife. During a 2-year interval, a Federal team led by the Bureau of Land Management is evaluating the effects of withdrawing these lands for extended periods. As part of this team, the U.S. Geological Survey (USGS) conducted a series of short-term studies to examine the historical effects of breccia-pipe uranium mining in the region. The USGS studies provide estimates of uranium resources affected by the possible land withdrawal, examine the effects of previous breccia-pipe mining, summarize water-chemistry data for streams and springs, and investigate potential biological pathways of exposure to uranium and associated contaminants. This fact sheet summarizes results through December 2009 and outlines further research needs.

Visualizing different uranium oxidation states during the surface alteration of uraninite and uranium tetrachloride.

PubMed

Grossmann, Kay; Arnold, Thuro; Steudtner, Robin; Weiss, Stefan; Bernhard, Gert

2009-08-01

Low-temperature alteration reactions on uranium phases may lead to the mobilization of uranium and thereby poses a potential threat to humans living close to uranium-contaminated sites. In this study, the surface alteration of uraninite (UO(2)) and uranium tetrachloride (UCl(4)) in air atmosphere was studied by confocal laser scanning microscopy (CLSM) and laser-induced fluorescence spectroscopy using an excitation wavelength of 408 nm. It was found that within minutes the oxidation state on the surface of the uraninite and the uranium tetrachloride changed. During the surface alteration process U(IV) atoms on the uraninite and uranium tetrachloride surface became stepwise oxidized by a one-electron step at first to U(V) and then further to U(VI). These observed changes in the oxidation states of the uraninite surface were microscopically visualized and spectroscopically identified on the basis of their fluorescence emission signal. A fluorescence signal in the wavelength range of 415-475 nm was indicative for metastable uranium(V), and a fluorescence signal in the range of 480-560 nm was identified as uranium(VI). In addition, the oxidation process of tetravalent uranium in aqueous solution at pH 0.3 was visualized by CLSM and U(V) was fluorescence spectroscopically identified. The combination of microscopy and fluorescence spectroscopy provided a very convincing visualization of the brief presence of U(V) as a metastable reaction intermediate and of the simultaneous coexistence of the three states U(IV), U(V), and U(VI). These results have a significant importance for fundamental uranium redox chemistry and should contribute to a better understanding of the geochemical behavior of uranium in nature.

Pore-scale characterization of biogeochemical controls on iron and uranium speciation under flow conditions.

PubMed

Pearce, Carolyn I; Wilkins, Michael J; Zhang, Changyong; Heald, Steve M; Fredrickson, Jim K; Zachara, John M

2012-08-07

Etched silicon microfluidic pore network models (micromodels) with controlled chemical and redox gradients, mineralogy, and microbiology under continuous flow conditions are used for the incremental development of complex microenvironments that simulate subsurface conditions. We demonstrate the colonization of micromodel pore spaces by an anaerobic Fe(III)-reducing bacterial species (Geobacter sulfurreducens) and the enzymatic reduction of a bioavailable Fe(III) phase within this environment. Using both X-ray microprobe and X-ray absorption spectroscopy, we investigate the combined effects of the precipitated Fe(III) phases and the microbial population on uranium biogeochemistry under flow conditions. Precipitated Fe(III) phases within the micromodel were most effectively reduced in the presence of an electron shuttle (AQDS), and Fe(II) ions adsorbed onto the precipitated mineral surface without inducing any structural change. In the absence of Fe(III), U(VI) was effectively reduced by the microbial population to insoluble U(IV), which was precipitated in discrete regions associated with biomass. In the presence of Fe(III) phases, however, both U(IV) and U(VI) could be detected associated with biomass, suggesting reoxidation of U(IV) by localized Fe(III) phases. These results demonstrate the importance of the spatial localization of biomass and redox active metals, and illustrate the key effects of pore-scale processes on contaminant fate and reactive transport.

Examination of the health status of populations from depleted-uranium-contaminated regions.

PubMed

Milacić, Snezana; Petrović, Dragana; Jovicić, Dubravka; Kovacević, Radomir; Simić, Jadranko

2004-05-01

During the NATO air strikes on the Federal Republic of Yugoslavia (Serbia and Montenegro) in 1999, depleted-uranium ammunition was used on 112 locations, mainly Kosovo, in the south of Serbia, and one location in Montenegro. Blood samples of residents from depleted-uranium-contaminated areas were gathered and blood cell and chromosomal aberrations were analyzed. During the last 3 years blood samples from 21 residents of Kosovo (Strpce), from 29 residents from the south of Serbia (the Vranje and Bujanovac regions), and from 19 technical television workers from the site of Pljackovica, in the vicinity of Vranje, were collected. Blood samples from 33 residents of central Serbia and 46 occupational workers exposed to X-rays were used as controls. All subjects studied were without any clinical symptoms of disease. The examinations included general clinical assessment; urine samples for alpha-and gamma-spectrometry analysis; complete blood counts; ratio-percentages of blood cells in stained (Giemsa) capillary smears, individual leukocyte line elements; morphological changes observed under a microscope; the presence of immature forms or blasts; and leukocyte enzyme activity [alkaline phosphatase leukocyte (APL)]. Chromosomal aberrations were evaluated in 200 peripheral blood lymphocytes in mitosis. An increased incidence of rogue cells and chromosomal aberrations was found in the blood of the residents of Vranje and Bujanovac, but this was below the incidence of chromosomal aberrations in individuals occupationally exposed to ionizing irradiation. Blast cells were not found. Blood counts were decreased in only a few samples, while morphological changes of both nuclei and cytoplasm were marked in individuals in south and central Serbia. Enzymatic activity (as measured by the APL score) was decreased in samples with chromosomal aberrations and cyto-morphological changes in subjects from the south of Serbia. The contamination level measured by this examination was low. Because of the presence of depleted uranium (uranium-238) in the soil and in plants, the prevention of consequences necessitates the identification of the initial biological effects on sensitive tissues. Early identification of serious blood cell changes is important for appropriate medical treatment.

Processing liquid organic wastes at the NNL Preston laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Coppersthwaite, Duncan; Greenwood, Howard; Docrat, Tahera

2013-07-01

Organic compounds of various kinds have been used in the nuclear industry for numerous duties in uranium chemical, metal and ceramic processing plants. In the course of the various operations undertaken, these organic compounds have become contaminated with uranic material, either accidentally or as an inevitable part of the process. Typically, the chemical/physical form and/or concentration of the uranic content of the organics has prevented disposal. In order to address the issue of contaminated liquid organic wastes, the National Nuclear Laboratory (NNL) has developed a suite of treatments designed to recover uranium and to render the waste suitable for disposal.more » The developed processes are operated at industrial scale via the NNL Preston Laboratory Residue Processing Plant. The Oil Waste Leaching (OWL) Process is a fully industrialised process used for the treatment of contaminated oils with approximately 200 tonnes of uranium contaminated oil being treated to date. The process was originally developed for the treatment of contaminated tributyl phosphate and odourless kerosene which had been adsorbed onto sawdust. However, over the years, the OWL process has been refined for a range of oils including 'water emulsifiable' cutting oils, lubricating oils, hydraulic oils/fluids and 'Fomblin' (fully fluorinated) oils. Chemically, the OWL process has proved capable of treating solvents as well as oils but the highly volatile/flammable nature of many solvents has required additional precautions compared with those required for oil treatment. These additional precautions led to the development of the Solvent Treatment Advanced Rig (STAR), an installation operated under an inert atmosphere. STAR is a small 'module' (100 dm{sup 3} volume) which allows the treatment of both water miscible and immiscible solvents. This paper discusses the challenges associated with the treatment of liquid organic wastes and the process developments which have allowed a wide range of materials to be successfully treated. (authors)« less

Detection of uranium using laser-induced breakdown spectroscopy.

PubMed

Chinni, Rosemarie C; Cremers, David A; Radziemski, Leon J; Bostian, Melissa; Navarro-Northrup, Claudia

2009-11-01

The goal of this work is a detailed study of uranium detection by laser-induced breakdown spectroscopy (LIBS) for application to activities associated with environmental surveillance and detecting weapons of mass destruction (WMD). The study was used to assist development of LIBS instruments for standoff detection of bulk radiological and nuclear materials and these materials distributed as contaminants on surfaces. Uranium spectra were analyzed under a variety of different conditions at room pressure, reduced pressures, and in an argon atmosphere. All spectra displayed a high apparent background due to the high density of uranium lines. Time decay curves of selected uranium lines were monitored and compared to other elements in an attempt to maximize detection capabilities for each species in the complicated uranium spectrum. A survey of the LIBS uranium spectra was conducted and relative emission line strengths were determined over the range of 260 to 800 nm. These spectra provide a guide for selection of the strongest LIBS analytical lines for uranium detection in different spectral regions. A detection limit for uranium in soil of 0.26% w/w was obtained at close range and 0.5% w/w was achieved at a distance of 30 m. Surface detection limits were substrate dependent and ranged from 13 to 150 microg/cm2. Double-pulse experiments (both collinear and orthogonal arrangements) were shown to enhance the uranium signal in some cases. Based on the results of this work, a short critique is given of the applicability of LIBS for the detection of uranium residues on surfaces for environmental monitoring and WMD surveillance.

Following the electroreduction of uranium dioxide to uranium in LiCl-KCl eutectic in situ using synchrotron radiation

NASA Astrophysics Data System (ADS)

Brown, L. D.; Abdulaziz, R.; Jervis, R.; Bharath, V. J.; Atwood, R. C.; Reinhard, C.; Connor, L. D.; Simons, S. J. R.; Inman, D.; Brett, D. J. L.; Shearing, P. R.

2015-09-01

The electrochemical reduction of uranium dioxide to metallic uranium has been investigated in lithium chloride-potassium chloride eutectic molten salt. Laboratory based electrochemical studies have been coupled with in situ energy dispersive X-ray diffraction, for the first time, to deduce the reduction pathway. No intermediate phases were identified using the X-ray diffraction before, during or after electroreduction to form α-uranium. This suggests that the electrochemical reduction occurs via a single, 4-electron-step, process. The rate of formation of α-uranium is seen to decrease during electrolysis and could be a result of a build-up of oxygen anions in the molten salt. Slow transport of O2- ions away from the UO2 working electrode could impede the electrochemical reduction.

Immobilization of uranium in biofilm microorganisms exposed to groundwater seeps over granitic rock tunnel walls in Olkiluoto, Finland

NASA Astrophysics Data System (ADS)

Krawczyk-Bärsch, Evelyn; Lünsdorf, Heinrich; Pedersen, Karsten; Arnold, Thuro; Bok, Frank; Steudtner, Robin; Lehtinen, Anne; Brendler, Vinzenz

2012-11-01

In an underground rock characterization facility, the ONKALO tunnel in Finland, massive 5-10-mm thick biofilms were observed attached to tunnel walls where groundwater was seeping from bedrock fractures at a depth of 70 m. In laboratory experiments performed in a flow cell with detached biofilms to study the effect of uranium on the biofilm, uranium was added to the circulating groundwater (CGW) obtained from the fracture feeding the biofilm. The final uranium concentration in the CGW was adjusted to 4.25 × 10-5 M, in the range expected from a leaking spent nuclear fuel (SNF) canister in a future underground repository. The effects were investigated using microelectrodes to measure pH and Eh, time-resolved laser fluorescence spectroscopy (TRLFS), energy-filtered transmission electron microscopy (EF-TEM), and electron energy-loss spectroscopy (EELS) studies and thermodynamic calculations were utilized as well. The results indicated that the studied biofilms constituted their own microenvironments, which differed significantly from that of the CGW. A pH of 5.37 was recorded inside the biofilm, approximately 3.5 units lower than the pH observed in the CGW, due to sulfide oxidation to sulfuric acid in the biofilm. Similarly, the Eh of +73 mV inside the biofilm was approximately 420 mV lower than the Eh measured in the CGW. Adding uranium increased the pH in the biofilm to 7.27 and reduced the Eh to -164 mV. The changes of Eh and pH influenced the bioavailability of uranium, since microbial metabolic processes are sensitive to metals and their speciation. EF-TEM investigations indicated that uranium in the biofilm was immobilized intracellularly in microorganisms by the formation of metabolically mediated uranyl phosphate, similar to needle-shaped autunite (Ca[UO2]2[PO4]2·2-6H2O) or meta-autunite (Ca[UO2]2[PO4]2·10-12H2O). In contrast, TRLFS studies of the contaminated CGW identified aqueous uranium carbonate species, likely (Ca2UO2[CO3]3), formed due to the high concentration of carbonate in the CGW. The results agreed with thermodynamic calculations of the theoretically predominant field of uranium species, formed in the uranium-contaminated CGW at the measured geochemical parameters. This investigation clearly demonstrated that biological systems must be considered as a part of natural systems that can significantly influence radionuclide behavior. The results improve our understanding of the mechanisms of biofilm response to radionuclides in relation to safety assessments of SNF repositories.

