Groundwater and surface-water interaction, water quality, and processes affecting loads of dissolved solids, selenium, and uranium in Fountain Creek near Pueblo, Colorado, 2012–2014

USGS Publications Warehouse

Arnold, L. Rick; Ortiz, Roderick F.; Brown, Christopher R.; Watts, Kenneth R.

2016-11-28

In 2012, the U.S. Geological Survey, in cooperation with the Arkansas River Basin Regional Resource Planning Group, initiated a study of groundwater and surface-water interaction, water quality, and loading of dissolved solids, selenium, and uranium to Fountain Creek near Pueblo, Colorado, to improve understanding of sources and processes affecting loading of these constituents to streams in the Arkansas River Basin. Fourteen monitoring wells were installed in a series of three transects across Fountain Creek near Pueblo, and temporary streamgages were established at each transect to facilitate data collection for the study. Groundwater and surface-water interaction was characterized by using hydrogeologic mapping, groundwater and stream-surface levels, groundwater and stream temperatures, vertical hydraulic-head gradients and ratios of oxygen and hydrogen isotopes in the hyporheic zone, and streamflow mass-balance measurements. Water quality was characterized by collecting periodic samples from groundwater, surface water, and the hyporheic zone for analysis of dissolved solids, selenium, uranium, and other selected constituents and by evaluating the oxidation-reduction condition for each groundwater sample under different hydrologic conditions throughout the study period. Groundwater loads to Fountain Creek and in-stream loads were computed for the study area, and processes affecting loads of dissolved solids, selenium, and uranium were evaluated on the basis of geology, geochemical conditions, land and water use, and evapoconcentration.During the study period, the groundwater-flow system generally contributed flow to Fountain Creek and its hyporheic zone (as a single system) except for the reach between the north and middle transects. However, the direction of flow between the stream, the hyporheic zone, and the near-stream aquifer was variable in response to streamflow and stage. During periods of low streamflow, Fountain Creek generally gained flow from groundwater. However, during periods of high streamflow, the hydraulic gradient between groundwater and the stream temporarily reversed, causing the stream to lose flow to groundwater.Concentrations of dissolved solids, selenium, and uranium in groundwater generally had greater spatial variability than surface water or hyporheic-zone samples, and constituent concentrations in groundwater generally were greater than in surface water. Constituent concentrations in the hyporheic zone typically were similar to or intermediate between concentrations in groundwater and surface water. Concentrations of dissolved solids, selenium, uranium, and other constituents in groundwater samples collected from wells located on the east side of the north monitoring well transect were substantially greater than for other groundwater, surface-water, and hyporheic-zone samples. With one exception, groundwater samples collected from wells on the east side of the north transect exhibited oxic to mixed (oxic-anoxic) conditions, whereas most other groundwater samples exhibited anoxic to suboxic conditions. Concentrations of dissolved solids, selenium, and uranium in surface water generally increased in a downstream direction along Fountain Creek from the north transect to the south transect and exhibited an inverse relation to streamflow with highest concentration occurring during periods of low streamflow and lowest concentrations occurring during periods of high streamflow.Groundwater loads of dissolved solids, selenium, and uranium to Fountain Creek were small because of the small amount of groundwater flowing to the stream under typical low-streamflow conditions. In-stream loads of dissolved solids, selenium, and uranium in Fountain Creek varied by date, primarily in relation to streamflow at each transect and were much larger than computed constituent loads from groundwater. In-stream loads generally decreased with decreases in streamflow and increased as streamflow increased. In-stream loads of dissolved solids and selenium increased between the north and middle transects but generally decreased between the middle and south transects. By contrast, uranium loads generally decreased between the north and middle transects but increased between the middle and south transects. In-stream load differences between transects appear primarily to be related to differences in streamflow. However, because groundwater typically flows to Fountain Creek under low-flow conditions, and groundwater has greater concentrations of dissolved solids, selenium, and uranium than surface water in Fountain Creek, increases in loads between transects likely are affected by inflow of groundwater to the stream, which can account for a substantial proportion of the in-stream load difference between transects. When loads decreased between transects, the primary cause likely was decreased streamflow as a result of losses to groundwater and flow through the hyporheic zone. However, localized groundwater inflow likely attenuated the magnitude by which the in-stream loads decreased.The combination of localized soluble geologic sources and oxic conditions likely is the primary reason for the occurrence of high concentrations of dissolved solids, selenium, and uranium in groundwater on the east side of the north monitoring well transect. To evaluate conditions potentially responsible for differences in water quality and redox conditions, physical characteristics such as depth to water, saturated thickness, screen depth below the water table, screen height above bedrock, and aquifer hydraulic conductivity were compared by using Wilcoxon rank-sum tests. Results indicated no significant difference between depth to water, screen height above bedrock, and hydraulic conductivity for groundwater samples collected from wells on the east side of the north transect and groundwater samples from all other wells. However, saturated thickness and screen depth below the water table both were significantly smaller for groundwater samples collected from wells on the east side of the north transect than for groundwater samples from other wells, indicating that these characteristics might be related to the elevated constituent concentrations found at that location. Similarly, saturated thickness and screen depth below the water table were significantly smaller for groundwater samples under oxic or mixed (oxic-anoxic) conditions than for those under anoxic to suboxic conditions.The greater constituent concentrations at wells on the east side of the north transect also could, in part, be related to groundwater discharge from an unnamed alluvial drainage located directly upgradient from that location. Although the quantity and quality of water discharging from the drainage is not known, the drainage appears to collect water from a residential area located upgradient to the east of the wells, and groundwater could become concentrated in nitrate and other dissolved constituents before flowing through the drainage. High levels of nitrate, whether from anthropogenic or natural geologic sources, could promote more soluble forms of selenium and other constituents by affecting the redox condition of groundwater. Whether oxic conditions at wells on the east side of the north transect are the result of physical characteristics or of groundwater inflow from the alluvial drainage, the oxic conditions appear to cause increased dissolution of minerals from the shallow shale bedrock at that location. Because ratios of hydrogen and oxygen isotopes indicate evaporation likely has not had a substantial effect on groundwater, constituent concentrations at that location likely are not the result of evapoconcentration. 

REMOVAL OF ALUMINUM COATINGS

DOEpatents

Peterson, J.H.

1959-08-25

A process is presented for dissolving aluminum jackets from uranium fuel elements without attack of the uranium in a boiling nitric acid-mercuric nitrate solution containing up to 50% by weight of nitrtc acid and mercuric nitrate in a concentration of between 0.05 and 1% by weight.

Uranium Fate and Transport Modeling, Guterl Specialty Steel Site, New York - 13545

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

Frederick, Bill; Tandon, Vikas

2013-07-01

The Former Guterl Specialty Steel Corporation Site (Guterl Site) is located 32 kilometers (20 miles) northeast of Buffalo, New York, in Lockport, Niagara County, New York. Between 1948 and 1952, up to 15,875 metric tons (35 million pounds) of natural uranium metal (U) were processed at the former Guterl Specialty Steel Corporation site in Lockport, New York. The resulting dust, thermal scale, mill shavings and associated land disposal contaminated both the facility and on-site soils. Uranium subsequently impacted groundwater and a fully developed plume exists below the site. Uranium transport from the site involves legacy on-site pickling fluid handling, themore » leaching of uranium from soil to groundwater, and the groundwater transport of dissolved uranium to the Erie Canal. Groundwater fate and transport modeling was performed to assess the transfer of dissolved uranium from the contaminated soils and buildings to groundwater and subsequently to the nearby Erie Canal. The modeling provides a tool to determine if the uranium contamination could potentially affect human receptors in the vicinity of the site. Groundwater underlying the site and in the surrounding area generally flows southeasterly towards the Erie Canal; locally, groundwater is not used as a drinking water resource. The risk to human health was evaluated outside the Guterl Site boundary from the possibility of impacted groundwater discharging to and mixing with the Erie Canal waters. This condition was evaluated because canal water is infrequently used as an emergency water supply for the City of Lockport via an intake located approximately 122 meters (m) (400 feet [ft]) southeast of the Guterl Site. Modeling was performed to assess whether mixing of groundwater with surface water in the Erie Canal could result in levels of uranium exceeding the U.S. Environmental Protection Agency (USEPA) established drinking water standard for total uranium; the Maximum Concentration Limit (MCL). Geotechnical test data indicate that the major portion of uranium in the soil will adsorb or remain bound to soil, yet leaching to groundwater appears as an on-site source. Soil leaching was modeled using low adsorption factors to replicate worst-case conditions where the uranium leaches to the groundwater. Results indicate that even after several decades, which is the period of time since uranium was processed at the Guterl Site, leaching from soil does not fully account for the currently observed levels of groundwater contamination. Modeling results suggest that there were historic releases of uranium from processing operations directly to the shallow fractured rock and possibly other geochemical conditions that have produced the current groundwater contamination. Groundwater data collected at the site between 1997 and 2011 do not indicate an increasing level of uranium in the main plume, thus the uranium adsorbed to the soil is in equilibrium with the groundwater geochemistry and transport conditions. Consequently, increases in the overall plume concentration or size are not expected. Groundwater flowing through fractures under the Guterl Site transports dissolved uranium from the site to the Erie Canal, where the groundwater has been observed to seep from the northern canal wall at some locations. The seeps discharge uranium at concentrations near or below the MCL to the Erie Canal. Conservative mixing calculations were performed using two worst-case assumptions: 1) the seeps were calculated as contiguous discharges from the Erie Canal wall and 2) the uranium concentration of the seepage is 274 micrograms per liter (μg/L) of uranium, which is the highest on-site uranium concentration in groundwater and nearly ten-fold the actual seep concentrations. The results indicate that uranium concentrations in the seep water would have to be more than 200 times greater than the highest observed on-site groundwater concentrations (or nearly 55,000 μg/L) to potentially exceed the drinking water standard (the MCL) for total uranium in the Erie Canal. (authors)« less

Temporal Variations in 234U/238U Activity Ratios in the Lower Mississippi River due to Changes in Source Tributary Discharges

NASA Astrophysics Data System (ADS)

Grzymko, T. J.; Marcantonio, F.; McKee, B. A.; Stewart, C. M.

2004-12-01

The world's 25 largest river systems contribute nearly 50% of all freshwater to the global ocean and carry large quantities of dissolved trace metals annually. Trace metal concentrations in these systems show large variances on seasonal time scales. In order to constrain the causes of these variations, consistent sampling on sub-seasonal time intervals is essential. Here, we focus on the Mississippi River, the seventh largest river in the world in terms of freshwater discharge and the third largest in terms of drainage basin area. Biweekly sampling of the lower Mississippi River at New Orleans was performed from January 2003 to August 2004. Uranium concentrations and 234U/238U activity ratios were measured for the dissolved component (<0.2 μ m-fraction) of river water. Over the course of this study, dissolved U activity ratios spanned a range of about 25%, from 1.23 to 1.60. Dissolved U concentrations ranged from 0.28 to 1.06 ppb. The relationship between concentrations, activity ratios, and lower river discharge is complicated, and no clear pattern is observed on both biweekly and seasonal timescales. However, there does seem to be a relationship between the larger seasonal trends in the lower Mississippi River and variations in the discharge of its upstream tributaries. To constrain this relationship, we have sampled water from the Missouri River, the upper Mississippi River above the confluence with the Missouri, the Ohio River, and the Arkansas River in February, April, and August of 2004. For the upstream samples measured thus far, the highest dissolved uranium concentrations are observed for the Missouri River at 2.02 ppb, while the lowest are found in the Ohio River at 0.38 ppb. Dissolved 234U/238U activity ratios are as unique for each tributary and vary from 1.36 in the Ohio River to 1.51 in the Missouri River. A preliminary mass balance analysis reveals that the lower river uranium activity ratios are controlled simply by the quantity and isotope signature of the waters discharged from the upstream tributaries. A discussion of the implications of this work for global ocean budgets of uranium will be presented.

Data on Streamflow and Quality of Water and Bottom Sediment in and near Humboldt Wildlife Management Area, Churchill and Pershing Counties, Nevada, 1998-2000

USGS Publications Warehouse

Paul, Angela P.; Thodal, Carl E.

2003-01-01

This study was initiated to expand upon previous findings that indicated concentrations of dissolved solids, arsenic, boron, mercury, molybdenum, selenium, and uranium were either above geochemical background concentrations or were approaching or exceeding ecological criteria in the lower Humboldt River system. Data were collected from May 1998 to September 2000 to further characterize streamflow and surface-water and bottom-sediment quality in the lower Humboldt River, selected agricultural drains, Upper Humboldt Lake, and Lower Humboldt Drain (ephemeral outflow from Humboldt Sink). During this study, flow in the lower Humboldt River was either at or above average. Flows in Army and Toulon Drains generally were higher than reported in previous investigations. An unnamed agricultural drain contributed a small amount to the flow measured in Army Drain. In general, measured concentrations of sodium, chloride, dissolved solids, arsenic, boron, molybdenum, and uranium were higher in water from agricultural drains than in Humboldt River water during this study. Mercury concentrations in water samples collected during the study period typically were below the laboratory reporting level. However, low-level mercury analyses showed that samples collected in August 1999 from Army Drain had higher mercury concentrations than those collected from the river or Toulon Drain or the Lower Humboldt Drain. Ecological criteria and effect concentrations for sodium, chloride, dissolved solids, arsenic, boron, mercury, and molybdenum were exceeded in some water samples collected as part of this study. Although water samples from the agricultural drains typically contained higher concentrations of sodium, chloride, dissolved solids, arsenic, boron, and uranium, greater instantaneous loads of these constituents were carried in the river near Lovelock than in agricultural drains during periods of high flow or non-irrigation. During this study, the high flows in the lower Humboldt River produced the maximum instantaneous loads of sodium, chloride, dissolved solids, arsenic, boron, molybdenum, and uranium at all river-sampling sites, except molybdenum near Imlay. Nevada Division of Environmental Protection monitoring reports on mine-dewatering discharge for permitted releases of treated effluent to the surface waters of the Humboldt River and its tributaries were reviewed for reported discharges and trace-element concentrations from June 1998 to September 1999. These data were compared with similar information for the river near Imlay. In all bottom sediments collected for this study, arsenic concentrations exceeded the Canadian Freshwater Interim Sediment-Quality Guideline for the protection of aquatic life and probable-effect level (concentration). Sediments collected near Imlay, Rye Patch Reservoir, Lovelock, and from Toulon Drain and Army Drain were found to contain cadmium and chromium concentrations that exceeded Canadian criteria. Chromium concentrations in sediments collected from these sites also exceeded the consensus-based threshold-effect concentration. The Canadian criterion for sediment copper concentration was exceeded in sediments collected from the Humboldt River near Lovelock and from Toulon, Army, and the unnamed agricultural drains. Mercury in sediments collected near Imlay and from Toulon Drain in August 1999 exceeded the U.S. Department of the Interior sediment probable-effect level. Nickel concentrations in sediments collected during this study were above the consensus-based threshold-effect concentration. All other river and drain sediments had constituent concentrations below protective criteria and toxicity thresholds. In Upper Humboldt Lake, chloride, dissolved solids, arsenic, boron, molybdenum, and uranium concentrations in surface-water samples collected near the mouth of the Humboldt River generally were higher than in samples collected near the mouth of Army Drain. Ecological criteria or effect con

Uranyl adsorption kinetics within silica gel: dependence on flow velocity and concentration

NASA Astrophysics Data System (ADS)

Dodd, Brandon M.; Tepper, Gary

2017-09-01

Trace quantities of a uranyl dissolved in water were measured using a simple optical method. A dilute solution of uranium nitrate dissolved in water was forced through nanoporous silica gel at fixed and controlled water flow rates. The uranyl ions deposited and accumulated within the silica gel and the uranyl fluorescence within the silica gel was monitored as a function of time using a light emitting diode as the excitation source and a photomultiplier tube detector. It was shown that the response time of the fluorescence output signal at a particular volumetric flow rate or average liquid velocity through the silica gel can be used to quantify the concentration of uranium in water. The response time as a function of concentration decreased with increasing flow velocity.

Chemistry of uranium, thorium, and radium isotopes in the Ganga-Brahmaputra river system: Weathering processes and fluxes to the Bay of Bengal

NASA Astrophysics Data System (ADS)

Sarin, M. M.; Krishnaswami, S.; somayajulu, B. L. K.; Moore, W. S.

1990-05-01

The most comprehensive data set on uranium, thorium, and radium isotopes in the Ganga-Brahmaputra, one of the major river systems of the world, is reported here. The dissolved 238U concentration in these river waters ranges between 0.44 and 8.32 μ/1, and it exhibits a positive correlation with major cations (Na + K + Mg + Ca). The 238U /∑Cations ratio in waters is very similar to that measured in the suspended sediments, indicating congruent weathering of uranium and major cations. The regional variations observed in the [ 234U /238U ] activity ratio are consistent with the lithology of the drainage basins. The lowland tributaries (Chambal, Betwa, Ken, and Son), draining through the igneous and metamorphic rocks of the Deccan Traps and the Vindhyan-Bundelkhand Plateau, have [ 234U /238U ] ratio in the range 1.16 to 1.84. This range is significantly higher than the near equilibrium ratio (~1.05) observed in the highland rivers which drain through sedimentary terrains. The dissolved 226Ra concentration ranges between 0.03 and 0.22 dpm/1. The striking feature of the radium isotopes data is the distinct difference in the 228Ra and 226Ra abundances between the highland and lowland rivers. The lowland waters are enriched in 228Ra while the highland waters contain more 226Ra. This difference mainly results from the differences in their weathering regimes. The discharge-weighted mean concentration of dissolved 238U in the Ganga (at Patna) and in the Brahmaputra (at Goalpara) are 1.81 and 0.63 μ/1, respectively. The Ganga-Brahmaputra river system constitutes the major source of dissolved uranium to the Bay of Bengal. These rivers transport annually about 1000 tons of uranium to their estuaries, about 10% of the estimated global supply of dissolved uranium to the oceans via rivers. The transport of uranium by these rivers far exceeds that of the Amazon, although their water discharge is only about 20% of that of the Amazon. The high intensity of weathering of uranium in the Ganga-Brahmapura River system can also be deduced from the [ 232Th /238U ] and [ 230Th /238U ] activity ratios measured in the suspended sediments. 230Th is enriched by about 19% in the suspended sediments relative to its parent 238U. The flux of excess 230Th supplied to the Bay of Bengal via these river sediments is 980 × 10 12 dpm/a, about six times more than its in situ production from seawater in the entire Bay of Bengal.

Influence of uranyl speciation and iron oxides on uranium biogeochemical redox reactions

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

Stewart, B.D.; Amos, R.T.; Nico, P.S.

2010-03-15

Uranium is a pollutant of concern to both human and ecosystem health. Uranium's redox state often dictates its partitioning between the aqueous- and solid-phases, and thus controls its dissolved concentration and, coupled with groundwater flow, its migration within the environment. In anaerobic environments, the more oxidized and mobile form of uranium (UO{sub 2}{sup 2+} and associated species) may be reduced, directly or indirectly, by microorganisms to U(IV) with subsequent precipitation of UO{sub 2}. However, various factors within soils and sediments may limit biological reduction of U(VI), inclusive of alterations in U(VI) speciation and competitive electron acceptors. Here we elucidate themore » impact of U(VI) speciation on the extent and rate of reduction with specific emphasis on speciation changes induced by dissolved Ca, and we examine the impact of Fe(III) (hydr)oxides (ferrihydrite, goethite and hematite) varying in free energies of formation on U reduction. The amount of uranium removed from solution during 100 h of incubation with S. putrefaciens was 77% with no Ca or ferrihydrite present but only 24% (with ferrihydrite) and 14% (no ferrihydrite) were removed for systems with 0.8 mM Ca. Imparting an important criterion on uranium reduction, goethite and hematite decrease the dissolved concentration of calcium through adsorption and thus tend to diminish the effect of calcium on uranium reduction. Dissimilatory reduction of Fe(III) and U(VI) can proceed through different enzyme pathways, even within a single organism, thus providing a potential second means by which Fe(III) bearing minerals may impact U(VI) reduction. We quantify rate coefficients for simultaneous dissimilatory reduction of Fe(III) and U(VI) in systems varying in Ca concentration (0 to 0.8 mM), and using a mathematical construct implemented with the reactive transport code MIN3P, we reveal the predominant influence of uranyl speciation, specifically the formation of uranyl-calcium-carbonato complexes, and ferrihydrite on the rate and extent of uranium reduction in complex geochemical systems.« less

Uranium delivery and uptake in a montane wetland, north-central Colorado, USA

USGS Publications Warehouse

Schumann, R. Randall; Zielinski, Robert A.; Otton, James K.; Pantea, Michael P.; Orem, William H.

2017-01-01

Comprehensive sampling of peat, underlying lakebed sediments, and coexisting waters of a naturally uraniferous montane wetland are combined with hydrologic measurements to define the important controls on uranium (U) supply and uptake. The major source of U to the wetland is groundwater flowing through locally fractured and faulted granite gneiss of Proterozoic age. Dissolved U concentrations in four springs and one seep ranged from 20 to 83 ppb (μg/l). Maximum U concentrations are ∼300 ppm (mg/kg) in lakebed sediments and >3000 ppm in peat. Uranium in lakebed sediments is primarily stratabound in the more organic-rich layers, but samples of similar organic content display variable U concentrations. Post-depositional modifications include variable additions of U delivered by groundwater. Uranium distribution in peat is heterogeneous and primarily controlled by proximity to groundwater-fed springs and seeps that act as local point sources of U, and by proximity to groundwater directed along the peat/lakebeds contact. Uranium is initially sorbed on various organic components of peat as oxidized U(VI) present in groundwater. Selective extractions indicate that the majority of sorbed U remains as the oxidized species despite reducing conditions that should favor formation of U(IV). Possible explanations are kinetic hindrances related to strong complex formation between uranyl and humic substances, inhibition of anaerobic bacterial activity by low supply of dissolved iron and sulfate, and by cold temperatures.

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

Mehta, Vrajesh; Maillot, Fabien; Wang, Zheming

Uranyl phosphate solids are often found with uranium ores, and their low solubility makes them promising target phases for in situ remediation of uranium-contaminated subsurface environments. The products and solubility of uranium(VI) precipitated with phosphate can be affected by the pH, dissolved inorganic carbon (DIC) concentration, and co-solute composition (e.g. Na+/Ca2+) of the groundwater. Batch experiments were performed to study the effect of these parameters on the products and extent of uranium precipitation induced by phosphate addition. In the absence of co-solute cations, chernikovite [H3O(UO2)(PO4)•3H2O] precipitated despite uranyl orthophosphate [(UO2)3(PO4)2•4H2O] being thermodynamically more favorable under certain conditions. As determined usingmore » X-ray diffraction, electron microscopy, and laser induced fluorescence spectroscopy, the presence of Na+ or Ca2+ as a co-solute led to the precipitation of sodium autunite ([Na2(UO2)2(PO4)2] and autunite [Ca(UO2)2(PO4)2]), which are structurally similar to chernikovite. In the presence of sodium, the dissolved U(VI) concentrations were generally in agreement with equilibrium predictions of sodium autunite solubility. However, in the calcium-containing systems, the observed concentrations were below the predicted solubility of autunite, suggesting the possibility of uranium adsorption to or incorporation in a calcium phosphate precipitate in addition to the precipitation of autunite.« less

Processing of irradiated, enriched uranium fuels at the Savannah River Plant

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

Hyder, M L; Perkins, W C; Thompson, M C

Uranium fuels containing /sup 235/U at enrichments from 1.1% to 94% are processed and recovered, along with neptunium and plutonium byproducts. The fuels to be processed are dissolved in nitric acid. Aluminum-clad fuels are disssolved using a mercury catalyst to give a solution rich in aluminum. Fuels clad in more resistant materials are dissolved in an electrolytic dissolver. The resulting solutions are subjected to head-end treatment, including clarification and adjustment of acid and uranium concentration before being fed to solvent extraction. Uranium, neptunium, and plutonium are separated from fission products and from one another by multistage countercurrent solvent extraction withmore » dilute tri-n-butyl phosphate in kerosene. Nitric acid is used as the salting agent in addition to aluminum or other metal nitrates present in the feed solution. Nuclear safety is maintained through conservative process design and the use of monitoring devices as secondary controls. The enriched uranium is recovered as a dilute solution and shipped off-site for further processing. Neptunium is concentrated and sent to HB-Line for recovery from solution. The relatively small quantities of plutonium present are normally discarded in aqueous waste, unless the content of /sup 238/Pu is high enough to make its recovery desirable. Most of the /sup 238/Pu can be recovered by batch extraction of the waste solution, purified by counter-current solvent extraction, and converted to oxide in HB-Line. By modifying the flowsheet, /sup 239/Pu can be recovered from low-enriched uranium in the extraction cycle; neptunium is then not recovered. The solvent is subjected to an alkaline wash before reuse to remove degraded solvent and fission products. The aqueous waste is concentrated and partially deacidified by evaporation before being neutralized and sent to the waste tanks; nitric acid from the overheads is recovered for reuse.« less

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.

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

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

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

Fast Oxidation Processes in a Naturally Reduced Aquifer Zone Caused by Dissolved Oxygen

NASA Astrophysics Data System (ADS)

Davis, J. A.; Jemison, N. E.; Williams, K. H.; Hobson, C.; Bush, R. P.

2014-12-01

The occurrence of naturally reduced zones is quite common in alluvial aquifers in the western U.S.A. due to the burial of woody debris in flood plains. The naturally reduced zones are heterogeneously dispersed in such aquifers and are characterized by high concentrations of organic carbon and reduced phases, including iron sulfides and reduced forms of metals, including uranium(IV). The persistence of high concentrations of dissolved uranium(VI) at uranium-contaminated aquifers on the Colorado Plateau has been attributed to slow oxidation of insoluble uranium(IV) mineral phases that are found in association with these natural reducing zones, although there is little understanding of the relative importance of various potential oxidants. Three field experiments were conducted within an alluvial aquifer adjacent to the Colorado River near Rifle, CO wherein groundwater associated with naturally reduced zones was pumped into a gas-impermeable tank, mixed with a conservative tracer (Br-), bubbled with a gas phase composed of 97% O2 and 3% CO2, and then returned to the subsurface in the same well from which it was withdrawn. Within minutes of re-injection of the oxygenated groundwater, dissolved uranium(VI) concentrations increased from less than 1 μM to greater than 2.5 μM, demonstrating that oxygen can be an important oxidant for uranium in these field systems if supplied to the naturally reduced zones. Small concentrations of nitrate were also observed in the previously nitrate-free groundwater, and Fe(II) decreased to the detection limit. These results contrast with other laboratory and field results in which oxygen was introduced to systems containing high concentrations of mackinawite (FeS) rather than the more crystalline iron sulfides found in aged, naturally reduced zones. The flux of oxygen to the naturally reduced zones in the alluvial aquifers occurs mainly through interactions between groundwater and gas phases at the water table, and seasonal variations of the water table at the Rifle, CO site may play an important role in introducing oxygen into the system. Although oxygen was introduced directly to the naturally reduced zones in these experiments, delivery of oxidants to the system may normally be controlled by other oxidative pathways in which oxygen plays an indirect role.

ISOTOPE FRACTIONATION PROCESS

DOEpatents

Clewett, G.H.; Lee, DeW.A.

1958-05-20

A new method is described for isotopic enrichment of uranium. It has been found that when an aqueous acidic solution of ionic tetravalent uraniunn is contacted with chelate complexed tetravalent uranium, the U/sup 238/ preferentially concentrates in the complexed phase while U/sup 235/ concentrates in the ionic phase. The effect is enhanced when the chelate compound is water insoluble and is dissolved in a water-immiscible organic solvent. Cupferron is one of a number of sultable complexing agents, and chloroform is a suitable organic solvent.

SEPARATION OF URANIUM FROM THORIUM

DOEpatents

Hellman, N.N.

1959-07-01

A process is presented for separating uranium from thorium wherein the ratio of thorium to uranium is between 100 to 10,000. According to the invention the thoriumuranium mixture is dissolved in nitric acid, and the solution is prepared so as to obtain the desired concentration within a critical range of from 4 to 8 N with regard to the total nitrate due to thorium nitrate, with or without nitric acid or any nitrate salting out agent. The solution is then contacted with an ether, such as diethyl ether, whereby uranium is extracted into ihe organic phase while thorium remains in the aqueous phase.

Radiochemical analyses of surface water from U.S. Geological Survey hydrologic bench-mark stations

USGS Publications Warehouse

Janzer, V.J.; Saindon, L.G.

1972-01-01

The U.S. Geological Survey's program for collecting and analyzing surface-water samples for radiochemical constituents at hydrologic bench-mark stations is described. Analytical methods used during the study are described briefly and data obtained from 55 of the network stations in the United States during the period from 1967 to 1971 are given in tabular form.Concentration values are reported for dissolved uranium, radium, gross alpha and gross beta radioactivity. Values are also given for suspended gross alpha radioactivity in terms of natural uranium. Suspended gross beta radioactivity is expressed both as the equilibrium mixture of strontium-90/yttrium-90 and as cesium-137.Other physical parameters reported which describe the samples include the concentrations of dissolved and suspended solids, the water temperature and stream discharge at the time of the sample collection.

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.

Ground-water quality and geochemistry, Carson Desert, western Nevada

USGS Publications Warehouse

Lico, Michael S.; Seiler, R.L.

1994-01-01

Aquifers in the Carson Desert are the primary source of drinking water, which is highly variable in chemical composition. In the shallow basin-fill aquifers, water chemistyr varies from a dilute calcium bicarbonate-dominated water beneath the irrigated areas to a saline sodium chloride- dominated water beneath unirrigated areas. Water samples from the shallow aquifers commonly have dissolved solids, chloride, magnesium, sulfate, arsenic, and manganese concentrations that exceed State of Nevada drinking-water standards. Water in the intermediante basin-fill aquifers is a dilute sodium bicarbonate type in the Fallon area and a distinctly more saline sodium chloride type in the Soda Lake-Upsal Hogback area. Dissolved solids, chloride, arsenic, fluoride, and manganese concen- trations commonly exceed drinking-water standards. The basalt aquifer contains a dilute sodium bicarbonate chloride water. Arsenic concentrations exceed standards in all sampled wells. The concen- trations of major constituents in ground water beneath the southern Carson Desert are the result of evapotranspiration and natural geochemical reactions with minerals derived mostly from igneous rocks. Water with higher concentrations of iron and manganese is near thermodynamic equilibrium with siderite and rhodochrosite and indicates that these elements may be limited by the solubility of their respective carbonate minerals. Naturally occurring radionuclides (uranium and radon-222) are present in ground water from the Carson Desert in concen- tratons higher than proposed drinking-water standards. High uranium concentrations in the shallow aquifers may be caused by evaporative concentration and the release of uranium during dissolution of iron and manganese oxides or the oxidation of sedimentary organic matter that typically has elevated uranium concentrations. Ground water in the Carson Desert does not appear to have be contaminated by synthetic organic chemicals.

Chemical quality of ground water in Salt Lake Valley, Utah, 1969-85

USGS Publications Warehouse

Waddell, K.M.; Seiler, R.L.; Solomon, D.K.

1986-01-01

During 1979-84, 35 wells completed in the principal aquifer in the Salt Lake Valley, Utah, that had been sampled during 1962-67 were resampled to determine if water quality changes had occurred. The dissolved solids concentration of the water from 13 of the wells has increased by more than 10% since 1962-67. Much of the ground water between the mouth of Bingham Canyon and the Jordan River about 10 mi to the east has been contaminated by seepage from reservoirs and evaporation ponds associated with mining activities. Many domestic and irrigation wells yield water with concentrations of dissolved solids that exceed 2,000 mg/L. A reservoir in the mouth of Bingham Canyon contains acidic waters with a pH of 3 to 4 and concentrations of dissolved solids ranging from 43,000 to 68,000 mg/L. Seepage from evaporation ponds, which are about 4.5 mi east of the reservoir, also is acidic and contains similar concentrations of dissolved solids. East of the reservoir, where a steep hydraulic gradient exists along the mountain front, the velocities of contaminant movement were estimated to range from about 680-1,000 ft/yr. Groundwater underlying part of the community of South Salt Lake near the Jordan River has been contaminated by leachate from uranium-mill tailings. The major effect of the leachate from the tailings of the Vitro Chemical Co. on the shallow unconfined aquifer downgradient from the tailings was the contribution of measurable quantities of dissolved solids, chloride, sulfate, iron, and uranium. The concentration of dissolved solids in uncontaminated water was 1,650 mg/L, whereas downgradient from the tailings area, the concentrations ranged from 2,320-21,000 mg/L. The maximum volume of contaminated water was estimated to be 7,800 acre-ft. The major effect of the leachate from the Vitro tailings on the confined aquifer was the contribution of measurable quantities of dissolved solids, chloride, sulfate, and iron. The concentration of dissolved solids upgradient from the tailings was 330 mg/L, and beneath and downgradient from the tailings the concentrations were 864 and 1,240 mg/L. The minimum volume of contaminated water in the confined aquifer was estimated to be about 12,000 acre-ft. (Lantz-PTT)

Diel Sampling of Groundwater and Surface Water for Trace Elements and Select Water-Quality Constituents at a Former Zinc Smelter Site near Hegeler, Illinois, August 1-3, 2007

USGS Publications Warehouse

Kay, Robert T.; Groschen, George E.; Dupre, David H.; Drexler, Timothy D.; Thingvold, Karen L.; Rosenfeld, Heather J.

2009-01-01

Surface water can exhibit substantial diel variations in the concentration of a number of constituents. Sampling regimens that do not characterize diel variations in water quality can result in an inaccurate understanding of site conditions and of the threat posed by the site to human health and the environment. Surface- and groundwater affected by acid drainage were sampled every 60 to 90 minutes over a 48-hour period at a former zinc smelter known as the Hegeler Zinc Superfund Site, in Hegeler, Ill. Groundwater-quality data from a well at the site indicate stable, low pH, weakly oxidizing geochemical conditions in the aquifer. With the exceptions of temperature and pH, no constituents exhibited diel variations in groundwater. Variations in temperature and pH likely were not representative of conditions in the aquifer. Surface water was sampled at a site on Grape Creek. Diel variations were observed in temperature, dissolved oxygen, pH, and specific conductance, and in the concentrations of nitrite, barium, iron, lead, vanadium, and possibly uranium. Concentrations during the diel cycles varied by about an order of magnitude for nitrite and varied by about a factor of two for barium, iron, lead, vanadium, and uranium. Temperature, dissolved oxygen, specific conductance, nitrite, barium, lead, and uranium generally reached maximum values during the afternoon and minimum values during the night. Iron, vanadium, and pH generally reached minimum values during the afternoon and maximum values during the night. These variations would need to be accounted for during sampling of surface-water quality in similar hydrologic settings. The temperature variations in surface water were affected by variations in air temperature. Concentrations of dissolved oxygen were affected by variations in the intensity of photosynthetic activity and respiration. Nitrite likely was formed by the oxidation of ammonium by dissolved oxygen and degraded by its anaerobic oxidation by ammonium or as part of the decomposition of organic matter. Variations in pH were affected by the photoreduction of Fe3+ to Fe2+ and the precipitation of iron oxyhydroxides. Diel variations in concentrations of iron and vanadium were likely caused by variations in the dissolution and precipitation of iron oxyhydroxides, oxyhydroxysulfates, and hydrous sulfates, which may have been affected by in the intensity of insolation, iron photoreduction, and the concentration of dissolved oxygen. The concentrations of lead, uranium, and perhaps barium in Grape Creek may have been affected by competition for sorption sites on iron oxyhydroxides. Competition for sorption sites was likely affected by variations in pH and the concentration of Fe2+. Constituent concentrations likely also were affected by precipitation and dissolution of minerals that are sensitive to changes in pH, temperature, oxidation-reduction conditions, and biologic activity. The chemical and biologic processes that resulted in the diel variations observed in Grape Creek occurred within the surface-water column or in the underlying sediments.

Impact of uranyl-calcium-carbonato complexes on uranium(VI) adsorption to synthetic and natural sediments.

PubMed

Stewart, Brandy D; Mayes, Melanie A; Fendorf, Scott

2010-02-01

Adsorption on soil and sediment solids may decrease aqueous uranium concentrations and limit its propensity for migration in natural and contaminated settings. Uranium adsorption will be controlled in large part by its aqueous speciation, with a particular dependence on the presence of dissolved calcium and carbonate. Here we quantify the impact of uranyl speciation on adsorption to both goethite and sediments from the Hanford Clastic Dike and Oak Ridge Melton Branch Ridgetop formations. Hanford sediments were preconditioned with sodium acetate and acetic acid to remove carbonate grains, and Ca and carbonate were reintroduced at defined levels to provide a range of aqueous uranyl species. U(VI) adsorption is directly linked to UO(2)(2+) speciation, with the extent of retention decreasing with formation of ternary uranyl-calcium-carbonato species. Adsorption isotherms under the conditions studied are linear, and K(d) values decrease from 48 to 17 L kg(-1) for goethite, from 64 to 29 L kg (-1) for Hanford sediments, and from 95 to 51 L kg(-1) for Melton Branch sediments as the Ca concentration increases from 0 to 1 mM at pH 7. Our observations reveal that, in carbonate-bearing waters, neutral to slightly acidic pH values ( approximately 5) and limited dissolved calcium are optimal for uranium adsorption.

Diel cycles in dissolved barium, lead, iron, vanadium, and nitrite in a stream draining a former zinc smelter site near Hegeler, Illinois

USGS Publications Warehouse

Kay, R.T.; Groschen, G.E.; Cygan, G.; Dupre, David H.

2011-01-01

Diel variations in the concentrations of a number of constituents have the potential to substantially affect the appropriate sampling regimen in acidic streams. Samples taken once during the course of the day cannot adequately reflect diel variations in water quality and may result in an inaccurate understanding of biogeochemical processes, ecological conditions, and of the threat posed by the water to human health and the associated wildlife. Surface water and groundwater affected by acid drainage were sampled every 60 to 90. min over a 48-hour period at a former zinc smelter known as the Hegeler Zinc Superfund Site, near Hegeler, Illinois. Diel variations related to water quality in the aquifer were not observed in groundwater. Diel variations were observed in the temperature, pH, and concentration of dissolved oxygen, nitrite, barium, iron, lead, vanadium, and possibly uranium in surface water. Temperature, dissolved oxygen, nitrite, barium, lead, and uranium generally attained maximum values during the afternoon and minimum values during the night. Iron, vanadium, and pH generally attained minimum values during the afternoon and maximum values during the night. Concentrations of dissolved oxygen were affected by the intensity of photosynthetic activity and respiration, which are dependent upon insolation. Nitrite, an intermediary in many nitrogen reactions, may have been formed by the oxidation of ammonium by dissolved oxygen and converted to other nitrogen species as part of the decomposition of organic matter. The timing of the pH cycles was distinctly different from the cycles found in Midwestern alkaline streams and likely was the result of the photoreduction of Fe3+ to Fe 2+ and variations in the intensity of precipitation of hydrous ferric oxide minerals. Diel cycles of iron and vanadium also were primarily the result of variations in the intensity of precipitation of hydrous ferric oxide minerals. The diel variation in the concentrations of lead, uranium, and barium may have been affected by competition with Fe+2 for sorption sites on hydrous ferric oxide minerals. ?? 2010.

Magnesium transport extraction of transuranium elements from LWR fuel

DOEpatents

Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Miller, William E.; Pierce, R. Dean

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl.sub.2 and a U-Fe alloy containing not less than about 84% by weight uranium at a temperature in the range of from about 800.degree. C. to about 850.degree. C. to produce additional uranium metal which dissolves in the U-Fe alloy raising the uranium concentration and having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein. The CaCl.sub.2 having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO.sub.2. The Ca metal and CaCl.sub.2 is recycled to reduce additional oxide fuel. The U-Fe alloy having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with Mg metal which takes up the actinide and rare earth fission product metals. The U-Fe alloy retains the noble metal fission products and is stored while the Mg is distilled and recycled leaving the transuranium actinide and rare earth fission products isolated.

Quantitative Analysis of Uranium Accumulation on Sediments during Field-scale Biostimulation under Variable Bicarbonate Concentrations at the Rifle IFRC Site

NASA Astrophysics Data System (ADS)

Fox, P. M.; Davis, J. A.; Bargar, J.; Williams, K. H.; Singer, D. M.; Long, P.

2011-12-01

Bioremediation of uranium in subsurface environments is an approach that has been used at numerous field sites throughout the U.S in an attempt to lower dissolved U(VI) concentrations in groundwater. At the Rifle IFRC research site in Colorado, biostimulation of the native microbial population through acetate amendment for various periods of time has been tested in order to immobilize uranium through reduction U(VI) to U(IV). While this approach has successfully decreased U(VI) concentrations in the dissolved phase, often to levels below the EPA's maximum contaminant level of 0.13 μM, little work has examined the solid-phase accumulation of U during field-scale biostimulation. The lack of information on solid-phase U accumulation is due in large part to the difficulty of obtaining comparable pre- and post-biostimulation field sediment samples. In addition, the relatively low (<10 ppm) U concentrations present in most sediments preclude the use of spectroscopic techniques such as XAS for examining solid-phase U speciation. However, a recently developed technique of performing column experiments in situ has allowed us to overcome both of these problems, obtaining sediment samples which were exposed to the same biogeochemical conditions as subsurface sediments during the course of biostimulation. During the 2010 Rifle IFRC field experiment (dubbed "Super 8"), a number of in situ columns were deployed in various wells representing regions of the aquifer affected by acetate amendment (ambient bicarbonate) and concomitant acetate and bicarbonate amendment (elevated bicarbonate). Elevated levels of bicarbonate have been shown to cause desorption of U(VI) from the solid phase at the Rifle site under non-stimulated conditions, resulting in higher dissolved U(VI) concentrations in the aquifer. The Super 8 field experiment was designed in part to test the effect of elevated bicarbonate concentrations on U sequestration during biostimulation. Results from this experiment provide a comparison of temporal aqueous and solid-phase U concentrations under ambient and elevated bicarbonate conditions during field-scale biostimulation. Additionally, a subset of in situ columns amended with 20 μM U(VI) were analyzed by XANES in order to determine the relative importance of U(VI) and U(IV) in the solid phase. While the elevated bicarbonate concentrations did not impede reduction and sequestration of U, differences in the behavior of dissolved U(VI) after acetate amendment was stopped demonstrate the importance of U adsorption-desorption reactions in controlling dissolved U concentrations post-biostimulation.

Molecular-scale characterization of uranium sorption by bone apatite materials for a permeable reactive barrier demonstration

USGS Publications Warehouse

Fuller, C.C.; Bargar, J.R.; Davis, J.A.

2003-01-01

Uranium binding to bone charcoal and bone meal apatite materials was investigated using U LIII-edge EXAFS spectroscopy and synchrotron source XRD measurements of laboratory batch preparations in the absence and presence of dissolved carbonate. Pelletized bone char apatite recovered from a permeable reactive barrier (PRB) at Fry Canyon, UT, was also studied. EXAFS analyses indicate that U(VI) sorption in the absence of dissolved carbonate occurred by surface complexation of U(VI) for sorbed concentrations ??? 5500 ??g U(VI)/g for all materials with the exception of crushed bone char pellets. Either a split or a disordered equatorial oxygen shell was observed, consistent with complexation of uranyl by the apatite surface. A second shell of atoms at a distance of 2.9 A?? was required to fit the spectra of samples prepared in the presence of dissolved carbonate (4.8 mM total) and is interpreted as formation of ternary carbonate complexes with sorbed U(VI). A U-P distance at 3.5-3.6 A?? was found for most samples under conditions where uranyl phosphate phases did not form, which is consistent with monodentate coordination of uranyl by phosphate groups in the apatite surface. At sorbed concentrations ??? 5500 ??g U(VI)/g in the absence of dissolved carbonate, formation of the uranyl phosphate solid phase, chernikovite, was observed. The presence of dissolved carbonate (4.8 mM total) suppressed the formation of chernikovite, which was not detected even with sorbed U(VI) up to 12 300 ??g U(VI)/g in batch samples of bone meal, bone charcoal, and reagent-grade hydroxyapatite. EXAFS spectra of bone char samples recovered from the Fry Canyon PRB were comparable to laboratory samples in the presence of dissolved carbonate where U(VI) sorption occurred by surface complexation. Our findings demonstrate that uranium uptake by bone apatite will probably occur by surface complexation instead of precipitation of uranyl phosphate phases under the groundwater conditions found at many U-contaminated sites.

Nominations for the 2017 NNSA Pollution Prevention Awards

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

Salzman, Sonja L.; Ballesteros Rodriguez, Sonia; Lopez, Lorraine Bonds

In the field of nuclear forensics, one of the biggest challenges is to dissolve postdetonation debris for analysis. Debris generated after a nuclear detonation is a glassy material that is difficult to dissolve with chemicals. Traditionally, concentrated nitric acid, hydrofluoric acid, or sulfuric acid are employed during the dissolution. These acids, due to their corrosive nature, are not suitable for in-field/on-site sample preparations. Uranium oxides are commonly present in nuclear fuel processing plants and nuclear research facilities. In uranium oxides, the level of uranium isotope enrichment is a sensitive indicator for nuclear nonproliferation and is monitored closely by the Internationalmore » Atomic Energy Agency (IAEA) to ensure there is no misuse of nuclear material or technology for nuclear weapons. During an IAEA on-site inspection at a facility, environmental surface swipe samples are collected and transported to the IAEA headquarters or network of analytical laboratories for further processing. Uranium oxide particles collected on the swipe medium are typically dissolved with inorganic acids and are then analyzed for uranium isotopic compositions. To improve the responsiveness of on-site inspections, in-field detection techniques have been recently explored. However, in-field analysis is bottlenecked by time-consuming and hazardous dissolution procedures, as corrosive inorganic acids must be used. Corrosive chemicals are difficult to use in the field due to personnel safety considerations, and the transportation of such chemicals is highly regulated. It was therefore necessary to develop fast uranium oxide dissolution methods using less hazardous chemicals in support of the rapid infield detection of anomalies in declared nuclear processes.« less

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

DISSOLUTION OF URANIUM FUELS BY MONOOR DIFLUOROPHOSPHORIC ACID

DOEpatents

Johnson, R.; Horn, F.L.; Strickland, G.

1963-05-01

A method of dissolving and separating uranium from a uranium matrix fuel element by dissolving the uraniumcontaining matrix in monofluorophosphoric acid and/or difluorophosphoric acid at temperatures ranging from 150 to 275 un. Concent 85% C, thereafter neutralizing the solution to precipitate uranium solids, and converting the solids to uranium hexafluoride by treatment with a halogen trifluoride is presented. (AEC)

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.

Uraniferous opal, Virgin Valley, Nevada: conditions of formation and implications for uranium exploration

USGS Publications Warehouse

Zielinski, R.A.

1982-01-01

Uraniferous, fluorescent opal, which occurs in tuffaceous sedimentary rocks at Virgin Valley, Nevada, records the temperature and composition of uranium-rich solutions as well as the time of uranium-silica coprecipitation. Results are integrated with previous geologic and geochronologic data for the area to produce a model for uranium mobility that may be used to explore for uranium deposits in similar geologic settings. Uraniferous opal occurs as replacements of diatomite, or silicic air-fall ash layers in tuffaceous lakebeds of the Virgin Valley Formation (Miocene) of Merriam (1907). Fission-track radiography shows uranium to be homogeneously dispersed throughout the opal structure, suggesting coprecipitation of dissolved uranium and silica gel. Fluid inclusions preserved within opal replacements of diatomite have homogenization temperatures in the epithermal range and are of low salinity. Four samples of opal from one locality all have U-Pb apparent ages which suggest uraniferous opal precipitation in late Pliocene time. These ages correspond to a period of local, normal faulting, and highangle faults may have served as vertical conduits for transport of deep, thermalized ground water to shallower levels. Lateral migration of rising solutions occurred at intersections of faults with permeable strata. Silica and some uranium were dissolved from silica-rich host strata of 5-20 ppm original uranium content and reprecipitated as the solutions cooled. The model predicts that in similar geologic settings, ore-grade concentrations of uranium will occur in permeable strata that intersect high-angle faults and that contain uranium source rocks as well as efficient reductant traps for uranium. In the absence of sufficient quantities of reductant materials, uranium will be flushed from the system or will accumulate in low-grade disseminated hosts such as uraniferous opal. ?? 1982.

PROCESS FOR THE RECOVERY OF URANIUM

DOEpatents

Morris, G.O.

1955-06-21

This patent relates to a process for the recovery of uranium from impure uranium tetrafluoride. The process consists essentially of the steps of dissolving the impure uranium tetrafluoride in excess dilute sulfuric acid in the presence of excess hydrogen peroxide, precipitating ammonium uranate from the solution so formed by adding an excess of aqueous ammonia, dissolving the precipitate in sulfuric acid and adding hydrogen peroxide to precipitate uranium peroxdde.

Uranium distribution in the coastal waters and pore waters of Tampa Bay, Florida

USGS Publications Warehouse

Swarzenski, P.W.; Baskaran, M.

2006-01-01

The geochemical reactivity of uranium (238U) and dissolved organic carbon (DOC), Fe, Mn, Ba, and V was investigated in the water column, pore waters, and across a river/estuarine mixing zone in Tampa Bay, Florida. This large estuary is impacted both by diverse anthropogenic activity and by extensive U-rich phosphatic deposits. Thus, the estuarine behavior of uranium may be examined relative to such known U enrichments and anthropogenic perturbations. Dissolved (< 0.45??m) uranium exhibited both removal and enrichment processes across the Alafia River/estuarine mixing zone relative to conservative mixing. Such non-conservative U behavior may be attributed to: i) physical mixing processes within the river; ii) U carrier phase reactivity; and/or iii) fluid exchange processes across sediment/water interface. In the bay proper, U concentrations were ?????2 to 3 times greater than those reported for other estuarine systems and are likely a result of erosional inputs from the extensive, underlying U-rich phosphatic deposits. Whereas dissolved U concentrations generally did not approach seawater values (13.6??nM) along the Alafia River salinity transect, water column U concentrations exceeded 16??nM in select regions of the bay. Within the hydrogeological framework of the bay, such enriched U may also be derived from advective fluid transport processes across the sediment/water interface, such as submarine groundwater discharge (SGD) or hyporheic exchange within coastal rivers. Pore water profiles of U in Tampa Bay show both a flux into and out of bottom sediments, and average, diffusive U pore water fluxes (Jdiff) ranged from - 82.0 to 116.6??mol d- 1. It is likely that negative U fluxes imply seawater entrainment or infiltration (i.e., submarine groundwater recharge), which may contribute to the removal of water column uranium. For comparison, a bay-wide, Ra-derived submarine groundwater discharge estimate for Tampa Bay (8??L m- 2 d- 1) yielded an average, advective (JSGD) U flux of 112.9??mol d- 1. In Tampa Bay, the estuarine distribution of U indicates a strong natural, geologic control that may also be influenced by enhanced fluid transport processes across the sediment/water interface. ?? 2006 Elsevier B.V. All rights reserved.

Geochemical reconnaissance study of Vassar Meadow (Adams Rib) wetlands and vicinity, Eagle County, Colorado

USGS Publications Warehouse

Owen, Douglass E.; Breit, George N.

1995-01-01

Wetlands are known to be efficient filters of metals dissolved in ground and surface waters. This paper presents the results of geochemical reconnaissance sampling done at the request of the U.S. Environmental Protection Agency in wetlands in Vassar Meadow, Eagle County, Colorado. Ten wetlands were sampled and found to be variously enriched in chromium, molybdenum, and uranium. The uranium and chromium concentrations (and, to a lesser extent, molybdenum) represent an environmental concern should they be released as a result of anthropogenic disturbance. The metal accumulation in these wetlands documents that the wetlands have been functioning as filters that protect water quality in East Brush Creek by lowering the dissolved metal content in water.

Control and distribution of uranium in coral reefs during diagenesis

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

Gvirtzman, G.; Friedman, G.M.; Miller, D.S.

1973-12-01

The concentration of about 2 ppM of uranium in the aragonitic skeletons of modern scleractinian corals which we studied is a constant value, regardless of occurrence, anatomy, or taxonomy. The presence of cement of aragonite or high- magnesian calcite usually raises the concentration of bulk samples to about 3 ppM. Modern corals may contain up to 50% of cementing minerals. Organisms, such as corals and coralline algae, while secreting their skeleton, discriminate against the uptake of uranium, whereas the uptake of uranium by mineral cements is less restrained. Aragonite cement contains about 3.6 ppM and highmagnesian calcite cement 2.6 ppMmore » uranium. During leaching by freshwater, the aragonite of the skeletons of corals dissolves out. This creates hollow molds which fill with drusy low-magnesian calcite. In emergent reefs from the shores of the Red Sea which display the ellects of progressive diagenesis this calcite is enriched in uranium (3.9 ppM) beyond that found in marine cements. Second-generation calcite, which fills original voids in the corals from the emergent reefs, contains a lower level of uranium concent ration (1.3 ppM). The level of concentration of uranium in low-magnesian calcite of diagenetically altered corals is a function of the availability of uranium in meteoric waters. In aragonite as well as in high- and low-magnesian calcite uranium replaces calcium or occupies lattice vacancies in the crystal lattice. (auth)« less

Impact of uranyl-calcium-carbonato complexes on uranium(VI) adsorption to synthetic and natural sediments

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

Stewart, B.D.; Mayes, Melanie; Fendorf, Scott

2010-01-01

Adsorption on soil and sediment solids may decrease aqueous uranium concentrations and limit its propensity for migration in natural and contaminated settings. Uranium adsorption will be controlled in large part by its aqueous speciation, with a particular dependence on the presence of dissolved calcium and carbonate. Here we quantify the impact of uranyl speciation on adsorption to both goethite and sediments from the Hanford Clastic Dike and Oak Ridge Melton Branch Ridgetop formations. Hanford sediments were preconditioned with sodium acetate and acetic acid to remove carbonate grains, and Ca and carbonate were reintroduced at defined levels to provide a rangemore » of aqueous uranyl species. U(VI) adsorption is directly linked to UO{sub 2}{sup 2+} speciation, with the extent of retention decreasing with formation of ternary uranyl-calcium-carbonato species. Adsorption isotherms under the conditions studied are linear, and K{sub d} values decrease from 48 to 17 L kg{sup -1} for goethite, from 64 to 29 L kg{sup -1} for Hanford sediments, and from 95 to 51 L kg{sup -1} for Melton Branch sediments as the Ca concentration increases from 0 to 1 mM at pH 7. Our observations reveal that, in carbonate-bearing waters, neutral to slightly acidic pH values ({approx}5) and limited dissolved calcium are optimal for uranium adsorption.« less

Radiation dose-dependent risk on individuals due to ingestion of uranium and radon concentration in drinking water samples of four districts of Haryana, India

NASA Astrophysics Data System (ADS)

Panghal, Amanjeet; Kumar, Ajay; Kumar, Suneel; Singh, Joga; Sharma, Sumit; Singh, Parminder; Mehra, Rohit; Bajwa, B. S.