Iron mineralogy and uranium-binding environment in the rhizosphere of a wetland soil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaplan, Daniel I.; Kukkadapu, Ravi; Seaman, John C.

Wetlands mitigate the migration of groundwater contaminants through the creation of biogeochemical gradients that enhance multiple contaminant-binding processes. Our hypothesis was that wetland plants not only contribute organic carbon, produce strong redox gradients, and elevate microbial populations to soils, but together these conditions also promote the formation of Fe (oxyhydr)oxides within the plant rhizosphere that may also contribute to contaminant immobilization. Mineralogy and U binding environments of the rhizosphere (plant-impacted soil zone) were evaluated in samples collected from contaminated and non-contaminated areas of a wetland on the Savannah River Site in South Carolina. Based on Mossbauer spectroscopy, rhizosphere soil collectedmore » from the field study site was greatly enriched with poorly crystalline nanoparticulate Fe-oxide/ferrihydrite-like materials and nano-goethite (<15-nm). X-ray computed tomography or various microscopy techniques showed that root plaques, tens-of microns thick, were consisted of highly oriented nanoparticles in an orientation suggestive that the roots were involved in the Fe-nanoparticle formation. Because of detection limits, SEM/EDS could not confirm whether U was enriched in the rhizosphere but did demonstrate that U was enriched on root plaques. Uranium in the plaques was always found in association with P and frequently with Fe. Together these findings suggest that plants may not only alter soil microbial and chemical conditions, but also mineralogical conditions that may be conducive to aqueous contaminant immobilization in wetlands.« less

Effects of organic carbon supply rates on uranium mobility in a previously bioreduced contaminated sediment.

PubMed

Wan, Jiamin; Tokunaga, Tetsu K; Kim, Yongman; Brodie, Eoin; Daly, Rebecca; Hazen, Terry C; Firestone, Mary K

2008-10-15

Bioreduction-based strategies for remediating uranium (U)-contaminated sediments face the challenge of maintaining the reduced status of U for long times. Because groundwater influxes continuously bring in oxidizing terminal electron acceptors (O2, NO3(-)), it is necessary to continue supplying organic carbon (OC) to maintain the reducing environment after U bioreduction is achieved. We tested the influence of OC supply rates on mobility of previously microbial reduced uranium U(IV) in contaminated sediments. We found that high degrees of U mobilization occurred when OC supply rates were high, and when the sediment still contained abundant Fe(III). Although 900 days with low levels of OC supply minimized U mobilization, the sediment redox potential increased with time as did extractable U(VI) fractions. Molecular analyses of total microbial activity demonstrated a positive correlation with OC supply and analyses of Geobacteraceae activity (RT-qPCR of 16S rRNA) indicated continued activity even when the effluent Fe(II) became undetectable. These data support our hypothesis on the mechanisms responsible for remobilization of U under reducing conditions; that microbial respiration caused increased (bi)carbonate concentration and formation of stable uranyl carbonate complexes, thereby shifted U(IV)/U(VI) equilibrium to more reducing potentials. The data also suggested that low OC concentrations could not sustain the reducing condition of the sediment for much longer time. Bioreduced U(IV) is not sustainable in an oxidizing environment for a very long time.

Weathering and evaporation controls on dissolved uranium concentrations in groundwater - A case study from northern Burundi.

PubMed

Post, V E A; Vassolo, S I; Tiberghien, C; Baranyikwa, D; Miburo, D

2017-12-31

The potential use of groundwater for potable water supply can be severely compromised by natural contaminants such as uranium. The environmental mobility of uranium depends on a suite of factors including aquifer lithology, redox conditions, complexing agents, and hydrological processes. Uranium concentrations of up to 734μg/L are found in groundwater in northern Burundi, and the objective of the present study was to identify the causes for these elevated concentrations. Based on a comprehensive data set of groundwater chemistry, geology, and hydrological measurements, it was found that the highest dissolved uranium concentrations in groundwater occur near the shores of Lake Tshohoha South and other smaller lakes nearby. A model is proposed in which weathering and evapotranspiration during groundwater recharge, flow and discharge exert the dominant controls on the groundwater chemical composition. Results of PHREEQC simulations quantitatively confirm this conceptual model and show that uranium mobilization followed by evapo-concentration is the most likely explanation for the high dissolved uranium concentrations observed. The uranium source is the granitic sand, which was found to have a mean elemental uranium content of 14ppm, but the exact mobilization process could not be established. Uranium concentrations may further be controlled by adsorption, especially where calcium-uranyl‑carbonate complexes are present. Water and uranium mass balance calculations for Lake Tshohoha South are consistent with the inferred fluxes and show that high‑uranium groundwater represents only a minor fraction of the overall water input to the lake. These findings highlight that the evaporation effects that cause radionuclide concentrations to rise to harmful levels in groundwater discharge areas are not only confined to arid regions, and that this should be considered when selecting suitable locations for water supply wells. Copyright © 2017 Elsevier B.V. All rights reserved.

Floquet Topological Insulators in Uranium Compounds

NASA Astrophysics Data System (ADS)

Pi, Shu-Ting; Savrasov, Sergey

2014-03-01

A major issue regarding the Uranium based nuclear fuels is to conduct the heat from the core area to its outer area. Unfortunately, those materials are notorious for their extremely low thermal conductivity due to the phonon-dominated-heat-transport properties in insulating states. Although metallic Uranium compounds are helpful in increasing the thermal conductivity, their low melting point still make those efforts in vain. In this report, we will figure out potential Uranium based Floquet topological insulators where the insulating bulk states accompanied with metallic surface states is achieved by applying periodic electrical fields which makes the coexistence of both benefits possible.

The effect of uranium on bacterial viability and cell surface morphology using atomic force microscopy in the presence of bicarbonate ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sepulveda-Medina, Paola; Katsenovich, Yelena; Musaramthota, Vishal

Nuclear production facilities during the Cold War have caused liquid waste to leak and soak into the ground creating multiple radionuclide plumes. The Arthrobacter bacteria are one of the most common groups in soils and are found in large numbers in subsurface environments contaminated with radionuclides. This study experimentally analyzed changes on the bacteria surface after uranium exposure and evaluated the effect of bicarbonate ions on U(VI) toxicity of a less uranium tolerant Arthrobacter strain, G968, by investigating changes in adhesion forces and cells dimensions via atomic force microscopy (AFM). AFM and viability studies showed that samples containing bicarbonate aremore » able to acclimate and withstand uranium toxicity. Samples containing no bicarbonate exhibited deformed surfaces and a low height profile, which might be an indication that the cells are not alive.« less

Testing of uranium nitride fuel in T-111 cladding at 1200 K cladding temperature

NASA Technical Reports Server (NTRS)

Rohal, R. G.; Tambling, T. N.; Smith, R. L.

1973-01-01

Two groups of six fuel pins each were assembled, encapsulated, and irradiated in the Plum Brook Reactor. The fuel pins employed uranium mononitride (UN) in a tantalum alloy clad. The first group of fuel pins was irradiated for 1500 hours to a maximum burnup of 0.7-atom-percent uranium. The second group of fuel pins was irradiated for about 3000 hours to a maximum burnup of 1.0-atom-percent uranium. The average clad surface temperature during irradiation of both groups of fuel pins was approximately 1200 K. The postirradiation examination revealed the following: no clad failures or fuel swelling occurred; less than 1 percent of the fission gases escaped from the fuel; and the clad of the first group of fuel pins experienced clad embrittlement whereas the second group, which had modified assembly and fabrication procedures to minimize contamination, had a ductile clad after irradiation.

Natural Bacterial Communities Serve as Quantitative Geochemical Biosensors

PubMed Central

Smith, Mark B.; Rocha, Andrea M.; Smillie, Chris S.; Olesen, Scott W.; Paradis, Charles; Wu, Liyou; Campbell, James H.; Fortney, Julian L.; Mehlhorn, Tonia L.; Lowe, Kenneth A.; Earles, Jennifer E.; Phillips, Jana; Joyner, Dominique C.; Elias, Dwayne A.; Bailey, Kathryn L.; Hurt, Richard A.; Preheim, Sarah P.; Sanders, Matthew C.; Yang, Joy; Mueller, Marcella A.; Brooks, Scott; Watson, David B.; Zhang, Ping; He, Zhili; Dubinsky, Eric A.; Adams, Paul D.; Arkin, Adam P.; Fields, Matthew W.; Zhou, Jizhong; Alm, Eric J.

2015-01-01

ABSTRACT Biological sensors can be engineered to measure a wide range of environmental conditions. Here we show that statistical analysis of DNA from natural microbial communities can be used to accurately identify environmental contaminants, including uranium and nitrate at a nuclear waste site. In addition to contamination, sequence data from the 16S rRNA gene alone can quantitatively predict a rich catalogue of 26 geochemical features collected from 93 wells with highly differing geochemistry characteristics. We extend this approach to identify sites contaminated with hydrocarbons from the Deepwater Horizon oil spill, finding that altered bacterial communities encode a memory of prior contamination, even after the contaminants themselves have been fully degraded. We show that the bacterial strains that are most useful for detecting oil and uranium are known to interact with these substrates, indicating that this statistical approach uncovers ecologically meaningful interactions consistent with previous experimental observations. Future efforts should focus on evaluating the geographical generalizability of these associations. Taken as a whole, these results indicate that ubiquitous, natural bacterial communities can be used as in situ environmental sensors that respond to and capture perturbations caused by human impacts. These in situ biosensors rely on environmental selection rather than directed engineering, and so this approach could be rapidly deployed and scaled as sequencing technology continues to become faster, simpler, and less expensive. PMID:25968645

Arsenic speciation and uranium concentrations in drinking water supply wells in Northern Greece: correlations with redox indicative parameters and implications for groundwater treatment.

PubMed

Katsoyiannis, Ioannis A; Hug, Stephan J; Ammann, Adrian; Zikoudi, Antonia; Hatziliontos, Christodoulos

2007-09-20

The cities in the Aksios and Kalikratia areas in Northern Greece rely on arsenic contaminated groundwater for their municipal water supply. As remedial action strongly depends on arsenic speciation, the presence of other possible contaminants, and on the general water composition, a detailed study with samples from 21 representative locations was undertaken. Arsenic concentrations were typically 10-70 microg/L. In the groundwaters of the Aksios area with lower Eh values (87-172 mV), pH 7.5-8.2 and 4-6 mM HCO(3) alkalinity, As(III) predominated. Manganese concentrations were mostly above the EC standard of 0.05 mg/L (0.1-0.7 mg/L). In groundwaters of the Kalikratia area with higher Eh values (272-352 mV), pH 6.7-7.5 and 6-12 mM HCO(3) alkalinity, As(V) was the main species. Uranium in the groundwaters was also investigated and correlations with total arsenic concentrations and speciation were examined to understand more of the redox chemistry of the examined groundwaters. Uranium concentrations were in the range 0.01-10 microg/L, with the higher concentrations to occur in the oxidizing groundwaters of the Kalikratia area. Uranium and total arsenic concentrations showed no correlation, whereas uranium concentrations correlated strongly with As(III)/As(tot) ratios, depicting their use as a possible indicator of groundwater redox conditions. Finally, boron was found to exceed the EC drinking water standard of 1 mg/L in some wells in the Kalikratia area and its removal should also be considered in the design of a remedial action.

Effects of dietary uranium on reproductive endpoints--fecundity, survival, reproductive success--of the fish Danio rerio.