2017-06-01

Uranium gets into drinking water when the minerals containing uranium are dissolved in groundwater. Uranium and radon concentrations have been measured in drinking water samples from different water sources such as hand pumps, tube wells and bore wells at different depths from various locations of four districts (Jind, Rohtak, Panipat and Sonipat) of Haryana, India, using the LED flourimetry technique and RAD7, electronic silicon solid state detector. The uranium (238U) and radon (222Rn) concentrations in water samples have been found to vary from 1.07 to 40.25 µg L-1 with an average of 17.91 µg L-1 and 16.06 ± 0.97 to 57.35 ± 1.28 Bq L-1 with an average of 32.98 ± 2.45 Bq L-1, respectively. The observed value of radon concentration in 43 samples exceeded the recommended limits of 11 Bq L-1 (USEPA) and all the values are within the European Commission recommended limit of 100 Bq L-1. The average value of uranium concentration is observed to be within the safe limit recommended by World Health Organization (WHO) and Atomic Energy Regulatory Board. The annual effective dose has also been measured in all the water samples and is found to be below the prescribed dose limit of 100 µSv y-1 recommended by WHO. Risk assessment of uranium in water is also calculated using life time cancer risk, life time average daily dose and hazard quotient. The high uranium concentration observed in certain areas is due to interaction of ground water with the soil formation of this region and the local subsurface geology of the region.

Uranium isotopes in rivers, estuaries and adjacent coastal sediments of western India: their weathering, transport and oceanic budget

NASA Astrophysics Data System (ADS)

Borole, D. V.; Krishnaswami, S.; Somayajulu, B. L. K.

1982-02-01

The two major river systems on the west coast of India, Narbada and Tapti, their estuaries and the coastal Arabian sea sediments have been extensively studied for their uranium concentrations and 238U /238U activity ratios. The 238U concentrations in the aqueous phase of these river systems exhibit a strong positive correlation with the sum of the major cations, σ Na + K + Mg + Ca, and with the HCO 3- ion contents. The abundance ratio of dissolved U to the sum of the major cations in these waters is similar to their ratio in typical crustal rocks. These findings lead us to conclude that 238U is brought into the aqueous phase along with major cations and bicarbonate. The strong positive correlation between 238U and total dissolved salts for selected rivers of the world yield an annual dissolved 238U flux of 0.88 × 10 10g/ yr to the oceans, a value very similar to its removal rate from the oceans, 1.05 × 10 10g/ yr, estimated based on its correlation with HCO 3- contents of rivers. In the estuaries, both 238U and its great-grand daughter 234U behave conservatively beyond chlorosities 0.14 g/l. These data confirm our earlier findings in other Indian estuaries. The behavior of uranium isotopes in the chlorosity zone 0.02-0.14 g/l, was studied in the Narbada estuary in some detail. The results, though not conclusive, seem to indicate a minor removal of these isotopes in this region. Reexamination of the results for the Gironde and Zaire estuaries (Martin et al., 1978a and b) also appear to confirm the conservative behavior of U isotopes in unpolluted estuaries. It is borne out from all the available data that estuaries beyond 0.14 g/l chlorosities act neither as a sink nor as a source for uranium isotopes, the behavior in the low chlorosity zones warrants further detailed investigation. A review of the uranium isotope measurements in river waters yield a discharge weighted-average 238U concentration of 0.22 μg/l with a 234U /238U activity ratio of 1.20 ± 0.06 ismissing. The residence time of uranium isotopes in the oceans estimated from the 238U concentration and the 234U /238U A. R. of the rivers yield conflicting results; the material balance of uranium isotopes in the marine environment still remains a paradox. If the disparity between the results is real, then an additional 234U flux of about 0.25 dpm/cm 2·10 3 yr into the oceans (about 20% of its river supply) is necessitated.

Long-term in situ oxidation of biogenic uraninite in an alluvial aquifer: impact of dissolved oxygen and calcium.

PubMed

Lezama-Pacheco, Juan S; Cerrato, José M; Veeramani, Harish; Alessi, Daniel S; Suvorova, Elena; Bernier-Latmani, Rizlan; Giammar, Daniel E; Long, Philip E; Williams, Kenneth H; Bargar, John R

2015-06-16

Oxidative dissolution controls uranium release to (sub)oxic pore waters from biogenic uraninite produced by natural or engineered processes, such as bioremediation. Laboratory studies show that uraninite dissolution is profoundly influenced by dissolved oxygen (DO), carbonate, and solutes such as Ca(2+). In complex and heterogeneous subsurface environments, the concentrations of these solutes vary in time and space. Knowledge of dissolution processes and kinetics occurring over the long-term under such conditions is needed to predict subsurface uranium behavior and optimize the selection and performance of uraninite-based remediation technologies over multiyear periods. We have assessed dissolution of biogenic uraninite deployed in wells at the Rifle, CO, DOE research site over a 22 month period. Uraninite loss rates were highly sensitive to DO, with near-complete loss at >0.6 mg/L over this period but no measurable loss at lower DO. We conclude that uraninite can be stable over decadal time scales in aquifers under low DO conditions. U(VI) solid products were absent over a wide range of DO values, suggesting that dissolution proceeded through complexation and removal of oxidized surface uranium atoms by carbonate. Moreover, under the groundwater conditions present, Ca(2+) binds strongly to uraninite surfaces at structural uranium sites, impacting uranium fate.

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

Radionuclides from past uranium mining in rivers of Portugal.

PubMed

Carvalho, Fernando P; Oliveira, João M; Lopes, Irene; Batista, Aleluia

2007-01-01

During several decades and until a few years ago, uranium mines were exploited in the Centre of Portugal and wastewaters from uranium ore milling facilities were discharged into river basins. To investigate enhancement of radioactivity in freshwater ecosystems, radionuclides of uranium and thorium series were measured in water, sediments, suspended matter, and fish samples from the rivers Vouga, Dão, Távora and Mondego. The results show that these rivers carry sediments with relatively high naturally occurring radioactivity, and display relatively high concentrations of radon dissolved in water, which is typical of a uranium rich region. Riverbed sediments show enhanced concentrations of radionuclides in the mid-section of the Mondego River, a sign of past wastewater discharges from mining and milling works at Urgeiriça confirmed by the enhanced values of (238)U/(232)Th radionuclide ratios in sediments. Radionuclide concentrations in water, suspended matter and freshwater fish from that section of Mondego are also enhanced in comparison with concentrations measured in other rivers. Based on current radionuclide concentrations in fish, regular consumption of freshwater species by local populations would add 0.032 mSv a(-1) of dose equivalent (1%) to the average background radiation dose. Therefore, it is concluded that current levels of enhanced radioactivity do not pose a significant radiological risk either to aquatic fauna or to freshwater fish consumers.

Alpha emitting radionuclides in drainage from Quinta do Bispo and Cunha Baixa uranium mines (Portugal) and associated radiotoxicological risk.

PubMed

Carvalho, Fernando P; Oliveira, João M; Faria, Isabel

2009-11-01

Two large uranium mines, Quinta do Bispo and Cunha Baixa, district of Viseu, North of Portugal, were exploited until 1991. Sulfuric acid was used for in situ uranium leaching in Cunha Baixa mine and for heap leaching of low grade ores at both mines. Large amounts of mining and milling residues were accumulated nearby. Since closure of mines, the treatment of acid mine waters has been maintained and treated water is released into surface water lines. Analysis of radionuclides in the soluble phase and in the suspended matter of water samples from the uranium mines, from the creeks receiving the discharges of mine effluents, from the rivers and from wells in this area, show an enhancement of radioactivity levels. For example, downstream the discharge of mine effluents into Castelo Stream, the concentrations of dissolved uranium isotopes and uranium daughters were up to 14 times the concentrations measured upstream; (238)U concentration in suspended particulate matter of Castelo Stream reached 72 kBq kg(-1), which is about 170 times higher than background concentrations in Mondego River. Nevertheless, radionuclide concentrations decreased rapidly to near background values within a distance of about 7 kilometers from the discharge point. Enhancement of radioactivity in underground waters was positively correlated with a decrease in water pH and with an increase of sulfate ion concentration, pointing out to Cunha Baixa mine as the source of groundwater contamination. The radiotoxic exposure risk arising from using these well waters as drinking water and as irrigation water is discussed and implementation of environmental remediation measures is advised.

The effect of hydrogen peroxide on uranium oxide films on 316L stainless steel

NASA Astrophysics Data System (ADS)

Wilbraham, Richard J.; Boxall, Colin; Goddard, David T.; Taylor, Robin J.; Woodbury, Simon E.

2015-09-01

For the first time the effect of hydrogen peroxide on the dissolution of electrodeposited uranium oxide films on 316L stainless steel planchets (acting as simulant uranium-contaminated metal surfaces) has been studied. Analysis of the H2O2-mediated film dissolution processes via open circuit potentiometry, alpha counting and SEM/EDX imaging has shown that in near-neutral solutions of pH 6.1 and at [H2O2] ⩽ 100 μmol dm-3 the electrodeposited uranium oxide layer is freely dissolving, the associated rate of film dissolution being significantly increased over leaching of similar films in pH 6.1 peroxide-free water. At H2O2 concentrations between 1 mmol dm-3 and 0.1 mol dm-3, formation of an insoluble studtite product layer occurs at the surface of the uranium oxide film. In analogy to corrosion processes on common metal substrates such as steel, the studtite layer effectively passivates the underlying uranium oxide layer against subsequent dissolution. Finally, at [H2O2] > 0.1 mol dm-3 the uranium oxide film, again in analogy to common corrosion processes, behaves as if in a transpassive state and begins to dissolve. This transition from passive to transpassive behaviour in the effect of peroxide concentration on UO2 films has not hitherto been observed or explored, either in terms of corrosion processes or otherwise. Through consideration of thermodynamic solubility product and complex formation constant data, we attribute the transition to the formation of soluble uranyl-peroxide complexes under mildly alkaline, high [H2O2] conditions - a conclusion that has implications for the design of both acid minimal, metal ion oxidant-free decontamination strategies with low secondary waste arisings, and single step processes for spent nuclear fuel dissolution such as the Carbonate-based Oxidative Leaching (COL) process.

Characteristics of NORM in the oil industry from eastern and western deserts of Egypt.

PubMed

Shawky, S; Amer, H; Nada, A A; El-Maksoud, T M; Ibrahiem, N M

2001-07-01

Naturally occurring radionuclides (NORs) from the 232Th- and 238U-series, which are omnipresent in the earth's crust, can be concentrated by technical activities, particularly those involving natural resources. Although, a great deal of work has been done in the field of radiation protection and remedial action on uranium and other mines, recent concern has been devoted to the hazard arising from naturally occurring radioactive materials (NORM) in oil and gas facilities. NORM wastes associated with oil and gas operations from scale deposits, separated sludge and water at different oil fields in the eastern and western deserts were investigated. Concentrations of the uranium, thorium, and potassium (40K) series have been determined from high-resolution gamma-ray spectrometry. Total uranium content of samples was determined using laser fluorimetry. The levels of radioactivity were mainly due to enhanced levels of dissolved radium ions. Only minute quantities of uranium and thorium were present. The disequilibrium factor for 238U/226Ra has been determined.

REMOVAL OF CHLORIDE FROM AQUEOUS SOLUTIONS

DOEpatents

Hyman, M.L.; Savolainen, J.E.

1960-01-01

A method is given for dissolving reactor fuel elements in which the uranium is associated with a relatively inert chromium-containing alloy such as stainless steel. An aqueous mixture of acids comprising 2 to 2.5 molar hydrochloric acid and 4 to 8 molar nitric acid is employed in dissolving the fuel element. In order io reduce corrosion in subsequent processing of the resulting solution, chloride values are removed from the solution by contacting it with concentrated nitric acid at an elevated temperature.

Chemical analysis of water samples and geophysical logs from cored test holes drilled in the central Oklahoma Aquifer, Oklahoma

USGS Publications Warehouse

Schlottmann, Jamie L.; Funkhouser, Ron A.

1991-01-01

Chemical analyses of water from eight test holes and geophysical logs for nine test holes drilled in the Central Oklahoma aquifer are presented. The test holes were drilled to investigate local occurrences of potentially toxic, naturally occurring trace substances in ground water. These trace substances include arsenic, chromium, selenium, residual alpha-particle activities, and uranium. Eight of the nine test holes were drilled near wells known to contain large concentrations of one or more of the naturally occurring trace substances. One test hole was drilled in an area known to have only small concentrations of any of the naturally occurring trace substances.Water samples were collected from one to eight individual sandstone layers within each test hole. A total of 28 water samples, including four duplicate samples, were collected. The temperature, pH, specific conductance, alkalinity, and dissolved-oxygen concentrations were measured at the sample site. Laboratory determinations included major ions, nutrients, dissolved organic carbon, and trace elements (aluminum, arsenic, barium, beryllium, boron, cadmium, chromium, hexavalent chromium, cobalt, copper, iron, lead, lithium, manganese, mercury, molybdenum, nickel, selenium, silver, strontium, vanadium and zinc). Radionuclide activities and stable isotope (5 values also were determined, including: gross-alpha-particle activity, gross-beta-particle activity, radium-226, radium-228, radon-222, uranium-234, uranium-235, uranium-238, total uranium, carbon-13/carbon-12, deuterium/hydrogen-1, oxygen-18/oxygen-16, and sulfur-34/sulfur-32. Additional analyses of arsenic and selenium species are presented for selected samples as well as analyses of density and iodine for two samples, tritium for three samples, and carbon-14 for one sample.Geophysical logs for most test holes include caliper, neutron, gamma-gamma, natural-gamma logs, spontaneous potential, long- and short-normal resistivity, and single-point resistance. Logs for test-hole NOTS 7 do not include long- and short-normal resistivity, spontaneous-potential, or single-point resistivity. Logs for test-hole NOTS 7A include only caliper and natural-gamma logs.

Uranium in foraminiferal calcite as a recorder of seawater uranium concentrations

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

Russell, A.D.; Emerson, S.; Nelson, B.K.

The authors present results of an investigation of uranium/calcium ratios in cleaned foraminiferal calcite as a recorder of seawater uranium concentrations. For accurate reconstruction of past seawater uranium content, shell calcite must incorporate uranium in proportion to seawater concentration and must preserve its original uranium composition over time. Laboratory culture experiments with live benthic (Amphistegina lobifera) and live planktonic (Globigerinell calida) foraminifera show that the U/Ca ratio of cleaned calcite tests is proportional to the concentration of uranium in solution. After correcting results for the presence of initial calcite, the apparent distribution coefficient D = (U/Ca[sub calcite])/(U/Ca)[sub solution] = 10.6more » [+-] 0.3 (x10[sup [minus]3]) for A. lobifera and D = 7.9 [+-] 0.1 (x10[sup [minus]3]) for G. calida. U/Ca ratios in planktonic foraminifera from core tops collected above 3900 m in the equatorial Atlantic and above 2100 m in the Pacific Ocean show no significant difference among the species analyzed. D estimated form core top samples ranges from 7.6 [+-] 0.4 (x10[sup [minus]3]) for O. universa to 8.4 [+-] 0.5 (x10[sup [minus]3]) for G. ruber. In benthic species C. wuellerstorfi, D = 7.0 [+-] 0.8 (x10[sup [minus]3]). U/Ca and Mg/Ca in G. tumida and G. sacculifer from core tops taken near and below the regional lysocline decrease with water depth. Smaller decreases in U/Ca and Mg/Ca with depth were observed in C. wuellerstorfi. In the planktonic species, the authors believe that U/CA and Mg/Ca are lower in the more dissolution-resistant fraction of calcite, leading to lower U/Ca in more highly dissolved samples.« less

Groundwater-quality characteristics for the Wyoming Groundwater-Quality Monitoring Network, November 2009 through September 2012

USGS Publications Warehouse

Boughton, Gregory K.

2014-01-01

Groundwater samples were collected from 146 shallow (less than or equal to 500 feet deep) wells for the Wyoming Groundwater-Quality Monitoring Network, from November 2009 through September 2012. Groundwater samples were analyzed for physical characteristics, major ions and dissolved solids, trace elements, nutrients and dissolved organic carbon, uranium, stable isotopes of hydrogen and oxygen, volatile organic compounds, and coliform bacteria. Selected samples also were analyzed for gross alpha radioactivity, gross beta radioactivity, radon, tritium, gasoline range organics, diesel range organics, dissolved hydrocarbon gases (methane, ethene, and ethane), and wastewater compounds. Water-quality measurements and concentrations in some samples exceeded numerous U.S. Environmental Protection Agency (EPA) drinking water standards. Physical characteristics and constituents that exceeded EPA Maximum Contaminant Levels (MCLs) in some samples were arsenic, selenium, nitrite, nitrate, gross alpha activity, and uranium. Total coliforms and Escherichia coli in some samples exceeded EPA Maximum Contaminant Level Goals. Measurements of pH and turbidity and concentrations of chloride, sulfate, fluoride, dissolved solids, aluminum, iron, and manganese exceeded EPA Secondary Maximum Contaminant Levels in some samples. Radon concentrations in some samples exceeded the alternative MCL proposed by the EPA. Molybdenum and boron concentrations in some samples exceeded EPA Health Advisory Levels. Water-quality measurements and concentrations also exceeded numerous Wyoming Department of Environmental Quality (WDEQ) groundwater standards. Physical characteristics and constituents that exceeded WDEQ Class I domestic groundwater standards in some samples were measurements of pH and concentrations of chloride, sulfate, dissolved solids, iron, manganese, boron, selenium, nitrite, and nitrate. Measurements of pH and concentrations of chloride, sulfate, dissolved solids, aluminum, iron, manganese, boron, and selenium exceeded WDEQ Class II agriculture groundwater standards in some samples. Measurements of pH and concentrations of sulfate, dissolved solids, aluminum, boron, and selenium exceeded WDEQ Class III livestock groundwater standards in some samples. The concentrations of dissolved solids in two samples exceeded the WDEQ Class IV industry groundwater standard. Measurements of pH and concentrations of dissolved solids, aluminum, iron, manganese, and selenium exceeded WDEQ Class special (A) fish and aquatic life groundwater standards in some samples. Stable isotopes of hydrogen and oxygen measured in water samples were compared to the Global Meteoric Water Line and Local Meteoric Water Lines. Results indicated that recharge to all of the wells was derived from precipitation and that the water has undergone some fractionation, possibly because of evaporation. Concentrations of organic compounds did not exceed any State or Federal water-quality standards. Few volatile organic compounds were detected in samples, whereas gasoline range organics, diesel range organics, and methane were detected most frequently. Concentrations of wastewater compounds did not exceed any State or Federal water-quality standards. The compounds N,N-diethyl-meta-toluamide (DEET), benzophenone, and phenanthrene were detected most frequently. Bacteria samples were collected, processed, incubated, and enumerated in the field or at the U.S. Geological Survey Wyoming-Montana Water Science Center. Total coliforms and Escherichia coli were detected in some samples.

Ground-Water Quality of the Northern High Plains Aquifer, 1997, 2002-04

USGS Publications Warehouse

Stanton, Jennifer S.; Qi, Sharon L.

2007-01-01

An assessment of ground-water quality in the northern High Plains aquifer was completed during 1997 and 2002-04. Ground-water samples were collected at 192 low-capacity, primarily domestic wells in four major hydrogeologic units of the northern High Plains aquifer-Ogallala Formation, Eastern Nebraska, Sand Hills, and Platte River Valley. Each well was sampled once, and water samples were analyzed for physical properties and concentrations of nitrogen and phosphorus compounds, pesticides and pesticide degradates, dissolved solids, major ions, trace elements, dissolved organic carbon (DOC), radon, and volatile organic compounds (VOCs). Tritium and microbiology were analyzed at selected sites. The results of this assessment were used to determine the current water-quality conditions in this subregion of the High Plains aquifer and to relate ground-water quality to natural and human factors affecting water quality. Water-quality analyses indicated that water samples rarely exceeded established U.S. Environmental Protection Agency public drinking-water standards for those constituents sampled; 13 of the constituents measured or analyzed exceeded their respective standards in at least one sample. The constituents that most often failed to meet drinking-water standards were dissolved solids (13 percent of samples exceeded the U.S. Environmental Protection Agency Secondary Drinking-Water Regulation) and arsenic (8 percent of samples exceeded the U.S. Environmental Protection Agency Maximum Contaminant Level). Nitrate, uranium, iron, and manganese concentrations were larger than drinking-water standards in 6 percent of the samples. Ground-water chemistry varied among hydrogeologic units. Wells sampled in the Platte River Valley and Eastern Nebraska units exceeded water-quality standards more often than the Ogallala Formation and Sand Hills units. Thirty-one percent of the samples collected in the Platte River Valley unit had nitrate concentrations greater than the standard, 22 percent exceeded the manganese standard, 19 percent exceeded the sulfate standard, 26 percent exceeded the uranium standard, and 38 percent exceeded the dissolved-solids standard. In addition, 78 percent of samples had at least one detectable pesticide and 22 percent of samples had at least one detectable VOC. In the Eastern Nebraska unit, 30 percent of the samples collected had dissolved-solids concentrations larger than the standard, 23 percent exceeded the iron standard, 13 percent exceeded the manganese standard, 10 percent exceeded the arsenic standard, 7 percent exceeded the sulfate standard, 7 percent exceeded the uranium standard, and 7 percent exceeded the selenium standard. No samples exceeded the nitrate standard. Thirty percent of samples had at least one detectable pesticide compound and 10 percent of samples had at least one detectable VOC. In contrast, the Sand Hills and Ogallala Formation units had fewer detections of anthropogenic compounds and drinking-water exceedances. In the Sand Hills unit, 15 percent of the samples exceeded the arsenic standard, 4 percent exceeded the nitrate standard, 4 percent exceeded the uranium standard, 4 percent exceeded the iron standard, and 4 percent exceeded the dissolved-solids standard. Fifteen percent of samples had at least one pesticide compound detected and 4 percent had at least one VOC detected. In the Ogallala Formation unit, 6 percent of water samples exceeded the arsenic standard, 4 percent exceeded the dissolved-solids standard, 3 percent exceeded the nitrate standard, 2 percent exceeded the manganese standard, 1 percent exceeded the iron standard, 1 percent exceeded the sulfate standard, and 1 percent exceeded the uranium standard. Eight percent of samples collected in the Ogallala Formation unit had at least one pesticide detected and 6 percent had at least one VOC detected. Differences in ground-water chemistry among the hydrogeologic units were attributed to variable depth to water, depth of the well screen below the water table, reduction-oxidation conditions, ground-water residence time, interactions with surface water, composition of aquifer sediments, extent of cropland, extent of irrigated land, and fertilizer application rates.

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.

Mechanisms of uranium interactions with hydroxyapatite: Implications for groundwater remediation

USGS Publications Warehouse

Fuller, C.C.; Bargar, J.R.; Davis, J.A.; Piana, M.J.

2002-01-01

The speciation of U(VI) sorbed to synthetic hydroxyapatite was investigated using a combination of U LIII-edge XAS, synchrotron XRD, batch uptake measurements, and SEM-EDS. The mechanisms of U(VI) removal by apatite were determined in order to evaluate the feasibility of apatitebased in-situ permeable reactive barriers (PRBs). In batch U(VI) uptake experiments with synthetic hydroxyapatite (HA), near complete removal of dissolved uranium (>99.5%) to <0.05 ??M was observed over a range of total U(VI) concentrations up to equimolar of the total P in the suspension. XRD and XAS analyses of U(VI)-reacted HA at sorbed concentrations ???4700 ppm U(VI) suggested that uranium(VI) phosphate, hydroxide, and carbonate solids were not present at these concentrations. Fits to EXAFS spectra indicate the presence of Ca neighbors at 3.81 A??. U-Ca separation, suggesting that U(VI) adsorbs to the HA surfaces as an inner-sphere complex. Uranium(VI) phosphate solid phases were not detected in HA with 4700 ppm sorbed U(VI) by backscatter SEM or EDS, in agreement with the surface complexation process. In contrast, U(VI) speciation in samples that exceeded 7000 ppm sorbed U(VI) included a crystalline uranium(VI) phosphate solid phase, identified as chernikovite by XRD. At these higher concentrations, a secondary, uranium(VI) phosphate solid was detected by SEM-EDS, consistent with chernikovite precipitation. Autunite formation occurred at total U:P molar ratios ???0.2. Our findings provide a basis for evaluating U(VI) sorption mechanisms by commercially available natural apatites for use in development of PRBs for groundwater U(VI) remediation.

Uranium series dating of Allan Hills ice

NASA Technical Reports Server (NTRS)

Fireman, E. L.

1986-01-01

Uranium-238 decay series nuclides dissolved in Antarctic ice samples were measured in areas of both high and low concentrations of volcanic glass shards. Ice from the Allan Hills site (high shard content) had high Ra-226, Th-230 and U-234 activities but similarly low U-238 activities in comparison with Antarctic ice samples without shards. The Ra-226, Th-230 and U-234 excesses were found to be proportional to the shard content, while the U-238 decay series results were consistent with the assumption that alpha decay products recoiled into the ice from the shards. Through this method of uranium series dating, it was learned that the Allen Hills Cul de Sac ice is approximately 325,000 years old.

Seasonal uranium distributions in the coastal waters off the Amazon and Mississippi Rivers

USGS Publications Warehouse

Swarzenski, P.W.; McKee, B.A.

1998-01-01

The chemical reactivity of uranium was investigated across estuarine gradients from two of the world's largest river systems: the Amazon and Mississippi. Concentrations of dissolved (<0.45 ??m) uranium (U) were measured in surface waters of the Amazon shelf during rising (March 1990), flood (June 1990) and low (November 1991) discharge regimes. The dissolved U content was also examined in surface waters collected across estuarine gradients of the Mississippi outflow region during April 1992, August 1993, and November (1993). All water samples were analyzed for U by isotope dilution inductively coupled plasma mass spectrometry (ICP-MS). In Amazon shelf surface waters uranium increased nonconservatively from about 0.01 ??g l-1 at the river's mouth to over 3 ??g l-1 at the distal site, irrespective of river discharge stage. Observed large-scale U removal at salinities generally less than 15 implies a) that riverine dissolved U was extensively adsorbed by freshly-precipitated hydrous metal oxides (e.g., FeOOH, MnO2) as a result of flocculation and aggregation, and b) that energetic resuspension and reworking of shelf sediments and fluid muds on the Amazon shelf released a chemically reactive particle/colloid to the water column which can further scavenge dissolved U across much of the estuarine gradient. In contrast, the estuarine chemistry of U is inconclusive within surface waters of the Mississippi shelf-break region. U behavior is most likely controlled less by traditional sorption and/or desorption reactions involving metal oxides or colloids than by the river's variable discharge regime (e.g., water parcel residence time during estuarine mixing, nature of particulates, sediment storage and resuspension in the confined lower river), and plume dispersal. Mixing of the thin freshwater lens into ambient seawater is largely defined by wind-driven rather than physical processes. As a consequence, in the Mississippi outflow region uranium predominantly displays ConserVative behavior; removal is evident only during anomalous river discharge regimes. 'Products-approach' mixing experiments conducted during the Flood of 1993 suggest the importance of small particles and/or colloids in defining a depleted U versus salinity distribution.

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.

Investigation of residual anode material after electrorefining uranium in molten chloride salt

NASA Astrophysics Data System (ADS)

Rose, M. A.; Williamson, M. A.; Willit, J.

2015-12-01

A buildup of material at uranium anodes during uranium electrorefining in molten chloride salts has been observed. Potentiodynamic testing has been conducted using a three electrode cell, with a uranium working electrode in both LiCl/KCl eutectic and LiCl each containing ∼5 mol% UCl3. The anodic current response was observed at 50° intervals between 450 °C and 650 °C in the eutectic salt. These tests revealed a buildup of material at the anode in LiCl/KCl salt, which was sampled at room temperature, and analyzed using ICP-MS, XRD and SEM techniques. Examination of the analytical data, current response curves and published phase diagrams has established that as the uranium anode dissolves, the U3+ ion concentration in the diffusion layer surrounding the electrode rises precipitously to levels, which may at low temperatures exceed the solubility limit for UCl3 or in the case of the eutectic salt for K2UCl5. The reduction in current response observed at low temperature in eutectic salt is eliminated at 650 °C, where K2UCl5 is absent due to its congruent melting and only simple concentration polarization effects are seen. In LiCl similar concentration effects are seen though significantly longer time at applied potential is required to effect a reduction in the current response as compared to the eutectic salt.

URANOUS IODATE AS A CARRIER FOR PLUTONIUM

DOEpatents

Miller, D.R.; Seaborg, G.T.; Thompson, S.G.

1959-12-15

A process is described for precipitating plutonium on a uranous iodate carrier from an aqueous acid solution conA plutonium solution more concentrated than the original solution can then be obtained by oxidizing the uranium to the hexavalent state and dissolving the precipitate, after separating the latter from the original solution, by means of warm nitric acid.

Dissolved radon and uranium in groundwater in a potential coal seam gas development region (Richmond River Catchment, Australia).

PubMed

Atkins, Marnie L; Santos, Isaac R; Perkins, Anita; Maher, Damien T

2016-04-01

The extraction of unconventional gas resources such as shale and coal seam gas (CSG) is rapidly expanding globally and often prevents the opportunity for comprehensive baseline groundwater investigations prior to drilling. Unconventional gas extraction often targets geological layers with high naturally occurring radioactive materials (NORM) and extraction practices may possibly mobilise radionuclides into regional and local drinking water resources. Here, we establish baseline groundwater radon and uranium levels in shallow aquifers overlying a potential CSG target formation in the Richmond River Catchment, Australia. A total of 91 groundwater samples from six different geological units showed highly variable radon activities (0.14-20.33 Bq/L) and uranium levels (0.001-2.77 μg/L) which were well below the Australian Drinking Water Guideline values (radon; 100 Bq/L and uranium; 17 μg/L). Therefore, from a radon and uranium perspective, the regional groundwater does not pose health risks to consumers. Uranium could not explain the distribution of radon in groundwater. Relatively high radon activities (7.88 ± 0.83 Bq/L) in the fractured Lismore Basalt aquifer coincided with very low uranium concentrations (0.04 ± 0.02 μg/L). In the Quaternary Sediments aquifers, a positive correlation between U and HCO3(-) (r(2) = 0.49, p < 0.01) implied the uranium was present as uranyl-carbonate complexes. Since NORM are often enriched in target geological formations containing unconventional gas, establishing radon and uranium concentrations in overlying aquifers comprises an important component of baseline groundwater investigations. Copyright © 2016 Elsevier Ltd. All rights reserved.

THE ANALYSIS OF URANIUM-ZIRCONIUM ALLOYS

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

Milner, G.W.C.; Skewies, A.F.

1953-03-01

A satisfactory procedure is described for the analysis of uranium-zirconium alloys containing up to 25% zirconium. It is based on the separation of the zirconium from the uranium by dissolving the cupferron complex of the former element into chloroform. After the evaporation of the solvent from the combined organic extracts, the residue is ignited to zirconium oxide. The latter is then re-dissolved and zirconium is separated from other elements co-extracted in the solvent extraction procedure by precipitation with mandelic acid. The zirconium mandelate is finally ignited to oxide at 960 deg C. The uranium is separated from the aqueous solutionmore » remaining from the cupferron extraction by precipitating with tannin at a pH of 8; the precipitate being removed by filtration and then ignited a t 800 deg C. The residue is dissolved in nitric acid and the uranium is finally determined by precipitating as ammonium diuranate and then igniting to U{sub 3}O{sub 8}. (auth)« less

The aqueous geochemistry of uranium in a drainage containing uraniferous organic-rich sediments, Lake Tahoe area, Nevada, USA

USGS Publications Warehouse

Zielinski, R.A.; Otton, J.K.; Wanty, R.B.; Pierson, C.T.

1988-01-01

Anomalously uraniferous waters occur in a small (4.2 km2) drainage in the west-central Carson Range, Nevada, on the eastern side of Lake Tahoe. The waters transport uranium from local U-rich soils and bedrock to organic-rich valley-fill sediments where it is concentrated, but weakly bound. The dissolved U and the U that is potentially available from coexisting sediments pose a threat to the quality of drinking water that is taken from the drainage. The U concentration in samples of 6 stream, 11 spring and 7 near-surface waters ranged from 0.1 V). Possible precipitation of U(IV) minerals is predicted under the more reducing conditions that are particularly likely in near-surface waters, but the inhibitory effects of sluggish kinetics or organic complexing are not considered. These combined results suggest that a process such as adsorption or ion exchange, rather than mineral saturation, is the most probable mechanism for uranium fixation in the sediments. -Authors

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

Determination of depleted uranium in urine via isotope ratio measurements using large-bore direct injection high efficiency nebulizer-inductively coupled plasma mass spectrometry.

PubMed

Westphal, Craig S; McLean, John A; Hakspiel, Shelly J; Jackson, William E; McClain, David E; Montaser, Akbar

2004-09-01

Inductively coupled plasma mass spectrometry (ICP-MS), coupled with a large-bore direct injection high efficiency nebulizer (LB-DIHEN), was utilized to determine the concentration and isotopic ratio of uranium in 11 samples of synthetic urine spiked with varying concentrations and ratios of uranium isotopes. Total U concentrations and (235)U/(238)U isotopic ratios ranged from 0.1 to 10 microg/L and 0.0011 and 0.00725, respectively. The results are compared with data from other laboratories that used either alpha-spectrometry or quadrupole-based ICP-MS with a conventional nebulizer-spray chamber arrangement. Severe matrix effects due to the high total dissolved solid content of the samples resulted in a 60 to 80% loss of signal intensity, but were compensated for by using (233)U as an internal standard. Accurate results were obtained with LB-DIHEN-ICP-MS, allowing for the positive identification of depleted uranium based on the (235)U/(238)U ratio. Precision for the (235)U/(238)U ratio is typically better than 5% and 15% for ICP-MS and alpha-spectrometry, respectively, determined over the concentrations and ratios investigated in this study, with the LB-DIHEN-ICP-MS system providing the most accurate results. Short-term precision (6 min) for the individual (235)U and (238)U isotopes in synthetic urine is better than 2% (N = 7), compared to approximately 5% for conventional nebulizer-spray chamber arrangements and >10% for alpha-spectrometry. The significance of these measurements is discussed for uranium exposure assessment of Persian Gulf War veterans affected by depleted uranium ammunitions.

Long-term anoxia and release of ancient, labile carbon upon thaw of Pleistocene permafrost

USGS Publications Warehouse

Ewing, Stephanie A.; O'Donnell, Jonathan A.; Aiken, George R.; Butler, Kenna D.; Butman, David; Windham-Myers, Lisamarie; Kanevskiy, Mikhail

2015-01-01

The fate of permafrost carbon upon thaw will drive feedbacks to climate warming. Here we consider the character and context of dissolved organic carbon (DOC) in yedoma permafrost cores from up to 20 m depth in central Alaska. We observed high DOC concentrations (4 to 129 mM) and consistent low molecular weight organic acid concentrations in three cores. We estimate a DOC production rate of 12 µmol DOC m−2 yr−1 based on model ages of up to ~200 kyr derived from uranium isotopes. Acetate C accounted for 24 ± 1% of DOC in all samples. This proportion suggests long-term anaerobiosis and is likely to influence thaw outcomes due to biolability of acetate upon release in many environments. The combination of uranium isotopes, ammonium concentrations, and calcium concentrations explained 86% of the variation in thaw water DOC concentrations, suggesting that DOC production may be related to both reducing conditions and mineral dissolution over time.

CONCENTRATION OF Pu USING OXALATE TYPE CARRIER

DOEpatents

Ritter, D.M.; Black, R.P.S.

1960-04-19

A method is given for dissolving and reprecipitating an oxalate carrier precipitate in a carrier precipitation process for separating and recovering plutonium from an aqueous solution. Uranous oxalate, together with plutonium being carried thereby, is dissolved in an aqueous alkaline solution. Suitable alkaline reagents are the carbonates and oxulates of the alkali metals and ammonium. An oxidizing agent selected from hydroxylamine and hydrogen peroxide is then added to the alkaline solution, thereby oxidizing uranium to the hexavalent state. The resulting solution is then acidified and a source of uranous ions provided in the acidified solution, thereby forming a second plutoniumcarrying uranous oxalate precipitate.

Uranium chloride extraction of transuranium elements from LWR fuel

DOEpatents

Miller, W.E.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R.; Pierce, R.D.

1992-08-25

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels containing rare earth and noble metal fission products as well as other fission products is disclosed. The oxide fuel is reduced with Ca metal in the presence of Ca chloride and a U-Fe alloy which is liquid at about 800 C to dissolve uranium metal and the noble metal fission product metals and transuranium actinide metals and rare earth fission product metals leaving Ca chloride having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein. The Ca chloride and CaO and the fission products contained therein are separated from the U-Fe alloy and the metal values dissolved therein. The U-Fe alloy having dissolved therein reduced metals from the spent nuclear fuel is contacted with a mixture of one or more alkali metal or alkaline earth metal halides selected from the class consisting of alkali metal or alkaline earth metal and Fe or U halide or a combination thereof to transfer transuranium actinide metals and rare earth metals to the halide salt leaving the uranium and some noble metal fission products in the U-Fe alloy and thereafter separating the halide salt and the transuranium metals dissolved therein from the U-Fe alloy and the metals dissolved therein. 1 figure.

Uranium chloride extraction of transuranium elements from LWR fuel

DOEpatents

Miller, William E.; Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Pierce, R. Dean

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels containing rare earth and noble metal fission products as well as other fission products is disclosed. The oxide fuel is reduced with Ca metal in the presence of Ca chloride and a U-Fe alloy which is liquid at about 800.degree. C. to dissolve uranium metal and the noble metal fission product metals and transuranium actinide metals and rare earth fission product metals leaving Ca chloride having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein. The Ca chloride and CaO and the fission products contained therein are separated from the U-Fe alloy and the metal values dissolved therein. The U-Fe alloy having dissolved therein reduced metals from the spent nuclear fuel is contacted with a mixture of one or more alkali metal or alkaline earth metal halides selected from the class consisting of alkali metal or alkaline earth metal and Fe or U halide or a combination thereof to transfer transuranium actinide metals and rare earth metals to the halide salt leaving the uranium and some noble metal fission products in the U-Fe alloy and thereafter separating the halide salt and the transuranium metals dissolved therein from the U-Fe alloy and the metals dissolved therein.

PROCESS FOR DISSOLVING BINARY URANIUM-ZIRCONIUM OR ZIRCONIUM-BASE ALLOYS

DOEpatents

Jonke, A.A.; Barghusen, J.J.; Levitz, N.M.

1962-08-14

A process of dissolving uranium-- zirconium and zircaloy alloys, e.g. jackets of fuel elements, with an anhydrous hydrogen fluoride containing from 10 to 32% by weight of hydrogen chloride at between 400 and 450 deg C., preferably while in contact with a fluidized inert powder, such as calcium fluoride is described. (AEC)

Environmental radioactivity assessment around old uranium mining sites near Mangualde (Viseu), Portugal

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

Carvalho, Fernando P.; Torres, Lubelia M.; Oliveira, Joao M.

2007-07-01

Uranium ore was extracted in the surroundings of Mangualde city, North of Portugal, in the mines of Cunha Baixa, Quinta do Bispo and Espinho until a few years ago. Mining waste, milling tailings and acid mine waters are the on site remains of this extractive activity. Environmental radioactivity measurements were performed in and around these sites in order to assess the dispersal of radionuclides from uranium mining waste and the spread of acidic waters resulting from the in situ uranium leaching with sulphuric acid. Results show migration of acid waters into groundwater around the Cunha Baixa mine. This groundwater ismore » tapped by irrigation wells in the agriculture area near the Cunha Baixa village. Water from wells displayed uranium ({sup 238}U) concentrations up to 19x10{sup 3} mBq L{sup -1} and sulphate ion concentrations up to 1070 mg L{sup -1}. These enhanced concentrations are positively correlated with low water pH, pointing to a common origin for radioactivity, dissolved sulphate, and acidity in underground mining works. Radionuclide concentrations were determined in horticulture and farm products from this area also and results suggest low soil to plant transfer of radionuclides and low food chain transfer of radionuclides to man. Analysis of aerosols in surface air showed re suspension of dust from mining and milling waste heaps. Therefore, it is recommended to maintain mine water treatment and to plan remediation of these mine sites in order to prevent waste dispersal in the environment. (authors)« less

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS FROM NEUTRON- BOMBARDED URANIUM

DOEpatents

Martin, A.E.; Johnson, I.; Burris, L. Jr.; Winsch, I.O.; Feder, H.M.

1962-11-13

A process is given for removing plutonium and/or fission products from uranium fuel. The fuel is dissolved in molten zinc--magnesium (10 to 18% Mg) alloy, more magnesium is added to obtain eutectic composition whereby uranium precipitates, and the uranium are separated from the Plutoniumand fission-product- containing eutectic. (AEC)

In situ bioremediation of uranium with emulsified vegetable oil as the electron donor.

PubMed

Watson, David B; Wu, Wei-Min; Mehlhorn, Tonia; Tang, Guoping; Earles, Jennifer; Lowe, Kenneth; Gihring, Thomas M; Zhang, Gengxin; Phillips, Jana; Boyanov, Maxim I; Spalding, Brian P; Schadt, Christopher; Kemner, Kenneth M; Criddle, Craig S; Jardine, Philip M; Brooks, Scott C

2013-06-18

A field test with a one-time emulsified vegetable oil (EVO) injection was conducted to assess the capacity of EVO to sustain uranium bioreduction in a high-permeability gravel layer with groundwater concentrations of (mM) U, 0.0055; Ca, 2.98; NO3(-), 0.11; HCO3(-), 5.07; and SO4(2-), 1.23. Comparison of bromide and EVO migration and distribution indicated that a majority of the injected EVO was retained in the subsurface from the injection wells to 50 m downgradient. Nitrate, uranium, and sulfate were sequentially removed from the groundwater within 1-2 weeks, accompanied by an increase in acetate, Mn, Fe, and methane concentrations. Due to the slow release and degradation of EVO with time, reducing conditions were sustained for approximately one year, and daily U discharge to a creek, located approximately 50 m from the injection wells, decreased by 80% within 100 days. Total U discharge was reduced by 50% over the one-year period. Reduction of U(VI) to U(IV) was confirmed by synchrotron analysis of recovered aquifer solids. Oxidants (e.g., dissolved oxygen, nitrate) flowing in from upgradient appeared to reoxidize and remobilize uranium after the EVO was exhausted as evidenced by a transient increase of U concentration above ambient values. Occasional (e.g., annual) EVO injection into a permeable Ca and bicarbonate-containing aquifer can sustain uranium bioreduction/immobilization and decrease U migration/discharge.

Natural or fertilizer-derived uranium in irrigation drainage: A case study in southeastern Colorado, U.S.A.

USGS Publications Warehouse

Zielinski, R.A.; Asher-Bolinder, S.; Meier, A.L.; Johnson, C.A.; Szabo, B. J.

1997-01-01

Drainage from heavily cultivated soils may be contaminated with U that is leached from the soil or added as a trace constituent of PO4-based commercial fertilizer. The effect of decades-long application of U-rich fertilizer on the U concentration of irrigation drainage was investigated in a small (14.2 km2) drainage basin in southeastern Colorado. The basin was chosen because previous reports indicated locally anomalous concentrations of dissolved NO3(6-36 mg l-1) and dissolved U (61 ??g l-1) at the mouth of the only stream. Results of this study indicated minimal impact of fertilizer-U compared to natural U leached from the local soils. Detailed sampling of the stream along a 6 mile (9.7 km) reach through heavily cultivated lands indicated marked decoupling of the buildup of dissolved NO3 and U. Dissolved U increased markedly in the upstream half of the reach and correlated positively with increases in Na, Mg, SO4, B and Li derived from leaching of surrounding shaley soils. In contrast, major increases in dissolved NO3 occurred farther downstream where stream water was heavily impacted by ground water return from extensively fertilized fields. Nitrogen isotopic measurements confirmed that dissolved NO3 originated from fertilizer and soil organic N (crop waste). Uranium isotopic measurements of variably uraniferous waters showed little evidence of contamination with fertilizer-derived U of isotopically distinct 234U/238U alpha activity ratio (A.R. = 1.0). Leaching experiments using local alkaline soil, irrigation water and U-rich fertilizer confirmed the ready leachability of soil-bound U and the comparative immobility of U added with liquid fertilizer. Relatively insoluble precipitates containing Ca-P-U were formed by mixing liquid fertilizer with water containing abundant dissolved Ca. In the local soils soluble Ca is provided by dissolution of abundant gypsum. Similar studies are needed elsewhere because the mobility of fertilizer-derived U is dependent on fertilizer type, porewater chemistry and soil properties (pH, moisture, mineralogy, texture).

High strength uranium-tungsten alloys

DOEpatents

Dunn, Paul S.; Sheinberg, Haskell; Hogan, Billy M.; Lewis, Homer D.; Dickinson, James M.

1991-01-01

Alloys of uranium and tungsten and a method for making the alloys. The amount of tungsten present in the alloys is from about 4 wt % to about 35 wt %. Tungsten particles are dispersed throughout the uranium and a small amount of tungsten is dissolved in the uranium.

High strength uranium-tungsten alloy process

DOEpatents

Dunn, Paul S.; Sheinberg, Haskell; Hogan, Billy M.; Lewis, Homer D.; Dickinson, James M.

1990-01-01

Alloys of uranium and tungsten and a method for making the alloys. The amount of tungsten present in the alloys is from about 4 wt % to about 35 wt %. Tungsten particles are dispersed throughout the uranium and a small amount of tungsten is dissolved in the uranium.

PROCESS OF PREPARING URANIUM CARBIDE

DOEpatents

Miller, W.E.; Stethers, H.L.; Johnson, T.R.

1964-03-24

A process of preparing uranium monocarbide is de scribed. Uranium metal is dissolved in cadmium, zinc, cadmium-- zinc, or magnesium-- zinc alloy and a small quantity of alkali metal is added. Addition of stoichiometric amounts of carbon at 500 to 820 deg C then precipitates uranium monocarbide. (AEC)

Geochemical Characterization of the Upper and Middle Floridan Aquifer System, South Florida

NASA Astrophysics Data System (ADS)

Mirecki, J.; Richardson, E.; Bennett, M.; Hendel, J.

2008-05-01

Our study focus is to characterize the water quality and geochemical environment of the Floridan Aquifer System (FAS) throughout the regional flowpath. A synoptic survey of 21 wells (n=15, upper FAS; n=6 middle FAS) was supplemented by additional samples (n=11) obtained during exploratory well development at 4 aquifer storage recovery (ASR) pilot sites. Synoptic survey samples were analyzed intensively, yielding a dataset that consists of major and trace dissolved constituents (including metals), stable isotopes (δ18O, δ13C, δD, δ34S in sulfate and sulfide), carbon species (carbonate alkalinity and organic carbon), uranium-series radionuclides, nutrients, and selected microbes and pathogens. The objectives of this study are three-fold: 1) to provide baseline water-quality and geochemical information prior to initiation of ASR activities that are part of the Comprehensive Everglades Restoration Plan; 2) to quantify the major controls on geochemical evolution along upper and middle FAS flowpaths using geochemical modeling methods; and 3) to identify areas where water- quality may limit the feasibility of ASR methods in the FAS. Preliminary interpretations water quality changes along the regional FAS flowpath can be summarized as follows. Concentrations of dissolved constituents increase from north to south along the flow path; generally, the upper FAS has lower total dissolved solids than the middle FAS at locations where well pairs were analyzed. The redox environment changes from oxic to strongly anoxic, very close to the recharge area. Redox measurements, dissolved iron, sulfide, and sulfur isotope data are consistent with sulfate-reducing conditions. Uranium-series isotope concentrations and activities generally are below regulatory criteria, with few exceptions in both the upper and middle FAS. Areas with greater radionuclide activity occur primarily at distal flowpath locations or at the coast.

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

Radioactivity and geochemistry of selected mineral-spring waters in the Western United States; basic data and multivariate statistical analysis

USGS Publications Warehouse

Felmlee, J.K.; Cadigan, R.A.

1982-01-01

Multivariate statistical analyses were performed on data from 156 mineral-spring sites in nine Western States to analyze relationships among the various parameters measured in the spring waters. Correlation analysis and R-mode factor analysis indicate that three major factors affect water composition in the spring systems studied: (1) duration of water circulation, (2) depth of water circulation, and (3) partial pressure of carbon dioxide. An examination of factor scores indicates that several types of hydrogeologic systems were sampled. Most of the samples are (1) older water from deeper circulating systems having relatively high salinity, high temperature, and low Eh or (2) younger water from shallower circulating systems having relatively low salinity, low temperature, and high Eh. The rest of the samples are from more complex systems. Any of the systems can have a relatively high or low content of dissolved carbonate species, resulting in a low or high pH, respectively. Uranium concentrations are commonly higher in waters of relatively low temperature and high Eh, and radium concentrations are commonly higher in waters having a relatively high carbonate content (low pH) and, secondarily, relatively high salinity. Water samples were collected and (or) measurements were taken at 156 of the 171 mineral-spring sites visited. Various samples were analyzed for radium, uranium, radon, helium, and radium-228 as well as major ions and numerous trace elements. On-site measurements for physical properties including temperature, specific conductance, pH, Eh, and dissolved oxygen were made. All constituents and properties show a wide range of values. Radium concentrations range from less than 0.01 to 300 picocuries per liter; they average 1.48 picocuries per liter and have an anomaly threshold value of 171 picocuries per liter for the samples studied. Uranium concentrations range from less than 0.01 to 120 micrograms per liter and average 0.26 micrograms per liter; they have an anomaly threshold value of 48.1 micrograms per liter. Radon content ranges from less than 10 to 110,000 picocuries per liter, averages 549 picocuries per liter and has an anomaly threshold of 20,400 picocuries per liter. Helium content ranges from -1,300 to +13,000 parts per billion relative to atmospheric helium; it averages +725 parts per billion and has an anomaly threshold of 10,000 parts per billion. Radium-228 concentrations range from less than 2.0 to 33 picocuries per liter; no anomaly threshold was determined owing to the small number of samples. All of the anomaly thresholds may be somewhat high because the sampling was biased toward springs likely to be radioactive. The statistical variance in radium and uranium concentrations unaccounted for by the identified factors testifies to the complexity of some hydrogeologic systems. Unidentified factors related to geologic setting and the presence of uranium-rich rocks in the systems also affect the observed concentrations of the radioactive elements in the water. The association of anomalous radioactivity in several springs with nearby known uranium occurrences indicates that other springs having anomalous radioactivity may also be associated with uranium occurrences as yet undiscovered.

Operational Range Assessment Program (ORAP) Phase II Overview for Active Installations

DTIC Science & Technology

2011-05-01

Dissolved Metals by EPA 1638M • Isotopic Uranium by EML A-01-R Mod  Sediment Analysis • None  Benthic Macroinvertebrates • Diversity Indices...Metals by EPA 200.8 • Dissolved Metals by EPA 200.8 (if turbid) • Isotopic Uranium by EML A-01- R Mod (if total U is > action limit) Groundwater

Analysis of maximum allowable fragment heights during dissolution of high flux isotope reactor fuel in an h-canyon dissolver

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

Daniel, G.; Rudisill, T.

2017-07-17

As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U 3O 8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H 2. The HFIR fuel cores will be dissolved using a flowsheet developed by the Savannahmore » River National Laboratory (SRNL) in either the 6.4D or 6.1D dissolver using a unique insert. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The recovered U will be down-blended into low-enriched U for subsequent use as commercial reactor fuel. During the development of the HFIR fuel dissolution flowsheet, the cycle time for the initial core was estimated at 28 to 40 h. Once the cycle is complete, H-Canyon personnel will open the dissolver and probe the HFIR insert wells to determine the height of any fuel fragments which did not dissolve. Before the next core can be charged to the dissolver, an analysis of the potential for H 2 gas generation must show that the combined surface area of the fuel fragments and the subsequent core will not generate H 2 concentrations in the dissolver offgas which exceeds 60% of the lower flammability limit (LFL) of H 2 at 200 °C. The objective of this study is to identify the maximum fuel fragment height as a function of the Al concentration in the dissolving solution which will provide criteria for charging successive HFIR cores to an H-Canyon dissolver.« less

RECOVERY OF URANIUM AND THORIUM FROM AQUEOUS SOLUTIONS

DOEpatents

Calkins, G.D.

1958-06-10

>A process is described for the recovery of uranium and thorium from monazite sand, which is frequently processed by treating it with a hot sodium hydroxide solution whereby a precipitate forms consisting mainly of oxides or hydroxides of the rare earths, thorium and uranium. The precipitate is dissolved in mineral acid, and the acid solution is then neutralized to a pH value of between 5.2 and 6.2 whereby both the uranium and thorium precipitate as the hydroxides, while substantially all the rare earth metal values present remain in the solution. The uranium and thoriunn can then be separated by dissolving the precipitate in a solution containing a mixture of alkali carbonate and alkali bicarbonate: and contacting the carbonate solution with a strong-base anion exchange resin whereby the uranium values are adsorbed on the resin while the thorium remains in solution.

DISSOLVED CONCENTRATION LIMITS OF RADIOACTIVE ELEMENTS

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

P. Bernot

The purpose of this study is to evaluate dissolved concentration limits (also referred to as solubility limits) of elements with radioactive isotopes under probable repository conditions, based on geochemical modeling calculations using geochemical modeling tools, thermodynamic databases, field measurements, and laboratory experiments. The scope of this activity is to predict dissolved concentrations or solubility limits for elements with radioactive isotopes (actinium, americium, carbon, cesium, iodine, lead, neptunium, plutonium, protactinium, radium, strontium, technetium, thorium, and uranium) relevant to calculated dose. Model outputs for uranium, plutonium, neptunium, thorium, americium, and protactinium are provided in the form of tabulated functions with pH andmore » log fCO{sub 2} as independent variables, plus one or more uncertainty terms. The solubility limits for the remaining elements are either in the form of distributions or single values. Even though selection of an appropriate set of radionuclides documented in Radionuclide Screening (BSC 2002 [DIRS 160059]) includes actinium, transport of Ac is not modeled in the total system performance assessment for the license application (TSPA-LA) model because of its extremely short half-life. Actinium dose is calculated in the TSPA-LA by assuming secular equilibrium with {sup 231}Pa (Section 6.10); therefore, Ac is not analyzed in this report. The output data from this report are fundamental inputs for TSPA-LA used to determine the estimated release of these elements from waste packages and the engineered barrier system. Consistent modeling approaches and environmental conditions were used to develop solubility models for the actinides discussed in this report. These models cover broad ranges of environmental conditions so they are applicable to both waste packages and the invert. Uncertainties from thermodynamic data, water chemistry, temperature variation, and activity coefficients have been quantified or otherwise addressed.« less

Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

DOE PAGES

Perdrial, Nicolas; Vázquez-Ortega, Angélica; Wang, Guohui; ...

2017-12-05

Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. Here, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO 4-reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K 2(UO 2) 6O 4(OH) 6·8H 2O]- and becquerelite [Ca(UO 2) 6O 4(OH) 6·8H 2O]-like species.more » Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO 2) 2O 4(HSiO 4) 2•0.5(H 2O)]-like species of uranium at 180 and 365 days. When present, PO 4 exerted a direct and strong control over U speciation. Furthermore, the detection of meta-ankoleite, [K 2(UO 2) 2O 4(PO 4) 2·6H 2O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO 4 is absent), after initial precipitation of more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO 4 present, nearly all uranium would have precipitated in the upper soil.« less

Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

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

Perdrial, Nicolas; Vázquez-Ortega, Angélica; Wang, Guohui

Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. In this study, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO(4)(-)reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K-2(UO2)(6)O-4(OH)(6)center dot 8H(2)O]-and becquerelite [Ca(UO2)(6)O-4(OH)(6)center dot 8H(2)O]-like species. Subsequent further removal of uranium coincided withmore » that of Si and accumulation of boltwoodite, [(K, Na)(UO2)(2)O-4(HSiO4)(2)center dot 0.5(H2O)]-like species of uranium at 180 and 365 days. When present, PO4 exerted a direct and strong control over U speciation. The detection of meta-ankoleite, [K-2(UO2)(2)O-4(PO4)(2)center dot 6H(2)O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO4 is absent), after initial precipitation of more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO4 present, nearly all uranium would have precipitated in the upper soil.« less

Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

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

Perdrial, Nicolas; Vázquez-Ortega, Angélica; Wang, Guohui

Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. Here, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO 4-reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K 2(UO 2) 6O 4(OH) 6·8H 2O]- and becquerelite [Ca(UO 2) 6O 4(OH) 6·8H 2O]-like species.more » Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO 2) 2O 4(HSiO 4) 2•0.5(H 2O)]-like species of uranium at 180 and 365 days. When present, PO 4 exerted a direct and strong control over U speciation. Furthermore, the detection of meta-ankoleite, [K 2(UO 2) 2O 4(PO 4) 2·6H 2O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO 4 is absent), after initial precipitation of more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO 4 present, nearly all uranium would have precipitated in the upper soil.« less

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1964-03-24

A process of recovering plutonium from fuel by dissolution in molten KAlCl/sub 4/ double salt is described. Molten lithium chloride plus stannous chloride is added to reduce plutonium tetrachloride to the trichloride, which is dissolved in a lithium chloride phase while the uranium, as the tetrachloride, is dissolved in a double-salt phase. Separation of the two phases is discussed. (AEC)

Reactivity of uranium(iii) with H2E (E = S, Se, Te): synthesis of a series of mononuclear and dinuclear uranium(iv) hydrochalcogenido complexes.

PubMed

Franke, Sebastian M; Rosenzweig, Michael W; Heinemann, Frank W; Meyer, Karsten

2015-01-01

We report the syntheses, electronic properties, and molecular structures of a series of mono- and dinuclear uranium(iv) hydrochalcogenido complexes supported by the sterically demanding but very flexible, single N-anchored tris(aryloxide) ligand ( Ad ArO) 3 N) 3- . The mononuclear complexes [(( Ad ArO) 3 N)U(DME)(EH)] (E = S, Se, Te) can be obtained from the reaction of the uranium(iii) starting material [(( Ad ArO) 3 N)U III (DME)] in DME via reduction of H 2 E and the elimination of 0.5 equivalents of H 2 . The dinuclear complexes [{(( Ad ArO) 3 N)U} 2 (μ-EH) 2 ] can be obtained by dissolving their mononuclear counterparts in non-coordinating solvents such as benzene. In order to facilitate the work with the highly toxic gases, we created concentrated THF solutions that can be handled using simple glovebox techniques and can be stored at -35 °C for several weeks.

Occurrence of Uranium and 222Radon in Glacial and Bedrock Aquifers in the Northern United States, 1993-2003

USGS Publications Warehouse

Ayotte, Joseph D.; Flanagan, Sarah M.; Morrow, William S.

2007-01-01

Water-quality data collected from 1,426 wells during 1993-2003 as part of the U.S. Geological Survey National Water-Quality Assessment (NAWQA) program were evaluated to characterize the water quality in glacial and bedrock aquifers of the northern United States. One of the goals of the NAWQA program is to synthesize data from individual studies across the United States to gain regional- and national-scale information about the behavior of contaminants. This study focused on the regional occurrence and distribution of uranium and 222radon in ground water in the glacial aquifer system of the United States as well as in the Cambrian-Ordovician and the New York and New England crystalline aquifer systems that underlie the glacial aquifer system. The occurrence of uranium and 222radon in ground water has long been a concern throughout the United States. In the glacial aquifers, as well as the Cambrian-Ordovician and the New York and New England crystalline aquifer systems of the United States, concentrations of uranium and 222radon were highly variable. High concentrations of uranium and 222radon affect ground water used for drinking water and for agriculture. A combination of information or data on (1) national-scale ground-water regions, (2) regional-scale glacial depositional models, (3) regional-scale geology, and (4) national-scale terrestrial gamma-ray emissions were used to confirm and(or) refine the regions used in the analysis of the water-chemistry data. Significant differences in the occurrence of uranium and 222radon, based primarily on geologic information were observed and used in this report. In general, uranium was highest in the Columbia Plateau glacial, West-Central glacial, and the New York and New England crystalline aquifer groups (75th percentile concentrations of 22.3, 7.7, and 2.9 micrograms per liter (ug/L), respectively). In the Columbia Plateau glacial and the West-Central glacial aquifer groups, more than 10 percent of wells sampled had concentrations of uranium that exceeded the U.S. Environmental Protection Agency (USEPA) Maximum Contaminant Level of 30 ug/L; in the New York and New England crystalline aquifer group, 4 percent exceeded 30 ug/L. Ground-water samples with high concentrations of uranium were commonly linked to geologic sources rich in uranium. In eight of nine aquifer groups defined for this study, concentrations of uranium correlated significantly with concentrations of sulfate in ground water (Spearman's rho = 0.20 to 0.56; p < 0.05). In the Columbia Plateau, glacial aquifers were derived in part from basaltic lava flows, some felsic volcanic rocks, and some paleo-lake bed materials that may be rich in uranium. In the Columbia Plateau and West-Central glacial aquifer groups, uranium correlated with total dissolved solids, bicarbonate, boron, lithium, selenium, and strontium. In the West-Central glacial aquifer group, rocks such as Cretaceous marine shales, which are abundant in uranium, probably contribute to the high concentrations in ground water; in the southern part of this group, which extends into Nebraska, the glacial or glacial-related sediment may be interbedded with uranium-rich materials that originated to the north and west and in the Rocky Mountains. In New England, crystalline bedrock that is granitic, such as two-mica granites, as well as other high-grade metamorphic rocks, has abundant uranium that is soluble in the predominantly oxic to sub-oxic geochemical conditions. This appears to contribute to high uranium concentrations in ground water. The highest 222radon concentrations were present in samples from wells completed in the New York and New England crystalline aquifer group; the median value (2,122 picocurries per liter (pCi/L)) was about 10 times the median values of all other aquifer groups. More than 25 percent of the samples from the New York and New England crystalline aquifer group wells had 222radon concentrations that exceeded the USEPA Alternative

The estuarine chemistry and isotope systematics of 234,238U in the Amazon and Fly Rivers

USGS Publications Warehouse

Swarzenski, P.; Campbell, P.; Porcelli, D.; McKee, B.

2004-01-01

Natural concentrations of 238U and ??234U values were determined in estuarine surface waters and pore waters of the Amazon and Fly (Papua New Guinea) Rivers to investigate U transport phenomena across river-dominated land-sea margins. Discharge from large, tropical rivers is a major source of dissolved and solid materials transported to the oceans, and are important in defining not only oceanic mass budgets, but also terrestrial weathering rates. On the Amazon shelf, salinity-property plots of dissolved organic carbon, pH and total suspended matter revealed two vastly contrasting water masses that were energetically mixed. In this mixing zone, the distribution of uranium was highly non-conservative and exhibited extensive removal from the water column. Uranium removal was most pronounced within a salinity range of 0-16.6, and likely the result of scavenging and flocculation reactions with inorganic (i.e., Fe/Mn oxides) and organic colloids/particles. Removal of uranium may also be closely coupled to exchange and resuspension processes at the sediment/water interface. An inner-shelf pore water profile indicated the following diagenetic processes: extensive (???1 m) zones of Fe(III) - and, to a lesser degree, Mn(IV) - reduction in the absence of significant S(II) concentrations appeared to facilitate the formation of various authigenic minerals (e.g., siderite, rhodocrosite and uraninite). The pore water dissolved 238U profile co-varied closely with Mn(II). Isotopic variations as evidenced in ??234U pore waters values from this site revealed information on the origin and history of particulate uranium. Only after a depth of about 1 m did the ??234U value approach unity (secular equilibrium), denoting a residual lattice bound uranium complex that is likely an upper-drainage basin weathering product. This suggests that the enriched ??234U values represent a riverine surface complexation product that is actively involved in Mn-Fe diagenetic cycles and surface complexation reactions. In the Fly River estuary, 238U appears to exhibit a reasonably conservative distribution as a function of salinity. The absence of observed U removal does not necessarily imply non-reactivity, but instead may record an integration of concurrent U removal and release processes. There is not a linear correlation between ??234U vs. 1/ 238U that would imply simple two component mixing. It is likely that resuspension of bottom sediments, prolonged residence times in the lower reaches of the Fly River, and energetic particle-colloid interactions contribute to the observed estuarine U distribution. The supply of uranium discharged from humid, tropical river systems to the sea appears to be foremost influenced by particle/water interactions that are ultimately governed by the particular physiographic and hydrologic characteristics of an estuary. ?? 2004 Elsevier Ltd. All rights reserved.

High strength and density tungsten-uranium alloys

DOEpatents

Sheinberg, Haskell

1993-01-01

Alloys of tungsten and uranium and a method for making the alloys. The amount of tungsten present in the alloys is from about 55 vol % to about 85 vol %. A porous preform is made by sintering consolidated tungsten powder. The preform is impregnated with molten uranium such that (1) uranium fills the pores of the preform to form uranium in a tungsten matrix or (2) uranium dissolves portions of the preform to form a continuous uranium phase containing tungsten particles.

IDAHO CHEMICAL PROCESSING PLANT TECHNICAL PROGRESS REPORT FOR APRIL THROUGH JUNE 1958

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

Stevenson, C.E.

1958-11-01

Processing of uranium -aluminum alloy was continued with slight process modifications. Means for recovering rare gases from dissolver off-gas are described. Results of extensive decontamination procedures required to enable entrance to the continuous dissolver cell are also indicated. Pilot plant studies of dissolving aluminum continuously showed that rates of dissolution were decreased by factors of 2 to 4 as the concentration of nitric acid fed was increased from 5.4 to 11N. The rate of aluminum dissolution was found to be proportional to initial area exposed for pieces of different shape. It was found possible to produce a highly basic aluminummore » nitrate solution at a reasonable rate by dissolving to low concentration in dilute acid, followed by evaporation to the desired level. Uranium exchange rate measurements for the TBP extraction process are described. A canned rotor pump under test with graphite bearings operated 6000 hours with nominal wear. Difficulties were experienced in testing a nutating disc pump. Measurements of the potential of zirconium in hydrofluoric acid as a function of pH confirmed the predicted equation. In teflon vessels, zirconium dissolves a little more rapidly in nitric-hydrofluoric acid mixtures than in glass vessels, presumably due to reaction of fluoride with silica. Titunium alloy Types 55A and 75A were found to resist corrosion by certain boiling nitric-hydrochloric acid mixtures. Initial tests have commenced with a NaK-heated 100 liter/hour pilot plant aluminum nitrate calciner to continue process demonstration. In tests in the smaller pilot plant unit, increasing feed spray air ratio was found to increase particle loading in the cyclone effluent. Laboratory studies indicated that a venturi scrubber using dilute nitric acid at 80 C should remove ruthenium effectively from calciner off-gas. In a pilot plant test in which a significant fraction of ruthenium feed was retained by the alumina, substantial absorption of volatilized ruthenium was obtained. Thermal conductivity of alumina near 3000 F was about 0.26 Btu/hr)(ft)( F). In leaching studies, very little strontium or plutonium was removed by water from alumina calcined at 550 C. Dilute nitric acid, however, extracted strontium from this material to the same degree (~ 50 percent) as from material calcined at 400 C. Concentrated basic aluminum nitrate was produced from simulated aluminum nitrate waste by slow hydrolysis with urea followed by evaporation. Aluminum was efficiently extracted from buffered aluminum nitrate solution by acetylacetone and was stripped back into nitric acid. A filterable aluminum phosphate was precipituted from aluminum nitrate solution by urea hydrolysis; the phosphate effectively carried fission products, however. Spectrophotometric methods were developed for macro and micro quantities of uranium, in the presence of high concentrations of other ions, based on tetrapropylammonium nitrate extraction. (For preceding period see ID0-14443.) (auth)« less

Isotopic Clues on Factors Controlling Geochemical Fluxes From Large Watersheds in Eastern Canada

NASA Astrophysics Data System (ADS)

Rosa, E.; Helie, J.; Ghaleb, B.; Hillaire-Marcel, C.; Gaillardet, J.

2008-12-01

A monitoring and monthly sampling program of the Nelson, Ottawa, St. Lawrence, La Grande and Great Whale rivers was started in September 2007. It provides information on the seasonality and sources of geochemical fluxes into the Hudson Bay and the North Atlantic from watersheds covering more than 2.6 106 km2 of the eastern Canadian boreal domain. Measurements of pH and alkalinity, analyses of major ions, strontium and dissolved silica, 2H and 18O of water, concentrations and isotopic properties of dissolved organic and inorganic carbon (13C) and uranium (234U/238U) were performed. Lithology more than latitudinal climatic gradients controls the river geochemistry. Rivers draining silicate terrains show lower dissolved U concentrations but greater 234U/238U disequilibria than rivers draining carbonates (average of 1.38 vs. 1.23). Groundwater supplies might exert some control on these U- isotope signatures. No clear seasonality is observed in 234U/238U ratios, but U concentrations are correlated to dissolved organic carbon (DOC) concentrations in most rivers. Rivers draining carbonates present higher total dissolved carbon concentrations and higher 13C-contents in dissolved inorganic carbon (DIC), in response to the dissolution of soil carbonates. DOC/DIC ratios above 2.4 are observed in rivers draining silicates; their lower 13C-DIC content directly reflects the organic matter oxidation in soils. Total dissolved solids are one order of magnitude or more greater in rivers draining carbonates, showing the strong difference in chemical weathering rates according to the geological setting. The stability in chemical fluxes and water isotopic compositions in the La Grande River, which hosts hydroelectric reservoirs covering more than 12 000 km2, indicates that it is the most buffered hydrological system among the investigated watersheds. Seasonal fluctuations are observed elsewhere, with maximum geochemical fluxes during the spring snowmelt. 2H-18O content of river water appears to be the only parameter presenting a strong latitudinal and climatic gradient (independent of lithology).

The determination of uranium (IV) in apatite

USGS Publications Warehouse

Clarke, Roy S.; Altschuler, Zalman S.

1956-01-01

Geologic and mineralogic evidence indicate that the uranium present in apatite may proxy for calcium in the mineral structure as U(IV). An experimental investigation was conducted and chemical evidence was obtained that establishes the presence of U(IV) in apatite. The following analytical procedure was developed for the determination of U(IV). Carbonate-fluorapatite is dissolved in cold 1.5M orthophosphoric acid and fluorapatite is dissolved in cold 1.2M hydrochloric acid containing 1.5 g of hydroxylamine hydrochloride per 100 ml. Uranium (IV) is precipitated by cupferron using titanium as a carrier. The uranium in the precipitate is separated by use of the ethyl acetate extraction procedure and determined fluorimetrically. The validity and the limitations of the method have been established by spike experiments.

Compilation and preliminary interpretation of hydrologic data for the Weldon Spring radioactive waste-disposal sites, St Charles County, Missouri; a progress report

USGS Publications Warehouse

Kleeschulte, M.J.; Emmett, L.F.

1986-01-01

The Weldon Spring Chemical Plant is located just north of the drainage divide separating the Mississippi River and the Missouri River in St. Charles County, Missouri. From 1957 to 1966 the plant converted uranium-ore concentrates and recycled scrap to pure uranium trioxide, uranium tetrafluoride, and uranium metal. Residues from these operations were pumped to four large pits that had been excavated near the plant. Small springs and losing streams are present in the area. Water overlying the residue in the pits has a large concentration of dissolved solids and a different chemical composition compared to the native groundwater and surface water. This difference is indicated by the concentrations of calcium, sodium, sulfate, nitrate, fluoride, uranium, radium, lithium, molybdenum, strontium, and vanadium, all of which are greater than natural or background concentrations. Water from Burgermeister Spring, located about 1.5 miles north of the chemical plant area, contains uranium and nitrate concentrations greater than background concentrations. Groundwater in the shallow bedrock aquifer moves northward from the vicinity of the chemical plant toward Dardenne Creek. An abandoned limestone quarry several miles southwest of the chemical plant also has been used for the disposal of radioactive waste and rubble. Groundwater flow from the quarry area is southward through the alluvium, away from the quarry and toward the Missouri River. The St. Charles County well field is located in the Missouri River flood plain near the quarry and the large yield wells are open to the Missouri River alluvial aquifer. Water from a well 4,000 ft southeast of the quarry was analyzed; there was no indication of contamination from the quarry. Additional water quality and water level data are needed to determine if water from the quarry moves toward the well field. Observation wells need to be installed in the area between the chemical plant, pits, and Dardenne Creek. The wells would be used to provide access for measurements of depth to ground water and for the collection of water samples from the shallow bedrock aquifer. (Lantz-PTT)

Dissolution flowsheet for high flux isotope reactor fuel

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

Foster, T.

2016-09-27

As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U 3O 8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H 2. The HFIR fuel cores will be dissolved and the recovered U will be down-blendedmore » into low-enriched U. HFIR fuel was previously processed in H-Canyon using a unique insert in both the 6.1D and 6.4D dissolvers. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The objective of this study was to identify flowsheet conditions through literature review and laboratory experimentation to safely and efficiently dissolve the HFIR fuel in H-Canyon. Laboratory-scale experiments were performed to evaluate the dissolution of HFIR fuel using both Al 1100 and Al 6061 T6 alloy coupons. The Al 1100 alloy was considered a representative surrogate which provided an upper bound on the generation of flammable (i.e., H 2) gas during the dissolution process. The dissolution of the Al 6061 T6 alloy proceeded at a slower rate than the Al 1100 alloy and was used to verify that the target Al concentration in solution could be achieved for the selected Hg concentration. Mass spectrometry and Raman spectroscopy were used to provide continuous monitoring of the concentration of H 2 and other permanent gases in the dissolution offgas allowing the development of H 2 generation rate profiles. The H 2 generation rates were subsequently used to evaluate if a full HFIR core could be dissolved in an H-Canyon dissolver without exceeding 60% of the calculated lower flammability limit (LFL) for H 2 at a given Hg concentration.« less

PRODUCTION OF PURIFIED URANIUM

DOEpatents

Burris, L. Jr.; Knighton, J.B.; Feder, H.M.

1960-01-26

A pyrometallurgical method for processing nuclear reactor fuel elements containing uranium and fission products and for reducing uranium compound; to metallic uranium is reported. If the material proccssed is essentially metallic uranium, it is dissolved in zinc, the sulution is cooled to crystallize UZn/sub 9/ , and the UZn/sub 9/ is distilled to obtain uranium free of fission products. If the material processed is a uranium compound, the sollvent is an alloy of zinc and magnesium and the remaining steps are the same.

Modelling of the dissolution and reprecipitation of uranium under oxidising conditions in the zone of shallow groundwater circulation.

PubMed

Dutova, Ekaterina M; Nikitenkov, Aleksei N; Pokrovskiy, Vitaly D; Banks, David; Frengstad, Bjørn S; Parnachev, Valerii P

2017-11-01

Generic hydrochemical modelling of a grantoid-groundwater system, using the Russian software "HydroGeo", has been carried out with an emphasis on simulating the accumulation of uranium in the aqueous phase. The baseline model run simulates shallow granitoid aquifers (U content 5 ppm) under conditions broadly representative of southern Norway and southwestern Siberia: i.e. temperature 10 °C, equilibrated with a soil gas partial CO 2 pressure (P CO2 , open system) of 10 -2.5 atm. and a mildly oxidising redox environment (Eh = +50 mV). Modelling indicates that aqueous uranium accumulates in parallel with total dissolved solids (or groundwater mineralisation M - regarded as an indicator of degree of hydrochemical evolution), accumulating most rapidly when M = 550-1000 mg L -1 . Accumulation slows at the onset of saturation and precipitation of secondary uranium minerals at M = c. 1000 mg L -1 (which, under baseline modelling conditions, also corresponds approximately to calcite saturation and transition to Na-HCO 3 hydrofacies). The secondary minerals are typically "black" uranium oxides of mixed oxidation state (e.g. U 3 O 7 and U 4 O 9 ). For rock U content of 5-50 ppm, it is possible to generate a wide variety of aqueous uranium concentrations, up to a maximum of just over 1 mg L -1 , but with typical concentrations of up to 10 μg L -1 for modest degrees of hydrochemical maturity (as indicated by M). These observations correspond extremely well with real groundwater analyses from the Altai-Sayan region of Russia and Norwegian crystalline bedrock aquifers. The timing (with respect to M) and degree of aqueous uranium accumulation are also sensitive to Eh (greater mobilisation at higher Eh), uranium content of rocks (aqueous concentration increases as rock content increases) and P CO2 (low P CO2 favours higher pH, rapid accumulation of aqueous U and earlier saturation with respect to uranium minerals). Copyright © 2017 Elsevier Ltd. All rights reserved.

Physical, chemical, and biological characteristics of Pueblo Reservoir, Colorado, 1985-89

USGS Publications Warehouse

Lewis, Michael E.; Edelmann, Patrick

1994-01-01

Physical, chemical, and biological characteristics of Pueblo Reservoir are described on the basis of data collected from spring 1985 through fall 1989. Also included are discussions of water quality of the upper Arkansas River Basin and the reservoir as they relate to reservoir operations. Pueblo Reservoir is a multipurpose, main-stem reservoir on the Arkansas River about 6 miles west of Pueblo, Colorado. At the top of its conservation pool, the reservoir is more than 9 miles long and ranges in depth from a few feet at the inflow to about 155 feet at the dam. Pueblo Reservoir derives most of its contents from the Arkansas River, which comprises native and transmountain flow. With respect to water temperature, the reservoir typically was well mixed to weakly stratified during the early spring and gradually became strongly stratified by May. The strong thermal stratification and underflow of the Arkansas River generally persisted into August, at which time the reservoir surface began to cool and the reservoir subsequently underwent fall turnover. Following fall turnover, the reservoir was stratified to some degree in the shallow upstream part and well mixed in the deeper middle and downstream parts. Reservoir residence times were affected by the extent of stratification present. When the reservoir was well mixed, residence times were as long as several months. During the summer when the reservoir was strongly stratified, reservoir releases were large, and when underflow was the prevalent flow pattern of the Arkansas River, reservoir residence times were as short as 30 days.Most particulate matter settled from the water column between the inflow and a distance of about 5 miles downstream. On occasions of large streamflows and sediment loads from the Arkansas River, particulate matter was transported completely through the reservoir. Water transparency, as measured with a Secchi disk, increased in a downstream direction from the reservoir inflow. The increase probably was a result of sediment settling from the water column in the upstream part of the reservoir. Secchi-disk depths in December through April were larger than those in May through November. Secchi-disk depths were small between May through August as inflow sediment loads and reservoir biomass increased. In the fall, Secchi-disk depths remained small possibly as the result of resuspension of sediment and detritus within the water column. Dissolved-oxygen concentrations generally were near supersaturation near the reservoir surface. Dissolved-oxygen concentrations decreased with increasing depth. On several occasions during the summer, dissolved oxygen became completely depleted in the hypolimnion of the downstream part of the reservoir. The most extensive period of anoxia that was measured was in August 1988; the bottom 12 to 30 feet of the downstream end of the reservoir was anoxic. Fall turnover typically resulted in well-oxygenated conditions throughout the water column from September or October through the spring. Values of pH ranged from 7.5 to 9.0 and typically were largest near the surface and decreased with depth.Dissolved-solids concentrations in the reservoir primarily are affected by dissolved solids in the inflow from the Arkansas River. Concentrations are largest during periods of decreased streamflows, September through April, and decrease with increasing streamflows in May through August. The median dissolved-solids concentration increased from 224 milligrams per liter at the inflow to 262 milligrams per liter at the outflow. However, a statistical analysis of dissolved solids indicated the apparent increase in dissolved-solids concentrations between the inflow and outflow was not significant. Calcium, sulfate, and bicarbonate are the major dissolved ions in Pueblo Reservoir.Concentrations of the major nutrients, nitrogen and phosphorus, varied within the reservoir because of settling of particulate matter, uptake by phytoplankton near the reservoir surface, and releases from the reservoir bottom sediments. Phosphorus was indicated to be a potentially growth-limiting nutrient in the reservoir because of its relatively small concentrations. During 1986 and 1987, the reservoir retained about 35 percent (359 tons) of the total nitrogen load and about 83 percent (203 tons) of the total phosphorus load. Settling of particulate matter from the water column and uptake by phytoplankton are the major nutrient sinks in the reservoir.Barium, iron, manganese, and zinc were the major trace elements in Pueblo Reservoir. Traceelement concentrations in the reservoir varied because of seasonality of trace-element concentrations in the Arkansas River, settling of particulate matter, and flux of trace elements from the bottom sediments. The aquatic-life standard in Pueblo Reservoir for total-recoverable iron (1,000 micrograms per liter) and the public water-supply standard for dissolved manganese (50 micrograms per liter) were exceeded on several occasions during the summer. Elevated concentrations of totalrecoverable iron and dissolved manganese in the Arkansas River during summer runoff contributed to exceedances in the upper part of the reservoir. Flux of manganese from the reservoir bottom sediments during periods of low or depleted dissolved-oxygen concentrations contributed to exceedances in the deeper, downstream parts of the reservoir. Concentrations of lead, mercury, and zinc were elevated in the reservoir bottom sediments and may be the result of metal-mine drainage in the upper Arkansas River Basin. Median concentrations of total organic carbon ranged from 3.1 to 4.5 milligrams per liter in May through September and from 2.5 to 3.5 milligrams per liter in October through April. Totalorganic-carbon concentrations in the reservoir were largest in the summer when streamflows and total-organic-carbon concentrations are largest in the Arkansas River. Total-organic-carbon concentrations in the reservoir decrease downstream from the reservoir inflow because of settling of particulate organic carbon. Levels of gross-alpha and gross-beta radioactivity generally were relatively low. In 7 of 31 samples collected, dissolved gross-alpha radioactivity, as natural uranium, exceeded 5 picocuries per liter, the level at which additional radiochemical analyses are recommended for drinking-water supplies. Potential sources of uranium in Pueblo Reservoir include weathering of exposed uranium ore deposits in the upper Arkansas River Basin and a uranium milling operation near Canon City.Phytoplankton densities and biovolumes measured during the winter, spring, and fall generally were indicative of a small to moderate algal biomass. Phytoplankton production tended to be largest during the summer. During the summer, phytoplankton densities and biovolumes generally were indicative of a moderate to large algal biomass. However, excessive algal production and biomass periodically occurred during the spring, summer, and fall. Three species of phytoplankton that are specifically associated with taste-and-odor problems in drinking water were identified on several occasions in water samples collected from Pueblo Reservoir. Reservoir operations and hydrodynamics can substantially affect processes that affect reservoir water quality. Stratification, underflow, and hypolimnetic withdrawals affect concentrations of dissolved solids, availability of nutrients, and concentrations of metals in the reservoir. Stratification impedes the mixing of epilimnetic and hypolimnetic waters, and the prevalent underflow that occurs during the summer results in a decrease in the potential dilution of inflowing river water with reservoir water. The underflow also decreases the maximum available nutrient load to the euphotic zone, which can, in turn, offset the maximum algal growth potential. Increased dissolved-solids, nutrient, and metal concentrations that occur in the hypolimnion during the summer are partially offset by hypolimnetic withdrawals.

Potential Aquifer Vulnerability in Regions Down-Gradient from Uranium In Situ Recovery (ISR) Sites

EPA Science Inventory

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 rock...

Chemical Equilibrium of the Dissolved Uranium in Groundwaters From a Spanish Uranium-Ore Deposit

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

Garralon, Antonio; Gomez, Paloma; Turrero, Maria Jesus

2007-07-01

The main objectives of this work are to determine the hydrogeochemical evolution of an uranium ore and identify the main water/rock interaction processes that control the dissolved uranium content. The Mina Fe uranium-ore deposit is the most important and biggest mine worked in Spain. Sageras area is located at the north part of the Mina Fe, over the same ore deposit. The uranium deposit was not mined in Sageras and was only perturbed by the exploration activities performed 20 years ago. The studied area is located 10 Km northeast of Ciudad Rodrigo (Salamanca) at an altitude over 650 m.a.s.l. Themore » uranium mineralization is related to faults affecting the metasediments of the Upper Proterozoic to Lower Cambrian schist-graywacke complex (CEG), located in the Centro-Iberian Zone of the Hesperian Massif . The primary uranium minerals are uraninite and coffinite but numerous secondary uranium minerals have been formed as a result of the weathering processes: yellow gummite, autunite, meta-autunite, torbernite, saleeite, uranotile, ianthinite and uranopilite. The water flow at regional scale is controlled by the topography. Recharge takes place mainly in the surrounding mountains (Sierra Pena de Francia) and discharge at fluvial courses, mainly Agueda and Yeltes rivers, boundaries S-NW and NE of the area, respectively. Deep flows (lower than 100 m depth) should be upwards due to the river vicinity, with flow directions towards the W, NW or N. In Sageras-Mina Fe there are more than 100 boreholes drilled to investigate the mineral resources of the deposit. 35 boreholes were selected in order to analyze the chemical composition of groundwaters based on their depth and situation around the uranium ore. Groundwater samples come from 50 to 150 m depth. The waters are classified as calcium-bicarbonate type waters, with a redox potential that indicates they are slightly reduced (values vary between 50 to -350 mV). The TOC varies between <0.1 and 4.0 mgC/L and the dissolved uranium has a maximum value of 7.7 mg/L. According the analytical data of dissolved uranium, the mineral closest to equilibrium seems to be UO{sub 2}(am). The tritium contents in the groundwaters vary between 1.5 and 7.3 T.U. Considering that the mean value of tritium in rainwater from the studied area has a value of 4 T.U., it can be concluded that the residence times of the groundwaters are relatively short, not longer than 50 years in the oldest case. (authors)« less

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.

Preparation of uranium compounds

DOEpatents

Kiplinger, Jaqueline L; Montreal, Marisa J; Thomson, Robert K; Cantat, Thibault; Travia, Nicholas E

2013-02-19

UI.sub.3(1,4-dioxane).sub.1.5 and UI.sub.4(1,4-dioxane).sub.2, were synthesized in high yield by reacting turnings of elemental uranium with iodine dissolved in 1,4-dioxane under mild conditions. These molecular compounds of uranium are thermally stable and excellent precursor materials for synthesizing other molecular compounds of uranium including alkoxide, amide, organometallic, and halide compounds.

Measurements of natural radioactivity concentration in drinking water samples of Shiraz city and springs of the Fars province, Iran, and dose estimation.

PubMed

Mehdizadeh, Simin; Faghihi, Reza; Sina, Sedigheh; Derakhshan, Shahrzad

2013-11-01

The Fars province is located in the south-west region of Iran where different nuclear sites has been established, such as Bushehr Nuclear Power Plant. In this research, 92 water samples from the water supplies of Shiraz city and springs of the Fars province were investigated with regard to the concentrations of natural radioactive elements, total uranium, (226)Ra, gross alpha and gross beta. (226)Ra concentration was determined by the (222)Rn emanation method. To measure the total uranium concentration, a laser fluorimetry analyzer (UA-3) was used. The mean concentration of (226)Ra in Shiraz's water resources was 23.9 mBq l(-1), while 93 % of spring waters have a concentration <2 mBq l(-1). The results of uranium concentration measurements show the mean concentrations of 7.6 and 6 μg l(-1) in the water of Shiraz and springs of Fars, respectively. The gross alpha and beta concentrations measured by the evaporation method were lower than the limit of detection of the measuring instruments used in this survey. The mean annual effective doses of infants, children and adults from (238)U and (226)Ra content of Shiraz's water and spring waters were estimated. According to the results of this study, the activity concentration in water samples were below the maximum permissible concentrations determined by the World Health Organization and the US Environmental Protection Agency. Finally, the correlation between (226)Ra and total U activity concentrations and geochemical properties of water samples, i.e. pH, total dissolve solids and SO4(-2), were estimated.

Water-quality data for Navajo National Monument, northeastern Arizona--2001-02

USGS Publications Warehouse

Thomas, Blakemore E.

2003-01-01

Water-quality data are provided for six sites in Navajo National Monument in northeastern Arizona. These data describe the current water quality and provide baseline water-quality information for monitoring future trends. Water samples were collected from six sites near three ancient Indian ruins during September 2001 to August 2002. Two springs and one well near Betatakin Ruin, one spring is near Keet Seel Ruin, and one spring and one stream are near Inspection House Ruin. Water from all the sites is from the N aquifer, a regional sandstone aquifer that is the source of drinking water for most members of the Navajo Nation and Hopi Tribe in northeastern Arizona. Concentrations of dissolved solids, major ions, trace elements, and uranium were low at the six sites. Dissolved-solids concentration ranged from 94 to 221 milligrams per liter. Concentrations of dissolved nitrate (as nitrogen) were generally low (less than 0.05 to 0.92 milligrams per liter) and were within the range of concentrations at other N-aquifer sites within 20 miles of the study area. Water samples from Inscription House Spring, Navajo Creek Tributary (near Inscription House Ruin), and Keet Seel Ruin Spring contained indicators of human or animal wastes--fecal coliform and Escherichia coli bacteria.

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

DOEpatents

Boyd, G.E.; Adamson, A.W.; Schubert, J.; Russell, E.R.

1958-10-01

A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This process provides a convenient and efficient means for isolating plutonium.

Biosorption of uranium by Pseudomonas aeruginosa strain CSU: Characterization and comparison studies

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

Hu, M.Z.C.; Norman, J.M.; Faison, B.D.

1996-07-20

Pseudomonas aeruginosa strain CSU, a nongenetically engineered bacterial strain known to bind dissolved hexavalent uranium (as UO{sub 2}{sup 2+} and/or its cationic hydroxo complexes) was characterized with respect to its sorptive activity. The uranium biosorption equilibrium could be described by the Langmuir isotherm. The rate of uranium adsorption increased following permeabilization of the outer and/or cytoplasmic membrane by organic solvents such as acetone. P. aeruginosa CSU biomass was significantly more sorptive toward uranium than certain novel, patented biosorbents derived from algal or fungal biomass sources. P. aeruginosa CSU biomass was also competitive with commercial cation-exchange resins, particularly in the presencemore » of dissolved transition metals. Uranium binding by P. aeruginosa CSU was clearly pH dependent. Uranium loading capacity increased with increasing pH under acidic conditions, presumably as a function of uranium speciation and due to the H{sup +} competition at some binding sites. Nevertheless, preliminary evidence suggests that this microorganism is also capable of binding anionic hexavalent uranium complexes. Ferric iron was a strong inhibitor of uranium binding to P. aeruginosa CSU biomass, and the presence of uranium also decreased the Fe{sup 3+} loading when the biomass was not saturated with Fe{sup 3+}. Thus, a two-state process in which iron and uranium are removed in consecutive steps was proposed for efficient use of the biomass as a biosorbent in uranium removal from mine wastewater, especially acidic leachates.« less

URANIUM BISMUTHIDE DISPERSION IN MOLTEN METAL

DOEpatents

Teitel, R.J.

1959-10-27

The formation of intermetallic bismuth compounds of thorium or uranium dispersed in a liquid media containing bismuth and lead is described. A bismuthide of uranium dispersed in a liquid metal medium is formed by dissolving uranium in composition of lead and bismuth containing less than 80% lead and lowering the temperature of the composition to a temperature below the point at which the solubility of uranium is exceeded and above the melting point of the composition.

Preparation, certification and validation of a stable solid spike of uranium and plutonium coated with a cellulose derivative for the measurement of uranium and plutonium content in dissolved nuclear fuel by isotope dilution mass spectrometry.

PubMed

Surugaya, Naoki; Hiyama, Toshiaki; Verbruggen, André; Wellum, Roger

2008-02-01

A stable solid spike for the measurement of uranium and plutonium content in nitric acid solutions of spent nuclear fuel by isotope dilution mass spectrometry has been prepared at the European Commission Institute for Reference Materials and Measurements in Belgium. The spike contains about 50 mg of uranium with a 19.838% (235)U enrichment and 2 mg of plutonium with a 97.766% (239)Pu abundance in each individual ampoule. The dried materials were covered with a thin film of cellulose acetate butyrate as a protective organic stabilizer to resist shocks encountered during transportation and to eliminate flaking-off during long-term storage. It was found that the cellulose acetate butyrate has good characteristics, maintaining a thin film for a long time, but readily dissolving on heating with nitric acid solution. The solid spike containing cellulose acetate butyrate was certified as a reference material with certified quantities: (235)U and (239)Pu amounts and uranium and plutonium amount ratios, and was validated by analyzing spent fuel dissolver solutions of the Tokai reprocessing plant in Japan. This paper describes the preparation, certification and validation of the solid spike coated with a cellulose derivative.

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.

A METHOD OF PREPARING URANIUM DIOXIDE

DOEpatents

Scott, F.A.; Mudge, L.K.

1963-12-17

A process of purifying raw, in particular plutonium- and fission- products-containing, uranium dioxide is described. The uranium dioxide is dissolved in a molten chloride mixture containing potassium chloride plus sodium, lithium, magnesium, or lead chloride under anhydrous conditions; an electric current and a chlorinating gas are passed through the mixture whereby pure uranium dioxide is deposited on and at the same time partially redissolved from the cathode. (AEC)

Geohydrologic, geochemical, and geologic controls on the occurrence of radon in ground water near Conifer, Colorado, USA

USGS Publications Warehouse

Lawrence, E.; Poeter, E.; Wanty, R.

1991-01-01

Integrated studies of geohydrology, geochemistry, and geology of crystalline rocks in the vicinity of Conifer, Colorado, reveal that radon concentrations do not correlate with variations in concentrations of other dissolved species. Concentrations of major ions show systematic variations along selected groundwater flowpaths, whereas radon concentrations are dependent on local geochemical and geologic phenomena (such as localized uranium concentration in the rock or the presence of faults or folds). When radon enters the flow system, concentrations do not increase along flowpaths because its decay rate is fast relative to groundwater flow rates. Radon-222 is not in secular equilibrium with 238U and 226Ra in the water. Therefore, most of the 238U and 226Ra necessary to support the waterborne 222Rn must be present locally in the rock. High concentrations of dissolved radon are not found in zones of high transmissivity, and transmissivity is not correlated with rock type in the study area. A higher transmissivity can be indicative of higher water-volume to rock-surface-area ratios, which could effectively dilute 222Rn entering the water and/or may indicate that emanated radon is carried away more rapidly. Water samples collected from individual wells over periods of several months showed significant fluctuations in the dissolved 222Rn content. This fluctuation may be controlled by changes in the contributions of water-producing zones within the well resulting from seasonal fluctuations of the water table and/or pumping stresses. ?? 1991.

Determination of the oxidation state of uranium in apatite and phosphorite deposits

USGS Publications Warehouse

Clarke, R.S.; Altschuler, Z.S.

1958-01-01

Geological and mineralogical evidence indicate that the uranium present in apatite may proxy for calcium in the mineral structure as U(IV). An experimental investigation was conducted and chemical evidence was obtained that establishes the presence of U(IV) in apatite. The following analytical procedure was developed for the determination of U(IV). Carbonatefluorapatite is dissolved in 1.5 M orthophosphoric acid at a temperature of 5??C or slightly below and fluorapatite is dissolved in cold 1.2 M hydrochloric acid (approximately 5??C) containing 1.5 g of hydroxylamine hydrochloride per 100 ml. Uranium(IV) is precipitated by cupferron using titanium as a carrier. The uranium in the precipitate is separated by use of the ethyl acetate extraction procedure and determined fluorimetrically. The validity and the limitations of the method have been established by spike experiments. ?? 1958.

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.

Process for recovering niobium from uranium-niobium alloys

DOEpatents

Wallace, Steven A.; Creech, Edward T.; Northcutt, Walter G.

1983-01-01

Niobium is recovered from scrap uranium-niobium alloy by melting the scrap with tin, solidifying the billet thus formed, heating the billet to combine niobium with tin therein, placing the billet in hydrochloric acid to dissolve the uranium and leave an insoluble residue of niobium stannide, then separating the niobium stannide from the acid.

Process for recovering niobium from uranium-niobium alloys

DOEpatents

Wallace, S.A.; Creech, E.T.; Northcutt, W.G.

1982-09-27

Niobium is recovered from scrap uranium-niobium alloy by melting the scrap with tin, solidifying the billet thus formed, heating the billet to combine niobium with tin therein, placing the billet in hydrochloric acid to dissolve the uranium and form a precipitate of niobium stannide, then separating the precipitate from the acid.

Webinar on the Removal of Uranium from Drinking Water by Small System Treatment Technology

EPA Science Inventory

Abstract: Radionuclides, such as uranium (U), occur naturally as trace elements in rocks and soils and thus can be found in dissolved forms in ground waters. Uranium has four oxidation states (+3, +4, +5, and +6) and is a very reactive element forming a variety of stable complexe...

METHOD OF DISSOLVING REFRACTORY ALLOYS

DOEpatents

Helton, D.M.; Savolainen, J.K.

1963-04-23

This patent relates to the dissolution of alloys of uranium with zirconium, thorium, molybdenum, or niobium. The alloy is contacted with an anhydrous solution of mercuric chloride in a low-molecular-weight monohydric alcohol to produce a mercury-containing alcohol slurry. The slurry is then converted to an aqueous system by adding water and driving off the alcohol. The resulting aqueous slurry is electrolyzed in the presence of a mercury cathode to remove the mercury and produce a uranium-bearing aqueous solution. This process is useful for dissolving irradiated nuclear reactor fuels for radiochemical reprocessing by solvent extraction. In addition, zirconium-alloy cladding is selectively removed from uranium dioxide fuel compacts by this means. (AEC)

Release of 226Ra from uranium mill tailings by microbial Fe(III) reduction

USGS Publications Warehouse

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

1991-01-01

Uranium mill tailings were anaerobically incubated in the presence of H2 with Alteromonas putrefaciens, a bacterium known to couple the oxidation of H2 and organic compounds to the reduction of Fe(III) oxides. There was a direct correlation between the extent of Fe(III) reduction and the accumulation of dissolved 226Ra. In sterile tailings in which Fe(III) was not reduced, there was negligible leaching of 226Ra. The behavior of Ba was similar to that of Ra in inoculated and sterile systems. These results demonstrate that under anaerobic conditions, microbial reduction of Fe(III) may result in the release of dissolved 226Ra from uranium mill tailings. ?? 1991.

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

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

Boyd, G.E.; Adamson, A.W.; Schubert, J.

A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This processmore » provides a convenient and efficient means for isolating plutonium.« less

Process for alloying uranium and niobium

DOEpatents

Holcombe, Cressie E.; Northcutt, Jr., Walter G.; Masters, David R.; Chapman, Lloyd R.

1991-01-01

Alloys such as U-6Nb are prepared by forming a stacked sandwich array of uraniun sheets and niobium powder disposed in layers between the sheets, heating the array in a vacuum induction melting furnace to a temperature such as to melt the uranium, holding the resulting mixture at a temperature above the melting point of uranium until the niobium dissolves in the uranium, and casting the uranium-niobium solution. Compositional uniformity in the alloy product is enabled by use of the sandwich structure of uranium sheets and niobium powder.

ELECTROCHEMICAL DECONTAMINATION AND RECOVERY OF URANIUM VALUES

DOEpatents

McLaren, J.A.; Goode, J.H.

1958-05-13

An electrochemical process is described for separating uranium from fission products. The method comprises subjecting the mass of uranium to anodic dissolution in an electrolytic cell containing aqueous alkali bicarbonate solution as its electrolyte, thereby promoting a settling from the solution of a solid sludge from about the electrodes and separating the resulting electrolyte solution containing the anodically dissolved uranium from the sludge which contains the rare earth fission products.

ELECTROLYTIC PRODUCTION OF URANIUM TETRAFLUORIDE

DOEpatents

Lofthouse, E.

1954-08-31

This patent relates to electrolytic methods for the production of uranium tetrafluoride. According to the present invention a process for the production of uranium tetrafluoride comprises submitting to electrolysis an aqueous solution of uranyl fluoride containing free hydrofluoric acid. Advantageously the aqueous solution of uranyl fluoride is obtained by dissolving uranium hexafluoride in water. On electrolysis, the uranyl ions are reduced to uranous tons at the cathode and immediately combine with the fluoride ions in solution to form the insoluble uranium tetrafluoride which is precipitated.

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

Washiya, Tadahiro; Komaki, Jun; Funasaka, Hideyuki

Japan Atomic Energy Agency (JAEA) has been developing the new aqueous reprocessing system named 'NEXT' (New Extraction system for TRU recovery)1-2, which provides many advantages as waste volume reduction, cost savings by advanced components and simplification of process operation. Advanced head-end systems in the 'NEXT' process consist of fuel disassembly system, fuel shearing system and continuous dissolver system. We developed reliable fuel disassembly system with innovative procedure, and short-length shearing system and continuous dissolver system can be provided highly concentrated dissolution to adapt to the uranium crystallization process. We have carried out experimental studies, and fabrication of engineering-scale test devicesmore » to confirm the systems performance. In this paper, research and development of advanced head-end systems are described. (authors)« less

Dissolution of synthetic uranium dibutyl phosphate deposits in oxidizing and reducing chemical formulations.

PubMed

Rufus, A L; Sathyaseelan, V S; Narasimhan, S V; Velmurugan, S

2013-06-15

Permanganate and nitrilotriacetic acid (NTA) based dilute chemical formulations were evaluated for the dissolution of uranium dibutyl phosphate (U-DBP), a compound that deposits over the surfaces of nuclear reprocessing plants and waste storage tanks. A combination of an acidic, oxidizing treatment (nitric acid with permanganate) followed by reducing treatment (NTA based formulation) efficiently dissolved the U-DBP deposits. The dissolution isotherm of U-DBP in its as precipitated form followed a logarithmic fit. The same chemical treatment was also effective in dissolving U-DBP coated on the surface of 304-stainless steel, while resulting in minimal corrosion of the stainless steel substrate material. Investigation of uranium recovery from the resulting decontamination solutions by ion exchange with a bed of mixed anion and cation resins showed quantitative removal of uranium. Copyright © 2013 Elsevier B.V. All rights reserved.

Review and interpretation of previous work and new data on the hydrogeology of the Schwartzwalder Uranium Mine and vicinity, Jefferson County, Colorado

USGS Publications Warehouse

Caine, Jonathan S.; Johnson, Raymond H.; Wild, Emily C.

2011-01-01

The Schwartzwalder deposit is the largest known vein type uranium deposit in the United States. Located about eight miles northwest of Golden, Colorado it occurs in Proterozoic metamorphic rocks and was formed by hydrothermal fluid flow, mineralization, and deformation during the Laramide Orogeny. A complex brittle fault zone hosts the deposit comprising locally brecciated carbonate, oxide, and sulfide minerals. Mining of pitchblende, the primary ore mineral, began in 1953 and an extensive network of underground workings was developed. Mine dewatering, treatment of the effluent and its discharge into the adjacent Ralston Creek was done under State permit from about 1990 through about 2008. Mining and dewatering ceased in 2000 and natural groundwater rebound has filled the mine workings to a current elevation that is above Ralston Creek but that is still below the lowest ground level adit. Water in the 'mine pool' has concentrations of dissolved uranium in excess of 1,000 times the U.S. Environmental Protection Agency drinking-water standard of 30 milligrams per liter. Other dissolved constituents such as molybdenum, radium, and sulfate are also present in anomalously high concentrations. Ralston Creek flows in a narrow valley containing Quaternary alluvium predominantly derived from weathering of crystalline bedrock including local mineralized rock. Just upstream of the mine site, two capped and unsaturated waste rock piles with high radioactivity sit on an alluvial terrace. As Ralston Creek flows past the mine site, a host of dissolved metal concentrations increase. Ralston Creek eventually discharges into Ralston Reservoir about 2.5 miles downstream. Because of highly elevated uranium concentrations, the State of Colorado issued an enforcement action against the mine permit holder requiring renewed collection and treatment of alluvial groundwater. As part of planned mine reclamation, abundant data were collected and compiled into a report by Wyman and Effner (2007), which was to be used as a basis for eventual mine site closure. In 2010 the U.S. Geological Survey was asked by the State of Colorado to provide an objective and independent review of the Wyman and Effner (2007) report and to identify gaps in knowledge regarding the hydrogeology of the mine site. Key findings from the U.S. Geological Survey assessment include geological structural analysis indicating that although the primary uranium-hosting fault likely does not cross under Ralston Creek, many complex subsidiary faults do cross under Ralston Creek. It is unknown if any of these faults act as conduits for mine pool water to enter Ralston Creek. Reported bedrock permeabilities are low, but local hydraulic gradients are sufficient to potentially drive groundwater flow from the mine pool to the creek. Estimated average linear velocities for the full range of reported hydraulic conductivities indicate groundwater transit times from the mine pool to the creek on the order of a few months to about 3,800 years or 11 to 65 years using mean reported input values. These estimates do not account for geochemical reactions along any given flow path that may differentially enhance or retard movement of individual dissolved constituents. New reconnaissance data including 34S isotope and 234U/238U isotopic activity ratios show potentially distinctive signatures for the mine pool compared to local groundwater and Ralston Creek water above the mine site. Although the mine pool may be near an equilibrium elevation, evidence for groundwater recharge transients indicates inflow to the workings that are greater than outflow. There is not enough hydraulic head data adjacent to the mine workings to adequately constrain a final equilibrium elevation or to predict how several wet years in succession might affect variations in mine pool elevation. Although ground level adits are sealed with bulkheads, if the mine pool elevation were to rise slightly to the elevation of or abo

The Niobrara Formation as a challenge to water quality in the Arkansas River, Colorado, USA

USGS Publications Warehouse

Bern, Carleton R.; Stogner, Sr., Robert W.

2017-01-01

Study regionArkansas River, east of the Rocky Mountains.Study focusCretaceous sedimentary rocks in the western United States generally pose challenges to water quality, often through mobilization of salts and trace metals by irrigation. However, in the Arkansas River Basin of Colorado, patchy exposure of multiple Cretaceous formations has made it difficult to identify which formations are most problematic. This paper examines water quality in surface-water inflows along a 26-km reach of the Arkansas River relative to the presence or absence of the Cretaceous Niobrara Formation within the watershed.New hydrological insights for the regionPrincipal component analysis (PCA) shows Niobrara-influenced inflows have distinctive geochemistry, particularly with respect to Na, Mg, SO42−, and Se. Uranium concentrations are also greater in Niobrara-influenced inflows. During the irrigation season, median dissolved solids, Se, and U concentrations in Niobrara-influenced inflows were 83%, 646%, and 55%, respectively, greater than medians where Niobrara Formation surface exposures were absent. During the non-irrigation season, which better reflects geologic influence, the differences were more striking. Median dissolved solids, Se, and U concentrations in Niobrara-influenced inflows were 288%, 863%, and 155%, respectively, greater than median concentrations where the Niobrara Formation was absent. Identification of the Niobrara Formation as a disproportionate source for dissolved solids, Se, and U will allow for more targeted studies and management, particularly where exposures underlie irrigated agriculture.

Effect of molybdenum ion implantation of the pitting corrosion of depleted uranium - 0.75 titanium alloy. (Reannouncement with new availability information). Final report

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

Lei, K.S.; Chang, F.; Levy, M.

1993-07-01

Pitting corrosion of molybdenum-ion-implanted, depleted uranium -0 75 Ti (DU -0 75 Ti) has been studied electrochemically in acidic, neutral, and alkaline solutions containing sodium chloride, and the results have been compared to those of the unimplanted DU -0 75 Ti. The data show that Mo implantation shifts the pitting potential of DU -0 75 Ti in the noble direction in acidic and alkaline solutions. In neutral 50 ppm Cl- solution, however, there is no beneficial effect of Mo implantation. Auger analysis studies show that before exposure to the solutions, all the molybdenum is in the oxide, which is approximatelymore » l000 A thick. After electrochemical scans in the acidic and alkaline chloride solutions, most of the Mo disappears from the oxide. However, no decrease in Mo concentration is found after exposure in neutral chloride solution. It is proposed that the implanted molybdenum dissolves in the acidic and alkaline solutions and forms simple or complex molybdates that inhibit pitting corrosion. The implanted molybdenum does not dissolve in the neutral chloride solution and inhibition does not occur.« less

Uranium isotopes in groundwater occurring at Amazonas State, Brazil.