PubMed

Simon, Olivier; Mottin, Elmina; Geffroy, Benjamin; Hinton, Thomas

2011-01-01

Exposure to metal-contaminated water has been shown to result in a number of reproductive abnormalities in adult and larvae fish, such as failure of oocyte maturation and teratogenic effects. Recently, dietary uptake of metals by fish has been recognized as a critical route of exposure, however, the mechanisms of metal uptake and toxicity are poorly understood and in need of further investigation. The objectives of the present study are to quantify uranium (U dietary transfers from spiked artificial diets) in Danio rerio tissues and embryos, as well as establish its effect on reproduction and embryonic development. Uranium's environmental prominence is currently increasing because of new mining and milling activities. Uranium concentrations range from 0.02 µg/L in natural waters to 2 mg/L. The focus of this study was to examine the trophic transfer and effects of U following exposure modalities (dose, exposure duration 1 to 20 d). Two different isotopes were used to distinguish between chemical and radioactivity toxicity of U. Results showed that U trophic transfer was low (0.52%). Uranium tissue distributions showed that accumulation occurred in digestive organs (liver, digestive tract) following dietary exposure. High levels of U were measured in the gonads (female in particular, >20% of relative burden). High U accumulation levels in eggs indicated maternal transfer of the contaminant. Moreover, U trophic exposure led to a reduction in reproduction success as a function of U accumulated levels. High U exposure conditions strongly reduced the total number of eggs (50%) and their viability at 10 d (reduction of the clutch number, low quality of eggs). © 2010 SETAC.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dam, William; Campbell, Sam; Johnson, Ray

Milling activities at a former uranium mill site near Riverton, Wyoming, USA, contaminated the shallow groundwater beneath and downgradient of the site. Although the mill operated for <6 years (1958-1963), its impact remains an environmental liability. Groundwater modeling predicted that contaminant concentrations were declining steadily, which confirmed the conceptual site model (CSM). However, local flooding in 2010 mobilized contaminants that migrated downgradient from the Riverton site and resulted in a dramatic increase in groundwater contaminant concentrations. This observation indicated that the original CSM was inadequate to explain site conditions and needed to be refined. In response to the new observationsmore » after the flood, a collaborative investigation to better understand site conditions and processes commenced. This investigation included installing 103 boreholes to collect soil and groundwater samples, sampling and analysis of evaporite minerals along the bank of the Little Wind River, an analysis of evaportranspiration in the shallow aquifer, and sampling naturally organic-rich sediments near groundwater discharge areas. The enhanced characterization revealed that the existing CSM did not account for high uranium concentrations in groundwater remaining on the former mill site and groundwater plume stagnation near the Little Wind River. Observations from the flood and subsequent investigations indicate that additional characterization is still needed to continue refining the CSM and determine the viability of the natural flushing compliance strategy. Additional sampling, analysis, and testing of soil and groundwater are necessary to investigate secondary contaminant sources, mobilization of contaminants during floods, geochemical processes, contaminant plume stagnation, distribution of evaporite minerals and organic-rich sediments, and mechanisms and rates of contaminant transfer from soil to groundwater. Future data collection will be used to continually revise the CSM and evaluate the compliance strategy at the site.« less

Column Testing and 1D Reactive Transport Modeling to Evaluate Uranium Plume Persistence Processes

NASA Astrophysics Data System (ADS)

Johnson, R. H.; Morrison, S.; Morris, S.; Tigar, A.; Dam, W. L.; Dayvault, J.

2015-12-01

At many U.S. Department of Energy Office of Legacy Management sites, 100 year natural flushing was selected as a remedial option for groundwater uranium plumes. However, current data indicate that natural flushing is not occurring as quickly as expected and solid-phase and aqueous uranium concentrations are persistent. At the Grand Junction, Colorado office site, column testing was completed on core collected below an area where uranium mill tailings have been removed. The total uranium concentration in this core was 13.2 mg/kg and the column was flushed with laboratory-created water with no uranium and chemistry similar to the nearby Gunnison River. The core was flushed for a total of 91 pore volumes producing a maximum effluent uranium concentration of 6,110 μg/L at 2.1 pore volumes and a minimum uranium concentration of 36.2 μg/L at the final pore volume. These results indicate complex geochemical reactions at small pore volumes and a long tailing affect at greater pore volumes. Stop flow data indicate the occurrence of non-equilibrium processes that create uranium concentration rebound. These data confirm the potential for plume persistence, which is occurring at the field scale. 1D reactive transport modeling was completed using PHREEQC (geochemical model) and calibrated to the column test data manually and using PEST (inverse modeling calibration routine). Processes of sorption, dual porosity with diffusion, mineral dissolution, dispersion, and cation exchange were evaluated separately and in combination. The calibration results indicate that sorption and dual porosity are major processes in explaining the column test data. These processes are also supported by fission track photographs that show solid-phase uranium residing in less mobile pore spaces. These procedures provide valuable information on plume persistence and secondary source processes that may be used to better inform and evaluate remedial strategies, including natural flushing.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Law, A.G.; Serkowski, J.A.; Schatz, A.L.

The Separations Area ground-water monitoring network consisted of 137 wells. Samples from wells in the monitoring network were collected on a monthly, quarterly, or semiannual schedule, depending on the history of the liquid waste disposal site. Samples were analyzed selectively for total alpha, total beta, tritium, /sup 90/Sr, /sup 137/Cs, /sup 60/Co, /sup 106/Ru, total uranium and nitrate. Average concentrations of contaminants in most wells were essentially the same in 1986 as in 1985. The DCG for tritium was exceeded at two PUREX cribs. The ACL specified for /sup 90/Sr was exceeded in three wells near the 216-A-25 Pond. Disposalmore » of effluents to the pond decreased as the main pond was reduced in width to a ditch leading the overflow pond. The ACL guidelines for uranium were exceeded although concentrations were below the DCG; the source of this uranium is probably the inactive 216-B-12 crib. Uranium concentrations above the ACL but below the DCG were also observed at the 216-U-14 ditch and the source is under evaluation. The inactive 216-B-5 reverse well exceeded the DCG for /sup 90/Sr and the ACL for /sup 137/Cs and uranium. Inactive facilities exceeding Rockwell guidelines were the 216-S-1/2 cribs, 216-U-1/2 cribs, the 216-U-10 pond, and the 216-U-6 crib. The 216-S-1/2 cribs have historically had high /sup 137/Cs concentrations because of localized contamination but are below the DCG. Uranium concentrations, which are above the DCG, have stabilized at the 216-U-1/2 cribs after the remedial pumping and uranium removal conducted in 1985. Possible additional action is currently being evaluated. Disposal of the effluent from the ion exchange column to the 216-S-25 crib resulted in ground-water concentrations that exceeded Rockwell guidelines but below the DCG. Ground water near the 216-U-10 pond remains elevated but below the DCG due to past disposal to the pond, which was deactivated in 1984. 23 refs., 25 figs., 26 tabs.« less

A Multifaceted Sampling Approach to Better Understanding Biogeochemical and Hydrogeological Controls on Uranium Mobility at a Former Uranium Mill Tailings Site in Riverton, Wyoming

NASA Astrophysics Data System (ADS)

Dam, W. L.; Johnson, R. H.; Campbell, S.; Bone, S. E.; Noel, V.; Bargar, J.

2015-12-01

Understanding uranium mobility in subsurface environments is not trivial. Obtaining sufficient data to accurately represent soil and aquifer characteristics can require unique approaches that evolve with added site knowledge. At Riverton, the primary source of uranium mill tailings remaining from ore processing was removed but contaminant plumes have persisted longer than predicted by groundwater modeling. What are the primary mechanisms controlling plume persistence? DOE is conducting new characterization studies to assist our understanding of underlying biogeochemical and hydrogeological mechanisms affecting secondary sources. A variety of field sampling techniques are being sequentially employed including augering, trenching, pore water sampling, and installing multi-level wells. In August 2012, vadose zone soil samples from 34 locations and groundwater from 103 boreholes were collected with Geoprobe ® direct push rods. Lower than expected uranium concentrations in composited shallow soils indicated the need for more focused and deeper samples. In May 2014, soil samples containing evaporites were collected along the bank of the Little Wind River; elevated uranium concentrations in evaporite minerals correlated with plume configurations and reflect contaminated groundwater discharge at the river. In September 2014, hand anger samples collected by the river and oxbow lake also indicated the presence of organic rich zones containing elevated uranium (>50 mg/kg). Subsequent samples collected from five backhoe trenches in May 2015 revealed a highly heterogeneous vadose zone composed of clay, silt, sand and cobbles containing evaporites and organic rich zones which may interact with groundwater plumes.Plans for August 2015 include sonic drilling to obtain continuous cores from the surface down to the base of the surficial aquifer with multi-level monitoring wells constructed in each borehole to assess vertical variation in groundwater chemistry. Temporary well-points will be installed adjacent to the river to assess geochemical and flow controls in the area of plume stagnation. Analyses include critical element speciation (C, S, Fe, and U), microbes, isotopes, diffusivity and flow characteristics. These activities support a dramatically improved understanding of plume persistence.

Modern Chemistry Techniques Applied to Metal Behavior and Chelation in Medical and Environmental Systems ? Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sutton, M; Andresen, B; Burastero, S R

2005-02-03

This report details the research and findings generated over the course of a 3-year research project funded by Lawrence Livermore National Laboratory (LLNL) Laboratory Directed Research and Development (LDRD). Originally tasked with studying beryllium chemistry and chelation for the treatment of Chronic Beryllium Disease and environmental remediation of beryllium-contaminated environments, this work has yielded results in beryllium and uranium solubility and speciation associated with toxicology; specific and effective chelation agents for beryllium, capable of lowering beryllium tissue burden and increasing urinary excretion in mice, and dissolution of beryllium contamination at LLNL Site 300; {sup 9}Be NMR studies previously unstudied atmore » LLNL; secondary ionization mass spec (SIMS) imaging of beryllium in spleen and lung tissue; beryllium interactions with aerogel/GAC material for environmental cleanup. The results show that chelator development using modern chemical techniques such as chemical thermodynamic modeling, was successful in identifying and utilizing tried and tested beryllium chelators for use in medical and environmental scenarios. Additionally, a study of uranium speciation in simulated biological fluids identified uranium species present in urine, gastric juice, pancreatic fluid, airway surface fluid, simulated lung fluid, bile, saliva, plasma, interstitial fluid and intracellular fluid.« less

PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER

DOEpatents

King, E.L.

1959-04-28

The separation and purification of plutonium from the radioactive elements of lower atomic weight is described. The process of this invention comprises forming a 0.5 to 2 M aqueous acidffc solution containing plutonium fons in the tetravalent state and elements with which it is normally contaminated in neutron irradiated uranium, treating the solution with a double thorium compound and a soluble pyrophosphate compound (Na/sub 4/P/sub 2/O/sub 7/) whereby a carrier precipitate of thorium A method is presented of reducing neptunium and - trite is advantageous since it destroys any hydrazine f so that they can be removed from solutions in which they are contained is described. In the carrier precipitation process for the separation of plutonium from uranium and fission products including zirconium and columbium, the precipitated blsmuth phosphate carries some zirconium, columbium, and uranium impurities. According to the invention such impurities can be complexed and removed by dissolving the contaminated carrier precipitate in 10M nitric acid, followed by addition of fluosilicic acid to about 1M, diluting the solution to about 1M in nitric acid, and then adding phosphoric acid to re-precipitate bismuth phosphate carrying plutonium.

Nuclear facility decommissioning and site remedial actions: A selected bibliography, Volume 13: Part 1, Main text

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goins, L.F.; Webb, J.R.; Cravens, C.D.

1992-09-01

This publication contains 1035 abstracted references on environmental restoration, nuclear facility decommissioning, uranium mill tailings management, and site remedial actions. These citations constitute the thirteenth in a series of reports prepared annually for the US Department of Energy (DOE) Environmental Restoration programs. Citations to foreign and domestic literature of all types. There are 13 major sections of the publication, including: (1) DOE Decontamination and Decommissioning Program; (2) Nuclear Facilities Decommissioning; (3) DOE Formerly Utilized Sites Remedial Action Program; (4) DOE Uranium Mill Tailings Remedial Action Project; (5) Uranium Mill Tailings Management; (6) DOE Environmental Restoration Program; (7) DOE Site-Specific Remedialmore » Actions; (8) Contaminated Site Restoration; (9) Remediation of Contaminated Soil and Groundwater; (10) Environmental Data Measurements, Management, and Evaluation; (11) Remedial Action Assessment and Decision-Making; (12) Technology Development and Evaluation; and (13) Environmental and Waste Management Issues. Bibliographic references are arranged in nine subject categories by geographic location and then alphabetically by first author, corporate affiliation, or publication title. Indexes are provided for author, corporate affiliation, title word, publication description, geographic location, subject category, and key word.« less

Environmental proteomics reveals early microbial community responses to biostimulation at a uranium- and nitrate-contaminated site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chourey, Karuna; Nissen, Silke; Vishnivetskaya, T.