PubMed

da Silva, Márcio Luiz; Bonotto, Daniel Marcos

2015-03-01

This paper reports the behavior of the dissolved U-isotopes (238)U and (234)U in groundwater providing from 15 cities in Amazonas State, Brazil. The isotope dilution technique accompanied by alpha spectrometry were utilized for acquiring the U content and (234)U/(238)U activity ratio (AR) data, 0.01-1.4µgL(-1) and 1.0-3.5, respectively. These results suggest that the water is circulating in a reducing environment and leaching strata containing minerals with low uranium concentration. A tendency to increasing ARs values following the groundwater flow direction is identified in Manaus city. The AR also increases according to the SW-NE directions: Uarini→Tefé; Manacapuru→Manaus; Presidente Figueiredo→São Sebastião do Uatumã; and Boa Vista do Ramos→Parintins. Such trends are possibly related to several factors, among them the increasing acid character of the waters. The waters analyzed are used for human consumption and the highest dissolved U content is much lower than the maximum established by the World Health Organization. Therefore, in view of this radiological parameter they can be used for drinking purposes. Copyright © 2014 Elsevier Ltd. All rights reserved.

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.

PRODUCTION OF URANIUM AND THORIUM COMPOUNDS

DOEpatents

Arden, T.V.; Burstall, F.H.; Linstead, R.P.; Wells, R.A.

1955-12-27

Compounds of Th and U are extracted with an organic solvent in the presence of an adsorbent substance which has greater retentivity for impurities present than for the uranium and/or thorium. The preferred adsorbent material is noted as being cellulose. The uranium and thoriumcontaining substances treated are preferably in the form of dissolved nitrates, and the preferred organic solvent is diethyl ether.

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS

DOEpatents

Nicholls, C.M.; Wells, I.; Spence, R.

1959-10-13

The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.

METHOD OF RECOVERING URANIUM COMPOUNDS

DOEpatents

Poirier, R.H.

1957-10-29

S>The recovery of uranium compounds which have been adsorbed on anion exchange resins is discussed. The uranium and thorium-containing residues from monazite processed by alkali hydroxide are separated from solution, and leached with an alkali metal carbonate solution, whereby the uranium and thorium hydrorides are dissolved. The carbonate solution is then passed over an anion exchange resin causing the uranium to be adsorbed while the thorium remains in solution. The uranium may be recovered by contacting the uranium-holding resin with an aqueous ammonium carbonate solution whereby the uranium values are eluted from the resin and then heating the eluate whereby carbon dioxide and ammonia are given off, the pH value of the solution is lowered, and the uranium is precipitated.

Thorium distributions in high- and low-dust regions and the significance for iron supply

NASA Astrophysics Data System (ADS)

Hayes, Christopher T.; Rosen, Jeffrey; McGee, David; Boyle, Edward A.

2017-02-01

Thorium and uranium isotopes (232Th, 230Th, 238U, and 234U) were investigated to refine their use for estimating mineral dust deposition and Fe delivery to the ocean. U concentrations and isotope ratios were consistent with conservative behavior and can safely be described using published U-salinity relationships and global average seawater isotopic composition. Near Barbados, waters affected by the Amazon outflow contained elevated 232Th. This signals one region where the thorium-dust method is inaccurate because of a confounding continental input. Dissolved 232Th fluxes in this region suggest that Amazonian Fe supply to the adjacent open ocean is much larger than local atmospheric deposition. The colloidal content of dissolved Th south of Bermuda was found to be quite small (2-6%), similar to that found north of Hawaii, despite the order of magnitude higher dust deposition in the Atlantic. This finding supports the assumption that dissolved 232Th and 230Th are scavenged at the same rate despite their different sources and also sheds light on the increase of dissolved 232Th fluxes with integrated depth. Outside the region influenced by Amazon River waters, dissolved 232Th fluxes are compared with Bermudan aerosol Fe deposition to estimate that fractional Th solubility is around 20% in this region. Finally, new dissolved and soluble Fe, Mn, and Cr data from the subtropical North Pacific support the idea that Fe concentrations in the remote ocean are highly buffered, whereas 232Th has a larger dynamic range between high- and low-dust regions.

Uranium speciation in biofilms studied by laser fluorescence techniques.

PubMed

Arnold, Thuro; Grossmann, Kay; Baumann, Nils

2010-03-01

Biofilms may immobilize toxic heavy metals in the environment and thereby influence their migration behaviour. The mechanisms of these processes are currently not understood, because the complexity of such biofilms creates many discrete geochemical microenvironments which may differ from the surrounding bulk solution in their bacterial diversity, their prevailing geochemical properties, e.g. pH and dissolved oxygen concentration, the presence of organic molecules, e.g. metabolites, and many more, all of which may affect metal speciation. To obtain such information, which is necessary for performance assessment studies or the development of new cost-effective strategies for cleaning waste waters, it is very important to develop new non-invasive methods applicable to study the interactions of metals within biofilm systems. Laser fluorescence techniques have some superior features, above all very high sensitivity for fluorescent heavy metals. An approach combining confocal laser scanning microscopy and laser-induced fluorescence spectroscopy for study of the interactions of biofilms with uranium is presented. It was found that coupling these techniques furnishes a promising tool for in-situ non-invasive study of fluorescent heavy metals within biofilm systems. Information on uranium speciation and uranium redox states can be obtained.

Quantifying differences in the impact of variable chemistry on equilibrium uranium(VI) adsorption properties of aquifer sediments

USGS Publications Warehouse

Stoliker, Deborah L.; Kent, Douglas B.; Zachara, John M.

2011-01-01

Uranium adsorption-desorption on sediment samples collected from the Hanford 300-Area, Richland, WA varied extensively over a range of field-relevant chemical conditions, complicating assessment of possible differences in equilibrium adsorption properties. Adsorption equilibrium was achieved in 500-1000 h although dissolved uranium concentrations increased over thousands of hours owing to changes in aqueous chemical composition driven by sediment-water reactions. A nonelectrostatic surface complexation reaction, >SOH + UO22+ + 2CO32- = >SOUO2(CO3HCO3)2-, provided the best fit to experimental data for each sediment sample resulting in a range of conditional equilibrium constants (logKc) from 21.49 to 21.76. Potential differences in uranium adsorption properties could be assessed in plots based on the generalized mass-action expressions yielding linear trends displaced vertically by differences in logKc values. Using this approach, logKc values for seven sediment samples were not significantly different. However, a significant difference in adsorption properties between one sediment sample and the fines (Kc uncertainty were improved by capturing all data points within experimental errors. The mass-action expression plots demonstrate that applying models outside the range of conditions used in model calibration greatly increases potential errors.

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.

Estimation of uranium migration parameters in sandstone aquifers.

PubMed

Malov, A I

2016-03-01

The chemical composition and isotopes of carbon and uranium were investigated in groundwater samples that were collected from 16 wells and 2 sources in the Northern Dvina Basin, Northwest Russia. Across the dataset, the temperatures in the groundwater ranged from 3.6 to 6.9 °C, the pH ranged from 7.6 to 9.0, the Eh ranged from -137 to +128 mV, the total dissolved solids (TDS) ranged from 209 to 22,000 mg L(-1), and the dissolved oxygen (DO) ranged from 0 to 9.9 ppm. The (14)C activity ranged from 0 to 69.96 ± 0.69 percent modern carbon (pmC). The uranium content in the groundwater ranged from 0.006 to 16 ppb, and the (234)U:(238)U activity ratio ranged from 1.35 ± 0.21 to 8.61 ± 1.35. The uranium concentration and (234)U:(238)U activity ratio increased from the recharge area to the redox barrier; behind the barrier, the uranium content is minimal. The results were systematized by creating a conceptual model of the Northern Dvina Basin's hydrogeological system. The use of uranium isotope dating in conjunction with radiocarbon dating allowed the determination of important water-rock interaction parameters, such as the dissolution rate:recoil loss factor ratio Rd:p (a(-1)) and the uranium retardation factor:recoil loss factor ratio R:p in the aquifer. The (14)C age of the water was estimated to be between modern and >35,000 years. The (234)U-(238)U age of the water was estimated to be between 260 and 582,000 years. The Rd:p ratio decreases with increasing groundwater residence time in the aquifer from n × 10(-5) to n × 10(-7) a(-1). This finding is observed because the TDS increases in that direction from 0.2 to 9 g L(-1), and accordingly, the mineral saturation indices increase. Relatively high values of R:p (200-1000) characterize aquifers in sandy-clayey sediments from the Late Pleistocene and the deepest parts of the Vendian strata. In samples from the sandstones of the upper part of the Vendian strata, the R:p value is ∼ 24, i.e., sorption processes are expressed more weakly, and uranium is possibly desorbed from the sediments. Overall, these results provide a better understanding of the evolution of uranium isotopes in groundwater systems. Copyright © 2015 Elsevier Ltd. All rights reserved.

Method for processing aqueous wastes

DOEpatents

Pickett, John B.; Martin, Hollis L.; Langton, Christine A.; Harley, Willie W.

1993-01-01

A method for treating waste water such as that from an industrial processing facility comprising the separation of the waste water into a dilute waste stream and a concentrated waste stream. The concentrated waste stream is treated chemically to enhance precipitation and then allowed to separate into a sludge and a supernate. The supernate is skimmed or filtered from the sludge and blended with the dilute waste stream to form a second dilute waste stream. The sludge remaining is mixed with cementitious material, rinsed to dissolve soluble components, then pressed to remove excess water and dissolved solids before being allowed to cure. The dilute waste stream is also chemically treated to decompose carbonate complexes and metal ions and then mixed with cationic polymer to cause the precipitated solids to flocculate. Filtration of the flocculant removes sufficient solids to allow the waste water to be discharged to the surface of a stream. The filtered material is added to the sludge of the concentrated waste stream. The method is also applicable to the treatment and removal of soluble uranium from aqueous streams, such that the treated stream may be used as a potable water supply.

Assessing selenium contamination in the irrigated stream-aquifer system of the Arkansas River, Colorado.

PubMed

Gates, Timothy K; Cody, Brent M; Donnelly, Joseph P; Herting, Alexander W; Bailey, Ryan T; Mueller Price, Jennifer

2009-01-01

Prudent interventions for reducing selenium (Se) in groundwater and streams within an irrigated river valley must be guided by a sound understanding of current field conditions. An emerging picture of the nature of Se contamination within the Lower Arkansas River Valley in Colorado is provided by data from a large number of groundwater and surface water sampling locations within two study regions along the river. Measurements show that dissolved Se concentrations in the river are about double the current Colorado Department of Public Health and Environment (CDPHE) chronic standard of 4.6 microg L(-1) for aquatic habitat in the upstream region and exceed the standard by a factor of 2 to 4 in the downstream region. Groundwater concentrations average about 57.7 microg L(-1) upstream and 33.0 microg L(-1) downstream, indicating a large subsurface source for irrigation-induced dissolution and mobilization of Se loads to the river and its tributaries. Inverse correlation was found between Se concentration and the distance to the closest identified shale in the direction upstream along the principal groundwater flow gradient. The data also exhibited, among other relationships, a moderate to strong correlation between dissolved Se and total dissolved solids in groundwater and surface water, a strong correlation with uranium in groundwater, and power relationships with nitrate in groundwater. The relationship to nitrate, derived primarily from N fertilizers, reveals the degree to which dissolved Se depends on oxidation and inhibited reduction due to denitrification and suggests that there are prospects for reducing dissolved Se through nitrate control. Current and future results from these ongoing studies will help provide a foundation for modeling and for the discovery of best management practices (BMPs) in irrigated agriculture that can diminish Se contamination.

SELECTIVE SEPARATION OF URANIUM FROM FERRITIC STAINLESS STEELS

DOEpatents

Beaver, R.J.; Cherubini, J.H.

1963-05-14

A process is described for separating uranium from a nuclear fuel element comprising a uranium-containing core and a ferritic stainless steel clad by heating said element in a non-carburizing atmosphere at a temperature in the range 850-1050 un. Concent 85% C, rapidly cooling the heated element through the temperature range 815 un. Concent 85% to 650 EC to avoid annealing said steel, and then contacting the cooled element with an aqueous solution of nitric acid to selectively dissolve the uranium. (AEC)

Recovery of uranium values

DOEpatents

Brown, K. B.; Crouse, Jr., D. J.; Moore, J. G.

1959-03-10

A liquid-liquid extraction method is presented for recovering uranium values from an aqueous acidic solution by means of certain high molecular weight amine fn the amine classes of primary, secondary, heterocyclic secondary, tertiary, or heterocyclic tertiary. The uranium bearing aqueous acidic solution is contacted with the selected anine dissolved in a nonpolar waterimmiscible organfc solvent such as kerosene. The uranium which is substantially completely extracted by the organic phase may be stripped therefrom by water, and recovered from the aqueous phase by treatment into ammonia to precipitate ammonium diuranate.

RECOVERY OF URANIUM VALUES

DOEpatents

Brown, K.B.; Crouse, D.J. Jr.; Moore, J.G.

1959-03-10

A liquid-liquid extraction method is presented for recovering uranium values from an aqueous acidic solution by means of certain high molecular weight amine in the amine classes of primary, secondary, heterocyclic secondary, tertiary, or heterocyclic tertiary. The uranium bearing aqueous acidic solution is contacted with the selected amine dissolved in a nonpolar water-immiscible organic solvent such as kerosene. The uranium which is substantially completely exiracted by the organic phase may be stripped therefrom by waters and recovered from the aqueous phase by treatment into ammonia to precipitate ammonium diuranate.

URANIUM SEPARATION PROCESS

DOEpatents

Lyon, W.L.

1962-04-17

A method of separating uranium oxides from PuO/sub 2/, ThO/sub 2/, and other actinide oxides is described. The oxide mixture is suspended in a fused salt melt and a chlorinating agent such as chlorine gas or phosgene is sparged through the suspension. Uranium oxides are selectively chlorinated and dissolve in the melt, which may then be filtered to remove the unchlorinated oxides of the other actinides. (AEC)

New Fiber Materials with Sorption Capacity at 5.0 g-U/kg Adsorbent under Marine Testing Conditions

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

Saito, Tomonori; Brown, S.; Das, Sadananda

The Fuel Resources program of the Fuel Cycle Research and Development program of the Office of Nuclear Energy (NE) has focused on assuring that nuclear fuel resources are available in the United States for a long term. An immense source of uranium is seawater, which contains an estimated amount of 4.5 billion tonnes of dissolved uranium. Extraction of the uranium resource in seawater can provide a price cap and ensure centuries of uranium supply for future nuclear energy production. NE initiated a multidisciplinary program with participants from national laboratories, universities, and research institutes to enable technical breakthroughs related to uraniummore » recovery from seawater. The goal is to develop advanced adsorbents to make the seawater uranium recovery technology a cost competitive, viable technology. Under this program, Oak Ridge National Laboratory (ORNL) has developed several novel adsorbents, which enhanced the uranium capacity 4-5 times from the state-of-the art Japanese adsorbents. Uranium exists uniformly at a concentration of ~3.3 ppb in seawater. Because of the vast volume of the oceans, the total estimated amount of uranium in seawater is approximately 1000 times larger than its amount in terrestrial resources. However, due to the low concentration, a significant challenge remains for making the extraction of uranium from seawater a commercially viable alternative technology. The biggest challenge for this technology to overcome to efficiently reduce the extraction cost is to develop adsorbents with increased uranium adsorption capacity. Two major approaches were investigated for synthesizing novel adsorbents with enhanced uranium adsorption capacity. One method utilized conventional radiation induced graft polymerization (RIGP) to synthesize adsorbents on high-surface area trunk fibers and the other method utilized a chemical grafting technique, atom-transfer radical polymerization (ATRP). Both approaches have shown promising uranium extraction capacities: RIGP adsorbent achieved 5.00 ± 0.15 g U/kg-ads., while ATRP adsorbent achieved 6.56 ± 0.33 g U/kg-ads., after 56 days of seawater exposure. These achieved values are the highest adsorption capacities ever reported for uranium extraction from seawater. The study successfully demonstrated new fiber materials with sorption capacity at 5.0 g-U/kg adsorbent under marine testing conditions. Further optimization, investigation of other new materials as well as deepening our understanding will develop adsorbents that have even higher uranium adsorption capacity, increased selectivity, and faster kinetics.« less

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.

Inherently safe in situ uranium recovery

DOEpatents

Krumhansl, James L; Brady, Patrick V

2014-04-29

An in situ recovery of uranium operation involves circulating reactive fluids through an underground uranium deposit. These fluids contain chemicals that dissolve the uranium ore. Uranium is recovered from the fluids after they are pumped back to the surface. Chemicals used to accomplish this include complexing agents that are organic, readily degradable, and/or have a predictable lifetime in an aquifer. Efficiency is increased through development of organic agents targeted to complexing tetravalent uranium rather than hexavalent uranium. The operation provides for in situ immobilization of some oxy-anion pollutants under oxidizing conditions as well as reducing conditions. The operation also artificially reestablishes reducing conditions on the aquifer after uranium recovery is completed. With the ability to have the impacted aquifer reliably remediated, the uranium recovery operation can be considered inherently safe.

The detailed analysis of natural radionuclides dissolved in spa waters of the Kłodzko Valley, Sudety Mountains, Poland.

PubMed

Walencik-Łata, A; Kozłowska, B; Dorda, J; Przylibski, T A

2016-11-01

A survey was conducted to measure natural radioactivity in spa waters from the Kłodzko Valley. The main goal of this study was to determine the activity concentration of uranium, radium and radon isotopes in the investigated groundwaters. Samples were collected several times from 35 water intakes from 5 spas and 2 mineral water bottling plants. The authors examined whether the increased gamma radiation background, as well as the elevated values of radium and uranium content in reservoir rocks, have a significant impact on the natural radioactivity of these waters. The second objective of this research was to provide information about geochemistry of U, Ra, Rn radionuclides and the radiological and chemical risks incurred by ingestion of isotopes with drinking water. On the basis of results obtained, it is feasible to assess the health hazard posed by ingestion of natural radioactivity with drinking waters. Moreover, the data yielded by this research may be helpful in the process of verification of the application of these waters in balneotherapy. In addition, annual effective radiation doses resulting from the isotopes consumption were calculated on the basis of the evaluated activity concentrations. In dose assessment for uranium and radium isotopes, the authors provided values for different human age groups. The obtained uranium content in the investigated waters was compared with the currently valid regulations concerning the quality of drinking water. Based on the activity concentrations data, the activity isotopic ratios (234)U/(238)U, (226)Ra/(238)U, (222)Rn/(238)U, (222)Rn/(226)Ra and the correlations between radionuclides content were then examined. In brief, it may be concluded on the basis of the obtained results that radon solubility is inversely proportional to radium and uranium dissolution in environmental water circulation. The presented study allows conclusions to be drawn on the radionuclide circulation among different environmental biota: from lithosphere through hydrosphere to biosphere. Copyright © 2016 Elsevier B.V. All rights reserved.

Interim Report: Field Demonstration Of Permeable Reactive Barriers To Remove Dissolved Uranium From Groundwater, Fry Canyon, Utah

EPA Pesticide Factsheets

The Fry Canyon site in southeastern Utah was selected in 1996 as a long-term field demonstration site to assess the performance of selected permeable reactive barriers for the removal of uranium (U) from groundwater.

PROCESS OF DISSOLVING FUEL ELEMENTS OF NUCLEAR REACTORS

DOEpatents

Wall, E.M.V.; Bauer, D.T.; Hahn, H.T.

1963-09-01

A process is described for dissolving stainless-steelor zirconium-clad uranium dioxide fuel elements by immersing the elements in molten lead chloride, adding copper, cuprous chloride, or cupric chloride as a catalyst and passing chlorine through the salt mixture. (AEC)

METHOD OF IMPREGNATING A POROUS MATERIAL

DOEpatents

Steele, G.N.

1960-06-01

A method of impregnating a porous body with an inorganic uranium- containing salt is outlined and comprises dissolving a water-soluble uranium- containing salt in water; saturating the intercommunicating pores of the porous body with the salt solution; infusing ammonia gas into the intercommunicating pores of the body, the ammonia gas in water chemically reacting with the water- soluble uranium-containing salt in the water solvent to form a nonwater-soluble uranium-containing precipitant; and evaporating the volatile unprecipitated products from the intercommunicating pores whereby the uranium-containing precipitate is uniformly distributed in the intercommunicating peres of the porous body.

Neutralization of Plutonium and Enriched Uranium Solutions Containing Gadolinium as a Neutron Poison

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

BRONIKOWSKI, MG.

2004-04-01

Materials currently being dissolved in the HB-Line Facility will result in an accumulated solution containing an estimated uranium:plutonium (U:Pu) ratio of 4.3:1 and an 235U enrichment estimated at 30 per cent The U:Pu ratio and the enrichment are outside the evaluated concentration range for disposition to high level waste (HLW) using gadolinium (Gd) as a neutron poison. To confirm that the solution generated during the current HB-Line dissolving campaign can be poisoned with Gd, neutralized and discarded to the Savannah River Site (SRS) high level waste (HLW) system without undue nuclear safety concerns the caustic precipitation of surrogate solutions wasmore » examined. Experiments were performed with a U/Pu/Gd solution representative of the HB-Line estimated concentration ratio and also a U/Gd solution. Depleted U was used in the experiments as the enrichment of the U will not affect the chemical behavior during neutralization, but will affect the amount of Gd added to the solution. Settling behavior of the neutralized solutions was found to be comparable to previous studies. The neutralized solutions mixed easily and had expected densities of typical neutralized waste. The neutralized solids were found to be homogeneous and less than 20 microns in size. Partially neutralized solids were more amorphous than the fully neutralized solids. Based on the results of these experiments, Gd was found to be a viable poison for neutralizing a U/Pu/Gd solution with a U:Pu mass ratio of 4.3:1 thus extending the U:Pu mass ratio from the previously investigated 0-3:1 to 4.3:1. However, further work is needed to allow higher U concentrations or U:Pu ratios greater than investigated in this work.« 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.

FUEL ELEMENTS AND METHOD OF MAKING

DOEpatents

Noland, R.A.; Marzano, C.

1958-08-19

A process is described of surface-impregnating bodies of metallic uranium with silicon. Silicon metal is added to or admixed with alkali metal selected from the group consisting of sodiunn, potassium, and sodiunnpotassium alloy. The uraniunn body is then immersed in the mixture obtained and the temperature is raised to between 425 and 600 deg C. The silicon is dissolved and deposits as a uranium-silicon compound on the uranium body.

Powder-based adsorbents having high adsorption capacities for recovering dissolved metals and methods thereof

DOEpatents

Janke, Christopher J.; Dai, Sheng; Oyola, Yatsandra

2016-05-03

A powder-based adsorbent and a related method of manufacture are provided. The powder-based adsorbent includes polymer powder with grafted side chains and an increased surface area per unit weight to increase the adsorption of dissolved metals, for example uranium, from aqueous solutions. A method for forming the powder-based adsorbent includes irradiating polymer powder, grafting with polymerizable reactive monomers, reacting with hydroxylamine, and conditioning with an alkaline solution. Powder-based adsorbents formed according to the present method demonstrated a significantly improved uranium adsorption capacity per unit weight over existing adsorbents.

Foam-based adsorbents having high adsorption capacities for recovering dissolved metals and methods thereof

DOEpatents

Janke, Christopher J.; Dai, Sheng; Oyola, Yatsandra

2015-06-02

Foam-based adsorbents and a related method of manufacture are provided. The foam-based adsorbents include polymer foam with grafted side chains and an increased surface area per unit weight to increase the adsorption of dissolved metals, for example uranium, from aqueous solutions. A method for forming the foam-based adsorbents includes irradiating polymer foam, grafting with polymerizable reactive monomers, reacting with hydroxylamine, and conditioning with an alkaline solution. Foam-based adsorbents formed according to the present method demonstrated a significantly improved uranium adsorption capacity per unit weight over existing adsorbents.

222Rn transport in a fractured crystalline rock aquifer: Results from numerical simulations

USGS Publications Warehouse

Folger, P.F.; Poeter, E.; Wanty, R.B.; Day, W.; Frishman, D.

1997-01-01

Dissolved 222Rn concentrations in ground water from a small wellfield underlain by fractured Middle Proterozoic Pikes Peak Granite southwest of Denver, Colorado range from 124 to 840 kBq m-3 (3360-22700 pCi L-1). Numerical simulations of flow and transport between two wells show that differences in equivalent hydraulic aperture of transmissive fractures, assuming a simplified two-fracture system and the parallel-plate model, can account for the different 222Rn concentrations in each well under steady-state conditions. Transient flow and transport simulations show that 222Rn concentrations along the fracture profile are influenced by 222Rn concentrations in the adjoining fracture and depend on boundary conditions, proximity of the pumping well to the fracture intersection, transmissivity of the conductive fractures, and pumping rate. Non-homogeneous distribution (point sources) of 222Rn parent radionuclides, uranium and 226Ra, can strongly perturb the dissolved 222Rn concentrations in a fracture system. Without detailed information on the geometry and hydraulic properties of the connected fracture system, it may be impossible to distinguish the influence of factors controlling 222Rn distribution or to determine location of 222Rn point sources in the field in areas where ground water exhibits moderate 222Rn concentrations. Flow and transport simulations of a hypothetical multifracture system consisting of ten connected fractures, each 10 m in length with fracture apertures ranging from 0.1 to 1.0 mm, show that 222Rn concentrations at the pumping well can vary significantly over time. Assuming parallel-plate flow, transmissivities of the hypothetical system vary over four orders of magnitude because transmissivity varies with the cube of fracture aperture. The extreme hydraulic heterogeneity of the simple hypothetical system leads to widely ranging 222Rn values, even assuming homogeneous distribution of uranium and 226Ra along fracture walls. Consequently, it is concluded that 222Rn concentrations vary, not only with the geometric and stress factors noted above, but also according to local fracture aperture distribution, local groundwater residence time, and flux of 222Rn from parent radionuclides along fracture walls.

PROCESSING OF URANIUM-METAL-CONTAINING FUEL ELEMENTS

DOEpatents

Moore, R.H.

1962-10-01

A process is given for recovering uranium from neutronbombarded uranium- aluminum alloys. The alloy is dissolved in an aluminum halide--alkali metal halide mixture in which the halide is a mixture of chloride and bromide, the aluminum halide is present in about stoichiometric quantity as to uranium and fission products and the alkali metal halide in a predominant quantity; the uranium- and electropositive fission-products-containing salt phase is separated from the electronegative-containing metal phase; more aluminum halide is added to the salt phase to obtain equimolarity as to the alkali metal halide; adding an excess of aluminum metal whereby uranium metal is formed and alloyed with the excess aluminum; and separating the uranium-aluminum alloy from the fission- productscontaining salt phase. (AEC)

PYROCHEMICAL DECONTAMINATION METHOD FOR REACTOR FUEL

DOEpatents

Buyers, A.G.

1959-06-30

A pyro-chemical method is presented for decontaminating neutron irradiated uranium and separating plutonium therefrom by contact in the molten state with a metal chloride salt. Uranium trichloride and uranium tetrachloride either alone or in admixture with alkaline metal and alkaline eanth metal fluorides under specified temperature and specified phase ratio conditions extract substantially all of the uranium from the irradiated uranium fuel together with certain fission products. The phases are then separated leaving purified uranium metal. The uranium and plutonium in the salt phase can be reduced to forin a highly decontaminated uraniumplutonium alloy. The present method possesses advantages for economically decontaminating irradiated nuclear fuel elements since irradiated fuel may be proccessed immediately after withdrawal from the reactor and the uranium need not be dissolved and later reduced to the metallic form. Accordingly, the uranium may be economically refabricated and reinserted into the reactor.

Neutralisation of an acidic pit lake by alkaline waste products.

PubMed

Allard, Bert; Bäckström, Mattias; Karlsson, Stefan; Grawunder, Anja

2014-01-01

A former open pit where black shale (alum shale) was excavated during 1942-1965 has been water filled since 1966. The water chemistry was dominated by calcium and sulphate and had a pH of 3.2-3.4 until 1997-1998, when pH was gradually increasing. This was due to the intrusion of leachates from alkaline cement waste deposited close to the lake. A stable pH of around 7.5 was obtained after 6-7 years. The chemistry of the pit lake has changed due to the neutralisation. Concentrations of some dissolved metals, notably zinc and nickel, have gone down, as a result of adsorption/co-precipitation on solid phases (most likely iron and aluminium hydroxides), while other metals, notably uranium and molybdenum, are present at elevated levels. Uranium concentration is reaching a minimum of around pH 6.5 and is increasing at higher pH, which may indicate a formation of neutral and anionic uranyl carbonate species at high pH (and total carbonate levels around 1 mM). Weathering of the water-exposed shale is still in progress.

Trace Element Mobility in Water and Sediments in a Hyporheic Zone Adjacent to an Abandoned Uranium Mine

NASA Astrophysics Data System (ADS)

Roldan, C.; Blake, J.; Cerrato, J.; Ali, A.; Cabaniss, S.

2015-12-01

The legacy of abandoned uranium mines lead to community concerns about environmental and health effects. This study focuses on a cross section of the Rio Paguate, adjacent to the Jackpile Mine on the Laguna Reservation, west-central New Mexico. Often, the geochemical interactions that occur in the hyporheic zone adjacent to these abandoned mines play an important role in trace element mobility. In order to understand the mobility of uranium (U), arsenic (As), and vanadium (V) in the Rio Paguate; surface water, hyporheic zone water, and core sediment samples were analyzed using inductively coupled plasma mass spectroscopy (ICP-MS). All water samples were filtered through 0.45μm and 0.22μm filters and analyzed. The results show that there is no major difference in concentrations of U (378-496μg/L), As (0.872-6.78μg/L), and V (2.94-5.01μg/L) between the filter sizes or with depth (8cm and 15cm) in the hyporheic zone. The unfiltered hyporheic zone water samples were analyzed after acid digestion to assess the particulate fraction. These results show a decrease in U concentration (153-202μg/L) and an increase in As (33.2-219μg/L) and V (169-1130μg/L) concentrations compared to the filtered waters. Surface water concentrations of U(171-184μg/L) are lower than the filtered hyporheic zone waters while As(1.32-8.68μg/L) and V(1.75-2.38μg/L) are significantly lower than the hyporheic zone waters and particulates combined. Concentrations of As in the sediment core samples are higher in the first 15cm below the water-sediment interface (14.3-3.82μg/L) and decrease (0.382μg/L) with depth. Uranium concentrations are consistent (0.047-0.050μg/L) at all depths. The over all data suggest that U is mobile in the dissolved phase and both As and V are mobile in the particular phase as they travel through the system.

METHOD FOR DISSOLVING ZIRCONIUM-URANIUM COMPOSITIONS

DOEpatents

Gens, T.A.

1961-07-18

A method is descrioed for treating a zirconium-- uranium composition to form a stable solution from which uranium and other values may be extracted by contacting the composition with at least a 4 molar aqueous solution of ammonium fluoride at a temperature of about 100 deg C, adding a peroxide, in incremental amounts, to the heated solution throughout the period of dissolution until all of the uranium is converted to soluble uranyl salt, adding nitric acid to the resultant solution to form a solvent extraction feed solution to convert the uranyl salt to a solvent extractable state, and thereafter recovering the uranium and other desired values from the feed solution by solvent extraction.

Major ions, nutrients, and trace elements in the Mississippi River near Thebes, Illinois, July through September 1993

USGS Publications Warehouse

Taylor, Howard E.; Antweiler, Ronald C.; Brinton, Terry I.; Roth, David A.; Moody, John A.

1994-01-01

Extensive flooding in the upper Mississippi River Basin during summer 1993 had a significant effect on the water quality of the Mississippi River. To evaluate the change in temporal distribution and transport of dissolved constituents in the Mississippi River, six water samples were collected by a discharge-weighted method from July through September 1993 near Thebes, Illinois. Sampling at this location provided water-quality information from the upper Mississippi, the Missouri, and the Illinois River Basins. Dissolved major constituents that were analyzed in each of the samples included bicarbonate, calcium (Ca), carbonate (C03), chloride (Cl), dissolved organic carbon, magnesium (Mg), potassium (K), silica NOD, sodium (Na), and sulfate (S04). Dissolved nutrients included ammonium ion (NH4), nitrate (N03), nitrite (N02), and orthophosphate (P04) . Dissolved trace elements included aluminum (Al), arsenic (As), barium (Ba), boron (B), beryllium (Be), bromide (Br), cadmium (Cd), chromium (Cr), cobalt, (Co), copper (Cu), fluoride (F), iron (Fe), lead, lithium (Li), manganese (Mn), mercury (Hg), molybdenum (Mo), nickel (Ni), strontium (Sr), thallium, uranium (U), vanadium (V), and zinc (Zn). Other physical properties of water that were measured included specific conductance, pH and suspended-sediment concentration (particle size, less than 63 micrometers). Results of this study indicated that large quantities of dissolved constituents were transported through the river system. Generally, pH, alkalinity, and specific conductance and the concentrations of B, Br, Ca, Cl, Cr, K, Li, Mg, Mo, Na, S04, Sr, U, and V increased as water discharge decreased, while concentrations of F, Hg, and suspended sediment sharply decreased as water discharge decreased after the crest of the flood. Concentrations of other constituents, such as Al, As, Ba, Be, Co, Cu, Ni, N03, N02, NH4, P04, and Si02, varied with time as discharge decreased after the crest of the flood. For most constituents, the load transported during floods generally is much greater than that transported during low-flow conditions. How ever, for Cd, Cr, Fe, Mn, V, and Zn, loads increased substantially as water discharge decreased after the crest of the flood.

Radiochemical sampling and analysis of shallow ground water and sediment at the BOMARC Missile Facility, east-central New Jersey, 1999-2000

USGS Publications Warehouse

Szabo, Zoltan; Zapecza, Otto S.; Oden, Jeannette H.; Rice, Donald E.

2005-01-01

A field sampling experiment was designed using low-flow purging with a portable pump and sample-collection equipment for the collection of water and sediment samples from observation wells screened in the Kirkwood-Cohansey aquifer system to determine radionuclide or trace-element concentrations for various size fractions. Selected chemical and physical characteristics were determined for water samples from observation wells that had not been purged for years. The sampling was designed to define any particulate, colloidal, and solution-phase associations of radionuclides or trace elements in ground water by means of filtration and ultrafiltration techniques. Turbidity was monitored and allowed to stabilize before samples were collected by means of the low-flow purging technique rather than by the traditional method of purging a fixed volume of water at high-flow rates from the observation well. A minimum of four water samples was collected from each observation well. The samples of water from each well were collected in the following sequence. (1) A raw unfiltered sample was collected within the first minutes of pumping. (2) A raw unfiltered sample was collected after at least three casing volumes of water were removed and turbidity stabilized. (3) A sample was collected after the water was filtered with a 0.45-micron filter. (4) A sample was collected after the water passed through a 0.45-micron filter and a 0.003-micron tangential-flow ultrafilter in sequence. In some cases, a fifth sample was collected after the water passed through a 0.45-micron filter and a 0.05-micron filter in sequence to test for colloids of 0.003 microns to 0.05 microns in size. The samples were analyzed for the concentration of manmade radionuclides plutonium-238 and -239 plus -240, and americium-241. The samples also were analyzed for concentrations of uranium-234, -235, and -238 to determine whether uranium-234 isotope enrichment (resulting from industrial processing) is present. A subset of samples was analyzed for concentrations of thorium-232, -230, and -228 to determine if thorium-228 isotope enrichment, also likely to result from industrial processing, is present. Concentrations of plutonium isotopes and americium-241 in the water samples were less than 0.1 picocurie per liter, the laboratory reporting level for these manmade radionuclides, with the exception of one americium-241 concentration from a filtered sample. A sequential split sample from the same well did not contain a detectable concentration of americium-241, however. Other filtered and unfiltered samples of water from the same well did not contain quantities of americium-241 nearly as high as 0.1 pCi/L. Therefore, the presence of americium-241 in a quantifiable concentration in water samples from this well could not be confirmed. Neither plutonium nor americium was detected in samples of settled sediment collected from the bottom of the wells. Concentrations of uranium isotopes (maximum of 0.05 and 0.08 picocuries per liter of uranium-238 and uranium-234, respectively) were measurable in unfiltered samples of turbid water from one well and in the settled bottom sediment from 6 wells (maximum concentrations of 0.25 and 0.20 picocuries per gram of uranium-238 and uranium-234, respectively). The uranium-234/uranium-238 isotopic ratio was near 1:1, which indicates natural uranium. The analytical results, therefore, indicate that no manmade radionuclide contamination is present in any of the well-bottom sediments, or unfiltered or filtered water samples from any of the sampled wells. No evidence of manmade radionuclide contamination was observed in the aquifer as settled or suspended particulates, colloids, or in the dissolved phase.

Sampling and analysis for radon-222 dissolved in ground water and surface water

USGS Publications Warehouse

DeWayne, Cecil L.; Gesell, T.F.

1992-01-01

Radon-222 is a naturally occurring radioactive gas in the uranium-238 decay series that has traditionally been called, simply, radon. The lung cancer risks associated with the inhalation of radon decay products have been well documented by epidemiological studies on populations of uranium miners. The realization that radon is a public health hazard has raised the need for sampling and analytical guidelines for field personnel. Several sampling and analytical methods are being used to document radon concentrations in ground water and surface water worldwide but no convenient, single set of guidelines is available. Three different sampling and analytical methods - bubbler, liquid scintillation, and field screening - are discussed in this paper. The bubbler and liquid scintillation methods have high accuracy and precision, and small analytical method detection limits of 0.2 and 10 pCi/l (picocuries per liter), respectively. The field screening method generally is used as a qualitative reconnaissance tool.

Modeling non-steady state radioisotope transport in the vadose zone--A case study using uranium isotopes at Pena Blanca, Mexico

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

Ku, T. L.; Luo, S.; Goldstein, S. J.

2009-06-01

Current models using U- and Th-series disequilibria to study radioisotope transport in groundwater systems mostly consider a steady-state situation. These models have limited applicability to the vadose zone (UZ) where the concentration and migratory behavior of radioisotopes in fluid are often transitory. We present here, as a first attempt of its kind, a model simulating the non-steady state, intermittent fluid transport in vadose layers. It provides quantitative constraints on in-situ migration of dissolved and colloidal radioisotopes in terms of retardation factor and rock-water interaction (or water transit) time. For uranium, the simulation predicts that intermittent flushing in the UZ leadsmore » to a linear relationship between reciprocal U concentration and {sup 234}U/{sup 238}U ratio in percolating waters, with the intercept and slope bearing information on the rates of dissolution and {alpha}-recoil of U isotopes, respectively. The general validity of the model appears to be borne out by the measurement of uranium isotopes in UZ waters collected at various times over a period during 1995-2006 from a site in the Pena Blanca mining district, Mexico, where the Nopal I uranium deposit is located. Enhanced {sup 234}U/{sup 238}U ratios in vadose-zone waters resulting from lengthened non-flushing time as prescribed by the model provide an interpretative basis for using {sup 234}U/{sup 238}U in cave calcites to reconstruct the regional changes in hydrology and climate. We also provide a theoretical account of the model's potential applications using radium isotopes.« less

Modeling non-steady state radioisotope transport in the vadose zone - A case study using uranium isotopes at Peña Blanca, Mexico

NASA Astrophysics Data System (ADS)

Ku, T. L.; Luo, S.; Goldstein, S. J.; Murrell, M. T.; Chu, W. L.; Dobson, P. F.

2009-10-01

Current models using U- and Th-series disequilibria to study radioisotope transport in groundwater systems mostly consider a steady-state situation. These models have limited applicability to the vadose zone (UZ) where the concentration and migratory behavior of radioisotopes in fluid are often transitory. We present here, as a first attempt of its kind, a model simulating the non-steady state, intermittent fluid transport in vadose layers. It provides quantitative constraints on in-situ migration of dissolved and colloidal radioisotopes in terms of retardation factor and rock-water interaction (or water transit) time. For uranium, the simulation predicts that intermittent flushing in the UZ leads to a linear relationship between reciprocal U concentration and 234U/ 238U ratio in percolating waters, with the intercept and slope bearing information on the rates of dissolution and α-recoil of U isotopes, respectively. The general validity of the model appears to be borne out by the measurement of uranium isotopes in UZ waters collected at various times over a period during 1995-2006 from a site in the Peña Blanca mining district, Mexico, where the Nopal I uranium deposit is located. Enhanced 234U/ 238U ratios in vadose-zone waters resulting from lengthened non-flushing time as prescribed by the model provide an interpretative basis for using 234U/ 238U in cave calcites to reconstruct the regional changes in hydrology and climate. We also provide a theoretical account of the model's potential applications using radium isotopes.

Distribution of uranium and thorium in groundwater of arid climate region

NASA Astrophysics Data System (ADS)

Murad, Ahmed; Alshamsi, Dalal; Aldahan, Ala; Hou, Xiaolin

2014-05-01

Uranium, thorium and their decay products are the most common radionuclides in groundwater in addition to potassium-40. Once groundwater is used for drinking, domestic and irrigation purposes, the radionuclides will then pose environmental and health related hazard originating from radioactivity and toxicity. In the investigation presented here, assessment of 238U, 235U and 232Th concentrations in groundwater across of the United Arab Emirates (UAE) is evaluated in terms of quality and sources. The region is dominated by arid climate conditions and radioactivity assessment of groundwater is essential for safe use of groundwater. Furthermore, the results were linked to data from other arid regions and worldwide. Groundwater samples (total dissolved solids,TDS, 142.5 mg L-1 to 12770 mg L-1) from 67 different wells were collected across geomorphologically different areas and most of the wells are actively used for agriculture. The aquifers are recent sand dunes, Quaternary (3 million years to present) sediments, and older carbonate rocks (230-10 million years). The 235U, 238U and 232Th measurements were carried out using ICP-MS system equipped with an Xt-skimmer cone and a concentric nebulizer under hot plasma conditions. Concentrations of 235U, 238U and 232Th range at (0.125-508.4) ng L-1, (25.81-69237) ng L-1 and (0.236-2529) ng L-1, respectively. Apparently, most 235U, 238U, 232Th concentrations in the sampled groundwater are below the WHO proposed permissible level of 60000 ng/L for total uranium (1 Bq L-1 for 235U and 10 Bq L-1 for 238U) and 5000 ng L-1 (1Bq L-1) for 232Th. A few samples show high concentrations of uranium that are associated with high TDS values and occur within interbedded limestones and shales aquifer. Comparison with worldwide groundwater data suggests that 238U concentration is highest in the arid regions groundwater where the recharge to aquifers is relatively low. The situation for 232Th concentrations seems less affected by climatic conditions, most likely is related to its less solubility in water compared to uranium. We calculated the accumulated TU and 232Th concentration in the irrigation water annually to estimate the cumulative concentrations after twenty years on specific agricultural areas. The TU and 232Th are expected not to reach more than 1.14 x 10-3 g (1.14 mg) and 4.32 x 10-6 g (4.32 μg) respectively after twenty years if the daily irrigation is at its maximum amount (10 m3). Despite these obtained values of concentrations in irrigation water, the transfer of uranium and thorium into crop is not readily and it is expected that only a tiny fraction of the element end into the body. However, further research is needed to quantify the dietary exposures in the UAE with detailed data from crops and consumers.

THE GRAVIMETRIC DETERMINATION OF MOLYBDENUM IN URANIUM-MOLYBDENUM ALLOYS

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

None

1959-03-01

The sample is dissolved in nitric and hydrochloric acids. After heating the solution with sulfuric acid, molybodenum is precipitated as the benzoin-oxime complex which is ignited to molybdic oxide. This is dissolved in ammonia, and the molybdenum is precipitated and weighed as lead molybdate. (auth)

Quantitative determination of environmental levels of uranium, thorium and plutonium in bone by solvent extraction and alpha spectrometry

NASA Astrophysics Data System (ADS)

Singh, Narayani P.; Zimmerman, Carol J.; Lewis, Laura L.; Wrenn, McDonald E.

1984-06-01

Solvent extraction and alpha-spectrometry have been emplyed in the quantitative simultaneous determination of uranium. thorium and plutonium. The bone specimens, spiked with 232U, 229Th and 242Pu tracers, are wet ashed with HNO 3 followed by alternate additions of a new drops of HNO 3 and H 2O 2. Uranium is reduced to the tetravalent state with 200 mg SnCl 2 and 25 ml HI. Uranium, thorium and plutonium are then coprecipitated with calcium as oxalate, heated to 550°C, dissolved in 50 ml HCl, and the acidity adjusted to 10 M. Uranium and plutonium are extracted into a 20% tri-lauryl amine (TLA) solution in xylene, leaving thorium in the aqueous phase. Plutonium is first back-extracted from the TLA phase by shaking with a 1:1.5 volume of 0.05 M NH 4I in 8 M HCl, which reduces Pu(IV) to Pu(III). Uranium is then back-extracted with an equal volume of 0.1 M HCl. Thorium, which was left in the aqueous phase, is evaporated to dryness, dissolved in 4 M HNO 3, and the acidity adjusted to 4 M. Thorium is then extracted into 20% TLA solution in xylene pre-equilibrated with 4 M HNO 3, and back-extracted with 10 M HCl. Uranium, thorium, and plutonium are then electrodeposited separately onto platinum discs and counted by an alpha-spectrometer with a multi-channel analyzer and surface barrier silicon diodes. The mean recoveries of uranium, thorium, and plutonium in bovine, dog, and human bones were over 70%.

Surface complexation modeling of U(VI) adsorption by aquifer sediments from a former mill tailings site at Rifle, Colorado

USGS Publications Warehouse

Hyun, S.P.; Fox, P.M.; Davis, J.A.; Campbell, K.M.; Hayes, K.F.; Long, P.E.

2009-01-01

A study of U(VI) adsorption by aquifer sediment samples from a former uranium mill tailings site at Rifle, Colorado, was conducted under oxic conditions as a function of pH, U(VI), Ca, and dissolved carbonate concentration. Batch adsorption experiments were performed using <2mm size sediment fractions, a sand-sized fraction, and artificial groundwater solutions prepared to simulate the field groundwater composition. To encompass the geochemical conditions of the alluvial aquifer at the site, the experimental conditions ranged from 6.8 ?? 10-8 to 10-5 M in [U(VI)]tot, 7.2 to 8.0 in pH, 3.0 ?? 10-3 to 6.0 ?? 10 -3 M in [Ca2+], and 0.05 to 2.6% in partial pressure of carbon dioxide. Surface area normalized U(VI) adsorption Kd values for the sand and <2 mm sediment fraction were similar, suggesting a similar reactive surface coating on both fractions. A two-site two-reaction, nonelectrostatic generalized composite surface complexation model was developed and successfully simulated the U(VI) adsorption data. The model successfully predicted U(VI) adsorption observed from a multilevel sampling well installed at the site. A comparison of the model with the one developed previously for a uranium mill tailings site at Naturita, Colorado, indicated that possible calcite nonequilibrium of dissolved calcium concentration should be evaluated. The modeling results also illustrate the importance of the range of data used in deriving the best fit model parameters. ?? 2009 American Chemical Society.

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.

Dissolution process for ZrO.sub.2 -UO.sub.2 -CaO fuels

DOEpatents

Paige, Bernice E.

1976-06-22

The present invention provides an improved dissolution process for ZrO.sub.2 -UO.sub.2 -CaO-type pressurized water reactor fuels. The zirconium cladding is dissolved with hydrofluoric acid, immersing the ZrO.sub.2 -UO.sub.2 -CaO fuel wafers in the resulting zirconium-dissolver-product in the dissolver vessel, and nitric acid is added to the dissolver vessel to facilitate dissolution of the uranium from the ZrO.sub.2 -UO.sub.2 -CaO fuel wafers.

Occurrence and hydrogeochemistry of radiochemical constituents in groundwater of Jefferson County and surrounding areas, southwestern Montana, 2007 through 2010

USGS Publications Warehouse

Caldwell, Rodney R.; Nimick, David A.; DeVaney, Rainie M.

2014-01-01

The U.S. Geological Survey, in cooperation with Jefferson County and the Jefferson Valley Conservation District, sampled groundwater in southwestern Montana to evaluate the occurrence and concentration of naturally-occurring radioactive constituents and to identify geologic settings and environmental conditions in which elevated concentrations occur. A total of 168 samples were collected from 128 wells within Broadwater, Deer Lodge, Jefferson, Lewis and Clark, Madison, Powell, and Silver Bow Counties from 2007 through 2010. Most wells were used for domestic purposes and were primary sources of drinking water for individual households. Water-quality samples were collected from wells completed within six generalized geologic units, and analyzed for constituents including uranium, radon, gross alpha-particle activity, and gross beta-particle activity. Thirty-eight wells with elevated concentrations or activities were sampled a second time to examine variability in water quality throughout time. These water-quality samples were analyzed for an expanded list of radioactive constituents including the following: three isotopes of uranium (uranium-234, uranium-235, and uranium-238), three isotopes of radium (radium-224, radium-226, and radium-228), and polonium-210. Existing U.S. Geological Survey and Montana Bureau of Mines and Geology uranium and radon water-quality data collected as part of other investigations through 2011 from wells within the study area were compiled as part of this investigation. Water-quality data from this study were compared to data collected nationwide by the U.S. Geological Survey through 2011. Radionuclide samples for this study typically were analyzed within a few days after collection, and therefore data for this study may closely represent the concentrations and activities of water being consumed locally from domestic wells. Radioactive constituents were detected in water from every well sampled during this study regardless of location or geologic unit. Nearly 41 percent of sampled wells had at least one radioactive constituent concentration that exceeded U.S. Environmental Protection Agency drinking-water standards or screening levels. Uranium concentrations were higher than the U.S. Environmental Protection Agency maximum contaminant level (MCL) of 30 micrograms per liter in samples from 14 percent of the wells. Radon concentrations exceeded a proposed MCL of 4,000 picocuries per liter in 27 percent of the wells. Combined radium (radium-226 and radium-228) exceeded the MCL of 5 picocuries per liter in samples from 10 of 47 wells. About 40 percent (42 of 104 wells) of the wells had gross alpha-particle activities (72-hour count) at or greater than a screening level of 15 pCi/L. Gross beta-particle activity exceeded the U.S. Environmental Protection Agency 50 picocuries per liter screening level in samples from 5 of 104 wells. Maximum radium-224 and polonium-210 activities in study wells were 16.1 and 3.08 picocuries per liter, respectively; these isotopes are constituents of human-health concern, but the U.S. Environmental Protection Agency has not established MCLs for them. Radioactive constituent concentrations or activities exceeded at least one established drinking-water standard, proposed drinking-water standard, or screening level in groundwater samples from five of six generalized geologic units assessed during this study. Radioactive constituent concentrations or activities were variable not only within each geologic unit, but also among wells that were completed in the same geologic unit and in close proximity to one another. Established or proposed drinking-water standards were exceeded most frequently in water from wells completed in the generalized geologic unit that includes rocks of the Boulder batholith and other Tertiary through Cretaceous igneous intrusive rocks (commonly described as granite). Specifically, of the wells completed in the Boulder batholith and related rocks sampled as part of this study, 24 percent exceeded the MCL of 30 micrograms per liter for uranium, 50 percent exceeded the proposed alternative MCL of 4,000 picocuries per liter for radon, and 27 percent exceeded the MCL of 5 micrograms per liter for combined radium-226 and radium-228. Elevated radioactive constituent values were detected in samples representing a large range of field properties and water types. Correlations between radioactive constituents and pH, dissolved oxygen, and most major ions were not statistically significant (p-value > 0.05) or were weakly correlated with Spearman correlation coefficients (rho) ranging from -0.5 to 0.5. Moderate correlations did exist between gross beta-particle activity and potassium (rho = 0.72 to 0.82), likely because one potassium isotope (potassium-40) is a beta-particle emitter. Total dissolved solids and specific conductance also were moderately correlated (rho = 0.62 to 0.71) with gross alpha-particle and gross beta-particle activity, indicating that higher radioactivity values can be associated with higher total dissolved solids. Correlations were evaluated among radioactive constituents. Moderate to strong correlations occurred between gross alpha-particle and beta-particle activities (rho = 0.77 to 0.96) and radium isotopes (rho = 0.78 to 0.92). Correlations between gross alpha-particle activity (72-hour count) and all analyzed radioactive constituents were statistically significant (p-value Radiochemical results varied temporally in samples from several of the thirty-eight wells sampled at least twice during the study. The time between successive sampling events ranged from about 1 to 10 months for 29 wells to about 3 years for the other 9 wells. Radiochemical constituents that varied by greater than 30 percent between sampling events included uranium (29 percent of the resampled wells), and radon (11 percent of the resampled wells), gross alpha-particle activity (38 percent of the resampled wells), and gross beta-particle activity (15 percent of the resampled wells). Variability in uranium concentrations from two wells was sufficiently large that concentrations were less than the MCL in the first set of samples and greater than the MCL in the second. Sample holding times affect analytical results in this study. Gross alpha-particle and gross beta-particle activities were measured twice, 72 hours and 30 days after sample collection. Gross alpha-particle activity decreased an average of 37 percent between measurements, indicating the presence of short-lived alpha-emitting radionuclides in these samples. Gross beta-particle activity increased an average of 31 percent between measurements, indicating ingrowth of longer-lived beta-emitting radionuclides.

Experiences with new neutralization technologies for remediation after ISL mining of uranium in Straz Pod Ralskem

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

Sedlakova, Veronika; Kaspar, Ludvik; Tykal, Tomas

2013-07-01

A big affection of the rock environment and groundwaters occurred during the chemical mining of uranium in the years 1966 to 1996 in the neighbourhood of the town Straz pod Ralskem in the Czech Republic. It is necessary to clean the residual technological solutions (RTS) from the underground. The pH of the solutions in some places is still less than 2 and the concentration of sulphates reaches up to 65 g/l. The remedial activities consist of pumping of the RTS from the ground and reprocessing of the RTS in the surface technologies. The implementation of the new neutralization technologies NDSmore » ML and NDS 10 help us with increasing of the efficiency of the remedial process. The NDS ML technology ('Mother liquor reprocessing station') started its operation in 2009 and it processes the concentrated technological solution from the evaporation station after the alum crystallization (mother liquor) with the concentration of total dissolved solids up to 250 g/l. The principle is the neutralization of the acid solutions with the aid of the lime milk. The suspension is then filtrated in the filter press, the filter cake is deposited in the tailings pond and the filtrate is injected back into the underground rock environment. The NDS 10 technology ('Neutralization and Decontamination Station NDS 10') started its operation in 2012 and it works on the same technological principle as the NDS ML station. The difference is that the NDS 10 station can process higher volume (4.4 m{sup 3}/min) of the RTS with lower concentration of total dissolved solids 20 - 25 g/l. This poster describes the experiences of the state enterprise DIAMO with putting of these two neutralization technologies into operation and with using of the lime milk neutralization in such a large scale. (authors)« less

Method for processing aqueous wastes

DOEpatents

Pickett, J.B.; Martin, H.L.; Langton, C.A.; Harley, W.W.

1993-12-28

A method is presented for treating waste water such as that from an industrial processing facility comprising the separation of the waste water into a dilute waste stream and a concentrated waste stream. The concentrated waste stream is treated chemically to enhance precipitation and then allowed to separate into a sludge and a supernate. The supernate is skimmed or filtered from the sludge and blended with the dilute waste stream to form a second dilute waste stream. The sludge remaining is mixed with cementitious material, rinsed to dissolve soluble components, then pressed to remove excess water and dissolved solids before being allowed to cure. The dilute waste stream is also chemically treated to decompose carbonate complexes and metal ions and then mixed with cationic polymer to cause the precipitated solids to flocculate. Filtration of the flocculant removes sufficient solids to allow the waste water to be discharged to the surface of a stream. The filtered material is added to the sludge of the concentrated waste stream. The method is also applicable to the treatment and removal of soluble uranium from aqueous streams, such that the treated stream may be used as a potable water supply. 4 figures.

METAL EXTRACTION PROCESS

DOEpatents

Lewis, G.W. Jr.; Rhodes, D.E.

1957-11-01

An improved method for extracting uranium from aqueous solutions by solvent extraction is presented. A difficulty encountered in solvent extraction operations using an organic extractant (e.g., tributyl phosphate dissolved in kerosene or carbon tetrachloride) is that emulsions sometimes form, and phase separation is difficult or impossible. This difficulty is overcome by dissolving the organic extractant in a molten wax which is a solid at operating temperatures. After cooling, the wax which now contains the extractant, is broken into small particles (preferably flakes) and this wax complex'' is used to contact the uranium bearing solutions and extract the metal therefrom. Microcrystalline petroleum wax and certain ethylene polymers have been found suitable for this purpose.

PROCESS FOR THE RECOVERY OF URANIUM FROM PHOSPHATIC ORE

DOEpatents

Long, R.L.

1959-04-14

A proccss is described for the recovery of uranium from phosphatic products derived from phosphatic ores. It has been discovered that certain alkyl phosphatic, derivatives can be employed in a direct solvent extraction operation to recover uranium from solid products, such as superphosphates, without first dissolving such solids. The organic extractants found suitable include alkyl derivatives of phosphoric, pyrophosphoric, phosof the derivative contains from 4 to 7 carbon atoms. A diluent such as kerosene is also used.

Uranium dioxide electrolysis

DOEpatents

Willit, James L [Batavia, IL; Ackerman, John P [Prescott, AZ; Williamson, Mark A [Naperville, IL

2009-12-29

This is a single stage process for treating spent nuclear fuel from light water reactors. The spent nuclear fuel, uranium oxide, UO.sub.2, is added to a solution of UCl.sub.4 dissolved in molten LiCl. A carbon anode and a metallic cathode is positioned in the molten salt bath. A power source is connected to the electrodes and a voltage greater than or equal to 1.3 volts is applied to the bath. At the anode, the carbon is oxidized to form carbon dioxide and uranium chloride. At the cathode, uranium is electroplated. The uranium chloride at the cathode reacts with more uranium oxide to continue the reaction. The process may also be used with other transuranic oxides and rare earth metal oxides.

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.

ANALYTICAL METHOD FOR THE ABSORPTIOMETRIC DETERMINATION OF BORON IN URANIUM METAL POWDER

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

None

1963-01-01

The U powder is dissolved in HCl and H/sub 2/O/sub 2/. The resulting solution is evaporated to dryness in the presence of H/sub 2/SO/sub 3/. Rosocyanin is formed, separated from the excess curcumin, and dissolved in ethanol for absorptiometric measurement. (auth)

Dry phase reactor for generating medical isotopes

DOEpatents

Mackie, Thomas Rockwell; Heltemes, Thad Alexander

2016-05-03

An apparatus for generating medical isotopes provides for the irradiation of dry-phase, granular uranium compounds which are then dissolved in a solvent for separation of the medical isotope from the irradiated compound. Once the medical isotope is removed, the dissolved compound may be reconstituted in dry granular form for repeated irradiation.

FUSED SALT PROCESS FOR RECOVERY OF VALUES FROM USED NUCLEAR REACTOR FUELS

DOEpatents

Moore, R.H.

1960-08-01

A process is given for recovering plutonium from a neutron-irradiated uranium mass (oxide or alloy) by dissolving the mass in an about equimolar alkali metalaluminum double chloride, adding aluminum metal to the mixture obtained at a temperature of between 260 and 860 deg C, and separating a uranium-containing metal phase and a plutonium-chloride- and fission-product chloridecontaining salt phase. Dissolution can be expedited by passing carbon tetrachloride vapors through the double salt. Separation without reduction of plutonium from neutron- bombarded uranium and that of cerium from uranium are also discussed.

THORIUM OXALATE-URANYL ACETATE COUPLED PROCEDURE FOR THE SEPARATION OF RADIOACTIVE MATERIALS

DOEpatents

Gofman, J.W.

1959-08-11

The recovery of fission products from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in acid and thorium oxalate is precipitated in ihe solution formed, whereby the fission products are carried on the thorium oxalate. The separated thorium oxalate precipitate is then dissolved in an aqueous oxalate solution and the solution formed is acidified, limiting ihe excess acidity to a maximum of 2 N, whereby thorium oxalate precipitates and carries lanthanum-rareearth- and alkaline-earth-metal fission products while the zirconium-fission-product remains in solution. This precipitate, too, is dissolved in an aqaeous oxalate solution at elevated temperature, and lanthanum-rare-earth ions are added to the solution whereby lanthanum-rare-earth oxalate forms and the lanthanum-rare-earth-type and alkalineearth-metal-type fission products are carried on the oxalate. The precipitate is separated from the solution.

Solubility classification of airborne uranium products collected at the perimeter of the Allied Chemical Plant, Metropolis, Illinois

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

Kalkwarf, D.R.

1980-05-01

Airborne uranium products were collected at the perimeter of the uranium-conversion plant operated by the Allied Chemical Corporation at Metropolis, Illinois, and the dissolution rates of these products were classified in terms of the ICRP Task Group Lung Model. Assignments were based on measurements of the dissolution half-times exhibited by uranium components of the dust samples as they dissolved in simulated lung fluid at 37/sup 0/C. Based on three trials, the dissolution behavior of dust with aerodynamic equivalent diameter (AED) less than 5.5 ..mu..m and collected nearest the closest residence to the plant was classified 0.40 D, 0.60 Y. Basedmore » on two trials, the dissolution behavior of dust with AED greater than 5.5 ..mu..m and collected at this location was classified 0.37 D, 0.63 Y. Based on one trial, the dissolution behavior of dust with AED less than 5.5 ..mu..m and collected at a location on the opposite side of the plant was classified 0.68 D, 0.32 Y. There was some evidence for adsorption of dissolved uranium onto other dust components during dissolution, and preliminary dissolution trials are recommended for future samples in order to optimize the fluid replacement schedule.« less

Uranium hydrogeochemical and stream sediment reconnaissance of the Newcastle NTMS Quadrangle, Wyoming, including concentrations of forty-two additional elements

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

Goff, S.J.; Sandoval, W.F.; Gallimore, D.L.

1980-06-01

Water and sediment samples were collected and each water sample was analyzed for U, and each sediment sample was analyzed for 43 elements, including U and Th. Uranium concentrations in water samples range from below the detection limit of 0.02 ppB to 702.26 ppB and have a median of 1.73 ppB and a mean of 11.76 ppB. Water samples containing high uranium concentrations generally are associated with known uranium mining activity or units known to be uranium bearing. About one-third of the water samples containing high uranium concentrations were collected from locations within the Pumpkin Buttes and Turnercrest-Ross Districts. Nearlymore » half of the water samples containing high uranium concentrations were collected from locations just west of the Monument Hill and Highland Flats-Box Creek Districts. Similar anomalous uranium concentrations in this region have been reported updip from Exxon's Highland uranium deposits. High uranium concentrations were also found associated with the Lance Creek-Old Woman Anticline District. Uranium concentrations in sediment samples range from 1.14 to 220.70 ppM and have a median of 3.37 ppM and a mean of 4.03 ppM. Throughout the major uranium mining districts of the Powder River Basin, sediment samples with high uranium concentrations were collected from dry streams located near wells producing water samples with high uranium concentrations. High uranium concentrations were also found associated with the Lance Creek oil field where uranium mineralization is known in the White River formation. High uranium concentrations were also found in sediment samples in areas where uranium mineralization is not known. These samples are from dry streams in areas underlain by the White River formation, the Niobrara formation, and the Pierre, Carlisle, Belle Fourche, and Mowry shales.« less

Diffusive gradient in thin FILMS (DGT) compared with soil solution and labile uranium fraction for predicting uranium bioavailability to ryegrass.

PubMed

Duquène, L; Vandenhove, H; Tack, F; Van Hees, M; Wannijn, J

2010-02-01

The usefulness of uranium concentration in soil solution or recovered by selective extraction as unequivocal bioavailability indices for uranium uptake by plants is still unclear. The aim of the present study was to test if the uranium concentration measured by the diffusive gradient in thin films (DGT) technique is a relevant substitute for plant uranium availability in comparison to uranium concentration in the soil solution or uranium recovered by ammonium acetate. Ryegrass (Lolium perenne L. var. Melvina) is grown in greenhouse on a range of uranium spiked soils. The DGT-recovered uranium concentration (C(DGT)) was correlated with uranium concentration in the soil solution or with uranium recovered by ammonium acetate extraction. Plant uptake was better predicted by the summed soil solution concentrations of UO(2)(2+), uranyl carbonate complexes and UO(2)PO(4)(-). The DGT technique did not provide significant advantages over conventional methods to predict uranium uptake by plants. Copyright 2009 Elsevier Ltd. All rights reserved.

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, John P.

1992-01-01

A process for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.

RECOVERY OF URANIUM FROM TUNGSTEN

DOEpatents

Newnam, K.

1959-02-01

A method is presented for the rccovery of uranium which has adhered to tungsten parts in electromagnetic isotope separation apparatus. Such a tungsten article is dissolved electrolytically in 20% NaOH by using the tungsten article as the anode. The resulting solution, containing soluble sodium lungstate and an insoluble slime, is then filtered. The slime residue is ignited successively with sodium nitrate and sodium pyrosulfate and leashed, and the resulting filtrates are combined with the original filtrate. Uranium is then recovered from the combined flltrates by diuranate precipitation.

River stage influences on uranium transport in a hydrologically dynamic groundwater-surface water transition zone

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

Zachara, John M.; Chen, Xingyuan; Murray, Chris

In this study, a well-field within a uranium (U) plume in the groundwater-surface water transition zone was monitored for a 3 year period for water table elevation and dissolved solutes. The plume discharges to the Columbia River, which displays a dramatic spring stage surge resulting from 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 (U aq), specific conductance (SpC), and other solutes, and to discriminate between transport, geochemical, and source term heterogeneity effects. Time seriesmore » trends for U aq and SpC were complex and displayed large temporal and 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 behaviors resulting from the intrusion dynamics of river water and the location of source terms. Hot-spots in U aq varied in location with increasing water table elevation through the combined effects of advection and source term location. Heuristic reactive transport modeling with PFLOTRAN demonstrated that mobilized U aq was transported between wells and source terms in complex trajectories, and was diluted as river water entered and exited the groundwater system. While U aq 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 river water intrusion.« less

River stage influences on uranium transport in a hydrologically dynamic groundwater-surface water transition zone

DOE PAGES

Zachara, John M.; Chen, Xingyuan; Murray, Chris; ...

2016-03-04

In this study, a well-field within a uranium (U) plume in the groundwater-surface water transition zone was monitored for a 3 year period for water table elevation and dissolved solutes. The plume discharges to the Columbia River, which displays a dramatic spring stage surge resulting from 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 (U aq), specific conductance (SpC), and other solutes, and to discriminate between transport, geochemical, and source term heterogeneity effects. Time seriesmore » trends for U aq and SpC were complex and displayed large temporal and 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 behaviors resulting from the intrusion dynamics of river water and the location of source terms. Hot-spots in U aq varied in location with increasing water table elevation through the combined effects of advection and source term location. Heuristic reactive transport modeling with PFLOTRAN demonstrated that mobilized U aq was transported between wells and source terms in complex trajectories, and was diluted as river water entered and exited the groundwater system. While U aq 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 river water intrusion.« less

Use of TEVA resin for the determination of U isotopes in water samples by Q-ICP-MS.

PubMed

Tagami, K; Uchida, S

2004-01-01

In order to measure uranium isotopic mass ratio in natural water samples by Q-ICP-MS, an application of TEVA resin (Eichrom) was studied to separate and concentrate U. After being evaporated to dryness, the sample residue was dissolved in 6 M HCl, then, TEVA extraction was carried out. U extracted on the resin could be removed with 20 ml of 1 M HCl (U fraction) when Fe content was lower than 2 mg. U recovery in U fraction showed a negative correlation with Fe content in the samples.

Cellular localization of uranium in the renal proximal tubules during acute renal uranium toxicity.

PubMed

Homma-Takeda, Shino; Kitahara, Keisuke; Suzuki, Kyoko; Blyth, Benjamin J; Suya, Noriyoshi; Konishi, Teruaki; Terada, Yasuko; Shimada, Yoshiya

2015-12-01

Renal toxicity is a hallmark of uranium exposure, with uranium accumulating specifically in the S3 segment of the proximal tubules causing tubular damage. As the distribution, concentration and dynamics of accumulated uranium at the cellular level is not well understood, here, we report on high-resolution quantitative in situ measurements by high-energy synchrotron radiation X-ray fluorescence analysis in renal sections from a rat model of uranium-induced acute renal toxicity. One day after subcutaneous administration of uranium acetate to male Wistar rats at a dose of 0.5 mg uranium kg(-1) body weight, uranium concentration in the S3 segment of the proximal tubules was 64.9 ± 18.2 µg g(-1) , sevenfold higher than the mean renal uranium concentration (9.7 ± 2.4 µg g(-1) ). Uranium distributed into the epithelium of the S3 segment of the proximal tubules and highly concentrated uranium (50-fold above mean renal concentration) in micro-regions was found near the nuclei. These uranium levels were maintained up to 8 days post-administration, despite more rapid reductions in mean renal concentration. Two weeks after uranium administration, damaged areas were filled with regenerating tubules and morphological signs of tissue recovery, but areas of high uranium concentration (100-fold above mean renal concentration) were still found in the epithelium of regenerating tubules. These data indicate that site-specific accumulation of uranium in micro-regions of the S3 segment of the proximal tubules and retention of uranium in concentrated areas during recovery are characteristics of uranium behavior in the kidney. Copyright © 2015 John Wiley & Sons, Ltd.

PROCESS FOR THE RECOVERY AND PURIFICATION OF URANIUM DEPOSITS

DOEpatents

Carter, J.M.; Kamen, M.D.

1958-10-14

A process is presented for recovering uranium values from UCl/sub 4/ deposits formed on calutrons. Such deposits are removed from the calutron parts by an aqueous wash solution which then contains the uranium values in addition to the following impurities: Ni, Cu, Fe, and Cr. This impurity bearing wash solution is treated with an oxidizing agent, and the oxidized solution is then treated with ammonia in order to precipitate the uranium as ammonium diuranate. The metal impurities of iron and chromium, which form insoluble hydroxides, are precipitated along with the uranium values. The precipitate is separated from the solution, dissolved in acid, and the solution again treated with ammonia and ammonium carbonate, which results in the precipitation of the metal impurities as hydroxides while the uranium values remain in solution.

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.

Mechanisms controlling lateral and vertical porewater migration of depleted uranium (DU) at two UK weapons testing sites.

PubMed

Graham, Margaret C; Oliver, Ian W; MacKenzie, Angus B; Ellam, Robert M; Farmer, John G

2011-04-15

Uranium associations with colloidal and truly dissolved soil porewater components from two Ministry of Defence Firing Ranges in the UK were investigated. Porewater samples from 2-cm depth intervals for three soil cores from each of the Dundrennan and Eskmeals ranges were fractionated using centrifugal ultrafiltration (UF) and gel electrophoresis (GE). Soil porewaters from a transect running downslope from the Dundrennan firing area towards a stream (Dunrod Burn) were examined similarly. Uranium concentrations and isotopic composition were determined using Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) and Multi-Collector-Inductively Coupled Plasma-Mass Spectrometry (MC-ICP-MS), respectively. The soils at Dundrennan were Fe- and Al-rich clay-loam soils whilst at Eskmeals, they were Fe- and Al-poor sandy soils; both, however, had similar organic matter contents due to the presence of a near-surface peaty layer at Eskmeals. These compositional features influenced the porewater composition and indeed the associations of U (and DU). In general, at Dundrennan, U was split between large (100kDa-0.2μm) and small (3-30kDa) organic colloids whilst at Eskmeals, U was mainly in the small colloidal and truly dissolved fractions. Especially below 10cm depth, association with large Fe/Al/organic colloids was considered to be a precursor to the removal of U from the Dundrennan porewaters to the solid phase. In contrast, the association of U with small organic colloids was largely responsible for inhibiting attenuation in the Eskmeals soils. Lateral migration of U (and DU) through near-surface Dundrennan soils will involve both large and small colloids but, at depth, transport of the smaller amounts of U remaining in the porewaters may involve large colloids only. For one of the Dundrennan cores the importance of redox-related processes for the re-mobilisation of DU was also indicated as Mn(IV) reduction resulted in the release of both Mn(II) and U(VI) into the truly dissolved phase. Copyright © 2011 Elsevier B.V. All rights reserved.

Repeated Storage of Respired Carbon in the Equatorial Pacific Ocean Over the Last Three Glacial Cycles

NASA Astrophysics Data System (ADS)

Jacobel, A. W.; McManus, J. F.; Anderson, R. F.; Winckler, G.

2017-12-01

As the largest reservoir of carbon actively exchanging with the atmosphere on glacial-interglacial timescales, the deep ocean has been implicated as the likely location of carbon dioxide sequestration during Pleistocene glaciations. Despite strong theoretical underpinnings for this expectation, it has been challenging to identify unequivocal evidence for respired carbon storage in the paleoceanographic record. Data on the rate of ocean ventilation derived from paired planktonic-benthic foraminifera radiocarbon ages conflict across the equatorial Pacific, and different proxy reconstructions contradict one another about the depth and origin of the watermass containing the respired carbon. Because any change in the storage of respiratory carbon must be accompanied by corresponding changes in dissolved oxygen concentrations, proxy data reflecting bottom water oxygenation are of value in addressing these apparent inconsistencies. We present new records of the redox sensitive metal uranium from the central equatorial Pacific to qualitatively identify intervals associated with respiratory carbon storage over the past 350 kyr. Our data reveal periods of deep ocean authigenic uranium deposition in association with each of the last three glacial maxima. Equatorial Pacific export productivity data show intervals with abundant authigenic uranium are not associated with local productivity increases, indicating episodic precipitation of authigenic uranium does not directly reflect increases in situ microbial respiration, but rather occurs in response to basin-wide decreases in deep water oxygen concentrations. We combine our new data with previously published results to propose a picture of glacial carbon storage and equatorial Pacific watermass structure that is internally consistent. We conclude that respired carbon storage in the Pacific was a persistent feature of Pleistocene glaciations.

PREPARATION OF REFRACTORY OXIDE CRYSTALS

DOEpatents

Grimes, W.R.; Shaffer, J.H.; Watson, G.M.

1962-11-13

A method is given for preparing uranium dioxide, thorium oxide, and beryllium oxide in the form of enlarged individual crystals. The surface of a fused alkali metal halide melt containing dissolved uranium, thorium, or beryllium values is contacted with a water-vapor-bearing inert gas stream at a rate of 5 to 10 cubic centimeters per minute per square centimeter of melt surface area. Growth of individual crystals is obtained by prolonged contact. Beryllium oxide-coated uranium dioxide crystals are prepared by disposing uranium dioxide crystals 5 to 20 microns in diameter in a beryllium-containing melt and contacting the melt with a water-vapor-bearing inert gas stream in the same manner. (AEC)

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).

Quantifying Differences in the Impact of Variable Chemistry on Equilibrium Uranium(VI) Adsorption Properties of Aquifer Sediments

PubMed Central

2011-01-01

Uranium adsorption–desorption on sediment samples collected from the Hanford 300-Area, Richland, WA varied extensively over a range of field-relevant chemical conditions, complicating assessment of possible differences in equilibrium adsorption properties. Adsorption equilibrium was achieved in 500–1000 h although dissolved uranium concentrations increased over thousands of hours owing to changes in aqueous chemical composition driven by sediment-water reactions. A nonelectrostatic surface complexation reaction, >SOH + UO22+ + 2CO32- = >SOUO2(CO3HCO3)2–, provided the best fit to experimental data for each sediment sample resulting in a range of conditional equilibrium constants (logKc) from 21.49 to 21.76. Potential differences in uranium adsorption properties could be assessed in plots based on the generalized mass-action expressions yielding linear trends displaced vertically by differences in logKc values. Using this approach, logKc values for seven sediment samples were not significantly different. However, a significant difference in adsorption properties between one sediment sample and the fines (<0.063 mm) of another could be demonstrated despite the fines requiring a different reaction stoichiometry. Estimates of logKc uncertainty were improved by capturing all data points within experimental errors. The mass-action expression plots demonstrate that applying models outside the range of conditions used in model calibration greatly increases potential errors. PMID:21923109

Quantifying differences in the impact of variable chemistry on equilibrium Uranium(VI) adsorption properties of aquifer sediments.

PubMed

Stoliker, Deborah L; Kent, Douglas B; Zachara, John M

2011-10-15

Uranium adsorption-desorption on sediment samples collected from the Hanford 300-Area, Richland, WA varied extensively over a range of field-relevant chemical conditions, complicating assessment of possible differences in equilibrium adsorption properties. Adsorption equilibrium was achieved in 500-1000 h although dissolved uranium concentrations increased over thousands of hours owing to changes in aqueous chemical composition driven by sediment-water reactions. A nonelectrostatic surface complexation reaction, >SOH + UO₂²⁺ + 2CO₃²⁻ = >SOUO₂(CO₃HCO₃)²⁻, provided the best fit to experimental data for each sediment sample resulting in a range of conditional equilibrium constants (logK(c)) from 21.49 to 21.76. Potential differences in uranium adsorption properties could be assessed in plots based on the generalized mass-action expressions yielding linear trends displaced vertically by differences in logK(c) values. Using this approach, logK(c) values for seven sediment samples were not significantly different. However, a significant difference in adsorption properties between one sediment sample and the fines (< 0.063 mm) of another could be demonstrated despite the fines requiring a different reaction stoichiometry. Estimates of logK(c) uncertainty were improved by capturing all data points within experimental errors. The mass-action expression plots demonstrate that applying models outside the range of conditions used in model calibration greatly increases potential errors.

URANIUM EXTRACTION

DOEpatents

Harrington, C.D.; Opie, J.V.

1958-07-01

The recovery of uranium values from uranium ore such as pitchblende is described. The ore is first dissolved in nitric acid, and a water soluble nitrate is added as a salting out agent. The resulting feed solution is then contacted with diethyl ether, whereby the bulk of the uranyl nitrate and a portion of the impurities are taken up by the ether. This acid ether extract is then separated from the aqueous raffinate, and contacted with water causing back extractioa of the uranyl nitrate and impurities into the water to form a crude liquor. After separation from the ether extract, this crude liquor is heated to about 118 deg C to obtain molten uranyl nitrate hexahydratc. After being slightly cooled the uranyl nitrate hexahydrate is contacted with acid free diethyl ether whereby the bulk of the uranyl nitrate is dissolved into the ethcr to form a neutral ether solution while most of the impurities remain in the aqueous waste. After separation from the aqueous waste, the resultant ether solution is washed with about l0% of its volume of water to free it of any dissolved impurities and is then contacted with at least one half its volume of water whereby the uranyl nitrate is extracted into the water to form an aqueous product solution.

Molybdenum, vanadium, and uranium weathering in small mountainous rivers and rivers draining high-standing islands

NASA Astrophysics Data System (ADS)

Gardner, Christopher B.; Carey, Anne E.; Lyons, W. Berry; Goldsmith, Steven T.; McAdams, Brandon C.; Trierweiler, Annette M.

2017-12-01

Rivers draining high standing islands (HSIs) and small mountainous rivers (SMRs) are known to have extremely high sediment fluxes, and can also have high chemical weathering yields, which makes them potentially important contributors to the global riverine elemental flux to the ocean. This work reports on the riverine concentrations, ocean flux, and weathering yields of Molybdenum (Mo), Vanadium (V), and Uranium (U) in a large number of small but geochemically important rivers using 338 river samples from ten lithologically-diverse regions. These redox-sensitive elements are used extensively to infer paleo-redox conditions in the ocean, and Mo and V are also important rock-derived micronutrients used by microorganisms in nitrogen fixation. Unlike in large river systems, in which dissolved Mo has been attributed predominately to pyrite dissolution, Mo concentrations in these rivers did not correlate with sulfate concentrations. V was found to correlate strongly with Si in terrains dominated by silicate rocks, but this trend was not observed in primarily sedimentary regions. Many rivers exhibited much higher V/Si ratios than larger rivers, and rivers draining young Quaternary volcanic rocks in Nicaragua had much higher dissolved V concentrations (mean = 1306 nM) than previously-studied rivers. U concentrations were generally well below the global average with the exception of rivers draining primarily sedimentary lithologies containing carbonates and shales. Fluxes of U and Mo from igneous terrains of intermediate composition are lower than the global average, while fluxes of V from these regions are higher, and up to two orders of magnitude higher in the Nicaragua rivers. Weathering yields of Mo and V in most regions are above the global mean, despite lower than average concentrations measured in some of those systems, indicating that the chemical weathering of these elements are higher in these SMR watersheds than larger drainages. In regions of active boundaries with andesite/dacite lithologies, rivers draining young Pleistocene rocks had higher concentrations than did older Miocene-Pliocene rocks of a similar composition. This work shows that weathering yields of Mo, V, and U from SMRs are slightly higher than from large rivers, and the age of igneous lithologies in these regions exhibits a measurable control on riverine concentrations of these elements.

PROCESS FOR REMOVING ALUMINUM COATINGS

DOEpatents

Flox, J.

1959-07-01

A process is presented for removing aluminum jackets or cans from uranium slugs. This is accomplished by immersing the aluminum coated uranium slugs in an aqueous solution of 9 to 20% sodium hydroxide and 35 to 12% sodium nitrate to selectively dissolve the aluminum coating, the amount of solution being such as to obtain a molar ratio of sodium hydroxide to aluminum of at least

EXTRACTION METHOD FOR SEPARATING URANIUM, PLUTONIUM, AND FISSION PRODUCTS FROM COMPOSITIONS CONTAINING SAME

DOEpatents

Seaborg, G.T.

1957-10-29

Methods for separating plutonium from the fission products present in masses of neutron irradiated uranium are reported. The neutron irradiated uranium is first dissolved in an aqueous solution of nitric acid. The plutonium in this solution is present as plutonous nitrate. The aqueous solution is then agitated with an organic solvent, which is not miscible with water, such as diethyl ether. The ether extracts 90% of the uraryl nitrate leaving, substantially all of the plutonium in the aqueous phase. The aqueous solution of plutonous nitrate is then oxidized to the hexavalent state, and agitated with diethyl ether again. In the ether phase there is then obtained 90% of plutonium as a solution of plutonyl nitrate. The ether solution of plutonyl nitrate is then agitated with water containing a reducing agent such as sulfur dioxide, and the plutonium dissolves in the water and is reduced to the plutonous state. The uranyl nitrate remains in the ether. The plutonous nitrate in the water may be recovered by precipitation.

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, J.P.

1992-03-17

A process is described for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.

SULFIDE METHOD PLUTONIUM SEPARATION

DOEpatents

Duffield, R.B.

1958-08-12

A process is described for the recovery of plutonium from neutron irradiated uranium solutions. Such a solution is first treated with a soluble sullide, causing precipitation of the plutoniunn and uraniunn values present, along with those impurities which form insoluble sulfides. The precipitate is then treated with a solution of carbonate ions, which will dissolve the uranium and plutonium present while the fission product sulfides remain unaffected. After separation from the residue, this solution may then be treated by any of the usual methods, such as formation of a lanthanum fluoride precipitate, to effect separation of plutoniunn from uranium.

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1962-04-10

A process of recovering plutonium from neutronbombarded uranium fuel by dissolving the fuel in equimolar aluminum chloride-potassium chloride; heating the mass to above 700 deg C for decomposition of plutonium tetrachloride to the trichloride; extracting the plutonium trichloride into a molten salt containing from 40 to 60 mole % of lithium chloride, from 15 to 40 mole % of sodium chloride, and from 0 to 40 mole % of potassium chloride or calcium chloride; and separating the layer of equimolar chlorides containing the uranium from the layer formed of the plutonium-containing salt is described. (AEC)

PROCESS OF RECOVERING URANIUM

DOEpatents

Kilner, S.B.

1959-12-29

A method is presented for separating and recovering uranium from a complex mixure of impurities. The uranium is dissolved to produce an aqueous acidic solution including various impurities. In accordance with one method, with the uranium in the uranyl state, hydrogen cyanide is introduced into the solution to complex the impurities. Subsequently, ammonia is added to the solution to precipitate the uraniunn as ammonium diuranate away from the impurities in the solution. Alternatively, the uranium is precipitated by adding an alkaline metal hydroxide. In accordance with the second method, the uranium is reduced to the uranous state in the solution. The reduced solution is then treated with solid alkali metal cyanide sufficient to render the solution about 0.1 to 1.0 N in cyanide ions whereat cyanide complex ions of the metal impurities are produced and the uranium is simultaneously precipituted as uranous hydroxide. Alternatively, hydrogen cyanide may be added to the reduced solution and the uranium precipitated subsequently by adding ammonium hydroxide or an alkali metal hydroxide. Other refinements of the method are also disclosed.

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

NASA Astrophysics Data System (ADS)

Reinoso-Maset, Estela; Steefel, Carl I.; Um, Wooyong; Chorover, Jon; O'Day, Peggy A.

2017-06-01

Uranyl oxyhydroxide minerals are important weathering products in uranium-contaminated surface and subsurface environments that regulate dissolved uranium (U) 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 work, the dissolution rates of K- and Na-compreignacite (K2(UO2)6O4(OH)6·8H2O and Na2(UO2)6O4(OH)6·8H2O, respectively) were measured using flow-through columns reacted with two simulated background porewater (BPW) solutions of low and high dissolved carbonate concentration (ca. 0.2 and 2.8 mmol 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 U mass from the columns, compared to <1% net loss in low carbonate BPW systems. Steady-state release of dissolved U 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 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 U 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. 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 U in porous geomedia.

Uranium hydrogeochemical and stream sediment reconnaissance of the Albuquerque NTMS Quadrangle, New Mexico, including concentrations of forty-three additional elements

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

Maassen, L.W.; Bolivar, S.L.

1979-06-01

The Los Alamos Scientific Laboratory conducted a hydrogeochemical and stream sediment reconnaissance for uranium. Totals of 408 water and 1538 sediment samples were collected from 1802 locations over a 20 100-km/sup 2/ area at an average density of one location per 11 km/sup 2/. Water samples were collected from springs, wells, and streams; sediments samples were collected predominantly from streams, but also from springs. All water samples were analyzed for uranium and 12 other elements. Sediment samples were analyzed for uranium and 42 additional elements. The uranium concentrations in water samples range from below the detection limit of 0.02 ppBmore » to 194.06 ppB. The mean uranium concentration for all water types containing < 40 ppB uranium is 1.98 ppB. Six samples contained uranium concentrations > 40.00 ppB. Well waters have the highest mean uranium concentration; spring waters have the lowest. Clusters of water samples that contain anomalous uranium concentrations are delineated in nine areas. Sediments collected from the quadrangle have uranium concentrations that range between 0.63 ppM and 28.52 ppM, with a mean for all sediments of 3.53 ppM. Eight areas containing clusters of sediments with anomalous uranium concentrations are delineated. One cluster contains sample locations within the Ambrosia Lake uranium district. Five clusters of sediment samples with anomalous uranium concentrations were collected from streams that drain the Jemez volcanic field. Another cluster defines an area just northeast of Albuquerque where streams drain Precambrian rocks, predominantly granites, of the Sandia Mountains. The last cluster, consisting of spring sediments from Mesa Portales, was collected near the contact of the Tertiary Ojo Alamo sandstone with underlying Cretaceous sediments. Sediments from these springs exhibit some of the highest uranium values reported and are associated with high uranium/thorium ratios.« less

Hydrogeochemical survey of groundwater for selected areas in the Arabian Shield and in cover rocks, Kingdom of Saudi Arabia

USGS Publications Warehouse

McHugh, John B.; Miller, W. Roger

1989-01-01

In the spring of 1984, a hydrogeochemical survey was conducted in the Kingdom of Saudi Arabia to test ground water as a sampling medium in exploration for mineral deposits. Eighty-one water samples (mostly from wells) were collected. The samples were analysed for the presence and concentration of major cations and anions, as well as a suite of trace elements. Most of the water samples contained high concentrations of dissolved salts. The majority of the samples showed no significant amounts of the trace elements. A few well-water samples contained moderately anomalous concentrations of zinc, molybdenum, and uranium. These anomalies could be due to salinity effects, contamination, or the proximity of mineral sources. This survey has established some baseline water-chemistry data, especially for the trace metals, which to date have not been reported in ground water in the Kingdom of Saudi Arabia.

Geochemical Characteristics of Aquifer system in Taichung Area, Central Taiwan

NASA Astrophysics Data System (ADS)

Tsai, Jui-Fen; Chen, Cheng-Hong; Liu, Tsung-Kwei

2016-04-01

For understanding the relationship between water bodies and host rocks and getting more information for groundwater in Taichung area, Central Taiwan, we systematically analyzed the stable isotopes (hydrogen and oxygen), helium isotopes and radon concentrations of dissolved gases from 54 groundwater, 39 river and 4 rain samples collected from Taichung Basin in wet and dry seasons of the year 2015. In the δ18O vs. δD plot, all samples present a linear trend similar to local meteoric water, indicating a meteoric origin. However, river samples are relative lighter than rain samples, it appears that the rivers are mainly recharged from precipitation of high-elevation areas with a lighter isotopic composition. Because the seasonal isotopic variation of river samples is significant, we calculated relative contribution of precipitation by seasons using the mass balance equation. Results show that the precipitation in the rainy season is the major source of groundwater. The helium isotopic ratio in dissolved gases of most groundwater samples are close to 1 RA (RA = 3He/4He ratio of air), except the sample from Wu-Feng well that exhibits 0.3 RA. This sample also has an older C-14 age (˜27000 yrs.) than others (<200 yrs.), implying that the dissolved helium is likely affected by radiogenic 4He of surrounding rocks. The average concentration of radon for groundwater in the northern section of Taichung Basin is 20.3 Bq/L, which is higher than that of the southern section (14.5 Bq/L). Variations of radon concentrations in the two sections may be related to the different drainage systems (Paleo-Dajia River vs. Wu River), in which sediments from Paleo-Dajia River may contain higher uranium concentrations. On the other hand, water in rivers usually contains undetectable radon (<0.37 Bq/L) because it rapidly escapes to the atmosphere. However, river samples from the central part of basin have radon concentrations ranging between 1 and 3 Bq/L, reflecting that the sampling sites are in the vicinity of points of groundwater inflow. This study illustrates the utility of hydrogen and oxygen isotopes to trace the groundwater source and determine the seasonal contribution ratios of precipitation to groundwater recharge, and demonstrates the advantage of using dissolved gas to investigate the groundwater-host rocks interaction. Key words: Central Taiwan, groundwater, dissolved gas, helium isotope, hydrogen and oxygen isotopes, water radon

Large decadal-scale changes in uranium and bicarbonate in groundwater of the irrigated western U.S

USGS Publications Warehouse

Burow, Karen R.; Belitz, Kenneth; Dubrovsky, Neil M.; Jurgens, Bryant C.

2017-01-01

Samples collected about one decade apart from 1105 wells from across the U.S. were compiled to assess whether uranium concentrations in the arid climate are linked to changing bicarbonate concentrations in the irrigated western U.S. Uranium concentrations in groundwater were high in the arid climate in the western U.S, where uranium sources are abundant. Sixty-four wells (6%) were above the U.S. EPA MCL of 30 μg/L; all but one are in the arid west. Concentrations were low to non-detectable in the humid climate. Large uranium and bicarbonate increases (differences are greater than the uncertainty in concentrations) occur in 109 wells between decade 1 and decade 2. Similarly, large uranium and bicarbonate decreases occur in 76 wells between the two decades. Significantly more wells are concordant (uranium and bicarbonate are both going the same direction) than discordant (uranium and bicarbonate are going opposite directions) (p < 0.001; Chi-square test). The largest percent difference in uranium concentrations occur in wells where uranium is increasing and bicarbonate is also increasing. These large differences occur mostly in the arid climate. Results are consistent with the hypothesis that changing uranium concentrations are linked to changes in bicarbonate in irrigated areas of the western U.S.

Uptake of uranium by aquatic plants growing in fresh water ecosystem around uranium mill tailings pond at Jaduguda, India.

PubMed

Jha, V N; Tripathi, R M; Sethy, N K; Sahoo, S K

2016-01-01

Concentration of uranium was determined in aquatic plants and substrate (sediment or water) of fresh water ecosystem on and around uranium mill tailings pond at Jaduguda, India. Aquatic plant/substrate concentration ratios (CRs) of uranium were estimated for different sites on and around the uranium mill tailings disposal area. These sites include upstream and downstream side of surface water sources carrying the treated tailings effluent, a small pond inside tailings disposal area and residual water of this area. Three types of plant groups were investigated namely algae (filamentous and non-filamentous), other free floating & water submerged and sediment rooted plants. Wide variability in concentration ratio was observed for different groups of plants studied. The filamentous algae uranium concentration was significantly correlated with that of water (r=0.86, p<0.003). For sediment rooted plants significant correlation was found between uranium concentration in plant and the substrate (r=0.88, p<0.001). Both for other free floating species and sediment rooted plants, uranium concentration was significantly correlated with Mn, Fe, and Ni concentration of plants (p<0.01). Filamentous algae, Jussiaea and Pistia owing to their high bioproductivity, biomass, uranium accumulation and concentration ratio can be useful for prospecting phytoremediation of stream carrying treated or untreated uranium mill tailings effluent. Copyright © 2015 Elsevier B.V. All rights reserved.

Uranium hydrogeochemical and stream sediment reconnaissance of the Newcastle NTMS quadrangle, Wyoming, including concentrations of forty-two additional elements

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

Goff, S.J.; Sandoval, W.F.; Gallimore, D.L.

1980-06-01

During the summer and fall of 1977, 533 water and 1226 sediment samples were collected from 1740 locations within the 18,000 km/sup 2/ area of the Newcastle quadrangle, Wyoming. Water samples were collected from wells and springs; sediment samples were collected from stream channels and from springs. Each water sample was analyzed for uranium, and each sediment sample was analyzed for 43 elements, including uranium and thorium. Uranium concentrations in water samples range from below the detection limit of 0.02 ppB to 702.26 ppB and have a median of 1.73 ppB and a mean of 11.76 ppB. Water samples containingmore » high uranium concentrations (>20 ppB) generally are associated with known uranium mining activity or units known to be uranium bearing. About one-third of the water samples containing high uranium concentrations were collected from locations within the Pumpkin Buttes and Turnercrest-Ross Districts. Nearly half of the water samples containing high uranium concentrations were collected from locations just west of the Monument Hill and Highland Flats-Box Creek Districts. Similar anomalous uranium concentrations in this region have been reported updip from Exxon's Highland uranium deposits. High uranium concentrations were also found associated with the Lance Creek-Old Woman Anticline District.« less

Water quality of surficial aquifers in the Georgia-Florida Coastal Plain

USGS Publications Warehouse

Crandall, C.A.; Berndt, M.P.

1996-01-01

The National Water Quality Assessment Program of the U.S. Geological Survey established the Georgia-Florida Coastal Plain study unit in 1991. The ground-water study-unit survey was conducted in 1993 to provide a broad over-view of water quality in surficial aquifers. Three land resource provinces were included in the Georgia-Florida Coastal Plain study-unit survey: the Central Florida Ridge, the Coastal Flatwoods, and the Southern Coastal Plain. The U.S. Geological Survey sampled 37 wells in surficial aquifers, 18 in the Coastal Flatwoods and 19 in the Southern Coastal Plain. The Florida Department of Environmental Protection sampled 27 wells tapping surficial aquifers in the Central Florida Ridge as part of the background ground-water quality monitoring network from 1985 through 1989. The data were used to characterize water quality in surficial aquifers of the Central Florida Ridge. Results of the study-unit survey indicated that dissolved solids concentrations in ground water were mostly less than 100 mg/L (milligrams per liter). Higher medians of pH, specific conductance, and concentrations of calcium, bicarbonate, and dissolved solids were measured in samples from the Central Florida Ridge compared to the Southern Coastal Plain and Coastal Flatwoods, probably because of a greater percentage of carbonate minerals in aquifer materials. The U.S. Environmental Protection Agency secondary maximum contaminant level for iron of 300 ug/L (micrograms per liter) in drinking water was exceeded in 15 of 45 samples. Concentrations of nitrate as nitrogen were less than 3.0 mg/L in most samples (74 percent), indicating little or no influence from human activity. Only five samples (9 percent) had concentrations above 10 mg/L, the U.S. Environmental Protection Agency maximum contaminant level for nitrate concentration in drinking water. Significantly lower median concentrations of nitrate were measured in samples from polyvinyl chloride monitoring wells with diameters less than 6 inches than in large diameter, uncased, or iron-cased wells. The median nitrate concentration was 0.05 mg/L in water from monitoring wells, 1.0 mg/L in samples from iron cased wells, and 2.0 mg/L in samples from uncased wells. Concentrations of volatile organic compounds were mostly less than the detection levels and exceeded 1 ug/L in only four samples. Compounds detected at concentrations greater than 1 ug/L were: tetrachloroethane (8.77 ug/L), toluene (23 ug/L) and chloromethane (21 ug/L). Atrazine, desethyl-atrazine, and metolachlor were the only pesticides detected; concentrations were less than 0.02 ug/L, except for metolachlor (2.5 ug/L). Detection of organic compounds in surficial aquifer may be associated with specific activities or sources near the well. Concentrations of radon exceeded the U.S. Environmental Protection Agency proposed maximum contaminant level of 300 picocuries per liter (pCi/L) in 33 samples from wells on the Coastal Flatwoods and the Southern Coastal Plain. Concentrations as high as 13,000 pCi/L were detected in northern Florida. Although uranium concentrations were less than 1 ug/L in all but one sample (1.3 ug/L) from the Southern Coastal Plain, elevated radon concentrations indicate that uranium is present in aquifer material. Uranium is most likely sorbed to iron oxides and clays in subsurface materials. Tritium concentrations indicated that ground water was recharged by precipitation during the past 40 years. Higher concentrations of tritium in ground water were found in the northern part of the study area and may be related to Savannah River Nuclear Facility.

Paleontological analysis of a lacustrine carbonaceous uranium deposit at the Anderson mine, Date Creek basin, west-central Arizona (U.S.A.)

USGS Publications Warehouse

Otton, J.K.; Bradbury, J.P.; Forester, R.M.; Hanley, J.H.

1990-01-01

The Tertiary sedimentary sequence of the Date Creek basin area of Arizona is composed principally of intertonguing alluvial-fan and lacustrine deposits. The lacustrine rocks contain large intermediate- to, locally, high-grade uranium deposits that form one of the largest uranium resources in the United States (an estimated 670,000 tons of U3O8 at an average grade of 0.023% is indicated by drilling to date). At the Anderson mine, about 50,000 tons of U3O8 occurs in lacustrine carbonaceous siltstones and mudstones (using a cutoff grade of 0.01%). The Anderson mine constitutes a new class of ore deposit, a lacustrine carbonaceous uranium deposit. Floral and faunal remains at the Anderson mine played a critical role in creating and documenting conditions necessary for uranium mineralization. Organic-rich, uraniferous rocks at the Anderson mine contain plant remains and ostracodes having remarkably detailed preservation of internal features because of infilling by opaline silica. This preservation suggests that the alkaline lake waters in the mine area contained high concentrations of dissolved silica and that silicification occurred rapidly, before compaction or cementation of the enclosing sediment. Uranium coprecipitated with the silica. Thinly laminated, dark-colored, siliceous beds contain centric diatoms preserved with carbonaceous material suggesting that lake waters at the mine were locally deep and anoxic. These alkaline, silica-charged waters and a stagnant, anoxic environment in parts of the lake were necessary conditions for the precipitation of large amounts of uranium in the lake-bottom sediments. Sediments at the Anderson mine contain plant remains and pollen that were derived from diverse vegetative zones suggesting about 1500 m of relief in the area at the time of deposition. The pollen suggests that the valley floor was semiarid and subtropical, whereas nearby mountains supported temperate deciduous forests. ?? 1990.

Reactive Transport of the Uranyl Ion in Soils, Sediments, and Groundwater Systems

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

Zachara, John M.; Ilton, Eugene S.; Liu, Chongxuan

2013-05-16

Uranium is a ubiquitous trace component in rocks ranging from 1.2 to 1.3 µg g-1 in sedimentary rocks, 2.2 to 15 µg g-1 in granites, and 20 to 120 µg g-1 in phosphates (Langmuir, 1997; Plant et al., 1999). Uranium (U) is released to natural waters in dilute concentrations (generally < 10-7 mole L-1) from the weathering of these sources, with water concentrations in uraniferous geologic terrains, such as the southwestern U.S. (USGS, 2011), being higher (~ 10-6.5 mol L-1). Elevated water-borne concentrations are associated with the weathering of natural ore bodies [~10-6 mol L-1; e.g, (Payne and Airey, 2006)],more » the extraction and mining of U for armaments (Jiang and Aschner, 2009; WHO, 2001) and nuclear fuels [10-6 to 10-3 mol L-1; (Abdelouas et al., 1999)], and the disposal of waste solids and liquids from nuclear fuels reprocessing and arms production [~ 10-6 to 10-2 mol L-1; e.g., (Wan et al., 2009; Zachara et al., 2007)]. The form of U present in natural waters at high concentration is generally the uranyl ion [e.g., UO22+] which is quite soluble. Groundwater in many parts of the world contains dissolved U originating from natural and anthropogenic sources (ATSDR, 2011; EFSA, 2009). Low levels of dissolved U in drinking water are considered a health concern, causing renal and other effects (Kurttio et al., 2002; Kurttio et al., 2005; Limson Zamora et al., 1998; Nriagu et al., 2012; Raymond-Whish et al., 2007; Selden et al., 2009). The U.S. Environmental Protection Agency has established a regulatory drinking water standard of 30 µg L-1 (1.26 x 10-7 mol L-1) or 30 pCi L-1, whichever is exceeded first. The World Health Organization has recommended an even lower drinking water standard of 15 µg L-1 [6.3 x 10-8 mol L-1; (WHO, 2005)]. Human exposure to U through drinking water is expected to rise as world-wide reliance on groundwater sources increase (ESS, 2010).« less

Water-quality assessment of the Kentucky River basin, Kentucky; results of investigations of surface-water quality, 1987-90

USGS Publications Warehouse

Haag, K.H.; Garcia, Rene; Jarrett, G.L.; Porter, S.D.

1995-01-01

The U.S. Geological Survey investigated the water quality of the Kentucky River Basin in Kentucky as part of the National Water-Quality Assessment program. Data collected during 1987-90 were used to describe the spatial and temporal variability of water-quality constituents including metals and trace elements, nutrients, sediments, pesticides, dissolved oxygen, and fecal-coliform bacteria. Oil-production activities were the source of barium, bromide, chloride, magnesium, and sodium in several watersheds. High concentrations of aluminum, iron, and zinc were related to surface mining in the Eastern Coal Field Region. High concentrations of lead and zinc occurred in streambed sediments in urban areas, whereas concentrations of arsenic, strontium, and uranium were associated with natural geologic sources. Concentrations of phosphorus were significantly correlated with urban and agricultural land use. The high phosphorus content of Bluegrass Region soils was an important source of phosphorus in streams. At many sites in urban areas, most of the stream nitrogen load was attributable to wastewater-treatment-plant effluent. Average suspended-sediment concentrations were positively correlated with discharge. There was a downward trend in suspended-sediment concentrations downstream in the Kentucky River main stem during the study. The most frequently detected herbicides in water samples were atrazine, 2,4-D, alachlor, metolachlor, and dicamba. Diazinon, malathion, and parathion were the most frequently detected organophosphate insecticides in water samples. Detectable concentrations of aldrin, chlordane, DDT, DDE, dieldrin, endrin, endosulfan, heptachlor, and lindane were found in streambed-sediment samples. Dissolved-oxygen concentrations were sometimes below the minimum concentration needed to sustain aquatic life. At some sites, high concentrations of fecal-indicator bacteria were found and water samples did not meet sanitary water-quality criteria.

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

RECOVERY OF VALUABLE MATERIAL FROM GRAPHITE BODIES

DOEpatents

Fromm, L.W. Jr.

1959-09-01

An electrolytic process for recovering uranium from a graphite fuel element is described. The uraniumcontaining graphite body is disposed as the anode of a cell containing a nitric acid electrolyte and a 5 amp/cm/sup 2/ current passed to induce a progressive disintegration of the graphite body. The dissolved uranium is quickly and easily separated from the resulting graphite particles by simple mechanical means, such as centrifugation, filtration, and decontamination.

Effects of surface applications of biosolids on groundwater quality and trace-element concentrations in crops near Deer Trail, Colorado, 2004-2010

USGS Publications Warehouse

Yager, Tracy J.B.; Crock, James G.; Smith, David B.; Furlong, Edward T.; Hageman, Philip L.; Foreman, William T.; Gray, James L.; ReVello, Rhiannon C.

2013-01-01

The U.S. Geological Survey (USGS), in cooperation with Metro Wastewater Reclamation District (Metro District), studied biosolids composition and the effects of biosolids applications on groundwater quality and trace-element concentrations in crops of the Metro District properties near Deer Trail, Colorado, during 2004 through 2010. Priority parameters for each monitoring component included the nine trace elements regulated by Colorado for biosolids (arsenic, cadmium, copper, lead, mercury, molybdenum, nickel, selenium, and zinc); other constituents also were analyzed. All concentrations for the priority parameters in monthly biosolids samples were less than Colorado regulatory limits, and the concentrations were relatively consistent. Biosolids likely were the largest source of nitrogen and phosphorus on the Metro District properties. Plutonium isotopes were not detected in the biosolids, but many organic wastewater compounds (organic wastewater compounds: wastewater indicators, pharmaceuticals, and hormones) were detected in substantial concentrations relative to minimum reporting levels and various surface-water concentrations. Bismuth, copper, mercury, nitrogen, phosphorus, silver, biogenic sterols, detergent degradates, disinfectants, fire retardants, fragrances, pharmaceuticals, and plasticizers would be the most likely biosolids signature to indicate the presence of Metro District biosolids in soil or streambed sediment from the study area. Antimony, cadmium, cobalt, copper, molybdenum, nickel, nitrogen, phosphorus, selenium, tungsten, vanadium, zinc, detergent degradates, disinfectants, fire retardants, fragrances, pharmaceuticals or their degradates, and plasticizers would be the most likely biosolids signature for groundwater and surface water in the study area. More biosolids-signature components detected and larger concentration differences from untreated materials, baseline, and blank samples indicate more evidence of biosolids presence or effects. Although the inorganic constituent concentrations were relatively large in samples from one monitoring well, the concentrations of organic wastewater compounds in groundwater samples were not correspondingly large. Concentrations of organic wastewater compounds in the groundwater samples from all five monitoring wells were less than the minimum reporting levels with only a few detections. Some of the organic wastewater compounds detected could have anthropogenic sources that are not biosolids. Concentrations of priority parameters in groundwater varied spatially and temporally but generally were less than Colorado regulatory limits. Concentrations of dissolved nitrate, arsenic, and selenium, in addition to chloride, sulfate, total dissolved solids, boron, iron, manganese, and uranium, in samples from some wells exceeded the Colorado standards. Concentrations of dissolved nitrate (three wells), molybdenum (one well), selenium (two wells), and uranium (one well) in shallow groundwater had significant (alpha = 0.05) upward trends in some parts of the study area. The biosolids-signature results indicate that the aquifers intercepted by the five routinely sampled wells likely have received some recharge through treated (biosolids-applied) fields or biosolids-affected ponds. Adverse effects from this biosolids-related recharge range from few (if any) at one well to large and significantly (alpha = 0.05) increasing nitrate concentrations at another well. A statistical evaluation of five paired wheat-grain samples from treated (biosolids-applied) fields and untreated (control) fields did not indicate any evidence that biosolids applications significantly (alpha = 0.05 or 0.10) increased concentration of any of these constituents in wheat grain. The wheat-grain concentrations from this study were similar to those from other studies for fields in North America where no biosolids were applied. The data for the limited crop samples indicate that biosolids applications are not increasing the concentrations of arsenic, cadmium, copper, lead, mercury, molybdenum, nickel, selenium, sulfur, and zinc in mature wheat grain from the study area.

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 concentrations in groundwater, northeastern Washington

USGS Publications Warehouse

Kahle, Sue C.; Welch, Wendy B.; Tecca, Alison E.; Eliason, Devin M.