2013-01-01

High performance mass spectrometry instrumentation coupled with improved protein extraction techniques enable metaproteomics to identify active members of soil and groundwater microbial communities. Metaproteomics workflows were applied to study the initial responses (i.e., 4 days post treatment) of the indigenous aquifer microbiota to biostimulation with emulsified vegetable oil (EVO) at a uranium-contaminated site. Members of the Betaproteobacteria (i.e., Dechloromonas, Ralstonia, Rhodoferax, Polaromonas, Delftia, Chromobacterium) and Firmicutes dominated the biostimulated aquifer community. Proteome characterization revealed distinct differences in protein expression between the microbial biomass collected from groundwater influenced by biostimulation and groundwater collected up-gradient of the EVO injection points. In particular,more » proteins involved in ammonium assimilation, EVO degradation, and polyhydroxybutyrate (PHB) granule formation were prominent following biostimulation. Interestingly, the atypical NosZ of a Dechloromonas sp. was highly expressed suggesting active nitrous oxide (N2O) respiration. c-type cytochromes were barely detected, as was citrate synthase, a biomarker for hexavalent uranium reduction activity, suggesting that metal reduction has not commenced 4 days post EVO delivery. Environmental metaproteomics identified microbial community responses to biostimulation and elucidated active pathways demonstrating the value of this technique for complementing nucleic acid-based approaches.« less

Unexpected Lack of Deleterious Effects of Uranium on Physiological Systems following a Chronic Oral Intake in Adult Rat

PubMed Central

Dublineau, Isabelle; Souidi, Maâmar; Gueguen, Yann; Lestaevel, Philippe; Bertho, Jean-Marc; Manens, Line; Delissen, Olivia; Grison, Stéphane; Paulard, Anaïs; Monin, Audrey; Kern, Yseult; Rouas, Caroline; Loyen, Jeanne; Gourmelon, Patrick; Aigueperse, Jocelyne

2014-01-01

Uranium level in drinking water is usually in the range of microgram-per-liter, but this value may be as much as 100 to 1000 times higher in some areas, which may raise question about the health consequences for human populations living in these areas. Our purpose was to improve knowledge of chemical effects of uranium following chronic ingestion. Experiments were performed on rats contaminated for 9 months via drinking water containing depleted uranium (0.2, 2, 5, 10, 20, 40, or 120 mg/L). Blood biochemical and hematological indicators were measured and several different types of investigations (molecular, functional, and structural) were conducted in organs (intestine, liver, kidneys, hematopoietic cells, and brain). The specific sensitivity of the organs to uranium was deduced from nondeleterious biological effects, with the following thresholds (in mg/L): 0.2 for brain, >2 for liver, >10 for kidneys, and >20 for intestine, indicating a NOAEL (No-Observed-Adverse-Effect Level) threshold for uranium superior to 120 m g/L. Based on the chemical uranium toxicity, the tolerable daily intake calculation yields a guideline value for humans of 1350 μg/L. This value was higher than the WHO value of 30 μg/L, indicating that this WHO guideline for uranium content in drinking water is very protective and might be reconsidered. PMID:24693537

Unexpected lack of deleterious effects of uranium on physiological systems following a chronic oral intake in adult rat.

PubMed

Dublineau, Isabelle; Souidi, Maâmar; Gueguen, Yann; Lestaevel, Philippe; Bertho, Jean-Marc; Manens, Line; Delissen, Olivia; Grison, Stéphane; Paulard, Anaïs; Monin, Audrey; Kern, Yseult; Rouas, Caroline; Loyen, Jeanne; Gourmelon, Patrick; Aigueperse, Jocelyne

2014-01-01

Uranium level in drinking water is usually in the range of microgram-per-liter, but this value may be as much as 100 to 1000 times higher in some areas, which may raise question about the health consequences for human populations living in these areas. Our purpose was to improve knowledge of chemical effects of uranium following chronic ingestion. Experiments were performed on rats contaminated for 9 months via drinking water containing depleted uranium (0.2, 2, 5, 10, 20, 40, or 120 mg/L). Blood biochemical and hematological indicators were measured and several different types of investigations (molecular, functional, and structural) were conducted in organs (intestine, liver, kidneys, hematopoietic cells, and brain). The specific sensitivity of the organs to uranium was deduced from nondeleterious biological effects, with the following thresholds (in mg/L): 0.2 for brain, >2 for liver, >10 for kidneys, and >20 for intestine, indicating a NOAEL (No-Observed-Adverse-Effect Level) threshold for uranium superior to 120 m g/L. Based on the chemical uranium toxicity, the tolerable daily intake calculation yields a guideline value for humans of 1350 μg/L. This value was higher than the WHO value of 30 μg/L, indicating that this WHO guideline for uranium content in drinking water is very protective and might be reconsidered.

Bioreduction and immobilization of uranium in situ: a case study at a USA Department of Energy radioactive waste site, Oak Ridge, Tennessee

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Weimin; Carley, Jack M; Watson, David B

Bioremediation of uranium contaminated groundwater was tested by delivery of ethanol as an electron donor source to stimulate indigenous microbial bioactivity for reduction and immobilization of uranium in situ, followed by tests of stability of uranium sequestration in the bioreduced area via delivery of dissolved oxygen or nitrate at the US Department of energy's Integrated Field Research Challenge site located at Oak Ridge, Tennessee, USA. After long term treatment that spanned years, uranium in groundwater was reduced from 40-60 mg {center_dot} L{sup -1} to <0.03 mg {center_dot} L{sup -1}, below the USA EPA standard for drinking water. The bioreduced uraniummore » was stable under anaerobic or anoxic conditions, but addition of DO and nitrate to the bioreduced zone caused U remobilization. The change in the microbial community and functional microorganisms related to uranium reduction and oxidation were characterized. The delivery of ethanol as electron donor stimulated the activities of indigenous microorganisms for reduction of U(VI) to U(IV). Results indicated that the immobilized U could be partially remobilized by D0 and nitrate via microbial activity. An anoxic environmental condition without nitrate is essential to maintain the stability of bioreduced uranium.« less

Summary of ground-water quality impacts of uranium mining and milling in the Grants mineral belt, New Mexico. Technical note (final)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaufmann, R.F.; Eadie, G.G.; Russell, C.R.

Ground-water contamination from uranium mining and milling results from the infiltration of radium-bearing mine, mill, and ion-exchange plant effluents. Radium, selenium, and nitrate were of most value as indicators of contamination. In recent years, mining has increased radium in mine effluents from several picocuries/liter (pCi/1) or less, to 100-150 pCi/1. The shallow aquifer in use in the vicinity of one mill was grossly contaminated with selenium, attributable to the mill tailings. Seepage from two other mill tailings ponds averaged 67,400,000 liters/year and, to date, has contributed an estimated 1.1 curies of radium to ground water. At one of these, anmore » injection well was used to dispose of over 3,400,000,000 liters of waste from 1960-1973. The wastes have not been properly monitored and have apparently migrated to more shallow, potable aquifers. No adverse impacts on municipal water quality in Paguate, Bluewater, Grants, Milan, and Gallup were observed. (GRA)« less

Radiation shielding materials and containers incorporating same

DOEpatents

Mirsky, Steven M.; Krill, Stephen J.; Murray, Alexander P.

2005-11-01

An improved radiation shielding material and storage systems for radioactive materials incorporating the same. The PYRolytic Uranium Compound ("PYRUC") shielding material is preferably formed by heat and/or pressure treatment of a precursor material comprising microspheres of a uranium compound, such as uranium dioxide or uranium carbide, and a suitable binder. The PYRUC shielding material provides improved radiation shielding, thermal characteristic, cost and ease of use in comparison with other shielding materials. The shielding material can be used to form containment systems, container vessels, shielding structures, and containment storage areas, all of which can be used to house radioactive waste. The preferred shielding system is in the form of a container for storage, transportation, and disposal of radioactive waste. In addition, improved methods for preparing uranium dioxide and uranium carbide microspheres for use in the radiation shielding materials are also provided.

Radiation Shielding Materials and Containers Incorporating Same

DOEpatents

Mirsky, Steven M.; Krill, Stephen J.; and Murray, Alexander P.

2005-11-01

An improved radiation shielding material and storage systems for radioactive materials incorporating the same. The PYRolytic Uranium Compound (''PYRUC'') shielding material is preferably formed by heat and/or pressure treatment of a precursor material comprising microspheres of a uranium compound, such as uranium dioxide or uranium carbide, and a suitable binder. The PYRUC shielding material provides improved radiation shielding, thermal characteristic, cost and ease of use in comparison with other shielding materials. The shielding material can be used to form containment systems, container vessels, shielding structures, and containment storage areas, all of which can be used to house radioactive waste. The preferred shielding system is in the form of a container for storage, transportation, and disposal of radioactive waste. In addition, improved methods for preparing uranium dioxide and uranium carbide microspheres for use in the radiation shielding materials are also provided.

U(VI) adsorption on aquifer sediments at the Hanford Site.

PubMed

Um, Wooyong; Serne, R Jeffrey; Brown, Christopher F; Last, George V

2007-08-15

Aquifer sediments collected via split-spoon sampling in two new groundwater wells in the 200-UP-1 operable unit at the Hanford Site were characterized and showed typical Ringold Unit E Formation properties dominated by gravel and sand. High iron-oxide content in Fe oxide/clay coatings caused the highest U(VI) adsorption as quantified by batch K(d) values, indicating iron oxides are the key solid adsorbent in the 200-UP-1 sediments that affect U(VI) fate and mobility. Even though U(VI) adsorption on the gravel-sized fraction of the sediments is considered to be negligible, careful characterization should be conducted to determine U(VI) adsorption on gravel, because of presence of Fe oxides coatings and diffusion-controlled adsorption into the gravel particles' interior surfaces. A linear adsorption isotherm was observed up to 10(-6) M (238 microg/L) of total U(VI) concentration in batch U(VI) adsorption tests with varying total U(VI) concentrations in spiked groundwater. U(VI) adsorption decreased with increasing concentrations of dissolved carbonate, because strong anionic aqueous uranium-carbonate complexes formed at high pH and high alkalinity conditions. Noticeable uranium desorption hysteresis was observed in a flow-through column experiment, suggesting that desorption K(d) values for aged uranium-contaminated sediments at the Hanford Site can be larger than adsorption K(d) values determined in short-term laboratory experiments and slow uranium release from contaminated sediments into the groundwater is expected.

Model-based Analysis of Mixed Uranium(VI) Reduction by Biotic and Abiotic Pathways During in Situ Bioremediation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Jiao; Scheibe, Timothy D.; Mahadevan, Radhakrishnan

2013-10-24

Uranium bioremediation has emerged as a potential strategy of cleanup of radionuclear contamination worldwide. An integrated geochemical & microbial community model is a promising approach to predict and provide insights into the bioremediation of a complicated natural subsurface. In this study, an integrated column-scale model of uranium bioremediation was developed, taking into account long-term interactions between biotic and abiotic processes. It is also combined with a comprehensive thermodynamic analysis to track the fate and cycling of biogenic species. As compared with other bioremediation models, the model increases the resolution of the connection of microbial community to geochemistry and establishes directmore » quantitative correlation between overall community evolution and geochemical variation, thereby accurately predicting the community dynamics under different sedimentary conditions. The thermodynamic analysis examined a recently identified homogeneous reduction of U(VI) by Fe(II) under dynamic sedimentary conditions across time and space. It shows that the biogenic Fe(II) from Geobacter metabolism can be removed rapidly by the biogenic sulphide from sulfate reducer metabolism, hence constituting one of the reasons that make the abiotic U(VI) reduction thermodynamically infeasible in the subsurface. Further analysis indicates that much higher influent concentrations of both Fe(II) and U(VI) than normal are required to for abiotic U(VI) reduction to be thermodynamically feasible, suggesting that the abiotic reduction cannot be an alternative to the biotic reduction in the remediation of uranium contaminated groundwater.« less

Radioactivity in Virgin Soils and Soils from Some Areas with Closed Uranium Mining Facilities in Bulgaria

NASA Astrophysics Data System (ADS)

Yordanova, I.; Staneva, D.; Misheva, L.; Bineva, Ts.; Banov, M.

2012-04-01

The soil radioecology is an important part of the environmental research in the country. Since the beginning of the 1970's regular monitoring of the content of different radionuclides in Bulgarian soils has been done. Objective of the studies were virgin soils from high mountain areas, hills and plains (the region of Kozloduy NPP and the Danube river valley). Natural and men-made radionuclides were observed. In the 25-year period after the the contamination with radionuclides due to the 1986 Chernobyl NPP accident a rich data base has been collected, recording the radiation status of the soils in Bulgaria. Special attention has been paid to the contamination with the long-lived technogenic radionuclides caesium-137 and strontium-90. This paper presents a summary of the obtained results. Caesium-137 and strontium-90 were the main men-made radionuclides detected in the examined Bulgarian soils few years after the Chernobyl NPP accident. Their content in the soils from high mountain areas (Rodopa and Rila mountains) is several times higher than that in the soils from North Bulgaria and Sofia fields. High non-homogenity in the pollution within small areas (even as small as several square meters) has been observed. Natural radioactivity was also studied. Averaged values for natural radionuclides like uranium-238, thorium-232, and radium-226 in virgin soils from different areas in the country are presented. A comparison of the dynamics of their behavior throughout the years is done. Bulgaria is a country with intensive uranium mining activities in the past years. That is why radiological monitoring of closed uranium mining facilities in different regions of the country are obligatory and of great interest. This work presents results from such investigations made in regions where remediation has been done. The results have been evaluated according to the Bulgarian radionuclide environment contamination legislation. The necessity of permanent environmental monitoring is assessed.

Use of electrical imaging and distributed temperature sensing methods to characterize surface water–groundwater exchange regulating uranium transport at the Hanford 300 Area, Washington

USGS Publications Warehouse

Slater, Lee D.; Ntarlagiannis, Dimitrios; Day-Lewis, Frederick D.; Mwakanyamale, Kisa; Versteeg, Roelof J.; Ward, Andy; Strickland, Christopher; Johnson, Carole D.; Lane, John W.

2010-01-01

We explored the use of continuous waterborne electrical imaging (CWEI), in conjunction with fiber‐optic distributed temperature sensor (FO‐DTS) monitoring, to improve the conceptual model for uranium transport within the Columbia River corridor at the Hanford 300 Area, Washington. We first inverted resistivity and induced polarization CWEI data sets for distributions of electrical resistivity and polarizability, from which the spatial complexity of the primary hydrogeologic units was reconstructed. Variations in the depth to the interface between the overlying coarse‐grained, high‐permeability Hanford Formation and the underlying finer‐grained, less permeable Ringold Formation, an important contact that limits vertical migration of contaminants, were resolved along ∼3 km of the river corridor centered on the 300 Area. Polarizability images were translated into lithologic images using established relationships between polarizability and surface area normalized to pore volume (Spor). The FO‐DTS data recorded along 1.5 km of cable with a 1 m spatial resolution and 5 min sampling interval revealed subreaches showing (1) temperature anomalies (relatively warm in winter and cool in summer) and (2) a strong correlation between temperature and river stage (negative in winter and positive in summer), both indicative of reaches of enhanced surface water–groundwater exchange. The FO‐DTS data sets confirm the hydrologic significance of the variability identified in the CWEI and reveal a pattern of highly focused exchange, concentrated at springs where the Hanford Formation is thickest. Our findings illustrate how the combination of CWEI and FO‐DTS technologies can characterize surface water–groundwater exchange in a complex, coupled river‐aquifer system.

River stage influences on uranium transport in a hydrologically dynamic groundwater-surface water transition zone: U TRANSPORT IN A GROUNDWATER-SURFACE WATER TRANSITION ZONE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zachara, John M.; Chen, Xingyuan; Murray, Chris

A tightly spaced well-field within a groundwater uranium (U) plume in the groundwater-surface water transition zone was monitored for a three year period for groundwater elevation and dissolved solutes. The plume discharges to the Columbia River, which displays a dramatic spring stage surge resulting from mountain snowmelt. Groundwater exhibits a low hydrologic gradient and chemical differences with river water. River water intrudes the site in spring. Specific aims were to assess the impacts of river intrusion on dissolved uranium (Uaq), specific conductance (SpC), and other solutes, and to discriminate between transport, geochemical, and source term heterogeneity effects. Time series trendsmore » for Uaq and SpC were complex and displayed large temporal well-to well variability as a result of water table elevation fluctuations, river water intrusion, and changes in groundwater flow directions. The wells were clustered into subsets exhibiting common temporal behaviors resulting from the intrusion dynamics of river water and the location of source terms. Concentration hot spots were observed in groundwater that varied in location with increasing water table elevation. Heuristic reactive transport modeling with PFLOTRAN demonstrated that mobilized U was transported between wells and source terms in complex trajectories, and was diluted as river water entered and exited the groundwater system. While uranium time-series concentration trends varied significantly from year to year as a result of climate-caused differences in the spring hydrograph, common and partly predictable response patterns were observed that were driven by water table elevation, and the extent and duration of the river water intrusion event.« less

Long-term fate of depleted uranium at Aberdeen and Yuma Proving Grounds: Human health and ecological risk assessments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ebinger, M.H.; Beckman, R.J.; Myers, O.B.

1996-09-01

The purpose of this study was to evaluate the immediate and long-term consequences of depleted uranium (DU) in the environment at Aberdeen Proving Ground (APG) and Yuma Proving Ground (YPG) for the Test and Evaluation Command (TECOM) of the US Army. Specifically, we examined the potential for adverse radiological and toxicological effects to humans and ecosystems caused by exposure to DU at both installations. We developed contaminant transport models of aquatic and terrestrial ecosystems at APG and terrestrial ecosystems at YPG to assess potential adverse effects from DU exposure. Sensitivity and uncertainty analyses of the initial models showed the portionsmore » of the models that most influenced predicted DU concentrations, and the results of the sensitivity analyses were fundamental tools in designing field sampling campaigns at both installations. Results of uranium (U) isotope analyses of field samples provided data to evaluate the source of U in the environment and the toxicological and radiological doses to different ecosystem components and to humans. Probabilistic doses were estimated from the field data, and DU was identified in several components of the food chain at APG and YPG. Dose estimates from APG data indicated that U or DU uptake was insufficient to cause adverse toxicological or radiological effects. Dose estimates from YPG data indicated that U or DU uptake is insufficient to cause radiological effects in ecosystem components or in humans, but toxicological effects in small mammals (e.g., kangaroo rats and pocket mice) may occur from U or DU ingestion. The results of this study were used to modify environmental radiation monitoring plans at APG and YPG to ensure collection of adequate data for ongoing ecological and human health risk assessments.« less

Coupling of iron and organic matter under fluctuation redox conditions: implications for carbon turnover, mineral formation, and contaminant transport

NASA Astrophysics Data System (ADS)

Nico, P. S.

2015-12-01

Interactions between naturally occurring organic matter and minerals surfaces play a determining role on the transport, chemical composition, and bio-availability of reduced carbon. These processes are controlled on the molecular scale by mineral dissolution and precipitation dynamics which are in turn controlled by both changing solution chemistry and redox regime. The presentation will highlight recent work by our group and others on elucidating some of these mechanisms with particular emphasis on the impacts of redox cycling and Fe mineral transformation. We are particular interested in how the form of organic matter impacts the formation and transformation of iron minerals and vis-a-versa under fluctuating redox conditions, and how that in turn impacts the transport of other elements controlled by Fe surfaces, e.g. uranium. In two different field conditions, in a ground water well and at a ground water-surface water interface, Fe(II) was oxidized in an organic rich environment leading to different types of Fe-organic matter co-precipitates. We followed the evolution of those participates under a return to reduced conditions in order to understand the transformations, or lack thereof, of the Fe minerals and the fate of the associated organic matter.

Plutonium Particle Migration in the Shallow Vadose Zone: The Nevada Test Site as an Analog Site

NASA Astrophysics Data System (ADS)

Hunt, J. R.; Smith, D. K.

2004-12-01

The upper meter of the vadose zone in desert environments is the horizon where wastes have been released and human exposure is determined through dermal, inhalation, and food uptake pathways. This region is also characterized by numerous coupled processes that determine contaminant transport, including precipitation infiltration, evapotranspiration, daily and annual temperature cycling, dust resuspension, animal burrowing, and geochemical weathering reactions. While there is considerable interest in colloidal transport of minerals, pathogenic organisms, and contaminants in the vadose zone, there are limited field sites where the actual occurrence of contaminant migration can be quantified over the appropriate spatial and temporal scales of interest. At the US Department of Energy Nevada Test Site, there have been numerous releases of radionuclides since the 1950's that have become field-scale tracer tests. One series of tests was the four safety shots conducted in an alluvial valley of Area 11 in the 1950's. These experiments tested the ability of nuclear materials to survive chemical explosions without initiating fission reactions. Four above-ground tests were conducted and they released plutonium and uranium on the desert valley floor with only one of the tests undergoing some fission. Shortly after the tests, the sites were surveyed for radionuclide distribution on the land surface using aerial surveys and with depth. Additional studies were conducted in the 1970's to better understand the fate of plutonium in the desert that included studies of depth distribution and dust resuspension. More recently, plutonium particle distribution in the soil profile was detected using autoradiography. The results to date demonstrate the vertical migration of plutonium particles to depths in excess of 30 cm in this arid vadose zone. While plutonium migration at the Nevada Test Site has been and continues to be a concern, these field experiments have become analog sites for the release of radiological materials potentially important to consequence management investigations. In particular, these 50-year old experiments with long and detailed site investigations under relative undisturbed conditions offer insights into transport pathways that must be represented in simulation models that evaluate responses to radiological dispersal devices (RDDs). A compilation of the available site characterization data suggests additional experimental and modeling programs that can ultimately quantify the fate of contaminant particles released at the soil surface.

Pattern of explosive reaction between uranium hexafluoride and hydrocarbon oils. Revision 1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rapp, K.E.

Examination of uranium hexafluoride release incidents occurring over the past three decades of ORGDP experience has identified only four which apparently involved an explosion of a container resulting from reaction between uranium hexafluoride and an impurity. These four incidents exhibit a certain degree of commonality. Each has involved: (1) condensed phase uranium hexafluoride, (2) a moderately elevated temperature, (3) a sufficient quantity of uranium hexafluoride for a significant partial pressure to be maintained independently above that which can be consumed by chemical reaction, and (4) an organic liquid (probably hydrocarbon oil) accidentally present in the container as a contaminant. Themore » purpose of this investigative search was to establish some conditional pattern for these four incidents to which their violent consequences could be attributed. Fortunately, the number of such incidents is relatively small, which emphasizes even more pointedly the unfortunate fact that documentation ranges from thorough to very limited. Documented sources of information are given in the bibliography. Copies of those which are not readily available are contained in six appendices. 8 refs.« less

Empirical calibration of uranium releases in the terrestrial environment of nuclear fuel cycle facilities.

PubMed

Pourcelot, Laurent; Masson, Olivier; Saey, Lionel; Conil, Sébastien; Boulet, Béatrice; Cariou, Nicolas

2017-05-01

In the present paper the activity of uranium isotopes measured in plants and aerosols taken downwind of the releases of three nuclear fuel settlements was compared between them and with the activity measured at remote sites. An enhancement of 238 U activity as well as 235 U/ 238 U anomalies and 236 U are noticeable in wheat, grass, tree leaves and aerosols taken at the edge of nuclear fuel settlements, which show the influence of uranium chronic releases. Further plants taken at the edge of the studied sites and a few published data acquired in the same experimental conditions show that the 238 U activity in plants is influenced by the intensity of the U atmospheric releases. Assuming that 238 U in plant is proportional to the intensity of the releases, we proposed empirical relationships which allow to characterize the chronic releases on the ground. Other sources of U contamination in plants such as accidental releases and "delayed source" of uranium in soil are also discussed in the light of uranium isotopes signatures. Copyright © 2017 Elsevier Ltd. All rights reserved.

Genetic and grade and tonnage models for sandstone-hosted roll-type uranium deposits, Texas Coastal Plain, USA

USGS Publications Warehouse

Hall, Susan M.; Mihalasky, Mark J.; Tureck, Kathleen; Hammarstrom, Jane M.; Hannon, Mark

2017-01-01

The coincidence of a number of geologic and climatic factors combined to create conditions favorable for the development of mineable concentrations of uranium hosted by Eocene through Pliocene sandstones in the Texas Coastal Plain. Here 254 uranium occurrences, including 169 deposits, 73 prospects, 6 showings and 4 anomalies, have been identified. About 80 million pounds of U3O8 have been produced and about 60 million pounds of identified producible U3O8 remain in place. The development of economic roll-type uranium deposits requires a source, large-scale transport of uranium in groundwater, and deposition in reducing zones within a sedimentary sequence. The weight of the evidence supports a source from thick sequences of volcanic ash and volcaniclastic sediment derived mostly from the Trans-Pecos volcanic field and Sierra Madre Occidental that lie west of the region. The thickest accumulations of source material were deposited and preserved south and west of the San Marcos arch in the Catahoula Formation. By the early Oligocene, a formerly uniformly subtropical climate along the Gulf Coast transitioned to a zoned climate in which the southwestern portion of Texas Coastal Plain was dry, and the eastern portion humid. The more arid climate in the southwestern area supported weathering of volcanic ash source rocks during pedogenesis and early diagenesis, concentration of uranium in groundwater and movement through host sediments. During the middle Tertiary Era, abundant clastic sediments were deposited in thick sequences by bed-load dominated fluvial systems in long-lived channel complexes that provided transmissive conduits favoring transport of uranium-rich groundwater. Groundwater transported uranium through permeable sandstones that were hydrologically connected with source rocks, commonly across formation boundaries driven by isostatic loading and eustatic sea level changes. Uranium roll fronts formed as a result of the interaction of uranium-rich groundwater with either (1) organic-rich debris adjacent to large long-lived fluvial channels and barrier–bar sequences or (2) extrinsic reductants entrained in formation water or discrete gas that migrated into host units via faults and along the flanks of salt domes and shale diapirs. The southwestern portion of the region, the Rio Grande embayment, contains all the necessary factors required for roll-type uranium deposits. However, the eastern portion of the region, the Houston embayment, is challenged by a humid environment and a lack of source rock and transmissive units, which may combine to preclude the deposition of economic deposits. A grade and tonnage model for the Texas Coastal Plain shows that the Texas deposits represent a lower tonnage subset of roll-type deposits that occur around the world, and required aggregation of production centers into deposits based on geologic interpretation for the purpose of conducting a quantitative mineral resource assessment.

Effects of chloride, sulfate and natural organic matter (NOM) on the accumulation and release of trace-level inorganic contaminants from corroding iron.