2018-04-18

A study of uranium in groundwater in northeastern Washington was conducted to make a preliminary assessment of naturally occurring uranium in groundwater relying on existing information and limited reconnaissance sampling. Naturally occurring uranium is associated with granitic and metasedimentary rocks, as well as younger sedimentary deposits, that occur in this region. The occurrence and distribution of uranium in groundwater is poorly understood. U.S. Environmental Protection Agency (EPA) regulates uranium in Group A community water systems at a maximum contaminant level (MCL) of 30 μg/L in order to reduce uranium exposure, protect from toxic kidney effects of uranium, and reduce the risk of cancer. However, most existing private wells in the study area, generally for single family use, have not been sampled for uranium. This document presents available uranium concentration data from throughout a multi-county region, identifies data gaps, and suggests further study aimed at understanding the occurrence of uranium in groundwater.The study encompasses about 13,000 square miles (mi2) in the northeastern part of Washington with a 2010 population of about 563,000. Other than the City of Spokane, most of the study area is rural with small towns interspersed throughout the region. The study area also includes three Indian Reservations with small towns and scattered population. The area has a history of uranium exploration and mining, with two inactive uranium mines on the Spokane Indian Reservation and one smaller inactive mine on the outskirts of Spokane. Historical (1977–2016) uranium in groundwater concentration data were used to describe and illustrate the general occurrence and distribution of uranium in groundwater, as well as to identify data deficiencies. Uranium concentrations were detected at greater than 1 microgram per liter (μg/L) in 60 percent of the 2,382 historical samples (from wells and springs). Uranium concentrations ranged from less than 1 to 88,600 μg/L, and the median concentration of uranium in groundwater for all sites was 1.4 μg/L.New (2017) uranium in groundwater concentration data were obtained by sampling 13 private domestic wells for uranium in areas without recent (2000s) water-quality data. Uranium was detected in all 13 wells sampled for this study; concentrations ranged from 1.03 to 1,180 μg/L with a median of 22 μg/L. Uranium concentrations of groundwater samples from 6 of the 13 wells exceeded the MCL for uranium. Uranium concentrations in water samples from two wells were 1,130 and 1,180 μg/L, respectively; nearly 40 times the MCL.Additional data collection and analysis are needed in rural areas where self-supplied groundwater withdrawals are the primary source of water for human consumption. Of the roughly 43,000 existing water wells in the study area, only 1,755 wells, as summarized in this document, have available uranium concentration data, and some of those data are decades old. Furthermore, analysis of area groundwater quality would benefit from a more extensive chemical-analysis suite including general chemistry in order to better understand local geochemical conditions that largely govern the mobility of uranium. Although the focus of the present study is uranium, it also is important to recognize that there are other radionuclides of concern that may be present in area groundwater.

Adsorbent Alkali Conditioning for Uranium Adsorption from Seawater. Adsorbent Performance and Technology Cost Evaluation

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

Tsouris, Costas; Mayes, Richard T.; Janke, Christopher James

The Fuel Resources program of the Fuel Cycle Research and Development program of the Office of Nuclear Energy (NE) is focused on identifying and implementing actions to assure that nuclear fuel resources are available in the United States. An immense source of uranium is seawater, which contains an estimated amount of 4.5 billion tonnes of dissolved uranium. This unconventional resource can provide a price cap and ensure centuries of uranium supply for future nuclear energy production. NE initiated a multidisciplinary program with participants from national laboratories, universities, and research institutes to enable technical breakthroughs related to uranium recovery from seawater.more » The goal is to develop advanced adsorbents to reduce the seawater uranium recovery technology cost and uncertainties. Under this program, Oak Ridge National Laboratory (ORNL) has developed a new amidoxime-based adsorbent of high surface area, which tripled the uranium capacity of leading Japanese adsorbents. Parallel efforts have been focused on the optimization of the physicochemical and operating parameters used during the preparation of the adsorbent for deployment. A set of parameters that need to be optimized are related to the conditioning of the adsorbent with alkali solution, which is necessary prior to adsorbent deployment. Previous work indicated that alkali-conditioning parameters significantly affect the adsorbent performance. Initiated in 2014, this study had as a goal to determine optimal parameters such as base type and concentration, temperature, and duration of conditioning that maximize the uranium adsorption performance of amidoxime functionalized adsorbent, while keeping the cost of uranium production low. After base-treatment at various conditions, samples of adsorbent developed at ORNL were tested in this study with batch simulated seawater solution of 8-ppm uranium concentration, batch seawater spiked with uranium nitrate at 75-100 ppb uranium, and continuous-flow natural seawater at the Pacific Northwest National Laboratory (PNNL). Fourier Transform Infrared (FTIR) spectroscopy, Nuclear Magnetic Resonance (NMR) spectroscopy, Scanning Electron Microscopy (SEM), and elemental analysis were used to characterize the adsorbent at different stages of adsorbent preparation and treatment. The study can be divided into two parts: (A) investigation of optimal parameters for KOH adsorbent conditioning and (B) investigation of other possible agents for alkali conditioning, including cost analysis on the basis of uranium production. In the first part of the study, tests with simulated seawater containing 8 ppm uranium showed that the uranium adsorption capacity increased with an increase in the KOH concentration and conditioning time and temperature at each of the KOH concentrations used. FTIR and solid state NMR studies indicated that KOH conditioning converts the amidoxime functional groups into more hydrophilic carboxylate. The longer the KOH conditioning time, up to three hours, the higher was the loading capacity from the simulated seawater solution which is composed of only uranyl, sodium, chloride, and carbonate ions. Marine testing with natural seawater, on the other hand, showed that the uranium adsorption capacity of the adsorbent increased with KOH conditioning temperature, and gradually decreased with increasing KOH conditioning time from one hour to three hours at 80 C. This behavior is due to the conversion of amidoxime to carboxylate. The carboxylate groups are needed to increase the hydrophilicity of the adsorbent; however, conversion of a significant amount of amidoxime to carboxylate leads to loss in selectivity toward uranyl ions. Thus, there is an optimum KOH conditioning time for each temperature at which an optimum ratio between amidoxime and carboxylate is reached. For the case of base conditioning with 0.44 M KOH at 80 C, the optimal conditioning time is 1 hour, with respect to the highest uranium loading capacity from natural seawater. Uptake of other metal ions such as V, Fe, and Cu follows the same trend as that of uranium. Also, the uptake of Ca, Mg, and Zn ions increased with increasing KOH conditioning time, probably due to formation of more carboxylates, which leads to conversion of uranium-selective binding sites to less selective sites. In the second part of the study, inorganic based reagents such as sodium hydroxide (NaOH), sodium carbonate (Na 2CO 3), cesium hydroxide (CsOH), as well as organic based reagents such as ammonium hydroxide (AOH), tetramethylammonium hydroxide (TMAOH), tetraethylammonium hydroxide (TEAOH), triethylmethylammonium hydroxide (TEMAOH), tetrapropylammonium hydroxide (TPAOH) and tetrabutylammonium hydroxide (TBAOH), in addition to KOH, were used for alkaline conditioning. NaOH has emerged as a better reagent for alkaline conditioning of amidoxime-based adsorbent because of higher uranium uptake capacity, higher uranium uptake selectivity ...« less

RECOVERY OF THORIUM AND URANIUM VALUES FROM AQUEOUS SOLUTIONS

DOEpatents

Calkins, G.D.

1958-02-18

This patent deals with the separation and recovery of uranium from monazite sand. After initial treatment of the sand with sodium hydroxide, a precipitate is obtuined which contains the uranium, thorium, rare earths and some phosphorus. This precipitate is then dissolved in nitric acid. The bulk of the rare earths are removed from thls soiution by adding aa excess of alkali carbonate, causing precipitation of the rare earths together with part of the thorium present. The solution still contains a considerable amount of thorium, some rare earths, and practically all of the uranium originally present. Thorium and rare earth values are readily precipitated from such solution, and the uranium values thus isolated, by the addition of an excess hydrogen peroxide. The pH value of the solution is preferably adjusted to at least 9 prior to the addition of the peroxide.

Characterization of low concentration uranium glass working materials

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

Eppich, G. R.; Wimpenny, J. B.; Leever, M. E.

A series of uranium-doped silicate glasses were created at (Lawrence Livermore National Laboratory) LLNL, to be used as working reference material analogs for low uranium concentration research. Specifically, the aim of this effort was the generation of well-characterized glasses spanning a range of concentrations and compositions, and of sufficient homogeneity in uranium concentration and isotopic composition, for instrumentation research and development purposes. While the glasses produced here are not intended to replace or become standard materials for uranium concentration or uranium isotopic composition, it is hoped that they will help fill a current gap, providing low-level uranium glasses sufficient formore » methods development and method comparisons within the limitations of the produced glass suite. Glasses are available for research use by request.« less

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

Hamzah, Zaini, E-mail: tengkuliana88@gmail.com; Rosli, Tengku Nurliana Tuan Mohd, E-mail: tengkuliana88@gmail.com; Saat, Ahmad, E-mail: tengkuliana88@gmail.com

An estuary is an area that has a free connection with the open sea and it is a dynamic semi-enclosed coastal bodies. Ex-mining, aquaculture and industrial areas in Selangor are the sources of pollutants discharged into the estuary water. Radionuclides are considered as pollutants to the estuary water. Gamma radiations emitted by natural radionuclides through their decaying process may give impact to human. The radiological effect of natural radionuclides which are {sup 226}Ra, {sup 228}Ra, {sup 40}K, {sup 238}U and {sup 232}Th, were explored by determining the respective activity concentrations in filtered water along the Langat estuary, Selangor. Meanwhile, in-more » situ water quality parameters such as temperature, dissolve oxygen (DO), salinity, total suspended solid (TSS), pH and turbidity were measured by using YSI portable multi probes meter. The activity concentration of {sup 226}Ra, {sup 228}Ra and {sup 40}K were determined by using gamma-ray spectrometry with high-purity germanium (HPGe) detector. The activity concentrations of {sup 226}Ra, {sup 228}Ra and {sup 40}K in samples are in the range of 0.17 - 0.67 Bq/L, 0.16 - 0.97 Bq/L and 1.22 - 5.57 Bq/L respectively. On the other hand, the concentrations of uranium-238 and thorium-232 were determined by using Energy Dispersive X-ray Fluorescence Spectrometry (EDXRF). The thorium concentrations are between 0.17 ppm to 0.28 ppm and uranium concentrations were 0.25 ppm to 0.31 ppm. The results show activity concentrations of radionuclides are slightly high near the river estuary. The Radium Equivalent, Absorbed Dose Rate, External Hazard Index, and Annual Effective Dose of {sup 226}Ra, {sup 228}Ra and {sup 40}K are also studied.« less

Safeguards on uranium ore concentrate? the impact of modern mining and milling process

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

Francis, Stephen

2013-07-01

Increased purity in uranium ore concentrate not only raises the question as to whether Safeguards should be applied to the entirety of uranium conversion facilities, but also as to whether some degree of coverage should be moved back to uranium ore concentrate production at uranium mining and milling facilities. This paper looks at uranium ore concentrate production across the globe and explores the extent to which increased purity is evident and the underlying reasons. Potential issues this increase in purity raises for IAEA's strategy on the Starting Point of Safeguards are also discussed.

Dissolution Flowsheet for High Flux Isotope Reactor Fuel

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

Daniel, W. E.; Rudisill, T. S.; O'Rourke, P. E.

2016-09-27

As part of the Spent Nuclear Fuel (SNF) processing campaign, H-Canyon is planning to begin dissolving High Flux Isotope Reactor (HFIR) fuel in late FY17 or early FY18. Each HFIR fuel core contains inner and outer fuel elements which were fabricated from uranium oxide (U 3O 8) dispersed in a continuous Al phase using traditional powder metallurgy techniques. Fuels fabricated in this manner, like other SNF’s processed in H-Canyon, dissolve by the same general mechanisms with similar gas generation rates and the production of H 2. The HFIR fuel cores will be dissolved and the recovered U will be down-blendedmore » into low-enriched U. HFIR fuel was previously processed in H-Canyon using a unique insert in both the 6.1D and 6.4D dissolvers. Multiple cores will be charged to the same dissolver solution maximizing the concentration of dissolved Al. The objective of this study was to identify flowsheet conditions through literature review and laboratory experimentation to safely and efficiently dissolve the HFIR fuel in H-Canyon. Laboratory-scale experiments were performed to evaluate the dissolution of HFIR fuel using both Al 1100 and Al 6061 T6 alloy coupons. The Al 1100 alloy was considered a representative surrogate which provided an upper bound on the generation of flammable (i.e., H 2) gas during the dissolution process. The dissolution of the Al 6061 T6 alloy proceeded at a slower rate than the Al 1100 alloy, and was used to verify that the target Al concentration in solution could be achieved for the selected Hg concentration. Mass spectrometry and Raman spectroscopy were used to provide continuous monitoring of the concentration of H 2 and other permanent gases in the dissolution offgas, allowing the development of H 2 generation rate profiles. The H 2 generation rates were subsequently used to evaluate if a full HFIR core could be dissolved in an H-Canyon dissolver without exceeding 60% of the calculated lower flammability limit (LFL) for H 2 at a given Hg concentration. Complete dissolution of the Al 1100 and Al 6061 T6 alloys up to a final Al concentration of 2 M was obtained using a 7 M HNO 3 solution containing a 0.002 M Hg catalyst. However, following the dissolutions, solids were observed in the solution. The solids were amorphous, but likely originated from the Si present in the alloys. No crystalline materials, such as Al(NO 3) 3 were observed. During the course of the dissolution experiments, it was determined that delaying the addition of Hg once the HNO 3 solution reached the boiling point can reduce the total offgas and H 2 generation rates. The delay in starting the Hg addition is not necessary for HFIR fuel dissolution, but could be useful in other research reactor dissolution campaigns. The potential to generate flammable concentrations of H 2 in the offgas during a HFIR fuel dissolution was evaluated using the experimental data. The predicted H 2 concentration in the dissolver offgas stream was compared with 60% of the calculated H 2 LFL at 200 °C using several prototypical experiments. The calculations showed that a full HFIR core can be dissolved using nominally 0.002 M Hg to catalyze the dissolution. The margin between the predicted H 2 concentration and the calculated LFL was greater when the solution was allowed to boil for 45 min prior to initiating the Hg addition. When the Hg was increased to 0.004 M, the predicted H 2 concentration exceeded the calculated LFL early in the dissolution. The dissolution experiments also demonstrated that additional Hg (beyond the initial 0.002 M) could be added as the Al concentration increases. The ability to add more Hg during a HFIR fuel dissolution could be beneficial if slow dissolution rates are observed at high Al concentrations. Experimental data were used to demonstrate that the predicted H 2 concentration in a dissolver was below 60% of the calculated LFL at 200 °C when 0.004 M Hg was used to catalyze the dissolution if the Al concentration is conservatively greater than 0.5 M. Data also show that the Hg concentration during a HFIR fuel dissolution can be increased from 0.002 to 0.008 M at an Al concentration of 1.3 M.« less

Characterization of selected radionuclides in sediment and surface water in Standley Lake, Great Western Reservoir, and Mower Reservoir, Jefferson County, Colorado, 1992

USGS Publications Warehouse

Clow, D.W.; Johncox, D.A.

1995-01-01

Lake sediment and surface water from Standley Lake, Great Western Reservoir, and Mower Reservoir, near Denver, Colorado, were sampled and analyzed for selected radionuclides during August through October, 1992. Sample concentrations were summarized and compared to results from a study conducted in 1983-84. Median plutonium-239,240 (239,240Pu) concentrations in lake-sediment grab samples from Standley Lake, Great Western Reservoir, and Mower Reservoir were 0.037, 0.105, and 0.351 picocuries per gram (pCi/g). The maximum concen- tration of 239,240Pu dissolved in lake water was 0.009 picocuries per liter, substantially below limits suggested by the Colorado Department of Health and the Environment. Dissolved concentrations of gross alpha and uranium isotopes were below National Drinking Water Standards in all water samples. There was no statistically significant difference between 239,240Pu concentration in lake-sediment grab samples collected from Standley Lake in 1983-84 and in 1992; however, there was a small, but statistically significant, difference at Great Western Reservoir (p<0.05). In 1992 at Great Western Reservoir, median 239,240Pu concentrations were 0.040 pCi/g lower than in 1983-84. There was a small, but statistically significant (p<0.05) difference in 239,240Pu concentrations in lake- bottom-sediment cores collected in 1983-84 and in 1992. Measured concentrations tended to be higher in 1983-84 than in 1992. The differences were greatest at concentrations above 1.5 pCi/g; in those samples concentrations were 10 to 30% higher in 1983-84 than in 1992.

Plant induced changes in concentrations of caesium, strontium and uranium in soil solution with reference to major ions and dissolved organic matter.

PubMed

Takeda, Akira; Tsukada, Hirofumi; Takaku, Yuichi; Akata, Naofumi; Hisamatsu, Shun'ichi

2008-06-01

For a better understanding of the soil-to-plant transfer of radionuclides, their behavior in the soil solution should be elucidated, especially at the interface between plant roots and soil particles, where conditions differ greatly from the bulk soil because of plant activity. This study determined the concentration of stable Cs and Sr, and U in the soil solution, under plant growing conditions. The leafy vegetable komatsuna (Brassica rapa L.) was cultivated for 26 days in pots, where the rhizosphere soil was separated from the non-rhizosphere soil by a nylon net screen. The concentrations of Cs and Sr in the rhizosphere soil solution decreased with time, and were controlled by K+NH(4)(+) and Ca, respectively. On the other hand, the concentration of U in the rhizosphere soil solution increased with time, and was related to the changes of DOC; however, this relationship was different between the rhizosphere and non-rhizosphere soil.

SEPARATION OF URANIUM FROM THORIUM AND PROTACTINIUM

DOEpatents

Musgrave, W.K.R.

1959-06-30

This patent relates to the separation of uranium from thorium and protactinium; such mixtures of elements usually being obtained by neutron irradiation of thorium. The method of separating the constituents has been first to dissolve the mixture of elements in concertrated nitric acid and then to remove the protactinium by absorption on manganese dioxide and the uranium by solvent extraction with ether. Prior to now, comparatively large amounts of thorium were extracted with the uranium. According to the invention this is completely prevented by adding sodium diethyldithiocarbamate to the mixture of soluble nitrate salts. The organic salt has the effect of reacting only with the uranyl nitrate to form the corresponding uranyl salt which can then be selectively extracted from the mixture with amyl acetate.

Variations of uranium concentrations in a multi-aquifer system under the impact of surface water-groundwater interaction

NASA Astrophysics Data System (ADS)

Wu, Ya; Li, Junxia; Wang, Yanxin; Xie, Xianjun

2018-04-01

Understanding uranium (U) mobility is vital to minimizing its concentrations in potential drinking water sources. In this study, we report spatial-seasonal variations in U speciation and concentrations in a multi-aquifer system under the impact of Sanggan River in Datong basin, northern China. Hydrochemical and H, O, Sr isotopic data, thermodynamic calculations, and geochemical modeling are used to investigate the mechanisms of surface water-groundwater mixing-induced mobilization and natural attenuation of U. In the study site, groundwater U concentrations are up to 30.2 μg/L, and exhibit strong spatial-seasonal variations that are related to pH and Eh values, as well as dissolved Ca2+, HCO3-, and Fe(III) concentrations. For the alkaline aquifers of this site (pH 7.02-8.44), U mobilization is due to the formation and desorption of Ca2UO2(CO3)30 and CaUO2(CO3)32- caused by groundwater Ca2+ elevation via mineral weathering and Na-Ca exchange, incorporated U(VI) release from calcite, and U(IV) oxidation by Fe(OH)3. U immobilization is linked to the adsorption of CaUO2(CO3)32- and UO2(CO3)34- shifted from Ca2UO2(CO3)30 because of HCO3- elevation and Ca2+ depletion, U(VI) co-precipitation with calcite, and U(VI) reduction by adsorbed Fe2+ and FeS. Those results are of great significance for the groundwater resource management of this and similar other surface water-groundwater interaction zones.

Investigating Uranium Concentrations in Groundwaters in the State of Idaho Using Kinetic Phosphorescence Analysis and Inductively Coupled Plasma Mass Spectrometry.

PubMed

Tkavadze, Levan; Dunker, Roy E; Brey, Richard R; Dudgeon, John

2016-11-01

The determination of uranium concentrations in natural water samples is of great interest due to the environmental consequences of this radionuclide. In this study, 380 groundwater samples from various locations within the state of Idaho were analyzed using two different techniques. The first method was Kinetic Phosphorescence Analysis (KPA), which gives the total uranium concentrations in water samples. The second analysis method was inductively coupled plasma mass spectrometry (ICP- MS). This method determines the total uranium concentration as well as the separate isotope concentrations of uranium. The U/U isotopic ratio was also measured for each sample to confirm that there was no depleted or enriched uranium present. The results were compared and mapped separately from each other. The study also found that in some areas of the state, natural uranium concentrations are relatively high.

Reconnaissance investigation of water quality, bottom sediment, and biota associated with irrigation drainage in Bowdoin National Wildlife Refuge and adjacent areas of the Milk River basin, northeastern Montana, 1986-87

USGS Publications Warehouse

Lambing, J.H.; Jones, W.E.; Sutphin, J.W.

1988-01-01

Concentrations of trace elements, radiochemicals, and pesticides in the Bowdoin National Wildlife Refuge lakes generally were not substantially larger than those in the water supplied from Dodson South Canal or in irrigation drainage. Concentrations of arsenic (47 micrograms/L), uranium (43 microg/L), and vanadium (51 microg/L) in Dry Lake Unit, and boron (1,000 microg/L) in Lake Bowdoin were notably larger than at other sites. Zinc concentrations in an irrigation drain (56 microg/L) and two shallow domestic wells (40 and 47 microg/L) were elevated relative to other sites. Concentrations of gross alpha radiation (64 picocuries/L) and gross beta radiation (71 picocuries/L) were elevated in Dry Lake Unit. Pesticides concentrations at all sites were 0.08 microg/L or less. Water use guidelines concentrations for boron, cadmium, uranium, zinc, and gross alpha radiation were slightly exceeded at several sites. In general, trace-constituent concentrations measured in the water do not indicate any potential toxicity problems in Bowdoin National Wildlife Refuge; however, highwater conditions in 1986 probably caused dilution of dissolved constituents compared to recent dry years. Trace element concentrations in bottom sediments of the refuge lakes were generally similar to background concentrations in the soils. The only exception was Dry Lake Unit, which had concentrations of chromium (99 micrograms/g), copper (37 microg/g), nickel (37 microg/g), vanadium (160 microg/g), and zinc (120 microg/g) that were about double the mean background concentrations. The maximum selenium concentration in bottom sediment was 0.6 microg/g. Pesticide concentrations in bottom sediments were less than analytical detection limits at all sites. With few exceptions, concentrations of trace elements and pesticides in biota generally were less than values known to produce harmful effects on growth or reproduction. (Lantz-PTT)

Water-quality characteristics in the Black Hills area, South Dakota

USGS Publications Warehouse

Williamson, Joyce E.; Carter, Janet M.

2001-01-01

This report summarizes the water-quality characteristics of ground-water and surface-water in the Black Hills area. Differences in groundwater quality by aquifer and differences in surfacewater quality by water source are presented. Ground-water characteristics are discussed individually for each of the major aquifers in the Black Hills area, referred to herein as the Precambrian, Deadwood, Madison, Minnelusa, Minnekahta, and Inyan Kara aquifers. Characteristics for minor aquifers also are discussed briefly. Surface-water characteristics are discussed for hydrogeologic settings including headwater springs, crystalline core sites, artesian springs, and exterior sites. To characterize the water quality of aquifers and streams in the Black Hills area, data from the U.S. Geological Survey National Water Information System water-quality database were examined. This included samples collected as part of the Black Hills Hydrology Study as well as for other studies within the time frame of October 1, 1930, to September 30, 1998. Tables of individual results are not presented in this report, only summaries. Constituents summarized and discussed include physical properties, common ions, nutrients, trace elements, and radionuclides. Comparisons of concentration levels are made to drinking-water standards as well as beneficial-use and aquatic-life criteria. Ground water within the Black Hills and surrounding area generally is fresh and hard to very hard. Concentrations exceeding various Secondary and Maximum Contaminant Levels may affect the use of the water in some areas for many aquifers within the study area. Concentrations that exceed Secondary Maximum Contaminant Levels (SMCL's) generally affect the water only aesthetically. Radionuclide concentrations may be especially high in some of the major aquifers used within the study area and preclude the use of water in some areas. The sodiumadsorption ratio and specific conductance may affect irrigation use for some wells. High concentrations of iron and manganese are the only concentrations that may hamper the use of water from Precambrian aquifers. The principal deterrents to use of water from the Deadwood aquifer are the high concentrations of radionuclides as well as iron and manganese. Iron, manganese, and hardness may deter use of water from the Madison aquifer as well as dissolved solids and sulfate in downgradient wells (generally deeper than 2,000 feet). Iron, manganese, and hardness may also deter use of the Minnelusa aquifer. Water from the Minnekahta aquifer generally is suitable for all water uses although it is hard to very hard. High concentrations of dissolved solids, iron, sulfate, and manganese may hamper the use of water from the Inyan Kara aquifer. In the southern Black Hills, radium-226 and uranium concentrations also may preclude use of water from the Inyan Kara aquifer. Suitability for irrigation may be affected by high specific conductance and sodium-adsorption ratio for the Inyan Kara. Surface-water quality within the Black Hills and surrounding area generally is very good but the water is hard to very hard. Concentrations of some constituents in the study area tend to be higher exterior to the Black Hills, primarily due to influences from the Cretaceous-age marine shales, including dissolved solids, sodium, sulfate, selenium, and uranium. Headwater springs have relatively constant discharge, specific conductance, dissolved solids, and concentrations of most other constituents. Concentrations at crystalline core sites are very similar to those found in samples from Precambrian aquifers. Some high nitrate concentrations greater than the Maximum Contaminant Level (MCL) of 10 mg/L (milligrams per liter) have occurred at Annie Creek near Lead, which have been attributed to mining impacts. Trace elements generally are low with the exception of arsenic, for which 60 percent of samples exceed the proposed MCL of 10 ug/L (micrograms per liter) and one sample

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.

Determining the release of radionuclides from tank waste residual solids. FY2015 report

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

King, William D.; Hobbs, David T.

Methodology development for pore water leaching studies has been continued to support Savannah River Site High Level Waste tank closure efforts. For FY2015, the primary goal of this testing was the achievement of target pH and Eh values for pore water solutions representative of local groundwater in the presence of grout or grout-representative (CaCO 3 or FeS) solids as well as waste surrogate solids representative of residual solids expected to be present in a closed tank. For oxidizing conditions representative of a closed tank after aging, a focus was placed on using solid phases believed to be controlling pH andmore » E h at equilibrium conditions. For three pore water conditions (shown below), the target pH values were achieved to within 0.5 pH units. Tank 18 residual surrogate solids leaching studies were conducted over an E h range of approximately 630 mV. Significantly higher Eh values were achieved for the oxidizing conditions (ORII and ORIII) than were previously observed. For the ORII condition, the target Eh value was nearly achieved (within 50 mV). However, E h values observed for the ORIII condition were approximately 160 mV less positive than the target. E h values observed for the RRII condition were approximately 370 mV less negative than the target. Achievement of more positive and more negative E h values is believed to require the addition of non-representative oxidants and reductants, respectively. Plutonium and uranium concentrations measured during Tank 18 residual surrogate solids leaching studies under these conditions (shown below) followed the general trends predicted for plutonium and uranium oxide phases, assuming equilibrium with dissolved oxygen. The highest plutonium and uranium concentrations were observed for the ORIII condition and the lowest concentrations were observed for the RRII condition. Based on these results, it is recommended that these test methodologies be used to conduct leaching studies with actual Tank 18 residual solids material. Actual waste testing will include leaching evaluations of technetium and neptunium, as well as plutonium and uranium.« less

[Uranium Concentration in Drinking Water from Small-scale Water Supplies in Schleswig-Holstein, Germany].

PubMed

Ostendorp, G

2015-04-01

In this study the drinking water of 212 small-scale water supplies, mainly situated in areas with intensive agriculture or fruit-growing, was analysed for uranium. The median uranium concentration amounted to 0.04 µg/lL, the 95(th) percentile was 2.5 µg/L. The maximum level was 14 µg/L. This sample exceeded the guideline value for uranium in drinking water. The uranium concentration in small-scale water supplies was found to be slightly higher than that in central water works in Schleswig-Holstein. Water containing more than 10 mg/L nitrate showed significantly higher uranium contents. The results indicate that the uranium burden in drinking water from small wells is mainly determined by geological factors. An additional anthropogenic effect of soil management cannot be excluded. Overall uranium concentrations were low and not causing health concerns. However, in specific cases higher concentrations may occur. © Georg Thieme Verlag KG Stuttgart · New York.

Bioreduction of U(VI) and stability of immobilized uranium under suboxic conditions.

PubMed

Hu, Nan; Ding, De-xin; Li, Shi-mi; Tan, Xiang; Li, Guang-yue; Wang, Yong-dong; Xu, Fei

2016-04-01

In order to study the bioreduction of U(VI) and stability of immobilized uranium under suboxic conditions, microcosm were amended with ethanol, lactate and glucose, and incubated under suboxic conditions. During the incubation, total dissolved U in amended microcosms decreased from 0.95 mg/L to 0.03 mg/L. Pyrosequencing results showed that, the proportion of anaerobic microorganisms capable of reducing U(VI) under suboxic conditions was small compared with that under anoxic conditions; the proportion of aerobic and facultative anaerobic microorganisms capable of consuming the dissolved oxygen was large; and some of the facultative anaerobic microorganisms could reduce U(VI). These results indicated that different microbial communities were responsible for the bioreduction of U(VI) under suboxic and anoxic conditions. After the electron donors were exhausted, total dissolved U in the amended microcosms remained unchanged, while the U(VI)/U(IV) ratio in the solid phase of sediments increased obviously. This implied that the performance of bioreduction of the U(VI) can be maintained under suboxic condition. Copyright © 2016 Elsevier Ltd. All rights reserved.

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.

SEPARATION PROCESS FOR THORIUM SALTS

DOEpatents

Bridger, G.L.; Whatley, M.E.; Shaw, K.G.

1957-12-01

A process is described for the separation of uranium, thorium, and rare earths extracted from monazite by digesting with sulfuric acid. By carefully increasing the pH of the solution, stepwise, over the range 0.8 to 5.5, a series of selective precipitations will be achieved, with the thorium values coming out at lower pH, the rare earths at intermediate pH and the uranium last. Some mixed precipitates will be obtained, and these may be treated by dissolving in HNO/sub 3/ and contacting with dibutyl phosphate, whereby thorium or uranium are taken up by the organic phase while the rare earths preferentially remain in the aqueous solution.

Naturally occurring contaminants in the Piedmont and Blue Ridge crystalline-rock aquifers and Piedmont Early Mesozoic basin siliciclastic-rock aquifers, eastern United States, 1994–2008

USGS Publications Warehouse

Chapman, Melinda J.; Cravotta, Charles A.; Szabo, Zoltan; Lindsay, Bruce D.

2013-01-01

Groundwater quality and aquifer lithologies in the Piedmont and Blue Ridge Physiographic Provinces in the eastern United States vary widely as a result of complex geologic history. Bedrock composition (mineralogy) and geochemical conditions in the aquifer directly affect the occurrence (presence in rock and groundwater) and distribution (concentration and mobility) of potential naturally occurring contaminants, such as arsenic and radionuclides, in drinking water. To evaluate potential relations between aquifer lithology and the spatial distribution of naturally occurring contaminants, the crystalline-rock aquifers of the Piedmont and Blue Ridge Physiographic Provinces and the siliciclastic-rock aquifers of the Early Mesozoic basin of the Piedmont Physiographic Province were divided into 14 lithologic groups, each having from 1 to 16 lithochemical subgroups, based on primary rock type, mineralogy, and weathering potential. Groundwater-quality data collected by the U.S. Geological Survey (USGS) National Water-Quality Assessment (NAWQA) Program from 1994 through 2008 from 346 wells and springs in various hydrogeologic and land-use settings from Georgia through New Jersey were compiled and analyzed for this study. Analyses for most constituents were for filtered samples, and, thus, the compiled data consist largely of dissolved concentrations. Concentrations were compared to criteria for protection of human health, such as U.S. Environmental Protection Agency (USEPA) drinking water maximum contaminant levels and secondary maximum contaminant levels or health-based screening levels developed by the USGS NAWQA Program in cooperation with the USEPA, the New Jersey Department of Environmental Protection, and Oregon Health & Science University. Correlations among constituent concentrations, pH, and oxidation-reduction (redox) conditions were used to infer geochemical controls on constituent mobility within the aquifers. Of the 23 trace-element constituents evaluated, arsenic, manganese, and zinc were detected in one or more water samples at concentrations greater than established human health-based criteria. Arsenic concentrations typically were less than 1 microgram per liter (µg/L) in most groundwater samples; however, concentrations of arsenic greater than 1 µg/L frequently were detected in groundwater from clastic lacustrine sedimentary rocks of the Early Mesozoic basin aquifers and from metamorphosed clastic sedimentary rocks of the Piedmont and Blue Ridge crystalline rock aquifers. Groundwater from these rock units had elevated pH compared to other rock units evaluated in this study. Of the nine samples for which arsenic concentration was greater than 10 µg/L, six were classified as oxic and three as anoxic, and seven had pH of 7.2 or greater. Manganese concentrations typically were less than 10 µg/L in most samples; however, 8.3 percent of samples from the Piedmont and Blue Ridge crystalline-rock aquifers and 3.0 percent of samples from the Early Mesozoic basin siliciclastic rock aquifers had manganese concentrations greater than the 300-µg/L health-based screening level. The positive correlation of manganese with iron and ammonia and the negative correlation of manganese with dissolved oxygen and nitrate are consistent with the reductive dissolution of manganese oxides in the aquifer. Zinc concentrations typically were less than 10 µg/L in the groundwater samples considered in the study, but 0.4 percent and 5.5 percent of the samples had concentrations greater than the health-based screening level of 2,000 µg/L and one-tenth of the health-based screening level, respectively. The mean rank concentration of zinc in groundwater from the quartz-rich sedimentary rock lithologic group was greater than that for other lithologic groups even after eliminating samples collected from wells constructed with galvanized casing. Approximately 90 percent of 275 groundwater samples had radon-222 concentrations that were greater than the proposed alternative maximum contaminant level of 300 picocuries per liter. In contrast, only 2.0 percent of 98 samples had combined radium (radium-226 plus radium-228) concentrations greater than the maximum contaminant level of 5.0 picocuries per liter, and 0.6 percent of 310 samples had uranium concentrations greater than the maximum contaminant level of 30 µg/L. Radon concentrations were highest in the Piedmont and Blue Ridge crystalline-rock aquifers, especially in granite, and elevated median concentrations were noted in the Piedmont Early Mesozoic basin aquifers, but without the extreme maximum concentrations found in the crystalline rocks (granites). Although the siliciclastic lithologies had a greater frequency of elevated uranium concentrations, radon and radium were commonly detected in water from both siliciclastic and crystalline lithologies. Uranium concentrations in groundwater from clastic sedimentary and clastic lacustrine/evaporite sedimentary lithologic groups within the Early Mesozoic basin aquifers, which had median concentrations of 3.6 and 3.1 µg/L, respectively, generally were higher than concentrations for other siliciclastic lithologic groups, which had median concentrations less than 1 µg/L. Although 89 percent of the 260 samples from crystalline-rock aquifers had uranium concentrations less than 1 µg/L, 0.8 percent had uranium concentrations greater than the 30-µg/L maximum contaminant level, and 6.5 percent had concentrations greater than 3 µg/L.

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.

Microbial communities associated with uranium in-situ recovery mining process are related to acid mine drainage assemblages.

PubMed

Coral, Thomas; Descostes, Michaël; De Boissezon, Hélène; Bernier-Latmani, Rizlan; de Alencastro, Luiz Felippe; Rossi, Pierre

2018-07-01

A large fraction (47%) of the world's uranium is mined by a technique called "In Situ Recovery" (ISR). This mining technique involves the injection of a leaching fluid (acidic or alkaline) into a uranium-bearing aquifer and the pumping of the resulting solution through cation exchange columns for the recovery of dissolved uranium. The present study reports the in-depth alterations brought to autochthonous microbial communities during acidic ISR activities. Water samples were collected from a uranium roll-front deposit that is part of an ISR mine in operation (Tortkuduk, Kazakhstan). Water samples were obtained at a depth of ca 500 m below ground level from several zones of the Uyuk aquifer following the natural redox zonation inherited from the roll front deposit, including the native mineralized orebody and both upstream and downstream adjacent locations. Samples were collected equally from both the entrance and the exit of the uranium concentration plant. Next-generation sequencing data showed that the redox gradient shaped the community structures, within the anaerobic, reduced, and oligotrophic habitats of the native aquifer zones. Acid injection induced drastic changes in the structures of these communities, with a large decrease in both cell numbers and diversity. Communities present in the acidified (pH values < 2) mining areas exhibited similarities to those present in acid mine drainage, with the dominance of Sulfobacillus sp., Leptospirillum sp. and Acidithiobacillus sp., as well as the archaean Ferroplasma sp. Communities located up- and downstream of the mineralized zone under ISR and affected by acidic fluids were blended with additional facultative anaerobic and acidophilic microorganisms. These mixed biomes may be suitable communities for the natural attenuation of ISR mining-affected subsurface through the reduction of metals and sulfate. Assessing the effect of acidification on the microbial community is critical to evaluating the potential for natural attenuation or active bioremediation strategies. Copyright © 2018 Elsevier B.V. All rights reserved.

Dissolved molybdenum and uranium in the Three Rivers of eastern Tibet

NASA Astrophysics Data System (ADS)

Noh, H.; Huh, Y.

2006-12-01

Three large rivers - the Chang Jiang (Yangtze), Mekong (Lancang Jiang) and Salween (Nu Jiang) - originate in eastern Tibet and run in close parallel over 300 km near the eastern Himalayan syntaxis. They flow across suture zones and faults generated by the collision of India and Eurasia. Sixty-five water samples were collected in summer of 1999 to 2004 and nine in winter of 2002 to 2003. The complex geologic makeup of the Three Rivers region (TRR) results in widely varying major and trace element compositions of the dissolved load. Two redox-sensitive elements, molybdenum (Mo) and uranium (U) were analyzed by ICP-MS, as potential proxies for weathering of sedimentary organic carbon and resultant generation of atmospheric carbon dioxide. Additionally, Mo constitutes an essential co-enzyme for biology. Mo concentration ranges from 0.76 to 21.3 nmol/kg (average: 6.24 nmol/kg, average of global rivers: ~5 nmol/kg (Martin and Meybeck, 1979)), and U concentration varies from 2.86 to 10.7 nmol/kg (average: 3.12 nmol/kg, average of global rivers: ~1 nmol/kg (Palmer and Edmond, 1993)). The highest values of Mo and U are observed in the headwater tributary sample of the Chang Jiang, where evaporite dissolution is dominant. Statistical analyses show that Mo is closely correlated with U (r = 0.713, p < 0.01) indicating similar source of Mo and U to river waters in the TRR. Inverse correlation with Si/total anions ratio suggests that their sources are non-silicate minerals. The correlation with sulfate supports the use Mo and U as proxies for weathering of reduced organic-rich sediments (Mo and SO4: r = 0.383, p < 0.01; U and SO4: r = 0.508, p < 0.01). Among the parameters tested (basin area, elevation, relief, slope, T, precipitation, potential-evapotranspiration, normalized difference vegetation index (NDVI), population density), best positive correlation (r>0.5) is shown between U and basin elevation, and negative correlation is shown between U and temperature, precipitation and potential- evapotranspiration. Martin J.-M. and Meybeck M. (1979) Elemental mass-balance of material carried by major world rivers. Mar. Chem. 7, 173-206. Palmer M. R. and Edmond J. M. (1993) Uranium in river water. Geochim. Cosmochim. Acta 57, 4947-4955.

In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions.

PubMed

Paradis, Charles J; Jagadamma, Sindhu; Watson, David B; McKay, Larry D; Hazen, Terry C; Park, Melora; Istok, Jonathan D

2016-04-01

Reoxidation and mobilization of previously reduced and immobilized uranium by dissolved-phase oxidants poses a significant challenge for remediating uranium-contaminated groundwater. Preferential oxidation of reduced sulfur-bearing species, as opposed to reduced uranium-bearing species, has been demonstrated to limit the mobility of uranium at the laboratory scale yet field-scale investigations are lacking. In this study, the mobility of uranium in the presence of nitrate oxidant was investigated in a shallow groundwater system after establishing conditions conducive to uranium reduction and the formation of reduced sulfur-bearing species. A series of three injections of groundwater (200 L) containing U(VI) (5 μM) and amended with ethanol (40 mM) and sulfate (20 mM) were conducted in ten test wells in order to stimulate microbial-mediated reduction of uranium and the formation of reduced sulfur-bearing species. Simultaneous push-pull tests were then conducted in triplicate well clusters to investigate the mobility of U(VI) under three conditions: 1) high nitrate (120 mM), 2) high nitrate (120 mM) with ethanol (30 mM), and 3) low nitrate (2 mM) with ethanol (30 mM). Dilution-adjusted breakthrough curves of ethanol, nitrate, nitrite, sulfate, and U(VI) suggested that nitrate reduction was predominantly coupled to the oxidation of reduced-sulfur bearing species, as opposed to the reoxidation of U(IV), under all three conditions for the duration of the 36-day tests. The amount of sulfate, but not U(VI), recovered during the push-pull tests was substantially more than injected, relative to bromide tracer, under all three conditions and further suggested that reduced sulfur-bearing species were preferentially oxidized under nitrate-reducing conditions. However, some reoxidation of U(IV) was observed under nitrate-reducing conditions and in the absence of detectable nitrate and/or nitrite. This suggested that reduced sulfur-bearing species may not be fully effective at limiting the mobility of uranium in the presence of dissolved and/or solid-phase oxidants. The results of this field study confirmed those of previous laboratory studies which suggested that reoxidation of uranium under nitrate-reducing conditions can be substantially limited by preferential oxidation of reduced sulfur-bearing species. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions

DOE PAGES

Paradis, Charles J.; Jagadamma, Sindhu; Watson, David B.; ...

2016-02-11

Reoxidation and mobilization of previously reduced and immobilized uranium by dissolved phase oxidants poses a significant challenge for remediating uranium-contaminated groundwater. Preferential oxidation of reduced sulfur-bearing species, as opposed to reduced uranium bearing species, has been demonstrated to limit the mobility of uranium at the laboratory scale yet field-scale investigations are lacking. Here in this study, the mobility of uranium in the presence of nitrate oxidant was investigated in a shallow groundwater system after establishing conditions conducive to uranium reduction and the formation of reduced sulfur-bearing species. A series of three injections of groundwater (200 L) containing U(VI) (5 μM)more » and amended with ethanol (40 mM) and sulfate (20 mM) were conducted in ten test wells in order to stimulate microbial mediated reduction of uranium and the formation of reduced sulfur-bearing species. Simultaneous push-pull tests were then conducted in triplicate well clusters to investigate the mobility of U(VI) under three conditions: 1) high nitrate (120 mM), 2) high nitrate (120 mM) with ethanol (30 mM), and 3) low nitrate (2 mM) with ethanol (30 mM). Dilution-adjusted breakthrough curves of ethanol, nitrate, nitrite, sulfate, and U(VI) suggested that nitrate reduction was predominantly coupled to the oxidation of reduced-sulfur bearing species, as opposed to the reoxidation of U(IV), under all three conditions for the duration of the 36-day tests. The amount of sulfate, but not U(VI), recovered during the push-pull tests was substantially more than injected, relative to bromide tracer, under all three conditions and further suggested that reduced sulfur-bearing species were preferentially oxidized under nitrate-reducing conditions. However, some reoxidation of U(IV) was observed under nitrate-reducing conditions and in the absence of detectable nitrate and/or nitrite. This suggested that reduced sulfur-bearing species may not be fully effective at limiting the mobility of uranium in the presence of dissolved and/or solid-phase oxidants. Lastly, the results of this field study confirmed those of previous laboratory studies which suggested that reoxidation of uranium under nitrate-reducing conditions can be substantially limited by preferential oxidation of reduced sulfur-bearing species.« less

Uranium and radium concentrations in plants growing on uranium mill tailings in South Dakota

Treesearch

Mark A. Rumble; Ardell J. Bjugstad

1986-01-01

Vegetation and soil samples were collected from a uranium mill tailings site and control sites in South Dakota. Uranium concentrations in soils from the mill tailings averaged 13.3 [micro]g g-1 compared to 5.1 [micro]g g-1 in soils from control sites. 226Ra concentrations in soils averaged 111.0 pCi g...

Progress in Chile in the development of the fission {sup 99}Mo production using modified CINTICHEM

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

Schrader, R.; Klein, J.; Medel, J.

2008-07-15

Fission {sup 99}Mo will be produced in Chile irradiating low-enriched uranium (LEU) foil in a MTR research reactor. For the purpose of developing the capability to fabricate the target, which is done of uranium foil enclosed in swaged concentric aluminum tubes, dummy targets are being fabricated using 130 {mu}m copper foil instead of the uranium foil, wrapped in a 14{mu}m nickel fission-recoil barrier. Dummy targets using several dimensions of copper foil have been assembled; however, the emphasis is being set in targets fabricated using the dimensions of the LEU foil that KAERI will provide, i.e. 50 mm x 100mm xmore » 0.130 mm. The assembling of target using the last dimensions has not been free of difficulties. Neutronic calculations and preliminary thermal and fluid analyses were performed to estimate the fission products activity and the heat removal capability for a 13 grams LEU-foil annular target, which will be irradiated in the RECH-1 research reactor at the level power of 5 MW during 48 hours. In a fume hood, Cintichem processing of natural uranium shavings with the addition of different carriers were performed, obtaining recovery over 90% of the added Mo carrier. Expertise has been gained in (a) foil dissolution process in a dissolver locally designed, (b) in Mo precipitation process, and (c) preparation of the purification columns with AgC, C and HZrO. Additionally, the irradiated target cutting machine with an innovative design was finally assembled. (author)« less

Elevated Uranium in Aquifers of the Jacobsville Sandstone

NASA Astrophysics Data System (ADS)

Sherman, H.; Gierke, J.

2003-12-01

The EPA has announced a new standard for uranium in drinking water of 30 parts per billion (ppb). This maximum contaminant level (MCL) takes effect for community water supplies December 2003. The EPA's ruling has heightened awareness among residential well owners that uranium in drinking water may increase the risk of kidney disease and cancer and has created a need for a quantified, scientific understanding of the occurrence and distribution of uranium isotopes in aquifers. The authors are investigating the occurrence of elevated uranium in northern Michigan aquifers of the Middle Proterozoic Jacobsville sandstone, a red to mottled sequence of sandstones, conglomerates, siltstones and shales deposited as basin fill in the 1.1 Ga Midcontinent rift. Approximately 25% of 300 well water samples tested for isotopic uranium have concentrations above the MCL. Elevated uranium occurrences are distributed throughout the Jacobsville sandstone aquifers stretching across Michigan's Upper Peninsula. However, there is significant variation in well water uranium concentrations (from 0.01 to 190 ppb) and neighboring wells do not necessarily have similar concentrations. The authors are investigating hydrogeologic controls on ground water uranium concentrations in the Jacobsville sandstone, e.g. variations in lithology, mineralogy, groundwater residence time and geochemistry. Approximately 2000' of Jacobsville core from the Amoco St. Amour well was examined in conjunction with the spectral gamma ray log run in the borehole. Spikes in equivalent uranium (eU) concentration from the log are frequently associated with clay and heavy mineral layers in the sandstone core. The lithology and mineralogy of these layers will be determined by analysis of thin sections and x-ray diffraction. A portable spectrometer, model GRS-2000/BL, will be used on the sandstone cliffs along Lake Superior to characterize depositional and lithologic facies of the Jacobsville sandstone in terms of concentrations and ratios of eU, eTh and K. Equipped with borehole accessories, the spectrometer will be used to log residential drinking wells to determine a relationship between the uranium concentration of well water and the eU concentration in the sandstone. Tritium/helium-3 dating will be used to determine whether ground water uranium concentrations increase with residence time. PHREEQCI will be used to model dominate aqueous species of uranium and saturation indices of uranium minerals.

Selected chemical analyses of water from formations of Mesozoic and Paleozoic age in parts of Oklahoma, northern Texas, and Union County, New Mexico

USGS Publications Warehouse

Parkhurst, R.S.; Christenson, S.C.

1987-01-01

Hydrochemical data were compiled into a data base as part of the Central Midwest Regional Aquifer System Analysis project. The data consist of chemical analyses of water samples collected from wells that are completed in formations of Mesozoic and Paleozoic age. The data base includes data from the National Water Data Storage and Retrieval System, the Petroleum Data System, the National Uranium Resource Evaluation, and selected publications. Chemical analyses were selected for inclusion within the hydrochemical data base if the total concentration of the cations differed from the total 10 percent or less of the total concentration of all ions. Those analyses which lacked the necessary data for an ionic balance were included if the ratios of dissolved-solids concentration to specific conductance were between 0.55 and 0.75. The tabulated chemical analyses, grouped by county, and a statistical summary of the analyses, listed by geologic unit, are presented.

Uranium hexafluoride public risk

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

Fisher, D.R.; Hui, T.E.; Yurconic, M.

1994-08-01

The limiting value for uranium toxicity in a human being should be based on the concentration of uranium (U) in the kidneys. The threshold for nephrotoxicity appears to lie very near 3 {mu}g U per gram kidney tissue. There does not appear to be strong scientific support for any other improved estimate, either higher or lower than this, of the threshold for uranium nephrotoxicity in a human being. The value 3 {mu}g U per gram kidney is the concentration that results from a single intake of about 30 mg soluble uranium by inhalation (assuming the metabolism of a standard person).more » The concentration of uranium continues to increase in the kidneys after long-term, continuous (or chronic) exposure. After chronic intakes of soluble uranium by workers at the rate of 10 mg U per week, the concentration of uranium in the kidneys approaches and may even exceed the nephrotoxic limit of 3 {mu}g U per gram kidney tissue. Precise values of the kidney concentration depend on the biokinetic model and model parameters assumed for such a calculation. Since it is possible for the concentration of uranium in the kidneys to exceed 3 {mu}g per gram tissue at an intake rate of 10 mg U per week over long periods of time, we believe that the kidneys are protected from injury when intakes of soluble uranium at the rate of 10 mg U per week do not continue for more than two consecutive weeks. For long-term, continuous occupational exposure to low-level, soluble uranium, we recommend a reduced weekly intake limit of 5 mg uranium to prevent nephrotoxicity in workers. Our analysis shows that the nephrotoxic limit of 3 {mu}g U per gram kidney tissues is not exceeded after long-term, continuous uranium intake at the intake rate of 5 mg soluble uranium per week.« less

Investigation of uranium geochemistry along groundwater flow path in the Continental Intercalaire aquifer (Southern Tunisia).

PubMed

Dhaoui, Z; Chkir, N; Zouari, K; Ammar, F Hadj; Agoune, A

2016-06-01

Environmental tracers ((2)H, (18)O, isotopes of Uranium) and geochemical processes occurring within groundwaters from the Continental Intercalaire (CI) in Southern Tunisia were used to understand the hydrodynamics and the recharge conditions of this aquifer. This study investigates the chemical and isotopic compositions of the CI groundwater. The water types are dominated by Na(+), SO4(2-), Cl(-) throughout most of the basin with a general increase in total dissolved solids from the Saharan Platform margins towards the Chotts region. Large scale groundwater flow paths are toward the Chotts region. The stable isotopes composition of the analyzed groundwater ranges from -8.8 to -6‰ vs V-SMOW for δ(18)O and from -67 to -40‰ vs V-SMOW for δ(2)H. The relatively enriched stable isotopes contents suggest the contribution of the Dahar sandstones outcrops in the current recharge of the CI aquifer in an arid context. However, the most depleted values in heavy isotopes indicate a paleorecharge of the aquifer under wetter conditions revealing a long residence time of groundwaters. The results from water samples using alpha spectrometry method indicate a range in (238)U concentrations and (234)U/(238)U activity ratios (AR) of 0.044-1.285 μg kg(-1) and 1.2 to 8.84 respectively. The geochemistry of uranium isotopes in groundwater is controlled by many factors, essentially, the influence of water rock interactions, the preferential dissolution of (234)U relative to (238)U due to alpha recoil and the mixing processes between different waters with distinct AR as well as (238)U concentrations. Copyright © 2016 Elsevier Ltd. All rights reserved.

Purification of uranium alloys by differential solubility of oxides and production of purified fuel precursors

DOEpatents

McLean, II, William; Miller, Philip E.

1997-01-01

A method for purifying metallic alloys of uranium for use as nuclear reactor fuels in which the metal alloy is first converted to an oxide and then dissolved in nitric acid. Initial removal of metal oxide impurities not soluble in nitric acid is accomplished by filtration or other physical means. Further purification can be accomplished by carbonate leaching of uranyl ions from the partially purified solution or using traditional methods such as solvent extraction.

Purification of uranium alloys by differential solubility of oxides and production of purified fuel precursors

DOEpatents

McLean, W. II; Miller, P.E.

1997-12-16

A method is described for purifying metallic alloys of uranium for use as nuclear reactor fuels in which the metal alloy is first converted to an oxide and then dissolved in nitric acid. Initial removal of metal oxide impurities not soluble in nitric acid is accomplished by filtration or other physical means. Further purification can be accomplished by carbonate leaching of uranyl ions from the partially purified solution or using traditional methods such as solvent extraction. 3 figs.

Radionuclide tracers of sediment-water interactions on the Amazon shelf

NASA Astrophysics Data System (ADS)

Moore, Willard S.; DeMaster, David J.; Smoak, Joseph M.; McKee, Brent A.; Swarzenski, Peter W.