PubMed

Peng, Ching-Yu; Ferguson, John F; Korshin, Gregory V

2013-09-15

This study examined effects of varying levels of anions (chloride and sulfate) and natural organic matter (NOM) on iron release from and accumulation of inorganic contaminants in corrosion scales formed on iron coupons exposed to drinking water. Changes of concentrations of sulfate and chloride were observed to affect iron release and, in lesser extent, the retention of representative inorganic contaminants (vanadium, chromium, nickel, copper, zinc, arsenic, cadmium, lead and uranium); but, effects of NOM were more pronounced. DOC concentration of 1 mg/L caused iron release to increase, with average soluble and total iron concentrations being four and two times, respectively, higher than those in the absence of NOM. In the presence of NOM, the retention of inorganic contaminants by corrosion scales was reduced. This was especially prominent for lead, vanadium, chromium and copper whose retention by the scales decreased from >80% in the absence of NOM to <30% in its presence. Some of the contaminants, notably copper, chromium, zinc and nickel retained on the surface of iron coupons in the presence of DOC largely retained their mobility and were released readily when ambient water chemistry changed. Vanadium, arsenic, cadmium, lead and uranium retained by the scales were largely unsusceptible to changes of NOM and chloride levels. Modeling indicated that the observed effects were associated with the formation of metal-NOM complexes and effects of NOM on the sorption of the inorganic contaminants on solid phases that are typical for iron corrosion in drinking water. Copyright © 2013 Elsevier Ltd. All rights reserved.

Geobacter Project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Derek Lovley; Maddalena Coppi; Stacy Ciufo

Analysis of the Genetic Potential and Gene Expression of Microbial Communities Involved in the In Situ Bioremediation of Uranium and Harvesting Electrical Energy from Organic Matter The primary goal of this research is to develop conceptual and computational models that can describe the functioning of complex microbial communities involved in microbial processes of interest to the Department of Energy. Microbial Communities to be Investigated: (1) Microbial community associated with the in situ bioremediation of uranium-contaminated groundwater; and (2) Microbial community that is capable of harvesting energy from waste organic matter in the form of electricity.

Small-scale geochemical cycles and the distribution of uranium in central and north Florida organic deposits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bond, P.A.

1993-03-01

The global geochemical cycle for an element tracks its path from its various sources to its sinks via processes of weathering and transportation. The cycle may then be quantified in a necessarily approximate manner. The geochemical cycle (thus quantified) reveals constraints (known and unknown) on an element's behavior imposed by the various processes which act on it. In the context of a global geochemical cycle, a continent becomes essentially a source term. If, however, an element's behavior is examined in a local or regional context, sources and their related sinks may be identified. This suggests that small-scale geochemical cycles maymore » be superimposed on global geochemical cycles. Definition of such sub-cycles may clarify the distribution of an element in the earth's near-surface environment. In Florida, phosphate minerals of the Hawthorn Group act as a widely distributed source of uranium. Uranium is transported by surface- and ground-waters. Florida is the site of extensive wetlands and peatlands. The organic matter associated with these deposits adsorbs uranium and may act as a local sink depending on its hydrogeologic setting. This work examines the role of organic matter in the distribution of uranium in the surface and shallow subsurface environments of central and north Florida.« less

Microbial Communities in Contaminated Sediments, Associated with Bioremediation of Uranium to Submicromolar Levels▿

PubMed Central

Cardenas, Erick; Wu, Wei-Min; Leigh, Mary Beth; Carley, Jack; Carroll, Sue; Gentry, Terry; Luo, Jian; Watson, David; Gu, Baohua; Ginder-Vogel, Matthew; Kitanidis, Peter K.; Jardine, Philip M.; Zhou, Jizhong; Criddle, Craig S.; Marsh, Terence L.; Tiedje, James M.

2008-01-01

Microbial enumeration, 16S rRNA gene clone libraries, and chemical analysis were used to evaluate the in situ biological reduction and immobilization of uranium(VI) in a long-term experiment (more than 2 years) conducted at a highly uranium-contaminated site (up to 60 mg/liter and 800 mg/kg solids) of the U.S. Department of Energy in Oak Ridge, TN. Bioreduction was achieved by conditioning groundwater above ground and then stimulating growth of denitrifying, Fe(III)-reducing, and sulfate-reducing bacteria in situ through weekly injection of ethanol into the subsurface. After nearly 2 years of intermittent injection of ethanol, aqueous U levels fell below the U.S. Environmental Protection Agency maximum contaminant level for drinking water and groundwater (<30 μg/liter or 0.126 μM). Sediment microbial communities from the treatment zone were compared with those from a control well without biostimulation. Most-probable-number estimations indicated that microorganisms implicated in bioremediation accumulated in the sediments of the treatment zone but were either absent or in very low numbers in an untreated control area. Organisms belonging to genera known to include U(VI) reducers were detected, including Desulfovibrio, Geobacter, Anaeromyxobacter, Desulfosporosinus, and Acidovorax spp. The predominant sulfate-reducing bacterial species were Desulfovibrio spp., while the iron reducers were represented by Ferribacterium spp. and Geothrix spp. Diversity-based clustering revealed differences between treated and untreated zones and also within samples of the treated area. Spatial differences in community structure within the treatment zone were likely related to the hydraulic pathway and to electron donor metabolism during biostimulation. PMID:18456853

Identifying and overcoming the constraints that prevent the full implementation of decommissioning and remediation programs in uranium mining sites.

PubMed

Franklin, Mariza Ramalho; Fernandes, Horst Monken

2013-05-01

Environmental remediation of radioactive contamination is about achieving appropriate reduction of exposures to ionizing radiation. This goal can be achieved by means of isolation or removal of the contamination source(s) or by breaking the exposure pathways. Ideally, environmental remediation is part of the planning phase of any industrial operation with the potential to cause environmental contamination. This concept is even more important in mining operations due to the significant impacts produced. This approach has not been considered in several operations developed in the past. Therefore many legacy sites face the challenge to implement appropriate remediation plans. One of the first barriers to remediation works is the lack of financial resources as environmental issues used to be taken in the past as marginal costs and were not included in the overall budget of the company. This paper analyses the situation of the former uranium production site of Poços de Caldas in Brazil. It is demonstrated that in addition to the lack of resources, other barriers such as the lack of information on site characteristics, appropriate regulatory framework, funding mechanisms, stakeholder involvement, policy and strategy, technical experience and mechanism for the appropriation of adequate technical expertise will play key roles in preventing the implementation of remediation programs. All these barriers are discussed and some solutions are suggested. It is expected that lessons learned from the Poços de Caldas legacy site may stimulate advancement of more sustainable options in the development of future uranium production centers. Copyright © 2011 Elsevier Ltd. All rights reserved.

Geochemistry of vanadium in an epigenetic, sandstone-hosted vanadium- uranium deposit, Henry Basin, Utah

USGS Publications Warehouse

Wanty, R.B.; Goldhaber, M.B.; Northrop, H.R.

1990-01-01

The epigenetic Tony M vanadium-uranium orebody in south-central Utah is hosted in fluvial sandstones of the Morrison Formation (Upper Jurassic). Measurements of the relative amounts of V+3 and V +4 in ore minerals show that V+3 is more abundant. Thermodynamic calculations show that vanadium was more likely transported to the site of mineralization as V+4. The ore formed as V+4 was reduced by hydrogen sulfide, followed by hydrolysis and precipitation of V+3 in oxide minerals or chlorite. Uranium was transported as uranyl ion (U+6), or some complex thereof, and reduced by hydrogen sulfide, forming coffinite. Detrital organic matter in the rocks served as the carbon source for sulfate-reducing bacteria. Vanadium most likely was derived from the dissolution of iron-titanium oxides. Uranium probably was derived from the overlying Brushy Basin Member of the Morrison Formation. Previous studies have shown that the ore formed at the density-stratified interface between a basinal brine and dilute meteoric water. The mineralization processes described above occurred within the mixing zone between these two fluids. -from Authors

Adsorption of uranium(VI) to manganese oxides: X-ray absorption spectroscopy and surface complexation modeling.

PubMed

Wang, Zimeng; Lee, Sung-Woo; Catalano, Jeffrey G; Lezama-Pacheco, Juan S; Bargar, John R; Tebo, Bradley M; Giammar, Daniel E

2013-01-15

The mobility of hexavalent uranium in soil and groundwater is strongly governed by adsorption to mineral surfaces. As strong naturally occurring adsorbents, manganese oxides may significantly influence the fate and transport of uranium. Models for U(VI) adsorption over a broad range of chemical conditions can improve predictive capabilities for uranium transport in the subsurface. This study integrated batch experiments of U(VI) adsorption to synthetic and biogenic MnO(2), surface complexation modeling, ζ-potential analysis, and molecular-scale characterization of adsorbed U(VI) with extended X-ray absorption fine structure (EXAFS) spectroscopy. The surface complexation model included inner-sphere monodentate and bidentate surface complexes and a ternary uranyl-carbonato surface complex, which was consistent with the EXAFS analysis. The model could successfully simulate adsorption results over a broad range of pH and dissolved inorganic carbon concentrations. U(VI) adsorption to synthetic δ-MnO(2) appears to be stronger than to biogenic MnO(2), and the differences in adsorption affinity and capacity are not associated with any substantial difference in U(VI) coordination.

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, particle size, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population andmore » composition, which mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfatereducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. The results of this study suggest that reductive immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

DOE PAGES

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.; ...

2016-12-29

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

MURMoT. Design and Application of Microbial Uranium Reduction Monitoring Tools

DOE Office of Scientific and Technical Information (OSTI.GOV)

Loeffler, Frank E.

2014-12-31

Uranium (U) contamination in the subsurface is a major remediation challenge at many DOE sites. Traditional site remedies present enormous costs to DOE; hence, enhanced bioremediation technologies (i.e., biostimulation and bioaugmentation) combined with monitoring efforts are being considered as cost-effective corrective actions to address subsurface contamination. This research effort improved understanding of the microbial U reduction process and developed new tools for monitoring microbial activities. Application of these tools will promote science-based site management decisions that achieve contaminant detoxification, plume control, and long-term stewardship in the most efficient manner. The overarching hypothesis was that the design, validation and application ofmore » a suite of new molecular and biogeochemical tools advance process understanding, and improve environmental monitoring regimes to assess and predict in situ U immobilization. Accomplishments: This project (i) advanced nucleic acid-based approaches to elucidate the presence, abundance, dynamics, spatial distribution, and activity of metal- and radionuclide-detoxifying bacteria; (ii) developed proteomics workflows for detection of metal reduction biomarker proteins in laboratory cultures and contaminated site groundwater; (iii) developed and demonstrated the utility of U isotopic fractionation using high precision mass spectrometry to quantify U(VI) reduction for a range of reduction mechanisms and environmental conditions; and (iv) validated the new tools using field samples from U-contaminated IFRC sites, and demonstrated their prognostic and diagnostic capabilities in guiding decision making for environmental remediation and long-term site stewardship.« less

Uranium Biomineralization by Natural Microbial Phosphatase Activities in the Subsurface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sobecky, Patricia A.

2015-04-06

In this project, inter-disciplinary research activities were conducted in collaboration among investigators at The University of Alabama (UA), Georgia Institute of Technology (GT), Lawrence Berkeley National Laboratory (LBNL), Brookhaven National Laboratory (BNL), the DOE Joint Genome Institute (JGI), and the Stanford Synchrotron Radiation Light source (SSRL) to: (i) confirm that phosphatase activities of subsurface bacteria in Area 2 and 3 from the Oak Ridge Field Research Center result in solid U-phosphate precipitation in aerobic and anaerobic conditions; (ii) investigate the eventual competition between uranium biomineralization via U-phosphate precipitation and uranium bioreduction; (iii) determine subsurface microbial community structure changes of Areamore » 2 soils following organophosphate amendments; (iv) obtain the complete genome sequences of the Rahnella sp. Y9-602 and the type-strain Rahnella aquatilis ATCC 33071 isolated from these soils; (v) determine if polyphosphate accumulation and phytate hydrolysis can be used to promote U(VI) biomineralization in subsurface sediments; (vi) characterize the effect of uranium on phytate hydrolysis by a new microorganism isolated from uranium-contaminated sediments; (vii) utilize positron-emission tomography to label and track metabolically-active bacteria in soil columns, and (viii) study the stability of the uranium phosphate mineral product. Microarray analyses and mineral precipitation characterizations were conducted in collaboration with DOE SBR-funded investigators at LBNL. Thus, microbial phosphorus metabolism has been shown to have a contributing role to uranium immobilization in the subsurface.« less

Screening of bacterial strains isolated from uranium mill tailings porewaters for bioremediation purposes.

PubMed

Sánchez-Castro, Iván; Amador-García, Ahinara; Moreno-Romero, Cristina; López-Fernández, Margarita; Phrommavanh, Vannapha; Nos, Jeremy; Descostes, Michael; Merroun, Mohamed L

2017-01-01

The present work characterizes at different levels a number of bacterial strains isolated from porewaters sampled in the vicinity of two French uranium tailing repositories. The 16S rRNA gene from 33 bacterial isolates, corresponding to the different morphotypes recovered, was almost fully sequenced. The resulting sequences belonged to 13 bacterial genera comprised in the phyla Firmicutes, Actinobacteria and Proteobacteria. Further characterization at physiological level and metals/metalloid tolerance provided evidences for an appropriate selection of bacterial strains potentially useful for immobilization of uranium and other common contaminants. By using High Resolution Transmission Electron Microscope (HRTEM), this potential ability to immobilize uranium as U phosphate mineral phases was confirmed for the bacterial strains Br3 and Br5 corresponding to Arthrobacter sp. and Microbacterium oxydans, respectively. Scanning Transmission Electron Microscope- High-Angle Annular Dark-Field (STEM-HAADF) analysis showed U accumulates on the surface and within bacterial cytoplasm, in addition to the extracellular space. Energy Dispersive X-ray (EDX) element-distribution maps demonstrated the presence of U and P within these accumulates. These results indicate the potential of certain bacterial strains isolated from porewaters of U mill tailings for immobilizing uranium, likely as uranium phosphates. Some of these bacterial isolates might be considered as promising candidates in the design of uranium bioremediation strategies. Copyright © 2016 Elsevier Ltd. All rights reserved.