1996-04-01

A comprehensive study of a variety of radionuclide tracers has been coupled with other geochemical investigations and with sedimentary and physical oceanographic measurements to elucidate processes and their characteristic time scales at the mouth of the Amazon River. This two-year field study on the Amazon continental shelf involved four cruises designed to provide information during different stages of the river hydrograph. Although the cruises were coordinated with river stage, other physical variables including spring-neap tidal stages, the flow of the North Brazil Current and trade-wind stress caused important effects on the shelf environment. Partitioning of uranium among dissolved, colloidal and particulate phases was investigated during AmasSeds. A detailed examination of uranium water-column behavior during low river discharge found that most (89%) of the uranium near the Amazon River mouth was associated with the particulate phase and that most (92%) of the riverine dissolved-phase uranium was in the colloidal size fraction (0.001-0.4 μm). A non-conservative uranium/salinity distribution was observed for dissolved uranium, indicating large-scale uranium removal from surface waters with salinities less than 20 ppt. Colloidal uranium was non-conservative across the entire salinity regime, exhibiting removal of colloidal uranium from waters with salinities less than 12 ppt and a significant input at higher salinities. A short-lived particle-reactive tracer, 234Th, was used to evaluate the rates of particle scavenging on the shelf. Suspended-sediment concentrations respond to each turn of the tide, thus limiting the time available for equilibrium to be established between the particles and the tracers. Experiments demonstrated that on the Amazon shelf the partitioning and distribution of trace elements are governed by particle dynamics (particle residence times < sorption times). The high suspended load, including fluid muds, retards the incorporation of adsorbed 234Th into the seabed. Once scavenged, 234Th remains part of the suspended-sediment and fluid-mud inventory for periods of at least 4-8 weeks. Another particle-reactive tracer, 210Pb, was used to evaluate the potential supply of reactive metals from offshore waters to the shelf. As open-ocean waters move into the Amazon mixing zone, in response to the estuarine-like circulation, they lose 210Ph through scavenging processes associated with delta formation. This oceanic input of 210Pb dominates other inputs to the Amazon shelf system. Based on 210Pb analyses from more than 40 ☐ and kasten cores, the flux of water moving shoreward and depositing 210Pb in the sediments was calculated to be on the order of 6 × 10 161y -1 ˜10 times the riverine flux from the Amazon. The distribution of 210Pb in the sediments suggests that if particle-reactive species (such as certain trace metals) are released in dissolved form on the shelf, they will be scavenged quickly in this turbid environment, with the largest inventories occurring in the foreset beds (although the highest concentrations occur in the bottomset beds). The large landward flow of water indicates that if particle-reactive species are released in the western equatorial Atlantic via aerosol transport or other mechanisms, there is a good chance that a sizeable portion will be buried in the Amazon delta. Fluxes of radium isotopes, 226Ra, 228Ra and 224Ra, from the bottom sediments were used to evaluate sediment resuspension across the shelf. The average flux of 226Ra from the Amazon shelf balanced the annual desorption of 226Ra from river-derived sediments; however, departures between the 226Ra flux and sediment necessary to support the flux occurred for different sampling periods. During falling and low discharge, less sediment entered the system than was required to support the sedimentary desorption 226Ra flux. During rising and high discharge, more sediment entered than was necessary to sustain the 226Ra flux. Considerable recycling of particles between the seabed and water column was required to wash away most of the desorbable 226Ra from the sediment. To support the sedimentary 228Ra flux, 3.4 × 10 16 g of sediment must be resuspended each year. Such mixing would resuspend the top 35 em of sediment over the entire shelf each year, or mix the surface layer (SL, the region of uniform sedimentary 210Pb depth profiles) to a depth of 90 cm annually. Such mixing would turn over the entire SL every 1-2 years. Desorption of sedimentary radium isotopes must be accompanied by the desorption of other exchangeable species including phosphate, cesium and cadmium. Correlations among phosphate and radium isotopes, infer that phosphate is being released from bottom sediments as the sediments are resuspended into the water column. As was the case for 226Ra, bottom sediment must be repeatedly suspended into the water column to release all of the exchangeable phosphate. The desorption of 224Ra from shelf sediments provides a tracer of the Amazon plume into the Atlantic. In July and September 1989, the ship crossed the Demerara retroflection 380 km from the Amazon shelf and excess 224Ra activities up to 8 dpm 100 kg -1 were measured. It was concluded that these waters were <5 days removed from the Amazon shelf. A sustained current of >80 em s -1 would be required to advect the water this distance in <5 days, an observation that agrees well with drogue releases during August 1989.

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

Morgan, T.L.; George, W.E.; Hensley, W.K.

As part of the Hydrogeochemical and Stream Sediment Reconnaissance (HSSR) of the National Uranium Resource Evaluation (NURE) sponsored by the US Department of Energy (DOE), the Los Alamos Scientific Laboratory (LASL) conducted a detailed hydrogeochemical survey of well waters in a 4250-km/sup 2/ area near Pie Town in west-central New Mexico. A total of 300 well samples was collected and analyzed for uranium and 23 other elements. The results of these analyses and carbonate and bicarbonate ion concentrations are presented in the Appendixes of this report. Uranium concentrations range from below the detection limit of 0.02 parts per billion (ppB)more » to 293.18 ppB and average 8.71 ppB. Samples containing high levels of uranium were collected from the Largo Creek valley west of Quemado, from a small area about 6 km east of Quemado, from a small area surrounding Pie Town, and from scattered locations in the area surrounding Adams Diggings north of Pie Town. Most of the samples containing high uranium concentrations were collected from wells associated with the volcanic sedimentary facies of the Datil formation. This formation is a likely source of mobile uranium that may be precipitating in the underlying Baca formation, a known uranium host unit. Bicarbonate ion concentration, while proportional to uranium concentration in some cases, is not a strong controlling factor in the uranium concentrations in samples from this area.« less

Impact of diatom growth on trace metal dynamics (Mn, Mo, V, U)

NASA Astrophysics Data System (ADS)

Osterholz, Helena; Simon, Heike; Beck, Melanie; Maerz, Joeran; Rackebrandt, Siri; Brumsack, Hans-Jürgen; Feudel, Ulrike; Simon, Meinhard

2014-03-01

In order to examine the specific role of diatoms in cycling of the trace metals manganese (Mn), molybdenum (Mo), vanadium (V), and uranium (U) Thalassiosira rotula, Skeletonema marinoi, Chaetoceros decipiens, and Rhizosolenia setigera were grown in batch cultures axenically and inoculated with three different bacterial strains isolated from the North Sea. Algal and bacterial growth, concentrations of trace metals and dissolved organic carbon (DOC) were monitored over time and showed that Mn and V were removed from the dissolved phase whereas Mo and U were not. R. setigera and T. rotula exhibited lowest growth and lowest removal whereas S. marinoi grew best and removed highest fractions of Mn and V. The high potential of Mn removal by S. marinoi was also evident from its 7 × higher Mn/P elemental ratio relative to T. rotula. The presence of bacteria modified the timing of the growth of S. marinoi but not directly trace metal removal whereas bacteria enhanced trace metal removal in the cultures of T. rotula and C. decipiens. Modeling of phytoplankton growth, concentrations of Mn and DOC fraction in axenic T. rotula cultures indicated that processes of binding and desorption of Mn to excreted organic components are important to explain the varying proportions of dissolved Mn and thus must be considered as an active component in Mn cycling. The results show distinct differences in the potential of the diatoms in the removal of Mn and V and that bacteria can play an active role in this context. S. marinoi presumably is an important player in Mn and V dynamics in coastal marine systems.

Room temperature electrodeposition of actinides from ionic solutions

DOEpatents

Hatchett, David W.; Czerwinski, Kenneth R.; Droessler, Janelle; Kinyanjui, John

2017-04-25

Uranic and transuranic metals and metal oxides are first dissolved in ozone compositions. The resulting solution in ozone can be further dissolved in ionic liquids to form a second solution. The metals in the second solution are then electrochemically deposited from the second solutions as room temperature ionic liquid (RTIL), tri-methyl-n-butyl ammonium n-bis(trifluoromethansulfonylimide) [Me.sub.3N.sup.nBu][TFSI] providing an alternative non-aqueous system for the extraction and reclamation of actinides from reprocessed fuel materials. Deposition of U metal is achieved using TFSI complexes of U(III) and U(IV) containing the anion common to the RTIL. TFSI complexes of uranium were produced to ensure solubility of the species in the ionic liquid. The methods provide a first measure of the thermodynamic properties of U metal deposition using Uranium complexes with different oxidation states from RTIL solution at room temperature.

Depleted uranium dust from fired munitions: physical, chemical and biological properties.

PubMed

Mitchel, R E J; Sunder, S

2004-07-01

This paper reports physical, chemical and biological analyses of samples of dust resulting from munitions containing depleted uranium (DU) that had been live-fired and had impacted an armored target. Mass spectroscopic analysis indicated that the average atom% of U was 0.198 +/- 0.10, consistent with depleted uranium. Other major elements present were iron, aluminum, and silicon. About 47% of the total mass was particles with diameters <300 microm, of which about 14% was <10 microm. X-ray diffraction analysis indicated that the uranium was present in the sample as uranium oxides-mainly U3O7 (47%), U3O8 (44%) and UO2 (9%). Depleted uranium dust, instilled into the lungs or implanted into the muscle of rats, contained a rapidly soluble uranium component and a more slowly soluble uranium component. The fraction that underwent dissolution in 7 d declined exponentially with increasing initial burden. At the lower lung burdens tested (<15 microg DU dust/lung) about 14% of the uranium appeared in urine within 7 d. At the higher lung burdens tested (~80-200 microg DU dust/lung) about 5% of the DU appeared in urine within 7 d. In both cases about 50% of that total appeared in urine within the first day. DU implanted in muscle similarly showed that about half of the total excreted within 7 d appeared in the first day. At the lower muscle burdens tested (<15 microg DU dust/injection site) about 9% was solubilized within 7 d. At muscle burdens >35 microg DU dust/injection site about 2% appeared in urine within 7 d. Natural uranium (NU) ore dust was instilled into rat lungs for comparison. The fraction dissolving in lung showed a pattern of exponential decline with increasing initial burden similar to DU. However, the decline was less steep, with about 14% appearing in urine for lung burdens up to about 200 microg NU dust/lung and 5% at lung burdens >1,100 microg NU dust/lung. NU also showed both a fast and a more slowly dissolving component. At the higher lung burdens of both DU and NU that showed lowered urine excretion rates, histological evidence of kidney damage was seen. Kidney damage was not seen with the muscle burdens tested. DU dust produced kidney damage at lower lung burdens and lower urine uranium levels than NU dust, suggesting that other toxic metals in DU dust may contribute to the damage.

METHOD OF SEPARATION

DOEpatents

Boyd, G.E.

1958-08-26

A process is presented fer separating uranium, plutonium, and fission products ions from uranyl nitrate solutions having a pH value between 1 and 3 obtained by dissolving neutron irradiated uranium. The method consists in passing such solutions through a bed of cation exchange resin, which may be a sulfonated phenol formaidehyde type. Following the adsorption step the resin is first treated with a solution of 0.2M to 0.3M sulfuric acid to desorb the uranium. Fission product ions are then desorbed by treating the resin in phosphoric acid and 1M in nitric acid. Lastly, the plutonium may be desorbed by treating the resin with a solution approximately 0.8M in phosphoric acid and 1M in nitric acid.

An artificially constructed Syngonium podophyllum-Aspergillus niger combinate system for removal of uranium from wastewater.

PubMed

He, Jia-dong; Wang, Yong-dong; Hu, Nan; Ding, Dexin; Sun, Jing; Deng, Qin-wen; Li, Chang-wu; Xu, Fei

2015-12-01

Aspergillus niger was inoculated to the roots of five plants, and the Syngonium podophyllum-A. niger combinate system (SPANCS) was found to be the most effective in removing uranium from hydroponic liquid with initial uranium concentration of 5 mg L(-1). Furthermore, the hydroponic experiments on the removal of uranium from the hydroponic liquids with initial uranium concentrations of 0.5, 1.0, and 3.0 mg L(-1) by the SPANCS were conducted, the inhibitory effect of A. niger on the growth of S. podophyllum in the SPANCS was studied, the accumulation characteristics of uranium by S. podophyllum in the SPANCS were analyzed, and the Fourier transform infrared (FT-IR) and extended X-ray absorption fine structure (EXAFS) spectra were measured. The results show that the removal of uranium by the SPANCS from the hydroponic liquids with initial uranium concentrations of 0.5, 1.0, and 3.0 mg L(-1) reached 98.20, 97.90, and 98.50%, respectively, after 37 days of accumulation of uranium; that the uranium concentrations in the hydroponic liquids decreased to 0.009, 0.021, and 0.045 mg L(-1), respectively, which are lower than the stipulated concentration for discharge of 0.050 mg L(-1) by the People's Republic of China; that A. niger helped to generate more groups in the root of S. podophyllum which can improve the complexing capability of S. podophyllum for uranium; and that the uranium accumulated in the root of S. podophyllum was in the form of phosphate uranyl and carboxylic uranyl.

DISSOLUTION OF ZIRCONIUM AND ALLOYS THEREFOR

DOEpatents

Swanson, J.L.

1961-07-11

The dissolution of zirconium cladding in a water solution of ammonium fluoride and ammonium nitrate is described. The method finds particular utility in processing spent fuel elements for nuclear reactors. The zirconium cladding is first dissolved in a water solution of ammonium fluoride and ammonium nitrate; insoluble uranium and plutonium fiuorides formed by attack of the solvent on the fuel materiai of the fuel element are then separated from the solution, and the fuel materiai is dissolved in another solution.

Assessing colloid-bound metal export in response to short term changes in runoff from a forested catchment

NASA Astrophysics Data System (ADS)

Neubauer, E.; Kammer, F. v. d.; Knorr, K.-H.; Pfeiffer, S.; Reichert, M.; Hofmann, T.

2012-04-01

Soils can act as a source of metals and natural organic matter (NOM) in runoff from catchments. Amounts and intensity of rainfall may influence NOM export from catchments. The presence of NOM and other colloids in water may not only enhance metal export, but also significantly change metal speciation. In this study, we investigated the response of metal-colloid associations to short-term discharge variations in the runoff from a small forested catchment (Lehstenbach, Bavaria, Germany). Here, the discharge from the catchment outlet responds within hours to rain events. Near-surface flow in organic-rich layers and peat soils has been identified to increase dissolved organic carbon (DOC) concentrations during stormwater runoff. Flow Field-Flow Fractionation coupled to ICP-MS (FlowFFF-ICPMS) is a high-resolution size separation technique which was used for the detection and quantification of colloids and associated metals. Colloid-associated metals, dissolved metals and metals associated with low-molecular weight organic ligands were also separated by filtration (0.2 µm) and ultrafiltration (1000 g/mol MWCO). During baseflow DOC concentration was <6 mg/L and the pH ranged between 4.6 and 5.0. The DOC concentration exported at a given discharge was subject to strong seasonal variation and depended on the water level before the discharge event. DOC concentrations were up to 8 fold higher during stormwater runoff compared to baseflow. The export of aluminum, arsenic, rare earth elements (REE) and uranium from the catchment increased during stormwater runoff showing a strong correlation with NOM concentrations. This result was supported by FlowFFF-ICPMS data revealing that NOM was the only colloid type available for metal complexation during all hydrological conditions. A clear temporal pattern in the association with the NOM was observed for most of the metals under study: During baseflow, 70-100% (Fe), 90% (Al), 60-100% (REE) and 80-85% (U) were associated with the NOM. During stormwater runoff, the dissolved species concentration and those associated with small organic ligands (<1000 g/mol) increased. The pH drop during the stormwater runoff (pH <4) is most likely the main factor for weaker metal-NOM binding. However, only 25 to 50% of the arsenic was associated with NOM, but no relation to discharge, or pH was exhibited. The results show that fluxes of most trace metals from the catchment are governed by NOM-colloids, even though substantial concentrations are dissolved or associated to low-molecular weight organic substances during stormwater runoff.

Selective Extraction of Uranium from Liquid or Supercritical Carbon Dioxide

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

Farawila, Anne F.; O'Hara, Matthew J.; Wai, Chien M.

2012-07-31

Current liquid-liquid extraction processes used in recycling irradiated nuclear fuel rely on (1) strong nitric acid to dissolve uranium oxide fuel, and (2) the use of aliphatic hydrocarbons as a diluent in formulating the solvent used to extract uranium. The nitric acid dissolution process is not selective. It dissolves virtually the entire fuel meat which complicates the uranium extraction process. In addition, a solvent washing process is used to remove TBP degradation products, which adds complexity to the recycling plant and increases the overall plant footprint and cost. A liquid or supercritical carbon dioxide (l/sc -CO2) system was designed tomore » mitigate these problems. Indeed, TBP nitric acid complexes are highly soluble in l/sc -CO2 and are capable of extracting uranium directly from UO2, UO3 and U3O8 powders. This eliminates the need for total acid dissolution of the irradiated fuel. Furthermore, since CO2 is easily recycled by evaporation at room temperature and pressure, it eliminates the complex solvent washing process. In this report, we demonstrate: (1) A reprocessing scheme starting with the selective extraction of uranium from solid uranium oxides into a TBP-HNO3 loaded Sc-CO2 phase, (2) Back extraction of uranium into an aqueous phase, and (3) Conversion of recovered purified uranium into uranium oxide. The purified uranium product from step 3 can be disposed of as low level waste, or mixed with enriched uranium for use in a reactor for another fuel cycle. After an introduction on the concept and properties of supercritical fluids, we first report the characterization of the different oxides used for this project. Our extraction system and our online monitoring capability using UV-Vis absorbance spectroscopy directly in sc-CO2 is then presented. Next, the uranium extraction efficiencies and kinetics is demonstrated for different oxides and under different physical and chemical conditions: l/sc -CO2 pressure and temperature, TBP/HNO3 complex used, reductant or complexant used for selectivity, and ionic liquids used as supportive media. To complete the extraction and recovery cycle, we then demonstrate uranium back extraction from the TBP loaded sc-CO2 phase into an aqueous phase and the characterization of the uranium complex formed at the end of this process. Another aspect of this project was to limit proliferation risks by either co-extracting uranium and plutonium, or by leaving plutonium behind by selectively extracting uranium. We report that the former is easily achieved, since plutonium is in the tetravalent or hexavalent oxidation state in the oxidizing environment created by the TBP-nitric acid complex, and is therefore co-extracted. The latter is more challenging, as a reductant or complexant to plutonium has to be used to selectively extract uranium. After undertaking experiments on different reducing or complexing systems (e.g., AcetoHydroxamic Acid (AHA), Fe(II), ascorbic acid), oxalic acid was chosen as it can complex tetravalent actinides (Pu, Np, Th) in the aqueous phase while allowing the extraction of hexavalent uranium in the sc-CO2 phase. Finally, we show results using an alternative media to commonly used aqueous phases: ionic liquids. We show the dissolution of uranium in ionic liquids and its extraction using sc-CO2 with and without the presence of AHA. The possible separation of trivalent actinides from uranium is also demonstrated in ionic liquids using neodymium as a surrogate and diglycolamides as the extractant.« less

PREPARATION OF URANIUM HEXAFLUORIDE

DOEpatents

Lawroski, S.; Jonke, A.A.; Steunenberg, R.K.

1959-10-01

A process is described for preparing uranium hexafluoride from carbonate- leach uranium ore concentrate. The briquetted, crushed, and screened concentrate is reacted with hydrogen fluoride in a fluidized bed, and the uranium tetrafluoride formed is mixed with a solid diluent, such as calcium fluoride. This mixture is fluorinated with fluorine and an inert diluent gas, also in a fluidized bed, and the uranium hexafluoride obtained is finally purified by fractional distillation.

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.

Controlling intake of uranium in the workplace: Applications of biokinetic modeling and occupational monitoring data

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

Leggett, Richard Wayne; Eckerman, Keith F; McGinn, Wilson

2012-01-01

This report provides methods for interpreting and applying occupational uranium monitoring data. The methods are based on current international radiation protection guidance, current information on the chemical toxicity of uranium, and best available biokinetic models for uranium. Emphasis is on air monitoring data and three types of bioassay data: the concentration of uranium in urine; the concentration of uranium in feces; and the externally measured content of uranium in the chest. Primary Reference guidance levels for prevention of chemical effects and limitation of radiation effects are selected based on a review of current scientific data and regulatory principles for settingmore » standards. Generic investigation levels and immediate action levels are then defined in terms of these primary guidance levels. The generic investigation and immediate actions levels are stated in terms of radiation dose and concentration of uranium in the kidneys. These are not directly measurable quantities, but models can be used to relate the generic levels to the concentration of uranium in air, urine, or feces, or the total uranium activity in the chest. Default investigation and immediate action levels for uranium in air, urine, feces, and chest are recommended for situations in which there is little information on the form of uranium taken into the body. Methods are prescribed also for deriving case-specific investigation and immediate action levels for uranium in air, urine, feces, and chest when there is sufficient information on the form of uranium to narrow the range of predictions of accumulation of uranium in the main target organs for uranium: kidneys for chemical effects and lungs for radiological effects. In addition, methods for using the information herein for alternative guidance levels, different from the ones selected for this report, are described.« less

Concentrations and activity ratios of uranium isotopes in groundwater from Doñana National Park, South of Spain

NASA Astrophysics Data System (ADS)

Bolívar, J. P.; Olías, M.; González-García, F.; García-Tenorio, R.

2008-08-01

The levels and distribution of natural radionuclides in groundwaters from the unconfined Almonte-Marismas aquifer, upon which Doñana National Park is located, have been analysed. Most sampled points were multiple piezometers trying to study the vertical distribution of the hydrogeochemical characteristics in the aquifer. Temperature, pH, electrical conductivity, dissolved oxygen and redox potential were determined in the field. A large number of parameters, physico-chemical properties, major and minor ions, trace elements and natural radionuclides (U-isotopes, Th-isotopes, Ra-isotopes and 210Po), were also analysed. In the southern zone, where aeolian sands crop out, water composition is of the sodium chloride type, and the lower U-isotopes concentrations have been obtained. As water circulates through the aquifer, bicarbonate and calcium concentrations increase slightly, and higher radionuclides concentrations were measured. Finally, we have demonstrated that 234U/238U activity ratios can be used as markers of the type of groundwater and bedrock, as it has been the case for old waters with marine origin confined by a marsh in the south-east part of aquifer.

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.

URANIUM RECOVERY PROCESS

DOEpatents

Hyman, H.H.; Dreher, J.L.

1959-07-01

The recovery of uranium from the acidic aqueous metal waste solutions resulting from the bismuth phosphate carrier precipitation of plutonium from solutions of neutron irradiated uranium is described. The waste solutions consist of phosphoric acid, sulfuric acid, and uranium as a uranyl salt, together with salts of the fission products normally associated with neutron irradiated uranium. Generally, the process of the invention involves the partial neutralization of the waste solution with sodium hydroxide, followed by conversion of the solution to a pH 11 by mixing therewith sufficient sodium carbonate. The resultant carbonate-complexed waste is contacted with a titanated silica gel and the adsorbent separated from the aqueous medium. The aqueous solution is then mixed with sufficient acetic acid to bring the pH of the aqueous medium to between 4 and 5, whereby sodium uranyl acetate is precipitated. The precipitate is dissolved in nitric acid and the resulting solution preferably provided with salting out agents. Uranyl nitrate is recovered from the solution by extraction with an ether such as diethyl ether.

Anodic behavior of uranium in AlCl3-1-ethyl-3-methyl-imidazolium chloride ionic liquid

NASA Astrophysics Data System (ADS)

Jiang, Yidong; Luo, Lizhu; Wang, Shaofei; Bin, Ren; Zhang, Guikai; Wang, Xiaolin

2018-01-01

The oxidation state of metals unambiguously affects its anodic behavior in ionic liquid. We systematically investigated the anodic behavior of uranium with different surface oxidation states by electrochemical measurements, spectroscopic methods and surface analysis techniques. In the anodic process, metal uranium can be oxidized to U3+. The corresponding products accumulated on the metal/ILs interface will form a viscous layer. The anodic behavior of uranium is also strongly dependent upon the surface oxide states including thickness and homogeneity of the oxide film. With an increase in the thickness of oxide film, it will be breached at potentials in excess of a critical value. A uniform oxide on uranium surface can be breached evenly, and then the underlying metal starts to dissolve forming a viscous layer which can facilitate uniformly stripping of oxide, thus giving an oxide-free surface. Otherwise, a nonuniform oxide can result in a severe pitted surface with residue oxygen.

Methods and Data Used to Investigate Polonium-210 as a Source of Excess Gross-Alpha Radioactivity in Ground Water, Churchill County, Nevada

USGS Publications Warehouse

Seiler, Ralph L.

2007-01-01

Ground water is the major source of drinking water in the Carson River Basin, California and Nevada. Previous studies have shown that uranium and gross-alpha radioactivities in ground water can be greater than U.S. Environmental Protection Agency Maximum Contaminant Levels, particularly in the Carson Desert, Churchill County, Nevada. Studies also have shown that the primary source of the gross-alpha radioactivity and alpha-emitting radionuclides in ground water is the dissolution of uranium-rich granitic rocks and basin-fill sediments that have their origins in the Sierra Nevada. However, ground water sampled from some wells in the Carson Desert had gross-alpha radioactivities greater than could be accounted for by the decay of dissolved uranium. The occurrence of polonium-210 (Po-210) was hypothesized to explain the higher than expected gross-alpha radioactivities. This report documents and describes the study design, field and analytical methods, and data used to determine whether Po-210 is the source of excess gross-alpha radioactivity in ground water underlying the Carson Desert in and around Fallon, Nevada. Specifically, this report presents: 1) gross alpha and uranium radioactivities for 100 wells sampled from June to September 2001; and 2) pH, dissolved oxygen, specific conductance, and Po-210 radioactivity for 25 wells sampled in April and June 2007. Results of quality-control samples for the 2007 dataset are also presented.

Investigation on Microbial Dissolution of Uranium (VI) from Autunite Mineral - 13421

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

Sepulveda, Paola; Katsenovich, Yelena; Lagos, Leonel

2013-07-01

Precipitating autunite minerals by polyphosphate injection was identified as a feasible remediation strategy for sequestering uranium in contaminated groundwater and soil in situ at the Hanford Site. Autunite stability under vadose and saturated zone environmental conditions can help to determine the long-term effectiveness of this remediation strategy. The Arthrobacter bacteria are one of the most common groups in soils and are found in large numbers in Hanford soil as well as other subsurface environments contaminated with radionuclides. Ubiquitous in subsurface microbial communities, these bacteria can play a significant role in the dissolution of minerals and the formation of secondary minerals.more » The main objective of this investigation was to study the bacterial interactions under oxidizing conditions with uranium (VI); study the potential role of bicarbonate, which is an integral complexing ligand for U(VI) and a major ion in groundwater compositions; and present data from autunite dissolution experiments using Arthrobacter strain G968, a less U(VI)-tolerant strain. Sterile 100 mL glass mixed reactors served as the major bioreactor for initial experimentation. These autunite-containing bioreactors were injected with bacterial cells after the autunite equilibrated with the media solution amended with 0 mM, 3 mM 5 mM and 10 mM concentrations of bicarbonate. G968 Arthrobacter cells in the amount of 10{sup 6} cells/mL were injected into the reactors after 27 days, giving time for the autunite to reach steady state. Abiotic non-carbonate controls were kept without bacterial inoculation to provide a control for the biotic samples. Samples of the solution were analyzed for dissolved U(VI) by means of kinetic phosphorescence analyzer KPA-11 (Chemcheck Instruments, Richland, WA). Analysis showed that as [HCO{sub 3}{sup -}] increases, a diminishing trend on the effect of bacteria on autunite leaching is observed. Viability of cells was conducted after 24 hours of cell incubation with the appropriate uranium and bicarbonate concentration treatment. As expected, the cells started to reduce after day 41 due to the nutritional exhaustion of the media. Moreover, viable bacteria accounted for more than 94% in the presence of 10 mM bicarbonate. Experiments showed that despite differences between the G975 and the G968 bacterial strains resistance to U(VI), in the presence of bicarbonate ions they are able to dissolute uranium from autunite mineral at the same capacity. The effect of both bacterial strains on autunite dissolution is reduced as the concentration of bicarbonate increases while the increase in soluble U(VI) concentration induced by G968 and G975 is dwarfed, for larger [HCO{sub 3}{sup -}]. (authors)« less

26 CFR 1.993-3 - Definition of export property.

Code of Federal Regulations, 2010 CFR

2010-04-01

...) Application of 50 percent test. The 50 percent test described in subparagraph (1) of this paragraph is applied... uranium concentrates (known in the industry as “yellow cake”), and nuclear fuel materials derived from the refining of uranium ore and uranium concentrates, or produced in a nuclear reaction, including— (a) Uranium...

26 CFR 1.993-3 - Definition of export property.

Code of Federal Regulations, 2011 CFR

2011-04-01

...) Application of 50 percent test. The 50 percent test described in subparagraph (1) of this paragraph is applied... uranium concentrates (known in the industry as “yellow cake”), and nuclear fuel materials derived from the refining of uranium ore and uranium concentrates, or produced in a nuclear reaction, including— (a) Uranium...

Potential of Melastoma malabathricum as bio-accumulator for uranium and thorium from soil

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

Saat, Ahmad, E-mail: ahmad183@salam.uitm.edu.my; Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam; Kamsani, Ain Shaqina

2015-04-29

Uranium and Thorium are naturally occuring radionuclides. However, due to anthropogenic activities in some locations their concentrations in the soils could be elevated. This study explores the potential of Melastoma malabathricum (locally known as ‘pokok senduduk’) as bio-accumulator of uranium and thorium from soils of three different study areas, namely former tin mining, industrial and residential/commercial areas in Peninsular Malaysia. The study found elevated concentrations of uranium and thorium in former tin mining soils as compared to natural abundance. However in industral and residential/commercial areas the concentrations are within the range of natural abundance. In terms of transfer factor (TF),more » in ex-mining areas TF > 1 for uranium in the leaf, stem and roots, indicating accumulation of uranium from soil. However for thorium TF < 1, indicating the occurence of transfer from soil to root, stem and leaf, but no accumulation. For other areas only transfer of uranium and thorium were observed. The results indicated the potential of Melastoma malabathricum to be used as bio-accumulatior of uranium, especially in areas of elevated concentration.« less

Can we predict uranium bioavailability based on soil parameters? Part 2: soil solution uranium concentration is not a good bioavailability index.

PubMed

Vandenhove, H; Van Hees, M; Wannijn, J; Wouters, K; Wang, L

2007-01-01

The present study aimed to quantify the influence of soil parameters on uranium uptake by ryegrass. Ryegrass was established on eighteen distinct soils, spiked with (238)U. Uranium soil-to-plant transfer factors (TF) ranged from 0.0003 to 0.0340kgkg(-1). There was no significant relation between the U soil-to-plant transfer (or total U uptake or flux) and the uranium concentration in the soil solution or any other soil factor measured, nor with the U recovered following selective soil extractions. Multiple linear regression analysis resulted in a significant though complex model explaining up to 99% of variation in TF. The influence of uranium speciation on uranium uptake observed was featured: UO(2)(+2), uranyl carbonate complexes and UO(2)PO(4)(-) seem the U species being preferentially taken up by the roots and transferred to the shoots. Improved correlations were obtained when relating the uranium TF with the summed soil solution concentrations of mentioned uranium species.

Uranium Associations with Kidney Outcomes Vary by Urine Concentration Adjustment Method

PubMed Central

Shelley, Rebecca; Kim, Nam-Soo; Parsons, Patrick J.; Lee, Byung-Kook; Agnew, Jacqueline; Jaar, Bernard G.; Steuerwald, Amy J.; Matanoski, Genevieve; Fadrowski, Jeffrey; Schwartz, Brian S.; Todd, Andrew C.; Simon, David; Weaver, Virginia M.

2017-01-01

Uranium is a ubiquitous metal that is nephrotoxic at high doses. Few epidemiologic studies have examined the kidney filtration impact of chronic environmental exposure. In 684 lead workers environmentally exposed to uranium, multiple linear regression was used to examine associations of uranium measured in a four-hour urine collection with measured creatinine clearance, serum creatinine- and cystatin-C-based estimated glomerular filtration rates, and N-acetyl-β-D-glucosaminidase (NAG). Three methods were utilized, in separate models, to adjust uranium levels for urine concentration - μg uranium/g creatinine; μg uranium/L and urine creatinine as separate covariates; and μg uranium/4 hr. Median urine uranium levels were 0.07 μg/g creatinine and 0.02 μg/4 hr and were highly correlated (rs =0.95). After adjustment, higher ln-urine uranium was associated with lower measured creatinine clearance and higher NAG in models that used urine creatinine to adjust for urine concentration but not in models that used total uranium excreted (μg/4 hr). These results suggest that, in some instances, associations between urine toxicants and kidney outcomes may be statistical, due to the use of urine creatinine in both exposure and outcome metrics, rather than nephrotoxic. These findings support consideration of non-creatinine-based methods of adjustment for urine concentration in nephrotoxicant research. PMID:23591699

Assessment of surface-water quantity and quality, Eagle River watershed, Colorado, 1947-2007

USGS Publications Warehouse

Williams, Cory A.; Moore, Jennifer L.; Richards, Rodney J.

2011-01-01

The spatial patterns for concentrations of trace metals (aluminum, cadmium, copper, iron, manganese, and zinc) indicate an increase in dissolved concentrations of these metals near historical mining areas in the Eagle River and several tributaries near Belden. In general, concentrations decrease downstream from mining areas. Concentrations typically are near or below reporting limits in Gore Creek and other tributaries within the watershed. Concentrations for trace elements (arsenic, selenium, and uranium) in the watershed usually are below the reporting limit, and no prevailing spatial patterns were observed in the data. Step-trend analysis and temporal-trend analysis provide evidence that remediation of historical mining areas in the upper Eagle River have led to observed decreases in metals concentrations in many surface-waters. Comparison of pre- and post-remediation concentrations for many metals indicates significant decreases in metals concentrations for cadmium, manganese, and zinc at sites downstream from the Eagle Mine Superfund Site. Some sites show order of magnitude reductions in median concentrations between these two periods. Evaluation of monotonic trends for dissolved metals concentrations show downward trends at numerous sites in, and downstream from, historic mining areas. The spatial pattern of nutrients shows lower concentrations on many tributaries and on the Eagle River upstream from Red Cliff with increases in nutrients downstream of major urban areas. Seasonal variations show that for many nutrient species, concentrations tend to be lowest May-June and highest January-March. The gradual changes in concentrations between seasons may be related to dilution effects from increases and decreases in streamflow. Upward trends in nutrients between the towns of Gypsum and Avon were detected for nitrate, orthophosphate, and total phosphorus. An upward trend in nitrite was detected in Gore Creek. No trends were detected in un-ionized ammonia within the ERW. Exceedances of State water-quality standards (nitrite, nitrate, and un-ionized ammonia) and levels higher than U.S. Environmental Protection Agency recommendations (total phosphorus) occur in several areas within the ERW. The majority of the exceedances are from comparisons to the U.S. Environmental Protection Agency total phosphorus recommendations. A positive correlation was observed between suspended sediment and total phosphorus. An upward trend in total dissolved solids in Gore Creek may be the result of increases in chloride salts. Highly significant trends were detected in sodium, potassium, and chloride with a significant upward trend in magnesium and a weakly significant upward trend in calcium. A quantitative analysis of the relative abundance of calcium, magnesium, sodium, and potassium to the available anions suggests that chloride salts likely are the source for the detected upward trends because chloride is the only commonly occurring anion with a trend in Gore Greek. A potential source for the observed chloride salts may be the chemical anti-icing and deicing products used during winter road maintenance in municipal areas and on Interstate-70. A downward trend in dissolved solids in the Eagle River between Gypsum and Avon may be contributing to the detected trend on the Eagle River at Gypsum. Significant downward trends were detected in specific ions such as calcium, magnesium, sulfate, and silica. Measures of total dissolved solids as well as comparisons to specific ions show that in water-quality samples within the ERW concentrations generally are lower in the headwaters, with increases downstream from Wolcott. Differences in concentrations likely result from increased abundance of salt-bearing geologic units downstream from Avon. Few sites had measured concentrations that exceeded the State standards for chloride.

Uranium hydrogeochemical and stream sediment reconnaissance of the Cortez NTMS Quadrangle, Colorado/Utah, including concentrations of forty-three additional elements

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

Warren, R.G.

1979-05-01

During the summers of 1976, 1977, and 1978, 598 water and 1657 sediment samples were collected from 1775 locations within the 19,600-km/sup 2/ area of the Cortez Quadrangle, Colorado and Utah. Water samples were collected from streams, springs, and wells; sediment samples were collected from stream channels (wet and dry) and from springs. Each water sample was analyzed for 13 elements, and each sediment sample was analyzed for 43 elements. Uranium concentrations in water samples range from below the detection limit of 0.02 to 241.47 ppB and have a median of 0.87 ppB and a mean of 3.80 ppB. Backgroundmore » uranium concentrations are 2 to 5 ppB in several nonmountainous regions but are much lower in mountainous areas, particularly in the northeastern portion of the quadrangle. Water samples containing high uranium concentrations (>20 ppB) generally are associated with high conductivities, high concentrations of other metallic elements, and geologic units, such as the Mancos shale, that are unfavorable for uranium mineralization. However, four ground-water samples exhibit high uranium concentrations without concomitant high conductivities or high concentrations of other metallic elements. Two of these samples were collected from sites in the Slick Rock U--V district, and two were collected in the Morrison formation in the southern portion of the quadrangle where large uranium deposits are not known. Water samples collected from the northwestern corner of the quadrangle uniformly exhibit background uranium values but generally contain high nickel concentrations. In this area, U--Cu (White Canyon-type) deposits are hosted primarily by the Shinarump member of the Chinle formation. Uranium concentrations in sediment samples range from 0.51 to 76.41 ppM and have a median of 2.76 ppM and a mean of 3.08 ppM. Background uranium and metallic element concentrations decrease to the southwest from the highest values in the northeastern portion of the quadrangle.« less

Status and understanding of groundwater quality in the two southern San Joaquin Valley study units, 2005-2006 - California GAMA Priority Basin Project

USGS Publications Warehouse

Burton, Carmen A.; Shelton, Jennifer L.; Belitz, Kenneth

2012-01-01

Groundwater quality in the southern San Joaquin Valley was investigated from October 2005 through March 2006 as part of the Priority Basin Project of the Groundwater Ambient Monitoring and Assessment (GAMA) Program. The GAMA Priority Basin Project is conducted by the U.S. Geological Survey (USGS) in collaboration with the California State Water Resources Control Board and the Lawrence Livermore National Laboratory. There are two study units located in the southern San Joaquin Valley: the Southeast San Joaquin Valley (SESJ) study unit and the Kern County Subbasin (KERN) study unit. The GAMA Priority Basin Project in the SESJ and KERN study units was designed to provide a statistically unbiased, spatially distributed assessment of untreated groundwater quality within the primary aquifers. The status assessment is based on water-quality and ancillary data collected in 2005 and 2006 by the USGS from 130 wells on a spatially distributed grid, and water-quality data from the California Department of Public Health (CDPH) database. Data was collected from an additional 19 wells for the understanding assessment. The aquifer systems (hereinafter referred to as primary aquifers) were defined as that part of the aquifer corresponding to the perforation interval of wells listed in the CDPH database for the SESJ and KERN study units. The status assessment of groundwater quality used data from samples analyzed for anthropogenic constituents such as volatile organic compounds (VOCs) and pesticides, as well as naturally occurring inorganic constituents such as major ions and trace elements. The status assessment is intended to characterize the quality of untreated groundwater resources within the primary aquifers in the SESJ and KERN study units, not the quality of drinking water delivered to consumers. Although the status assessment applies to untreated groundwater, Federal and California regulatory and non-regulatory water-quality benchmarks that apply to drinking water are used to provide context for the results. Relative-concentrations (sample concentration divided by benchmark concentration) were used for evaluating groundwater. A relative-concentration greater than 1.0 indicates a concentration greater than the benchmark and is classified as high. The relative-concentration threshold for classifying inorganic constituents as moderate or low was 0.5; for organic constituents the threshold between moderate and low was 0.1. Aquifer-scale proportion was used as the primary metric for assessing the quality of untreated groundwater for the study units. High aquifer-scale proportion is defined as the areal percentage of the primary aquifers with a high relative-concentration for a particular constituent or class of constituents. Moderate and low aquifer-scale proportions were defined as the areal percentage of the primary aquifers with moderate and low relative-concentrations, respectively. Two statistical approaches—grid-based and spatially weighted—were used to evaluate aquifer-scale proportions for individual constituents and classes of constituents. Grid-based and spatially weighted estimates were comparable for the two study units in the southern San Joaquin Valley (within 90 percent confidence intervals). The status assessment showed that inorganic constituents were more prevalent than organic constituents and that relative-concentrations were higher for inorganic constituents than for organic constituents. For inorganic constituents with human-health benchmarks, the relative-concentration of at least one constituent in the SESJ study unit was high in 30 percent of the primary aquifers. In the KERN study unit, the relative-concentration of at least one constituent was high in 23 percent of the primary aquifers. In the SESJ and KERN study units, the inorganic constituents with human-health benchmarks detected at high relative-concentrations in more than 2 percent of the primary aquifers were arsenic, boron, vanadium, nitrate, uranium, and gross alpha radioactivity. Additional constituents with human-health benchmarks—antimony, radium, and fluoride—were detected at high relative-concentrations in the KERN study unit. For inorganic constituents with aesthetic benchmarks (secondary maximum contaminant levels, SMCLs), the relative-concentration of at least one constituent in the SESJ study unit was high in 6.6 percent of the primary aquifers. In the KERN study unit, the relative-concentration of at least one constituent was high in 22 percent of the primary aquifers. Inorganic constituents with aesthetic benchmarks detected at high relative-concentrations in the primary aquifers in the SESJ and KERN study units were iron and manganese. Additional constituents with aesthetic benchmarks—total dissolved solids (TDS), sulfate, and chloride—were detected at high relative-concentrations in the KERN study unit. In contrast, the status assessment for organic constituents with human-health benchmarks showed that relative-concentrations were high in 4.8 percent and 2.1 percent of the primary aquifers in the SESJ and KERN study units, respectively. The special-interest constituent, perchlorate, was detected at high relative-concentrations in 1.2 percent of the primary aquifers in the SESJ study unit. Twenty-eight of the 78 VOCs (not including fumigants) analyzed were detected. Of these 28 VOCs, benzene had high relative-concentrations in the SESJ study unit, and relative-concentrations for the other 27 VOCs were moderate and low. Five of the 10 fumigants were detected; 1,2-dibromo-3-chloropropane (DBCP) was the only fumigant with high relative-concentrations in the SESJ and KERN study units. Of the 136 pesticides and pesticide degradates analyzed, 33 were detected. Human-health benchmarks were established for eighteen of the detected pesticides. Dieldrin was detected at moderate relative-concentrations in the SESJ and KERN study units. All other pesticides detected with human-health benchmarks were present at low relative-concentrations. The detection frequencies for two of these pesticides—simazine and atrazine—were greater than or equal to 10 percent in the SESJ and KERN study units. The understanding assessment of groundwater quality included an analysis of correlations of selected water-quality constituents or classes of constituents with potential explanatory factors. The understanding assessment indicated that the concentrations of many trace elements and major ions were correlated to well depth, groundwater age, and/or geochemical conditions. Many trace elements were positively correlated with depth. Arsenic, boron, vanadium, fluoride, manganese, and iron concentrations increased with well depth or depth to top-of-perforations. The concentrations for these trace elements also were higher in older (pre-modern) groundwater. In contrast, uranium concentrations decreased with increasing depth and groundwater age. Most trace elements were correlated to geochemical conditions. Arsenic, antimony, boron, fluoride, manganese, and iron concentrations generally were higher wherever the pH of the groundwater was greater than 7.6. Concentrations for these constituents generally were higher at low concentrations of dissolved oxygen (DO). Uranium was the exception; uranium concentrations generally were lower at high pH and at high concentrations of DO. Nitrate concentrations generally were lower in deeper wells. Nitrate concentrations also were higher in groundwater with higher DO. Total dissolved solids, sulfate, and chloride concentrations were higher in the KERN study unit than in the SESJ study unit. Total dissolved solids were negatively correlated with pH in the KERN study unit. Total dissolved solids and sulfate were higher in areas with more agricultural land use. Chloride concentrations increased with depth to top-of-perforations in the KERN study unit. Organic constituents and constituents of special interest, like many inorganic constituents, were correlated with well depth, groundwater age, and DO. Unlike most trace elements, however, solvent and pesticide detections, and total trihalomethanes (THM), DBCP, and perchlorate concentrations decreased with increasing well depth. Volatile organic compound, solvent, and pesticide detections, and THM concentrations also were lower in older (pre-modern) groundwater than in modern-age groundwater. Solvent detections and total THM, DBCP, and perchlorate concentrations increased with increasing DO concentrations.

Preparation of High Purity, High Molecular-Weight Chitin from Ionic Liquids for Use as an Adsorbate for the Extraction of Uranium from Seawater

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

Rogers, Robin

Ensuring a domestic supply of uranium is a key issue facing the wider implementation of nuclear power. Uranium is mostly mined in Kazakhstan, Australia, and Canada, and there are few high-grade uranium reserves left worldwide. Therefore, one of the most appealing potential sources of uranium is the vast quantity dissolved in the oceans (estimated to be 4.4 billion tons worldwide). There have been research efforts centered on finding a means to extract uranium from seawater for decades, but so far none have resulted in an economically viable product, due in part to the fact that the materials that have beenmore » successfully demonstrated to date are too costly (in terms of money and energy) to produce on the necessary scale. Ionic Liquids (salts which melt below 100{degrees}C) can completely dissolve raw crustacean shells, leading to recovery of a high purity, high molecular weight chitin powder and to fibers and films which can be spun directly from the extract solution suggesting that continuous processing might be feasible. The work proposed here will utilize the unprecedented control this makes possible over the chitin fiber a) to prepare electrospun nanofibers of very high surface area and in specific architectures, b) to modify the fiber surfaces chemically with selective extractant capacity, and c) to demonstrate their utility in the direct extraction and recovery of uranium from seawater. This approach will 1) provide direct extraction of chitin from shellfish waste thus saving energy over the current industrial process for obtaining chitin; 2) allow continuous processing of nanofibers for very high surface area fibers in an economical operation; 3) provide a unique high molecular weight chitin not available from the current industrial process, leading to stronger, more durable fibers; and 4) allow easy chemical modification of the large surface areas of the fibers for appending uranyl selective functionality providing selectivity and ease of stripping. The resulting sorbent should prove economically feasible, as well as providing an overall net energy gain.« less

NEUTRALIZATIONS OF HIGH ALUMINUM LOW URANIUM USED NUCLEAR FUEL SOLUTIONS CONTAINING GADOLINIUM AS A NEUTRON POISON

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

Taylor-Pashow, K.

2011-06-08

H-Canyon will begin dissolving High Aluminum - Low Uranium (High Al/Low U) Used Nuclear Fuel (UNF) following approval by DOE which is anticipated in CY2011. High Al/Low U is an aluminum/enriched uranium UNF with small quantities of uranium relative to aluminum. The maximum enrichment level expected is 93% {sup 235}U. The High Al/Low U UNF will be dissolved in H-Canyon in a nitric acid/mercury/gadolinium solution. The resulting solution will be neutralized and transferred to Tank 39H in the Tank Farm. To confirm that the solution generated could be poisoned with Gd, neutralized, and discarded to the Savannah River Site (SRS)more » high level waste (HLW) system without undue nuclear safety concerns the caustic precipitation of simulant solutions was examined. Experiments were performed with three simulant solutions representative of the H-Canyon estimated concentrations in the final solutions after dissolution. The maximum U, Gd, and Al concentration were selected for testing from the range of solution compositions provided. Simulants were prepared in three different nitric acid concentrations, ranging from 0.5 to 1.5 M. The simulant solutions were neutralized to four different endpoints: (1) just before a solid phase was formed (pH 3.5-4), (2) the point where a solid phase was obtained, (3) 0.8 M free hydroxide, and (4) 1.2 M free hydroxide, using 50 wt % sodium hydroxide (NaOH). The settling behavior of the neutralized solutions was found to be slower compared to previous studies, with settling continuing over a one week period. Due to the high concentration of Al in these solutions, precipitation of solids was observed immediately upon addition of NaOH. Precipitation continued as additional NaOH was added, reaching a point where the mixture becomes almost completely solid due to the large amount of precipitate. As additional NaOH was added, some of the precipitate began to redissolve, and the solutions neutralized to the final two endpoints mixed easily and had expected densities of typical neutralized waste. Based on particle size and scanning electron microscopy analyses, the neutralized solids were found to be homogeneous and less than 20 microns in size. The majority of solids were less than 4 microns in size. Compared to previous studies, a larger percentage of the Gd was found to precipitate in the partially neutralized solutions (at pH 3.5-4). In addition the Gd:U mass ratio was found to be at least 1.0 in all of the solids obtained after partial or full neutralization. The hydrogen to U (H:U) molar ratios for two accident scenarios were also determined. The first was for transient neutralization and agitator failure. Experimentally this scenario was determined by measuring the H:U ratio of the settled solids. The minimum H:U molar ratio for solids from fully neutralized solutions was 388:1. The second accident scenario is for the solids drying out in an unagitiated pump box. Experimentally, this scenario was determined by measuring the H:U molar ratio in centrifuged solids. The minimum H:U atom ratios for centrifuged precipitated solids was 250:1. It was determined previously that a 30:1 H:Pu atom ratio was sufficient for a 1:1 Gd:Pu mass ratio. Assuming a 1:1 equivalence with {sup 239}Pu, the results of these experiments show Gd is a viable poison for neutralizing U/Gd solutions with the tested compositions.« 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.

Micro-SHINE Uranyl Sulfate Irradiations at the Linac

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

Youker, Amanda J.; Kalensky, Michael; Chemerisov, Sergey

2016-08-01

Peroxide formation due to water radiolysis in a uranyl sulfate solution is a concern for the SHINE Medical Technologies process in which Mo-99 is generated from the fission of dissolved low enriched uranium. To investigate the effects of power density and fission on peroxide formation and uranyl-peroxide precipitation, uranyl sulfate solutions were irradiated using a 50-MeV electron linac as part of the micro-SHINE experimental setup. Results are given for uranyl sulfate solutions with both high and low enriched uranium irradiated at different linac powers.

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.

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

PubMed

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65 and 24%, respectively.

Groundwater-Quality Assessment, Pike County, Pennsylvania, 2007

USGS Publications Warehouse

Senior, Lisa A.

2009-01-01

Pike County, a 545 square-mile area in northeastern Pennsylvania, has experienced the largest relative population growth of any county in the state from 1990 to 2000 and its population is projected to grow substantially through 2025. This growing population may result in added dependence and stresses on water resources, including the potential to reduce the quantity and degrade the quality of groundwater and associated stream base flow with changing land use. Groundwater is the main source of drinking water in the county and is derived primarily from fractured-rock aquifers (shales, siltstones, and sandstones) and some unconsolidated glacial deposits that are recharged locally from precipitation. The principal land uses in the county as of 2005 were public, residential, agricultural, hunt club/private recreational, roads, and commercial. The public lands cover a third of the county and include national park, state park, and other state lands, much of which are forested. Individual on-site wells and wastewater disposal are common in many residential areas. In 2007, the U.S. Geological Survey, in cooperation with the Pike County Conservation District, began a study to provide current information on groundwater quality throughout the county that will be helpful for water-resource planning. The countywide reconnaissance assessment of groundwater quality documents current conditions with existing land uses and may serve as a baseline of groundwater quality for future comparison. Twenty wells were sampled in 2007 throughout Pike County to represent groundwater quality in the principal land uses (commercial, high-density and moderate-density residential with on-site wastewater disposal, residential in a sewered area, pre-development, and undeveloped) and geologic units (five fractured-rock aquifers and one glacial unconsolidated aquifer). Analyses selected for the groundwater samples were intended to identify naturally occurring constituents from the aquifer or constituents introduced by human activities that pose a health risk or otherwise were of concern in groundwater in the county. The analyses included major ions, nutrients, selected trace metals, volatile organic compounds (VOCs), selected organic wastewater compounds, gross alpha-particle and gross beta-particle activity, uranium, and radon-222. Analyses of the 20 samples were primarily for dissolved constituents, but six samples were analyzed for both dissolved and total metals. Results of the 2007 sampling indicated few water-quality problems, although concentrations of some constituents indicated influence of human activities on groundwater. No constituent analyzed exceeded any primary drinking-water standard or maximum contaminant level (MCL) established by the U.S. Environmental Protection Agency. Radon-222 levels were greater than, or equal to, the proposed MCL of 300 picocuries per liter (pCi/L) in water from 15 (75 percent) of the 20 wells. Radon-222 levels did not exceed the alternative MCL of 4,000 pCi/L in any groundwater sample. Radon-222 is naturally occurring, and the greatest concentrations (up to 2,650 pCi/L) were in water samples from wells in members of the Catskill Formation, a fractured-rock aquifer. The dissolved arsenic concentration of 3.9 micrograms per liter (ug/L) in one sample was greater than the health-advisory (HA) level of 2 ug/L but less than the MCL of 10 ug/L. Recommended or secondary maximum contaminant levels (SMCLs) were exceeded for pH, dissolved iron, and dissolved manganese. In six samples analyzed for dissolved and total concentrations of selected metals, total concentrations commonly were much greater than dissolved concentrations of iron, and to a lesser degree, for arsenic, lead, copper, and manganese. Concentrations of iron above the SMCL of 300 ug/L may be more widespread in the county for particulate iron than for dissolved iron. The total arsenic concentration in one of the six samples was greater than the HA level of

Quantification of Kinetic Rate Law Parameters of Uranium Release from Sodium Autunite as a Function of Aqueous Bicarbonate Concentrations

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

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn M.

2013-09-05

ABSTRACT: Hydrogen carbonate is one of the most significant components within the uranium geochemical cycle. In aqueous solutions, hydrogen carbonate forms strong complexes with uranium. As such, aqueous bicarbonate may significantly increase the rate of uranium release from uranium minerals. Quantifying the relationship of aqueous hydrogen carbonate solutions to the rate of uranium release during dissolution is critical to understanding the long-term fate of uranium within the environment. Single-pass flow-through (SPTF) experiments were conducted to estimate the rate of uranium release from Na meta-autunite as a function of bicarbonate solutions (0.0005-0.003 M) under the pH range of 6-11 and temperaturesmore » of 5-60oC. Consistent with the results of previous investigation, the rate of uranium release from sodium autunite exhibited minimal dependency on temperature; but were strongly dependent on pH and increasing concentrations of bicarbonate solutions. Most notably at pH 7, the rate of uranium release exhibited 370 fold increases relative to the rate of uranium release in the absence of bicarbonate. However, the effect of increasing concentrations of bicarbonate solutions on the release of uranium was significantly less under higher pH conditions. It is postulated that at high pH values, surface sites are saturated with carbonate, thus the addition of more bicarbonate would have less effect on uranium release. Results indicate the activation energies were unaffected by temperature and bicarbonate concentration variations, but were strongly dependent on pH conditions. As pH increased from 6 to 11, activation energy values were observed to decrease from 29.94 kJ mol-1 to 13.07 kJ mol-1. The calculated activation energies suggest a surface controlled dissolution mechanism.« less

Inhibition of poly(ADP-ribose)polymerase-1 and DNA repair by uranium

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

Cooper, Karen L.; Dashner, Erica J.; Tsosie, Ranalda

Uranium has radiological and non-radiological effects within biological systems and there is increasing evidence for genotoxic and carcinogenic properties attributable to uranium through its heavy metal properties. In this study, we report that low concentrations of uranium (as uranyl acetate; < 10 μM) is not cytotoxic to human embryonic kidney cells or normal human keratinocytes; however, uranium exacerbates DNA damage and cytotoxicity induced by hydrogen peroxide, suggesting that uranium may inhibit DNA repair processes. Concentrations of uranyl acetate in the low micromolar range inhibited the zinc finger DNA repair protein poly(ADP-ribose) polymerase (PARP)-1 and caused zinc loss from PARP-1 protein.more » Uranyl acetate exposure also led to zinc loss from the zinc finger DNA repair proteins Xeroderma Pigmentosum, Complementation Group A (XPA) and aprataxin (APTX). In keeping with the observed inhibition of zinc finger function of DNA repair proteins, exposure to uranyl acetate enhanced retention of induced DNA damage. Co-incubation of uranyl acetate with zinc largely overcame the impact of uranium on PARP-1 activity and DNA damage. These findings present evidence that low concentrations of uranium can inhibit DNA repair through disruption of zinc finger domains of specific target DNA repair proteins. This may provide a mechanistic basis to account for the published observations that uranium exposure is associated with DNA repair deficiency in exposed human populations. - Highlights: • Low micromolar concentration of uranium inhibits polymerase-1 (PARP-1) activity. • Uranium causes zinc loss from multiple DNA repair proteins. • Uranium enhances retention of DNA damage caused by ultraviolet radiation. • Zinc reverses the effects of uranium on PARP activity and DNA damage repair.« less

The association of uranium with organic matter in Holocene peat: An experimental leaching study

USGS Publications Warehouse

Zielinski, R.A.; Meier, A.L.