Molecular-Scale Characterization of Natural Organic Matter From A Uranium Contaminated Aquifer and its Utilization by Native Microbial Communities

NASA Astrophysics Data System (ADS)

Mouser, P. J.; Wilkins, M. J.; Williams, K. H.; Smith, D. F.; Paša-Tolić, L.

2011-12-01

The availability and form of natural organic matter (NOM) strongly influences rates of microbial metabolism and associated redox processes in subsurface environments. This is an important consideration in metal-contaminated aquifers, such as the DOE's Rifle Integrated Field Research Challenge (IFRC) site, where naturally occurring suboxic conditions in groundwater may play an important function in controlling uranium mobility, and therefore the long-term stewardship of the site. Currently, the biophysiochemical processes surrounding the nature of the aquifer and its role in controlling the fate and transport of uranium are poorly understood. Using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) with electrospray ionization (ESI), we characterized dissolved organic matter (DOM) chemistry for three surface and groundwater sources at Rifle and assessed microbial utilization in batch incubation experiments. FT-ICR-MS uniquely offers ultrahigh mass measurement accuracy and resolving power for polar organics, in addition to enabling elemental composition assignments of these compounds. Samples were collected from the Colorado River, a shallow groundwater aquifer adjacent to the river, and a spring/seep discharge point upgradient from the aquifer. DOM was concentrated and purified from each source and analyzed using FT-ICR-MS with ESI. We identified between 6,000 and 7,000 formulae at each location, with the river sample having the smallest and the spring sample having the largest number of identified peaks. The groundwater and spring samples contained DOM with a large percentage of formulae containing nitrogen and sulfur species, while the river sample was dominated by carbon, hydrogen, and oxygen species. Less than 38% of the formulae were shared between any two samples, indicating a significant level of uniqueness across the samples. Unsaturated hydrocarbons, cellulose, and lipids were rapidly utilized by indigenous bacteria during a 24-day incubation period, and presumably transformed to more recalcitrant lignins and protein-type molecules. These findings indicate that FT-ICR-MS with ESI is an effective method for characterizing molecular-scale differences in DOM from complex environments. We also provide preliminary evidence that certain DOM fractions are more efficiently utilized by indigenous microbial communities and likely play an important role in controlling reducing conditions in heterogeneous subsurface environments.

Validation of uranium determination in urine by ICP-MS.

PubMed

Bouvier-Capely, C; Baglan, N; Montègue, A; Ritt, J; Cossonnet, C

2003-08-01

A rapid procedure--dilution of urine+ICP-MS measurement--for the determination of uranium in urine was validated. Large ranges of concentration and isotopic composition were studied on urine samples excreted by occupationally exposed workers. The results were consistent with those obtained by fluorimetry and by alpha spectrometry after a purification procedure, two currently used techniques. However, the proposed procedure is limited for determination of the minor isotope 234U. Thus for worker monitoring, the conversion of 234U mass concentration into activity concentration can lead to an erroneous value of the effective dose, in particular for a contamination at very low level with highly enriched uranium. A solution to avoid this hazard is to perform a chemical purification prior to ICP-MS measurement to lower uncertainty and detection limit for 234U.

BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS

DOEpatents

Seaborg, G.T.; Perlman, I.

1959-02-10

A process is described for the separation from each other of uranyl values, tetravalent plutonium values and fission products contained in an aqueous acidic solution. First the pH of the solution is adjusted to between 2.5 and 8 and hydrogen peroxide is then added to the solution causing precipitation of uranium peroxide which carries any plutonium values present, while the fission products remain in solution. Separation of the uranium and plutonium values is then effected by dissolving the peroxide precipitate in an acidic solution and incorporating a second carrier precipitate, selective for plutonium. The plutonium values are thus carried from the solution while the uranium remains flissolved. The second carrier precipitate may be selected from among the group consisting of rare earth fluorides, and oxalates, zirconium phosphate, and bismuth lihosphate.

Pore-Scale Characterization of Biogeochemical Controls on Iron and Uranium Speciation under Flow Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pearce, Carolyn I.; Wilkins, Michael J.; Zhang, Changyong

2012-09-17

Etched silicon microfluidic pore network models (micromodels) with controlled chemical and redox gradients, mineralogy, and microbiology under continuous flow conditions are used for the incremental development of complex microenvironments that simulate subsurface conditions. We demonstrate the colonization of micromodel pore spaces by an anaerobic Fe(III)-reducing bacterial species (Geobacter sulfurreducens) and the enzymatic reduction of a bioavailable Fe(III) phase within this environment. Using both X-ray Microprobe and X-ray Absorption Spectroscopy, we investigate the combined effects of the precipitated Fe(III) phases and the microbial population on uranium biogeochemistry under flow conditions. Precipitated Fe(III) phases within the micromodel were most effectively reduced inmore » the presence of an electron shuttle (AQDS), and Fe(II) ions adsorbed onto the precipitated mineral surface without inducing any structural change. In the absence of Fe(III), U(VI) was effectively reduced by the microbial population to insoluble U(IV), which was precipitated in discrete regions associated with biomass. In the presence of Fe(III) phases, however, both U(IV) and U(VI) could be detected associated with biomass, suggesting re-oxidation of U(IV) by localized Fe(III) phases. These results demonstrate the importance of the spatial localization of biomass and redox active metals, and illustrate the key effects of pore-scale processes on contaminant fate and reactive transport.« less

Monitoring Physical and Biogeochemical Dynamics of Uranium Bioremediation at the Intermediate Scale

NASA Astrophysics Data System (ADS)

Tarrell, A. N.; Figueroa, L. A.; Rodriguez, D.; Haas, A.; Revil, A.

2011-12-01

Subsurface uranium above desired levels for aquifer use categories exists naturally and from historic mining and milling practices. In situ bioimmobilization offers a cost effective alternative to conventional pump and treat methods by stimulating growth of microorganisms that lead to the reduction and precipitation of uranium. Vital to the long-term success of in situ bioimmobilization is the ability to successfully predict and demonstrate treatment effectiveness to assure that regulatory goals are met. However, successfully monitoring the progress over time is difficult and requires long-term stewardship to ensure effective treatment due to complex physical and biogeochemical heterogeneity. In order to better understand these complexities and the resultant effect on uranium immobilization, innovative systematic monitoring approaches with multiple performance indicators must be investigated. A key issue for uranium bioremediation is the long term stability of solid-phase reduction products. It has been shown that a combination of data from electrode-based monitoring, self-potential monitoring, oxidation reduction potential (ORP), and water level sensors provides insight for identifying and localizing bioremediation activity and can provide better predictions of deleterious biogeochemical change such as pore clogging. In order to test the proof-of-concept of these sensing techniques and to deconvolve redox activity from other electric potential changing events, an intermediate scale 3D tank experiment has been developed. Well-characterized materials will be packed into the tank and an artificial groundwater will flow across the tank through a constant-head boundary. The experiment will utilize these sensing methods to image the electrical current produced by bacteria as well as indications of when and where electrical activity is occurring, such as with the reduction of radionuclides. This work will expand upon current knowledge by exploring the behavior of uranium bioremediation at an intermediate scale, as well as examining the effects from introducing a flow field in a laboratory setting. Data collected from this experiment will help further characterize which factors are contributing to current increases. Additional information concerning the effect of geochemical changes in porosity may also be observed. The results of this work will allow the creation of a new data set collected from a more comprehensive laboratory monitoring network and will allow stakeholders to develop effective decision-making tools on the long-term remediation management at uranium contaminated sites. The data will also aid in the long-term prediction abilities of a reactive transport models. As in situ bioremediation offers a low cost alternative to ex situ treatment methods, the results of this work will help to both reduce cost at existing sites and enable treatment of sites that otherwise have no clear solution.

Translocation of uranium from water to foodstuff while cooking.

PubMed

Krishnapriya, K C; Baksi, Ananya; Chaudhari, Swathi; Gupta, Soujit Sen; Pradeep, T

2015-10-30

The present work report the unusual uranium uptake by foodstuff, especially those rich in carbohydrates like rice when they are cooked in water, contaminated with uranium. The major staple diet in South Asia, rice, was chosen to study its interaction with UO2(2+), the active uranium species in water, using inductively coupled plasma mass spectrometry. Highest uptake limit was checked by cooking rice at very high uranium concentration and it was found to be good scavenger of uranium. To gain insight into the mechanism of uptake, direct interaction of UO2(2+) with monosaccharides was also studied, using electrospray ionization mass spectrometry taking mannose as a model. The studies have been done with dissolved uranium salt, uranyl nitrate hexahydrate (UO2(NO3)2·6H2O), as well as the leachate of a stable oxide of uranium, UO2(s), both of which exist as UO2(2+) in water. Among the eight different rice varieties investigated, Karnataka Ponni showed the maximum uranium uptake whereas unpolished Basmati rice showed the minimum. Interaction with other foodstuffs (potato, carrot, peas, kidney beans and lentils) with and without NaCl affected the extent of chemical interaction but was not consistent with the carbohydrate content. Uranium interaction with D-mannose monitored through ESI-MS, under optimized instrumental parameters, identified the peaks corresponding to uranyl adduct with mannose monomer, dimer and trimer and the species were confirmed by MS/MS studies. The product ion mass spectra showed peaks illustrating water loss from the parent ion as the collision energy was increased, an evidence for the strong interaction of uranium with mannose. This study would constitute the essential background for understanding interaction of uranium with various foods. Extension of this work would involve identification of foodstuff as green heavy metal scavengers. Copyright © 2015. Published by Elsevier B.V.

Ground water contamination with (238)U, (234)U, (235)U, (226)Ra and (210)Pb from past uranium mining: cove wash, Arizona.

PubMed

Dias da Cunha, Kenya Moore; Henderson, Helenes; Thomson, Bruce M; Hecht, Adam A

2014-06-01

The objectives of the study are to present a critical review of the (238)U, (234)U, (235)U, (226)Ra and (210)Pb levels in water samples from the EPA studies (U.S. EPA in Abandoned uranium mines and the Navajo Nation: Red Valley chapter screening assessment report. Region 9 Superfund Program, San Francisco, 2004, Abandoned uranium mines and the Navajo Nation: Northern aum region screening assessment report. Region 9 Superfund Program, San Francisco, 2006, Health and environmental impacts of uranium contamination, 5-year plan. Region 9 Superfund Program, San Franciso, 2008) and the dose assessment for the population due to ingestion of water containing (238)U and (234)U. The water quality data were taken from Sect. "Data analysis" of the published report, titled Abandoned Uranium Mines Project Arizona, New Mexico, Utah-Navajo Lands 1994-2000, Project Atlas. Total uranium concentration was above the maximum concentration level for drinking water (7.410-1 Bq/L) in 19 % of the water samples, while (238)U and (234)U concentrations were above in 14 and 17 % of the water samples, respectively. (226)Ra and (210)Pb concentrations in water samples were in the range of 3.7 × 10(-1) to 5.55 × 102 Bq/L and 1.11 to 4.33 × 102 Bq/L, respectively. For only two samples, the (226)Ra concentrations exceeded the MCL for total Ra for drinking water (0.185 Bq/L). However, the (210)Pb/(226)Ra ratios varied from 0.11 to 47.00, and ratios above 1.00 were observed in 71 % of the samples. Secular equilibrium of the natural uranium series was not observed in the data record for most of the water samples. Moreover, the (235)U/(total)U mass ratios ranged from 0.06 to 5.9 %, and the natural mass ratio of (235)U to (total)U (0.72 %) was observed in only 16 % of the water samples, ratios above or below the natural ratio could not be explained based on data reported by U.S. EPA. In addition, statistical evaluations showed no correlations among the distribution of the radionuclide concentrations in the majority of the water samples, indicating more than one source of contamination could contribute to the sampled sources. The effective doses due to ingestion of the minimum uranium concentrations in water samples exceed the average dose considering inhalation and ingestion of regular diet for other populations around the world (1 μSv/year). The maximum doses due to ingestion of (238)U or (234)U were above the international limit for effective dose for members of the public (1 mSv/year), except for inhabitants of two chapters. The highest effective dose was estimated for inhabitants of Cove, and it was almost 20 times the international limit for members of the public. These results indicate that ingestion of water from some of the sampled sources poses health risks.

Redox behavior of uranium at the nanoporous aluminum oxide-water interface: implications for uranium remediation.

PubMed

Jung, Hun Bok; Boyanov, Maxim I; Konishi, Hiromi; Sun, Yubing; Mishra, Bhoopesh; Kemner, Kenneth M; Roden, Eric E; Xu, Huifang

2012-07-03

Sorption-desorption experiments show that the majority (ca. 80-90%) of U(VI) presorbed to mesoporous and nanoporous alumina could not be released by extended (2 week) extraction with 50 mM NaHCO(3) in contrast with non-nanoporous α alumina. The extent of reduction of U(VI) presorbed to aluminum oxides was semiquantitatively estimated by comparing the percentages of uranium desorbed by anoxic sodium bicarbonate between AH(2)DS-reacted and unreacted control samples. X-ray absorption spectroscopy confirmed that U(VI) presorbed to non-nanoporous alumina was rapidly and completely reduced to nanoparticulate uraninite by AH(2)DS, whereas reduction of U(VI) presorbed to nanoporous alumina was slow and incomplete (<5% reduction after 1 week). The observed nanopore size-dependent redox behavior of U has important implications in developing efficient remediation techniques for the subsurface uranium contamination because the efficiency of in situ bioremediation depends on how effectively and rapidly U(VI) bound to sediment or soil can be converted to an immobile phase.

Uptake of trace elements and radionuclides from uranium mill tailings by four-wing saltbush (Atriplex canescens) and alkali sacaton (Sporobolus airoides). [Radium 226; Uranium; Molybdenum; Selenium; Vanadium; Astatine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dreesen, D.R.; Marple, M.L.

1979-01-01

A greenhouse experiment was performed to determine the uptake of trace elements and radionuclides from uranium mill tailings by native plant species. Four-wing saltbush and alkali sacaton were grown in alkaline tailings covered with soil and in soil alone as controls. The tailings material was highly enriched in Ra-226, Mo, U, Se, V, and As compared with three local soils. The shrub grown in tailings had elevated concentrations of Mo, Se, Ra-226, U, As, and Na compared with the controls. Alkali sacaton contained high concentrations of Mo, Se, Ra-226, and Ni when grown on tailings. Molybdenum and selenium concentrations inmore » plants grown in tailings are above levels reported to be toxic to grazing animals. These results indicate that the bioavailability of Mo and Se in alkaline environments makes these elements among the most hazardous contaminants present in uranium mill wastes.« less

A neutron activation analysis procedure for the determination of uranium, thorium and potassium in geologic samples

USGS Publications Warehouse

Aruscavage, P. J.; Millard, H.T.

1972-01-01

A neutron activation analysis procedure was developed for the determination of uranium, thorium and potassium in basic and ultrabasic rocks. The three elements are determined in the same 0.5-g sample following a 30-min irradiation in a thermal neutron flux of 2??1012 n??cm-2??sec-1. Following radiochemical separation, the nuclides239U (T=23.5 m),233Th (T=22.2 m) and42K (T=12.36 h) are measured by ??-counting. A computer program is used to resolve the decay curves which are complex owing to contamination and the growth of daughter activities. The method was used to determine uranium, throium and potassium in the U. S. Geological Survey standard rocks DTS-1, PCC-1 and BCR-1. For 0.5-g samples the limits of detection for uranium, throium and potassium are 0.7, 1.0 and 10 ppb, respectively. ?? 1972 Akade??miai Kiado??.

Different pattern of brain pro-/anti-oxidant activity between depleted and enriched uranium in chronically exposed rats.

PubMed

Lestaevel, P; Romero, E; Dhieux, B; Ben Soussan, H; Berradi, H; Dublineau, I; Voisin, P; Gourmelon, P

2009-04-05

Uranium is not only a heavy metal but also an alpha particle emitter. The main toxicity of uranium is expected to be due to chemiotoxicity rather than to radiotoxicity. Some studies have demonstrated that uranium induced some neurological disturbances, but without clear explanations. A possible mechanism of this neurotoxicity could be the oxidative stress induced by reactive oxygen species imbalance. The aim of the present study was to determine whether a chronic ingestion of uranium induced anti-oxidative defence mechanisms in the brain of rats. Rats received depleted (DU) or 4% enriched (EU) uranyl nitrate in the drinking water at 2mg(-1)kg(-1)day(-1) for 9 months. Cerebral cortex analyses were made by measuring mRNA and protein levels and enzymatic activities. Lipid peroxidation, an oxidative stress marker, was significantly enhanced after EU exposure, but not after DU. The gene expression or activity of the main antioxidant enzymes, i.e. superoxide dismutase (SOD), catalase (CAT) and glutathione peroxidase (GPx), increased significantly after chronic exposure to DU. On the contrary, oral EU administration induced a decrease of these antioxidant enzymes. The NO-ergic pathway was almost not perturbed by DU or EU exposure. Finally, DU exposure increased significantly the transporters (Divalent-Metal-Transporter1; DMT1), the storage molecule (ferritin) and the ferroxidase enzyme (ceruloplasmin), but not EU. These results illustrate that oxidative stress plays a key role in the mechanism of uranium neurotoxicity. They showed that chronic exposure to DU, but not EU, seems to induce an increase of several antioxidant agents in order to counteract the oxidative stress. Finally, these results demonstrate the importance of the double toxicity, chemical and radiological, of uranium.

Using complex resistivity imaging to infer biogeochemical processes associated with bioremediation of an uranium-contaminated aquifer

NASA Astrophysics Data System (ADS)

Flores Orozco, AdriáN.; Williams, Kenneth H.; Long, Philip E.; Hubbard, Susan S.; Kemna, Andreas

2011-09-01

Experiments at the Department of Energy's Integrated Field Research Challenge (IFRC) site near Rifle, Colorado, have demonstrated the ability to remove uranium from groundwater by stimulating the growth and activity of Geobacter species through acetate amendment. Prolonging the activity of these strains in order to optimize uranium bioremediation has prompted the development of minimally invasive and spatially extensive monitoring methods diagnostic of their in situ activity and the end products of their metabolism. Here we demonstrate the use of complex resistivity imaging for monitoring biogeochemical changes accompanying stimulation of indigenous aquifer microorganisms during and after a prolonged period (100+ days) of acetate injection. A thorough raw data statistical analysis of discrepancies between normal and reciprocal measurements and incorporation of a new power law phase-error model in the inversion were used to significantly improve the quality of the resistivity phase images over those obtained during previous monitoring experiments at the Rifle IFRC site. The imaging results reveal spatiotemporal changes in the phase response of aquifer sediments, which correlate with increases in Fe(II) and precipitation of metal sulfides (e.g., FeS) following the iterative stimulation of iron and sulfate-reducing microorganisms. Only modest changes in resistivity magnitude were observed over the monitoring period. The largest phase anomalies (>40 mrad) were observed hundreds of days after halting acetate injection, in conjunction with accumulation of Fe(II) in the presence of residual FeS minerals, reflecting preservation of geochemically reduced conditions in the aquifer, a prerequisite for ensuring the long-term stability of immobilized, redox-sensitive contaminants such as uranium.

Vanadium Respiration by Geobacter metallireducens: Novel Strategy for In Situ Removal of Vanadium from Groundwater

PubMed Central

Ortiz-Bernad, Irene; Anderson, Robert T.; Vrionis, Helen A.; Lovley, Derek R.

2004-01-01

Vanadium can be an important contaminant in groundwaters impacted by mining activities. In order to determine if microorganisms of the Geobacteraceae, the predominant dissimilatory metal reducers in many subsurface environments, were capable of reducing vanadium(V), Geobacter metallireducens was inoculated into a medium in which acetate was the electron donor and vanadium(V) was the sole electron acceptor. Reduction of vanadium(V) resulted in the production of vanadium(IV), which subsequently precipitated. Reduction of vanadium(V) was associated with cell growth with a generation time of 15 h. No vanadium(V) was reduced and no precipitate was formed in heat-killed or abiotic controls. Acetate was the most effective of all the electron donors evaluated. When acetate was injected into the subsurface to enhance the growth and activity of Geobacteraceae in an aquifer contaminated with uranium and vanadium, vanadium was removed from the groundwater even more effectively than uranium. These studies demonstrate that G. metallireducens can grow via vanadium(V) respiration and that stimulating the activity of Geobacteraceae, and hence vanadium(V) reduction, can be an effective strategy for in situ immobilization of vanadium in contaminated subsurface environments. PMID:15128571

The measurement of alpha particle emissions from semiconductor memory materials

NASA Astrophysics Data System (ADS)

Bouldin, D. P.

1981-07-01

With the increasing concern for the affects of alpha particles on the reliability of semiconductor memories, an interest has arisen in characterizing semiconductor manufacturing materials for extremely low-level alpha-emitting contaminants. It is shown that four elements are of primary concern: uranium, thorium, radium, and polonium. Measurement of contamination levels are given relevance by first correlating them with alpha flux emission levels and then corre1ating these flux values with device soft error rates. Measurement techniques involve either measurements of elemental concentrations-applicable to only uranium and thorium - or direct measurements of alpha emission fluxes. Alpha fluxes are most usefully measured by means of ZnS scintillation counting, practical details of which are discussed. Materials measurements are reported for ceramics, solder, silicon, quartz, and various metals and organic materials. Ceramics and most metals have contamination levels of concern, but the high temperature processing normally used in semiconductor manufacturing and low total amounts reduce problems, at least for metals. Silicon, silicon compounds, and organic materials have been found to have no detectable alpha emitters. Finally, a brief discussion of the calibration of alpha sources for accelerated device testing is given, including practical details on the affects of source/chip separation and alignment variations.

Semianalytical solutions for contaminant transport under variable velocity field in a coastal aquifer

NASA Astrophysics Data System (ADS)

Koohbor, Behshad; Fahs, Marwan; Ataie-Ashtiani, Behzad; Simmons, Craig T.; Younes, Anis

2018-05-01

Existing closed-form solutions of contaminant transport problems are limited by the mathematically convenient assumption of uniform flow. These solutions cannot be used to investigate contaminant transport in coastal aquifers where seawater intrusion induces a variable velocity field. An adaptation of the Fourier-Galerkin method is introduced to obtain semi-analytical solutions for contaminant transport in a confined coastal aquifer in which the saltwater wedge is in equilibrium with a freshwater discharge flow. Two scenarios dealing with contaminant leakage from the aquifer top surface and contaminant migration from a source at the landward boundary are considered. Robust implementation of the Fourier-Galerkin method is developed to efficiently solve the coupled flow, salt and contaminant transport equations. Various illustrative examples are generated and the semi-analytical solutions are compared against an in-house numerical code. The Fourier series are used to evaluate relevant metrics characterizing contaminant transport such as the discharge flux to the sea, amount of contaminant persisting in the groundwater and solute flux from the source. These metrics represent quantitative data for numerical code validation and are relevant to understand the effect of seawater intrusion on contaminant transport. It is observed that, for the surface contamination scenario, seawater intrusion limits the spread of the contaminant but intensifies the contaminant discharge to the sea. For the landward contamination scenario, moderate seawater intrusion affects only the spatial distribution of the contaminant plume while extreme seawater intrusion can increase the contaminant discharge to the sea. The developed semi-analytical solution presents an efficient tool for the verification of numerical models. It provides a clear interpretation of the contaminant transport processes in coastal aquifers subject to seawater intrusion. For practical usage in further studies, the full open source semi-analytical codes are made available at the website https://lhyges.unistra.fr/FAHS-Marwan.

Impact of natural organic matter on uranium transport through saturated geologic materials: from molecular to column scale.

PubMed

Yang, Yu; Saiers, James E; Xu, Na; Minasian, Stefan G; Tyliszczak, Tolek; Kozimor, Stosh A; Shuh, David K; Barnett, Mark O

2012-06-05

The risk stemming from human exposure to actinides via the groundwater track has motivated numerous studies on the transport of radionuclides within geologic environments; however, the effects of waterborne organic matter on radionuclide mobility are still poorly understood. In this study, we compared the abilities of three humic acids (HAs) (obtained through sequential extraction of a peat soil) to cotransport hexavalent uranium (U) within water-saturated sand columns. Relative breakthrough concentrations of U measured upon elution of 18 pore volumes increased from undetectable levels (<0.001) in an experiment without HAs to 0.17 to 0.55 in experiments with HAs. The strength of the HA effect on U mobility was positively correlated with the hydrophobicity of organic matter and NMR-detected content of alkyl carbon, which indicates the possible importance of hydrophobic organic matter in facilitating U transport. Carbon and uranium elemental maps collected with a scanning transmission X-ray microscope (STXM) revealed uneven microscale distribution of U. Such molecular- and column-scale data provide evidence for a critical role of hydrophobic organic matter in the association and cotransport of U by HAs. Therefore, evaluations of radionuclide transport within subsurface environments should consider the chemical characteristics of waterborne organic substances, especially hydrophobic organic matter.