1988-01-01

Uraniferous peat was sampled from surface layers of a Holocene U deposit in northeastern Washington State. Dried, sized, and homogenized peat that contained 5980 ??307 ppm U was subjected to a variety of leaching conditions to determine the nature and strength of U-organic bonding in recently accumulated organic matter. The results complement previous experimental studies of U uptake on peat and suggest some natural or anthropogenic disturbances that are favorable for remobilizing U. The fraction of U leached in 24 h experiments at 25??C ranged from 0 to 95%. The most effective leach solutions contained anions capable of forming stable dissolved complexes with uranyl (UO2+2) cation. These included H2SO4 (pH = 1.5) and concentrated (>0.01 M) solutions of sodium bicarbonate-carbonate (pH = 7.0-10.0), or sodium pyrophosphate (pH = 10). Effective leaching by carbonate and pyrophosphate in the absence of added oxidant, and the insignificant effect of added oxidant (as pressurized O2) strongly suggest that U is initially fixed on organic matter as an oxidized U(VI) species. Uranium is more strongly bound than some other polyvalent cations, based on its resistance to exchange in the presence of large excesses of dissolved Ca2+ and Cu2+. Measurements of the rate of U leaching indicate faster rates in acid solution compared to carbonate solution, and are consisten with simultaneous attack of sites with different affinities for U. Sulfuric acid appears a good choice for commercial extraction of U from mined peat. In situ disturbances such as overliming of peat soils, addition of fertilizers containing pyrophosphate, or incursions of natural carbonate-rich waters could produce significant remobilization of U, and possibly compromise the quality of local domestic water supplies. ?? 1988.

Analysis of 2H-Evaporator Acid Cleaning Samples

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

Hay, M.; Diprete, D.; Edwards, T.

The 2H-Evaporator acid cleaning solution samples were analyzed by SRNL to determine a composition for the scale present in the evaporator before recent acid cleaning. Composite samples were formed from the solution samples from the two acid cleaning cycles. The solution composition was converted to a weight percent scale solids basis under an assumed chemical composition. The scale composition produced from the acid cleaning solution samples indicates a concentration of 6.85 wt% uranium. An upper bound, onesided 95% confidence interval on the weight percent uranium value may be given as 6.9 wt% + 1.645 × 0.596 wt% = 7.9 wt%.more » The comparison of the composition from the current acid cleaning solutions with the composition of recent scale samples along with the thermodynamic modeling results provides reasonable assurance that the sample results provide a good representation of the overall scale composition in the evaporator prior to acid cleaning. The small amount of scale solids dissolved in the 1.5 M nitric acid during the evaporator cleaning process likely produced only a small amount of precipitation based on modeling results and the visual appearance of the samples.« less

Application of phytoextraction for uranium contaminated soil in korea

NASA Astrophysics Data System (ADS)

Ryu, Y.; Han, Y.; Lee, M.

2013-12-01

The soils having high concentration of uranium, sampled from Goesan Deokpyungri area in Korea, were identified with the uranium removal efficiency of phytoextraction by using several plants. According to the results of physicochemical properties, uranium concentration from soil was 28.85mg/kg, pH 5.43 and soil texture was "Sand". Results of SEP(Sequential Extraction Procedure) test, uranium concentrations ratio of soil in the status of exchangeable/carbonate was 13.4%. Five plants such as Lettuce (Lactuca sativa L.), Chinese cabbage (Brassica campestris L.), Sweet potato (Ipomoea batatas (L.) Lam), Radish (Raphanus sativus), Sesame (Perilla frutescens var. japonica) were cultivated during 56 days in phytotron. All the cultivation processes were conducted in a growth chamber at 25 degrees celsius, 70% relative humidity, 4000 Lux illumination (16 hours/day) and CO2 concentration of 600 ppm. Four times at intervals of 2 weeks leaves and roots collected were analyzed for uranium concentration. Ranges of uranium concentration of the roots and leaves from the five plants were measured to 206.81-721.22μg/kg and 3.45-10.21μg/kg respectively. The majority of uranium was found to accumulate in the roots. Uranium concentration in the leaves, regardless of the type of plants were presented below standard of drinking water(30μg/l) by U.S EPA. Phytoextraction pot experiments with citric acid were conducted. Citric acid as chelating agent was applied to soil to enhance uranium accumulation in five crop plants. 6 days before harvest crops, Each citric acid 25mM and 50mM was injected into the soil by 300ml. After injecting citric acid 25mM , pH of the soil was reduced to 4.95. Uranium concentration of leaves and roots collected from five plants was increased to 2-4times and 7-30times compared to control soil. Injected with citric acid 50mM , pH of the soil was reduced to 4.79. Uranium concentration of leaves and roots collected from five plants was increased to 3-10times and 10-50times compared to control soil. The results of TOC (Total Organic Carbon content), CEC (Cation Exchange Capacity), T-N and T-P analysis of the soil with citric acid 25mM and 50mM were similar to control soil. Finally, the chelating agent was effective to use a citric acid 50mM .

Impact of anaerobic oxidation of methane on the geochemical cycle of redox-sensitive elements at cold-seep sites of the northern South China Sea

NASA Astrophysics Data System (ADS)

Hu, Yu; Feng, Dong; Liang, Qianyong; Xia, Zhen; Chen, Linying; Chen, Duofu

2015-12-01

Cold hydrocarbon seepage is a frequently observed phenomenon along continental margins worldwide. However, little is known about the impact of seeping fluids on the geochemical cycle of redox-sensitive elements. Pore waters from four gravity cores (D-8, D-5, D-7, and D-F) collected from cold-seep sites of the northern South China Sea were analyzed for SO42-, Mg2+, Ca2+, Sr2+, dissolved inorganic carbon (DIC), δ13CDIC, dissolved Fe, Mn, and trace elements (e.g. Mo, U). The sulfate concentration-depth profiles, δ13CDIC values and (ΔDIC+ΔCa2++ΔMg2+)/ΔSO42- ratios suggest that organoclastic sulfate reduction (OSR) is the dominant process in D-8 core. Besides OSR, anaerobic oxidation of methane (AOM) is partially responsible for depletion of sulfate at D-5 and D-7 cores. The sulfate consumption at D-F core is predominantly caused by AOM. The depth of sulfate-methane interface (SMI) and methane diffusive flux of D-F core are calculated to be ~7 m and 0.035 mol m-2 yr-1, respectively. The relatively shallow SMI and high methane flux at D-F core suggest the activity of gas seepage in this region. The concentrations of dissolved uranium (U) were inferred to decrease significantly within the iron reduction zone. It seems that AOM has limited influence on the U geochemical cycling. In contrast, a good correlation between the consumption of sulfate and the removal of molybdenum (Mo) suggests that AOM has a significantly influence on the geochemical cycle of Mo at cold seeps. Accordingly, cold seep environments may serve as an important potential sink in the marine geochemical cycle of Mo.

Uranium removal from aqueous solution by coir pith: equilibrium and kinetic studies.

PubMed

Parab, Harshala; Joshi, Shreeram; Shenoy, Niyoti; Verma, Rakesh; Lali, Arvind; Sudersanan, M

2005-07-01

Basic aspects of uranium adsorption by coir pith have been investigated by batch equilibration. The influence of different experimental parameters such as final solution pH, adsorbent dosage, sorption time, temperature and various concentrations of uranium on uptake were evaluated. Maximum uranium adsorption was observed in the pH range 4.0-6.0. The Freundlich and Langmuir adsorption models were used for the mathematical description of the adsorption equilibrium. The equilibrium data fitted well to both the equilibrium models in the studied concentration range of uranium (200-800 mg/l) and temperatures (305-336 K). The coir pith exhibited the highest uptake capacity for uranium at 317 K, at the final solution pH value of 4.3 and at the initial uranium concentration of 800 mg/l. The kinetics of the adsorption process followed a second-order adsorption. The adsorbent used proved to be suitable for removal of uranium from aqueous solutions. 0.2 N HCl was effective in uranium desorption. The results indicated that the naturally abundant coir pith of otherwise nuisance value exhibited considerable potential for application in removal of uranium from aqueous solution.

Can we predict uranium bioavailability based on soil parameters? Part 1: effect of soil parameters on soil solution uranium concentration.

PubMed

Vandenhove, H; Van Hees, M; Wouters, K; Wannijn, J

2007-01-01

Present study aims to quantify the influence of soil parameters on soil solution uranium concentration for (238)U spiked soils. Eighteen soils collected under pasture were selected such that they covered a wide range for those parameters hypothesised as being potentially important in determining U sorption. Maximum soil solution uranium concentrations were observed at alkaline pH, high inorganic carbon content and low cation exchange capacity, organic matter content, clay content, amorphous Fe and phosphate levels. Except for the significant correlation between the solid-liquid distribution coefficients (K(d), L kg(-1)) and the organic matter content (R(2)=0.70) and amorphous Fe content (R(2)=0.63), there was no single soil parameter significantly explaining the soil solution uranium concentration (which varied 100-fold). Above pH=6, log(K(d)) was linearly related with pH [log(K(d))=-1.18 pH+10.8, R(2)=0.65]. Multiple linear regression analysis did result in improved predictions of the soil solution uranium concentration but the model was complex.

Selected trace elements in the Sacramento River, California: occurrence and distribution.

PubMed

Taylor, H E; Antweiler, R C; Roth, D A; Alpers, C N; Dileanis, P

2012-05-01

The impact of trace elements from the Iron Mountain Superfund site on the Sacramento River and selected tributaries is examined. The concentration and distribution of many trace elements-including aluminum, arsenic, boron, barium, beryllium, bismuth, cadmium, cerium, cobalt, chromium, cesium, copper, dysprosium, erbium, europium, iron, gadolinium, holmium, potassium, lanthanum, lithium, lutetium, manganese, molybdenum, neodymium, nickel, lead, praseodymium, rubidium, rhenium, antimony, selenium, samarium, strontium, terbium, thallium, thulium, uranium, vanadium, tungsten, yttrium, ytterbium, zinc, and zirconium-were measured using a combination of inductively coupled plasma-mass spectrometry and inductively coupled plasma-atomic emission spectrometry. Samples were collected using ultraclean techniques at selected sites in tributaries and the Sacramento River from below Shasta Dam to Freeport, California, at six separate time periods from mid-1996 to mid-1997. Trace-element concentrations in dissolved (ultrafiltered [0.005-μm pore size]) and colloidal material, isolated at each site from large volume samples, are reported. For example, dissolved Zn ranged from 900 μg/L at Spring Creek (Iron Mountain acid mine drainage into Keswick Reservoir) to 0.65 μg/L at the Freeport site on the Sacramento River. Zn associated with colloidal material ranged from 4.3 μg/L (colloid-equivalent concentration) in Spring Creek to 21.8 μg/L at the Colusa site on the Sacramento River. Virtually all of the trace elements exist in Spring Creek in the dissolved form. On entering Keswick Reservoir, the metals are at least partially converted by precipitation or adsorption to the particulate phase. Despite this observation, few of the elements are removed by settling; instead the majority is transported, associated with colloids, downriver, at least to the Bend Bridge site, which is 67 km from Keswick Dam. Most trace elements are strongly associated with the colloid phase going downriver under both low- and high-flow conditions.

Selected trace elements in the Sacramento River, California: Occurrence and distribution

USGS Publications Warehouse

Taylor, Howard E.; Antweiler, Ronald C.; Roth, David A.; Dileanis, Peter D.; Alpers, Charles N.

2012-01-01

The impact of trace elements from the Iron Mountain Superfund site on the Sacramento River and selected tributaries is examined. The concentration and distribution of many trace elements—including aluminum, arsenic, boron, barium, beryllium, bismuth, cadmium, cerium, cobalt, chromium, cesium, copper, dysprosium, erbium, europium, iron, gadolinium, holmium, potassium, lanthanum, lithium, lutetium, manganese, molybdenum, neodymium, nickel, lead, praseodymium, rubidium, rhenium, antimony, selenium, samarium, strontium, terbium, thallium, thulium, uranium, vanadium, tungsten, yttrium, ytterbium, zinc, and zirconium—were measured using a combination of inductively coupled plasma-mass spectrometry and inductively coupled plasma-atomic emission spectrometry. Samples were collected using ultraclean techniques at selected sites in tributaries and the Sacramento River from below Shasta Dam to Freeport, California, at six separate time periods from mid-1996 to mid-1997. Trace-element concentrations in dissolved (ultrafiltered [0.005-μm pore size]) and colloidal material, isolated at each site from large volume samples, are reported. For example, dissolved Zn ranged from 900 μg/L at Spring Creek (Iron Mountain acid mine drainage into Keswick Reservoir) to 0.65 μg/L at the Freeport site on the Sacramento River. Zn associated with colloidal material ranged from 4.3 μg/L (colloid-equivalent concentration) in Spring Creek to 21.8 μg/L at the Colusa site on the Sacramento River. Virtually all of the trace elements exist in Spring Creek in the dissolved form. On entering Keswick Reservoir, the metals are at least partially converted by precipitation or adsorption to the particulate phase. Despite this observation, few of the elements are removed by settling; instead the majority is transported, associated with colloids, downriver, at least to the Bend Bridge site, which is 67 km from Keswick Dam. Most trace elements are strongly associated with the colloid phase going downriver under both low- and high-flow conditions.

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

Application of bimodal distribution to the detection of changes in uranium concentration in drinking water collected by random daytime sampling method from a large water supply zone.

PubMed

Garboś, Sławomir; Święcicka, Dorota

2015-11-01

The random daytime (RDT) sampling method was used for the first time in the assessment of average weekly exposure to uranium through drinking water in a large water supply zone. Data set of uranium concentrations determined in 106 RDT samples collected in three runs from the water supply zone in Wroclaw (Poland), cannot be simply described by normal or log-normal distributions. Therefore, a numerical method designed for the detection and calculation of bimodal distribution was applied. The extracted two distributions containing data from the summer season of 2011 and the winter season of 2012 (nI=72) and from the summer season of 2013 (nII=34) allowed to estimate means of U concentrations in drinking water: 0.947 μg/L and 1.23 μg/L, respectively. As the removal efficiency of uranium during applied treatment process is negligible, the effect of increase in uranium concentration can be explained by higher U concentration in the surface-infiltration water used for the production of drinking water. During the summer season of 2013, heavy rains were observed in Lower Silesia region, causing floods over the territory of the entire region. Fluctuations in uranium concentrations in surface-infiltration water can be attributed to releases of uranium from specific sources - migration from phosphate fertilizers and leaching from mineral deposits. Thus, exposure to uranium through drinking water may increase during extreme rainfall events. The average chronic weekly intakes of uranium through drinking water, estimated on the basis of central values of the extracted normal distributions, accounted for 3.2% and 4.1% of tolerable weekly intake. Copyright © 2015 Elsevier Ltd. All rights reserved.

Behavior of uranium under conditions of interaction of rocks and ores with subsurface water

NASA Astrophysics Data System (ADS)

Omel'Yanenko, B. I.; Petrov, V. A.; Poluektov, V. V.

2007-10-01

The behavior of uranium during interaction of subsurface water with crystalline rocks and uranium ores is considered in connection with the problem of safe underground insulation of spent nuclear fuel (SNF). Since subsurface water interacts with crystalline rocks formed at a high temperature, the mineral composition of these rocks and uranium species therein are thermodynamically unstable. Therefore, reactions directed toward the establishment of equilibrium proceed in the water-rock system. At great depths that are characterized by hindered water exchange, where subsurface water acquires near-neutral and reducing properties, the interaction is extremely sluggish and is expressed in the formation of micro- and nanoparticles of secondary minerals. Under such conditions, the slow diffusion redistribution of uranium with enrichment in absorbed forms relative to all other uranium species is realized as well. The products of secondary alteration of Fe- and Ti-bearing minerals serve as the main sorbents of uranium. The rate of alteration of minerals and conversion of uranium species into absorbed forms is slow, and the results of these processes are insignificant, so that the rocks and uranium species therein may be regarded as unaltered. Under reducing conditions, subsurface water is always saturated with uranium. Whether water interacts with rock or uranium ore, the equilibrium uranium concentration in water is only ≤10-8 mol/l. Uraninite ore under such conditions always remains stable irrespective of its age. The stability conditions of uranium ore are quite suitable for safe insulation of SNF, which consists of 95% uraninite (UO2) and is a confinement matrix for all other radionuclides. The disposal of SNF in massifs of crystalline rocks at depths below 500 m, where reducing conditions are predominant, is a reliable guarantee of high SNF stability. Under oxidizing conditions of the upper hydrodynamic zone, the rate of interaction of rocks with subsurface water increases by orders of magnitude and subsurface water is commonly undersaturated with uranium. Uranium absorbed by secondary minerals, particularly by iron hydroxides and leucoxene, is its single stable species under oxidizing conditions. The impact of oxygen-bearing water leads to destruction of uranium ore. This process is realized simultaneously at different hypsometric levels even if the permeability of the medium is variable in both the lateral and vertical directions. As a result, intervals containing uranyl minerals and relics of primary uranium ore are combined in ore-bearing zones with intervals of completely dissolved uranium minerals. A wide halo of elevated uranium contents caused by sorption is always retained at the location of uranium ore entirely destroyed by weathering. Uranium ore commonly finds itself in the aeration zone due to technogenic subsidence of the groundwater table caused by open-pit mining or pumping out of water from underground mines. The capillary and film waters that interact with rocks and ores in this zone are supplemented by free water filtering along fractures when rain falls or snow is thawing. The interaction of uranium ore with capillary water results in oxidation of uraninite, accompanied by loosening of the mineral surface, formation of microfractures, and an increase in solubility with enrichment of capillary water in uranium up to 10-4 mol/l. Secondary U(VI) minerals, first of all, uranyl hydroxides and silicates, replace uraninite, and uranium undergoes local diffusion redistribution with its sorption by secondary minerals of host rocks. The influx of free water facilitates the complete dissolution of primary and secondary uranium minerals, the removal of uranium at the sites of groundwater discharge, and its redeposition under reducing conditions at a greater depth. It is evident that the conditions of the upper hydrodynamic zone and the aeration zone are unfit for long-term insulation of SNF and high-level wastes because, after the failure of containers, the leakage of radionuclides into the environment becomes inevitable.

Uranium in granitic magmas: Part 2. Experimental determination of uranium solubility and fluid-melt partition coefficients in the uranium oxide-haplogranite-H 2O-NaX (X = Cl, F) system at 770°C, 2 kbar

NASA Astrophysics Data System (ADS)

Peiffert, Chantal; nguyen-Trung, Chinh; Cuney, Michel

1996-05-01

The solubility of uranium oxide was investigated in both aqueous halide (Cl, F) fluid and granitic melt in equilibrium in the system uranium oxide-haplogranite-H 2O-NaCl (0.1-5.0 molal), NaF (0.1-0.5 molal) at 770°C, 2 kbar, and fO 2 conditions controlled by Ni-NiO, Fe 3O 4-Fe 2O 3, and Cu 2O- CuO buffers. Three distinct uranium oxides UO (2+ x) with x = 0.01 ± 0.01; 0.12 ± 0.02; and 0.28 ± 0.02, respec- tively, were obtained in both chloride and fluoride systems, under the three fO 2 conditions cited above. Changes in the composition of aqueous solutions and silicate melt were observed after the runs. These changes were more pronounced for the fluoride-bearing experiments. Quench pH decreased from 5.9 to 2.1 with increasing chloride molality from 0.085-4.38 molal. For fluoride solutions, the decrease of pH from 5.4 to 3.4 corresponded to the increase of fluoride molality from 0.02-0.23 molal. The U solubility in chloride solutions was in the range 10-967 ppm. For the same molality, fluoride solutions appeared to dissolve up to twenty times more uranium than chloride solutions. The increase of halide molality and oxidation led to increase the U solubility. The U solubility in silicate glasses was in the range 10-1.8 × 10 4 ppm and increased with increasing oxidation and halide concentration. In addition, increasing agpaicity also increased U solubility in the chloride system. This effect was not observed in the fluoride system. The chloride concentration in the silicate melt increased from 100-790 ppm with increasing initial aqueous chloride concentration from 0.1-5.0 m. The fluoride concentration in the silicate melt increased from 2.8 × 10 3 to 1.1 × 10 4 ppm with increasing initial fluoride concentra- tion from 0.1-0.5 m. In the chloride system, the partition coefficient of U (log D)(U) fluid/melt) increased from -1.2-0 with increasing agpaicity from 0.92-1.36, for increasing chloride concentration from 0.085-4.38 molal and for increasing fO 2 from 10 -15 to 10 -4 bar. In the fluoride system, a linear correlation was established between the partition coefficient of U and the log fO 2. In F-rich system, D(U) fluid/melt values was in the range 2.4 × 10 -2-4.2 × 10 -2 for increasing fluoride concentration from 0.02-0.22 molal and for the same increasing of fO 2. In the chloride system, the partition coefficients of Na ( D (Na) fluid/melt) and K ( D) (K) fluid/melt) are in good agreement up to 1.0 m NaCl with the two linear equations established by Holland (1972) : D (Na) fluid/melt = 0.46 × (Cl)(m) (1) and D(Na) fluid/melt = 0.34 × (Cl)(m) (2). However, in initial 5.0 m NaCl, slopes of Eqns. 1 and 2 decreased to 0.41 and 0.16, respectively. Data obtained in the present study provide useful information for the understanding of the behaviour of U in the fractionation processes of halide rich magmas. Fluid/melt partition coefficients higher than one, favorable for the genesis of magmatic U mineralization, can be reached for peraluminous leucogran- ites in equilibrium with chloride-rich solutions.

Fiber-based adsorbents having high adsorption capacities for recovering dissolved metals and methods thereof

DOEpatents

Janke, Christopher J.; Dai, Sheng; Oyola, Yatsandra

2016-09-06

A fiber-based adsorbent and a related method of manufacture are provided. The fiber-based adsorbent includes polymer fibers with grafted side chains and an increased surface area per unit weight over known fibers to increase the adsorption of dissolved metals, for example uranium, from aqueous solutions. The polymer fibers include a circular morphology in some embodiments, having a mean diameter of less than 15 microns, optionally less than about 1 micron. In other embodiments, the polymer fibers include a non-circular morphology, optionally defining multiple gear-shaped, winged-shaped or lobe-shaped projections along the length of the polymer fibers. A method for forming the fiber-based adsorbents includes irradiating high surface area polymer fibers, grafting with polymerizable reactive monomers, reacting the grafted fibers with hydroxylamine, and conditioning with an alkaline solution. High surface area fiber-based adsorbents formed according to the present method demonstrated a significantly improved uranium adsorption capacity per unit weight over existing adsorbents.

Fiber-based adsorbents having high adsorption capacities for recovering dissolved metals and methods thereof

DOEpatents

Janke, Christopher J; Dai, Sheng; Oyola, Yatsandra

2014-05-13

A fiber-based adsorbent and a related method of manufacture are provided. The fiber-based adsorbent includes polymer fibers with grafted side chains and an increased surface area per unit weight over known fibers to increase the adsorption of dissolved metals, for example uranium, from aqueous solutions. The polymer fibers include a circular morphology in some embodiments, having a mean diameter of less than 15 microns, optionally less than about 1 micron. In other embodiments, the polymer fibers include a non-circular morphology, optionally defining multiple gear-shaped, winged-shaped or lobe-shaped projections along the length of the polymer fibers. A method for forming the fiber-based adsorbents includes irradiating high surface area polymer fibers, grafting with polymerizable reactive monomers, reacting the grafted fibers with hydroxylamine, and conditioning with an alkaline solution. High surface area fiber-based adsorbents formed according to the present method demonstrated a significantly improved uranium adsorption capacity per unit weight over existing adsorbents.

Determination of the elemental concentration of uranium and thorium in the products and by-products of amang tin tailings process

NASA Astrophysics Data System (ADS)

Alnour, I. A.; Wagiran, H.; Ibrahim, N.; Hamzah, S.; Elias, M. S.

2017-01-01

Amang or tin tailing is processed into concentrated ores and other economical valuable minerals such as monazite, zircon, xenotime, ilmenite etc. Besides that, the tailings from these ores may have a significant potential source of radiation exposure to amang plants' workers. This study was conducted to determine the elemental concentration of uranium and thorium in mineral samples collected from five amang tailing factories. The concentration of uranium and thorium was carried out by using instrumental neutron activation analysis (INAA) relative technique. The concentration of uranium and thorium in ppm obtained in this study are as follows: raw (189-1064) and (622-4965); monazite (1076-1988) and (3467-33578); xenotime 4053 and 5540; zircon (309-3090) and (387-6339); ilmenite (104-583) and (88-1205); rutile (212-889) and (44-1119); pyrite (7-43) and (9-132); and waste (5-338) and (9-1218) respectively. The analysis results shows that the monazite, xenotime and zircon have high content of uranium and thorium, whereas ilmenite, rutile, pyrite and waste have lower concentration compare with raw materials after tailing process. The highest values of uranium and thorium concentrations (4053 ± 428 ppm and 33578 ± 873 ppm, respectively) were observed in xenotime and monazite; whereas the lowest value was 5.48 ± 0.86 ppm of uranium recorded in waste (sand) and 9 ± 0.32 ppm of thorium for waste (sand) and pyrite.

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.

Improving gross count gamma-ray logging in uranium mining with the NGRS probe

NASA Astrophysics Data System (ADS)

Carasco, C.; Pérot, B.; Ma, J.-L.; Toubon, H.; Dubille-Auchère, A.

2018-01-01

AREVA Mines and the Nuclear Measurement Laboratory of CEA Cadarache are collaborating to improve the sensitivity and precision of uranium concentration measurement by means of gamma ray logging. The determination of uranium concentration in boreholes is performed with the Natural Gamma Ray Sonde (NGRS) based on a NaI(Tl) scintillation detector. The total gamma count rate is converted into uranium concentration using a calibration coefficient measured in concrete blocks with known uranium concentration in the AREVA Mines calibration facility located in Bessines, France. Until now, to take into account gamma attenuation in a variety of boreholes diameters, tubing materials, diameters and thicknesses, filling fluid densities and compositions, a semi-empirical formula was used to correct the calibration coefficient measured in Bessines facility. In this work, we propose to use Monte Carlo simulations to improve gamma attenuation corrections. To this purpose, the NGRS probe and the calibration measurements in the standard concrete blocks have been modeled with MCNP computer code. The calibration coefficient determined by simulation, 5.3 s-1.ppmU-1 ± 10%, is in good agreement with the one measured in Bessines, 5.2 s-1.ppmU-1. Based on the validated MCNP model, several parametric studies have been performed. For instance, the rock density and chemical composition proved to have a limited impact on the calibration coefficient. However, gamma self-absorption in uranium leads to a nonlinear relationship between count rate and uranium concentration beyond approximately 1% of uranium weight fraction, the underestimation of the uranium content reaching more than a factor 2.5 for a 50 % uranium weight fraction. Next steps will concern parametric studies with different tubing materials, diameters and thicknesses, as well as different borehole filling fluids representative of real measurement conditions.

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.

Risk evaluation of uranium mining: A geochemical inverse modelling approach

NASA Astrophysics Data System (ADS)

Rillard, J.; Zuddas, P.; Scislewski, A.

2011-12-01

It is well known that uranium extraction operations can increase risks linked to radiation exposure. The toxicity of uranium and associated heavy metals is the main environmental concern regarding exploitation and processing of U-ore. In areas where U mining is planned, a careful assessment of toxic and radioactive element concentrations is recommended before the start of mining activities. A background evaluation of harmful elements is important in order to prevent and/or quantify future water contamination resulting from possible migration of toxic metals coming from ore and waste water interaction. Controlled leaching experiments were carried out to investigate processes of ore and waste (leached ore) degradation, using samples from the uranium exploitation site located in Caetité-Bahia, Brazil. In experiments in which the reaction of waste with water was tested, we found that the water had low pH and high levels of sulphates and aluminium. On the other hand, in experiments in which ore was tested, the water had a chemical composition comparable to natural water found in the region of Caetité. On the basis of our experiments, we suggest that waste resulting from sulphuric acid treatment can induce acidification and salinization of surface and ground water. For this reason proper storage of waste is imperative. As a tool to evaluate the risks, a geochemical inverse modelling approach was developed to estimate the water-mineral interaction involving the presence of toxic elements. We used a method earlier described by Scislewski and Zuddas 2010 (Geochim. Cosmochim. Acta 74, 6996-7007) in which the reactive surface area of mineral dissolution can be estimated. We found that the reactive surface area of rock parent minerals is not constant during time but varies according to several orders of magnitude in only two months of interaction. We propose that parent mineral heterogeneity and particularly, neogenic phase formation may explain the observed variation of the reactive mineral surface area. The formation of coatings on dissolving mineral surfaces significantly reduces the amount of surface available to react with fluids. Our results show that negatively charged ion complexes, responsible for U transport, decreases when alkalinity and rock buffer capacity is similarly lower. Carbonate ion pairs however, may increase U mobility when radionuclide concentration is high and rock buffer capacity is low. The present work helps to orient future monitoring of this site in Brazil as well as of other sites where uranium is linked to igneous rock formations, without the presence of sulphides. Monitoring SO4 migration (in acidic leaching uranium sites) seems to be an efficient and simple way to track different hazards, especially in tropical conditions, where the succession of dry and wet periods increases the weathering action of the residual H2SO4. Nevertheless, models of risk evaluation should take into account reactive surface areas and neogenic minerals since they determine the U ion complex formation, which in turn, controls uranium mobility in natural systems. Keywords: uranium mining, reactive mineral surface area, uranium complexes, inverse modelling approach, risk evaluation

Uranyl nitrate-exposed rat alveolar macrophages cell death: Influence of superoxide anion and TNF α mediators

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

Orona, N.S.; Tasat, D.R., E-mail: deborah.tasat@unsam.edu.ar; School of Dentistry, University of Buenos Aires, M. T. de Alvear 2142

2012-06-15

Uranium compounds are widely used in the nuclear fuel cycle, military and many other diverse industrial processes. Health risks associated with uranium exposure include nephrotoxicity, cancer, respiratory, and immune disorders. Macrophages present in body tissues are the main cell type involved in the internalization of uranium particles. To better understand the pathological effects associated with depleted uranium (DU) inhalation, we examined the metabolic activity, phagocytosis, genotoxicity and inflammation on DU-exposed rat alveolar macrophages (12.5–200 μM). Stability and dissolution of DU could differ depending on the dissolvent and in turn alter its biological action. We dissolved DU in sodium bicarbonate (NaHCO{submore » 3} 100 mM) and in what we consider a more physiological vehicle resembling human internal media: sodium chloride (NaCl 0.9%). We demonstrate that uranyl nitrate in NaCl solubilizes, enters the cell, and elicits its cytotoxic effect similarly to when it is diluted in NaHCO{sub 3}. We show that irrespective of the dissolvent employed, uranyl nitrate impairs cell metabolism, and at low doses induces both phagocytosis and generation of superoxide anion (O{sub 2}{sup −}). At high doses it provokes the secretion of TNFα and through all the range of doses tested, apoptosis. We herein suggest that at DU low doses O{sub 2}{sup −} may act as the principal mediator of DNA damage while at higher doses the signaling pathway mediated by O{sub 2}{sup −} may be blocked, prevailing damage to DNA by the TNFα route. The study of macrophage functions after uranyl nitrate treatment could provide insights into the pathophysiology of uranium‐related diseases. -- Highlights: ► Uranyl nitrate effect on cultured macrophages is linked to the doses and independent of its solubility. ► At low doses uranyl nitrate induces generation of superoxide anion. ► At high doses uranyl nitrate provokes secretion of TNFα. ► Uranyl nitrate induces apoptosis through all the range of doses tested.« less

WET FLUORIDE SEPARATION METHOD

DOEpatents

Seaborg, G.T.; Gofman, J.W.; Stoughton, R.W.

1958-11-25

The separation of U/sup 233/ from thorium, protactinium, and fission products present in neutron-irradiated thorium is accomplished by dissolving the irradiated materials in aqueous nitric acid, adding either a soluble fluoride, iodate, phosphate, or oxalate to precipltate the thorium, separating the precipltate from the solution, and then precipitating uranlum and protactinium by alkalizing the solution. The uranium and protactinium precipitate is removcd from the solution and dissolved in nitric acid. The uranyl nitrate may then be extracted from the acid solution by means of ether, and the protactinium recovered from the aqueous phase.

National uranium resource evaluation: Newark Quadrangle, Pennsylvania and New Jersey

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

Popper, G.H.P.; Martin, T.S.

1982-04-01

The Newark Quadrangle, Pennsylvania and New Jersey, was evaluated to a depth of 1500 m to identify geologic environments and delineate areas favorable for uranium deposits. Criteria used were those developed for the National Uranium Resource Evaluation program. Results of the investigation indicate that the Precambrian Reading Prong contains environments favorable for anatectic and allogenic uranium deposits. Two suites of rocks are favorable for anatectic-type concentrations: An alaskite-magnetite-gneiss association, and red granite and quartz monzonite. Allogenic uranium concentrations occur in rocks of the marble-skarn-serpentinite association. Environments favorable for peneconcordant sandstone-type uranium deposits occur in the upper one-third of the Catskillmore » Formation, the Mississippian-Pennsylvanian Mauch Chunk-Pottsville transition beds, and the upper half of the Triassic Stockton Formation. The Triassic Lockatong Formation contains environments favorable for carbonaceous shale-type uranium concentrations. The Ordovician Epler Formation and the Cretaceous-Tertiary strata of the Coastal Plain were not evaluated due to time restrictions and lack of outcroup. All other geologic environments are considered unfavorable for uranium deposits.« less

Investigating uranium distribution in surface sediments and waters: a case study of contamination from the Juniper Uranium Mine, Stanislaus National Forest, CA.

PubMed

Kayzar, Theresa M; Villa, Adam C; Lobaugh, Megan L; Gaffney, Amy M; Williams, Ross W

2014-10-01

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. The ((234)U)/((238)U) composition of Red Rock Creek is altered downstream of the Juniper Mine. As a result of mine-derived contamination, water ((234)U)/((238)U) ratios are 67% lower than in water upstream of the mine (1.114-1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activity ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041-1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (∼70-80% of uranium in leachable fraction). Contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment. Published by Elsevier Ltd.

Investigating uranium distribution in surface sediments and waters: a case study of contamination from the Juniper Uranium Mine, Stanislaus National Forest, CA

DOE PAGES

Kayzar, Theresa M.; Villa, Adam C.; Lobaugh, Megan L.; ...

2014-06-07

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. Furthermore, we alter the (234U)/(238U) composition of Red Rock Creek downstream of the Juniper Mine. As a result of mine-derived contamination, water (234U)/(238U) ratios are 67% lower than in water upstream of the mine (1.114–1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activitymore » ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041–1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (~70–80% of uranium in leachable fraction). Furthermore, contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment.« less

Experimental study on thermal hazard of tributyl phosphate-nitric acid mixtures using micro calorimeter technique.

PubMed

Sun, Qi; Jiang, Lin; Gong, Liang; Sun, Jin-Hua

2016-08-15

During PUREX spent nuclear fuel reprocessing, mixture of tributyl phosphate (TBP) and hydrocarbon solvent are employed as organic solvent to extract uranium in consideration of radiation contaminated safety and resource recycling, meanwhile nitric acid is utilized to dissolve the spent fuel into small pieces. However, once TBP contacts with nitric acid or nitrates above 130°C, a heavy "red oil" layer would occur accompanied by thermal runaway reactions, even caused several nuclear safety accident. Considering nitric acid volatility and weak exothermic detection, C80micro calorimeter technique was used in this study to investigate thermal decomposition of TBP mixed with nitric acid. Results show that the concentration of nitric acid greatly influences thermal hazard of the system by direct reactions. Even with a low heating rate, if the concentration of nitric acid increases due to evaporation of water or improper operations, thermal runaway in the closed system could start at a low temperature. Copyright © 2016 Elsevier B.V. All rights reserved.

Uranium concentration and distribution in six peridotite inclusions of probable mantle origin

NASA Technical Reports Server (NTRS)

Haines, E. L.; Zartman, R. E.

1973-01-01

Fission-track activation was used to investigate uranium concentration and distribution in peridotite inclusions in alkali basalt from six localities. Whole-rock uranium concentrations range from 24 to 82 ng/g. Most of the uranium is uniformly distributed in the major silicate phases - olivine, orthopyroxene, and clinopyroxene. Chromian spinels may be classified into two groups on the basis of their uranium content - those which have less than 10 ng/g and those which have 100 to 150 ng/g U. In one sample accessory hydrous phases, phlogopite and hornblende, contain 130 and 300 ng/g U, respectively. The contact between the inclusion and the host basalt is usually quite sharp. Glassy or microcrystalline veinlets found in some samples contain more than 1 microgram/g. Very little uranium is associated with microcrystals of apatite. These results agree with some earlier investigators, who have concluded that suboceanic peridotites contain too little uranium to account for normal oceanic heat flow by conduction alone.

Hydrogeochemical and stream sediment reconnaissance basic data for Waco NTMS quadrangle, Texas

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

Not Available

1981-07-31

Results of a reconnaissance geochemical survey of the Waco Quadrangle are reported. Field and laboratory data are presented for 218 groundwater and 614 stream sediment samples. Statistical and areal distribution of uranium and possible uranium-related variables are displayed. A generalized geologic map of the survey area is provided, and pertinent geologic factors which may be of significance in evaluating the potential for uranium mineralization are briefly discussed. Groundwater data indicate that uranium concentrations above the 85th percentile occur primarily in the Upper cretaceous units (Navarro, Taylor, and Woodbine Groups) and Lower Cretaceous carbonate units (Fredricksburg and Wilcox Groups). Saline watermore » trends are also prominent in these units. Stream sediment data indicate high uranium concentrations occur in the western portion of the quadrangle. Most of the samples with high uranium values are collected from the Upper and Lower Cretaceous and Tertiary units. Associated with the high uranium values are high concentrations of aluminum, chromium, iron, scandium, yttrium, zinc, and zirconium.« less

Experiments and Modeling of Uranium Adsorption in the Presence of Other Ions in Simulated Seawater

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

Ladshaw, Austin; Das, Sadananda; Liao, Wei-Po

2015-11-19

Seawater contains uranium at an average concentration of 3.3 ppb, as well as a variety of other ions at either overwhelmingly higher or similar concentrations, which complicate the recovery of uranium. This report describes an investigation of the effects of various factors such as uranium speciation and presence of salts including sodium, calcium, magnesium, and bicarbonate, as well as trace elements such as vanadium on uranium adsorption kinetics in laboratory experiments. Adsorption models are also developed to describe the experimental data of uranium extraction from seawater. Results show that the presence of calcium and magnesium significantly slows down the uraniummore » adsorption kinetics. Vanadium can replace uranium from amidoxime-based adsorbent in the presence of sodium in the solution. Results also show that bicarbonate in the solution strongly competes with amidoxime for binding uranium, and thus slows down the uranium adsorption kinetics. Developed on the basis of the experimental findings, the model is capable of describing the effects of pH, ionic strength, temperature, and concentration of various species. The results of this work are useful in the understanding of the important factors that control the adsorbent capacity and kinetics of uranium uptake by amidoxime-based adsorbents.« less

Spatial distribution of uranium and basic water quality parameter in the capital of Bihar and consequent ingestion dose.

PubMed

Kumar, Deepak; Singh, Anshuman; Jha, Rishi Kumar

2018-04-21

Investigation of presence of Uranium (U) in groundwater/drinking water is an active are of research due to its chemical and radiological toxicity as well as long-term health effects. The current study had the objective of estimating U as a naturally occurring radioactive element in groundwater samples and assessment of ingestion dose, when groundwater is the source of drinking water. The random sampling method was chosen for the collection of samples based on population density. The estimation of U was done using LED fluorimeter. Statistical tools were applied to analyze the data and its spatial distribution. The U concentrations in three blocks of urban Patna were well below the permissible limits suggested by different health agencies of the world. A correlation test was performed to analyze the association of U with other physiochemical parameters of water samples. It was found that the sulfate, chloride, calcium, hardness, alkalinity, TDS, salinity, and ORP were positively correlated, whereas fluoride, phosphate, magnesium, dissolved oxygen, and pH were negatively correlated with U concentrations. The ingestion dose due to U, occurring in groundwater, was found to vary from 0.2-27.0 μSv y -1 with a mean of 4.2 μSv y - 1 , which was well below the recommended limit of 0.1 mSv (WHO WHO Chron 38:104-108, 2012).Therefore, the water in this region is fit for drinking purposes.

Uranium and barium cycling in a salt wedge subterranean estuary: The influence of tidal pumping

USGS Publications Warehouse

Santos, I.R.; Burnett, W.C.; Misra, S.; Suryaputra, I.G.N.A.; Chanton, J.P.; Dittmar, T.; Peterson, R.N.; Swarzenski, P.W.

2011-01-01

The contribution of submarine groundwater discharge (SGD) to oceanic metal budgets is only beginning to be explored. Here, we demonstrate that biogeochemical processes in a northern Florida subterranean estuary (STE) significantly alter U and Ba concentrations entering the coastal ocean via SGD. Tidal pumping controlled the distribution of dissolved metals in shallow beach groundwater. Hourly observations of intertidal groundwaters revealed high U and low Ba concentrations at high tide as a result of seawater infiltration into the coastal aquifer. During ebb tide, U decreased and Ba increased due to freshwater dilution and, more importantly, biogeochemical reactions that removed U and added Ba to solution. U removal was apparently a result of precipitation following the reduction of U(VI) to U(IV). A significant correlation between Ba and dissolved organic carbon (DOC) in shallow beach groundwaters implied a common source, likely the mineralization of marine particulate organic matter driven into the beach face by tidal pumping. In deeper groundwaters, where the labile organic matter had been depleted, Ba correlated with Mn. We estimate that net SGD fluxes were − 163 and + 1660 μmol m− 1 d− 1 for U and Ba, respectively (or − 1 and + 8 μmol m− 2 d− 1 if a 200-m wide seepage area is considered). Our results support the emerging concept that subterranean estuaries are natural biogeochemical reactors where metal concentrations are altered relative to conservative mixing between terrestrial and marine endmembers. These deviations from conservative mixing significantly influence SGD-derived trace metal fluxes.

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

Kayzar, Theresa M.; Villa, Adam C.; Lobaugh, Megan L.

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. Furthermore, we alter the (234U)/(238U) composition of Red Rock Creek downstream of the Juniper Mine. As a result of mine-derived contamination, water (234U)/(238U) ratios are 67% lower than in water upstream of the mine (1.114–1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activitymore » ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041–1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (~70–80% of uranium in leachable fraction). Furthermore, contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment.« less

Uranium Isotopes in Calcium Carbonate: A Possible Proxy for Paleo-pH and Carbonate Ion Concentration?

NASA Astrophysics Data System (ADS)

Chen, X.; Romaniello, S. J.; Herrmann, A. D.; Wasylenki, L. E.; Anbar, A. D.

2015-12-01

Natural variations of 238U/235U in marine carbonates are being explored as a paleoredox proxy. However, in order for this proxy to be robust, it is important to understand how pH and alkalinity affect the fractionation of 238U/235U during coprecipitation with calcite and aragonite. Recent work suggests that the U/Ca ratio of foraminiferal calcite may vary with seawater [CO32-] concentration due to changes in U speciation[1]. Here we explore analogous isotopic consequences in inorganic laboratory co-precipitation experiments. Uranium coprecipitation experiments with calcite and aragonite were performed at pH 8.5 ± 0.1 and 7.5 ± 0.1 using a constant addition method [2]. Dissolved U in the remaining solution was periodically collected throughout the experiments. Samples were purified with UTEVA resin and 238U/235U was determined using a 233U-236U double-spike and MC-ICP-MS, attaining a precision of ± 0.10 ‰ [3]. Small but resolvable U isotope fractionation was observed in aragonite experiments at pH ~8.5, preferentially enriching heavier U isotopes in the solid phase. 238U/235U of the dissolved U in these experiments can be fit by Rayleigh fractionation curves with fractionation factors of 1.00002 - 1.00009. In contrast, no resolvable U isotope fractionation was detected in an aragonite experiment at pH ~7.5 or in calcite experiments at either pH. Equilibrium isotope fractionation among dissolved U species is the most likely mechanism driving these isotope effects. Our quantitative model of this process assumes that charged U species are preferentially incorporated into CaCO3 relative to the neutral U species Ca2UO2(CO3)3(aq), which we hypothesize to have a lighter equilibrium U isotope composition than the charged U species. According to this model, the magnitude of U isotope fractionation should scale with the fraction of the neutral U species in the solution, in agreement with our experimental results. These findings suggest that U isotope variations in abiotic CaCO3 reflect changes in aqueous U(VI) speciation, which are in turn a function of carbonate ion chemistry and pH. Hence, the door is opened to the development of a possible 238U/235U proxy for the carbonate ion system. [1] DeCarlo et al., (2015), GCA, 162,151-165. [2] Reeder et a., (2001), GCA, 65, 3491-3503. [3] Weyer et al., (2008) GCA 72, 345-359.

Removing oxygen from a solvent extractant in an uranium recovery process

DOEpatents

Hurst, Fred J.; Brown, Gilbert M.; Posey, Franz A.

1984-01-01

An improvement in effecting uranium recovery from phosphoric acid solutions is provided by sparging dissolved oxygen contained in solutions and solvents used in a reductive stripping stage with an effective volume of a nonoxidizing gas before the introduction of the solutions and solvents into the stage. Effective volumes of nonoxidizing gases, selected from the group consisting of argon, carbon dioxide, carbon monoxide, helium, hydrogen, nitrogen, sulfur dioxide, and mixtures thereof, displace oxygen from the solutions and solvents thereby reduce deleterious effects of oxygen such as excessive consumption of elemental or ferrous and accumulation of complex iron phosphates or cruds.

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.

Uranium hydrogeochemical and stream sediment reconnaissance of the Durango NTMS quadrangle, Colorado

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

Dawson, H.E.; Weaver, T.A.

1979-01-01

During the spring and summer of 1976, 1518 water and 1604 waterborne sediment samples were collected from 1804 locations in the Durango NTMS quadrangle, Colorado. The samples obtained from this 19 940-km/sup 2/ area were analyzed at the Los Alamos Scientific Laboratory for total uranium. The uranium concentrations in waters ranged from less than the detectable limit of 0.2 ppB to 25.7 ppB, with a mean value of 0.84 ppB. The concentrations in sediments ranged from 1.0 ppM to 71.6 ppM, with a mean value of 4.2 ppM. Study of total water and total sediment populations indicated that both aremore » actually mixtures of several populations. Consequently, samples were chosen for discussion on the basis of their having conspicuously high uranium concentrations relative to surrounding background values. Thirty-four water samples (approximately 2.2% of the total water population) had uranium concentrations above 5.00 ppB, the highest of which were well water samples from the San Luis Valley. Thirty-seven sediment samples (approximately 2.3% of the total sediment population) had uranium concentrations above 12.0 ppM. The majority of these were taken from sites in Precambrian rocks, but several came from Paleozoic and Mesozoic strate and Tertiary volcanics. The uranium concentrations in sediment samples from areas of Precambrian rock were especially high and these areas may warrant further, more detailed investigations.« less

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.

Direct determination of uranium in seawater by laser fluorimetry.

PubMed

Kumar, Sanjukta A; Shenoy, Niyoti S; Pandey, Shailaja; Sounderajan, Suvarna; Venkateswaran, G

2008-10-19

A method for estimation of uranium in seawater by using steady state laser flourimetry is described. Uranium present in seawater, in concentration of approximately 3 ng ml(-1) was estimated without prior separation of matrix. Quenching effect of major ions (Cl(-), Na(+), SO(4)(-), Mg(+), Ca(+), K(+), HCO(3)(-), Br(-)) present in seawater on fluorescence intensity of uranium was studied. The concentration of phosphoric acid required for maximum enhancement of fluorescence intensity was optimized and was found to be 5%. Similarly the volume of concentrated nitric acid required to eliminate the quenching effect of chloride and bromide completely from 5 ml of seawater were optimized and was found to be 3 ml. A simple equation was derived using steady state fluorescence correction method and was used for calculation of uranium concentration in seawater samples. The method has a precesion of 1% (1s, n=3). The values obtained from laser fluorimetry were validated by analyzing the same samples by linear sweep adsorptive stripping voltametry (LSASV) of the uranium-chloranilic acid (2,5-dichloro-3,6-dihydroxy-1,4-benzoquinone) complex. Both the values are well in agreement.

Bone as a Possible Target of Chemical Toxicity of Natural Uranium in Drinking Water

PubMed Central

Kurttio, Päivi; Komulainen, Hannu; Leino, Aila; Salonen, Laina; Auvinen, Anssi; Saha, Heikki

2005-01-01

Uranium accumulates in bone, affects bone metabolism in laboratory animals, and when ingested in drinking water increases urinary excretion of calcium and phosphate, important components in the bone structure. However, little is known about bone effects of ingested natural uranium in humans. We studied 146 men and 142 women 26–83 years of age who for an average of 13 years had used drinking water originating from wells drilled in bedrock, in areas with naturally high uranium content. Biochemical indicators of bone formation were serum osteocalcin and amino-terminal propeptide of type I procollagen, and a marker for bone resorption was serum type I collagen carboxy-terminal telopeptide (CTx). The primary measure of uranium exposure was uranium concentration in drinking water, with additional information on uranium intake and uranium concentration in urine. The data were analyzed separately for men and women with robust regression (which suppresses contributions of potential influential observations) models with adjustment for age, smoking, and estrogen use. The median uranium concentration in drinking water was 27 μg/L (interquartile range, 6–116 μg/L). The median of daily uranium intake was 36 μg (7–207 μg) and of cumulative intake 0.12 g (0.02–0.66 g). There was some suggestion that elevation of CTx (p = 0.05) as well as osteocalcin (p = 0.19) could be associated with increased uranium exposure (uranium in water and intakes) in men, but no similar relationship was found in women. Accordingly, bone may be a target of chemical toxicity of uranium in humans, and more detailed evaluation of bone effects of natural uranium is warranted. PMID:15626650

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.

The Problem of Preconcentration of Uranium Ores by Physical Processes; LES PROBLEMES DE LA PRECONCENTRATION DES MINERAIS D'URANIUM PAR VOIE PHYSIQUE. LE TRIAGE ELECTRONIQUE

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

Vuchot, L.; Ginocchio, A. et al.

1959-10-31

As uranium ores, like most other ores, are not definite substances which can be treated directly for the production of the metal, the ores must be concentrated. The common physical processes used for all ores, such as sieving, gravimetric separation, flotation, electromagnetic separation, and electrostatic separation, are applicable to the beneficiation of uranium. The radioactivity of uranium ores has led to a radiometric method for the concentration. This method is described in detail. As an example, the preconcentration of Forez ores is discussed. (J.S.R.)

Unraveling uranium induced oxidative stress related responses in Arabidopsis thaliana seedlings. Part II: responses in the leaves and general conclusions.

PubMed

Vanhoudt, Nathalie; Cuypers, Ann; Horemans, Nele; Remans, Tony; Opdenakker, Kelly; Smeets, Karen; Bello, Daniel Martinez; Havaux, Michel; Wannijn, Jean; Van Hees, May; Vangronsveld, Jaco; Vandenhove, Hildegarde

2011-06-01

The cellular redox balance seems an important modulator under heavy metal stress. While for other heavy metals these processes are well studied, oxidative stress related responses are also known to be triggered under uranium stress but information remains limited. This study aimed to further unravel the mechanisms by which plants respond to uranium stress. Seventeen-day-old Arabidopsis thaliana seedlings, grown on a modified Hoagland solution under controlled conditions, were exposed to 0, 0.1, 1, 10 and 100 μM uranium for 1, 3 and 7 days. While in Part I of this study oxidative stress related responses in the roots were discussed, this second Part II discusses oxidative stress related responses in the leaves and general conclusions drawn from the results of the roots and the leaves will be presented. As several responses were already visible following 1 day exposure, when uranium concentrations in the leaves were negligible, a root-to-shoot signaling system was suggested in which plastids could be important sensing sites. While lipid peroxidation, based on the amount of thiobarbituric acid reactive compounds, was observed after exposure to 100 μM uranium, affecting membrane structure and function, a transient concentration dependent response pattern was visible for lipoxygenase initiated lipid peroxidation. This transient character of uranium stress responses in leaves was emphasized by results of lipoxygenase (LOX2) and antioxidative enzyme transcript levels, enzyme capacities and glutathione concentrations both in time as with concentration. The ascorbate redox balance seemed an important modulator of uranium stress responses in the leaves as in addition to the previous transient responses, the total ascorbate concentration and ascorbate/dehydroascorbate redox balance increased in a concentration and time dependent manner. This could represent either a slow transient response or a stable increase with regard to plant acclimation to uranium stress. Copyright © 2011 Elsevier Ltd. All rights reserved.

Uranium hydrogeochemical and stream sediment reconnaissance of the Arminto NTMS quadrangle, Wyoming, including concentrations of forty-three additional elements

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

Morgan, T.L.

1979-11-01

During the summers of 1976 and 1977, 570 water and 1249 sediment samples were collected from 1517 locations within the 18,000-km/sup 2/ area of the Arminto NTMS quadrangle of central Wyoming. Water samples were collected from wells, springs, streams, and artifical ponds; sediment samples were collected from wet and dry streams, springs, and wet and dry ponds. All water samples were analyzed for 13 elements, including uranium, and each sediment sample was analyzed for 43 elements, including uranium and thorium. Uranium concentrations in water samples range from below the detection limit to 84.60 parts per billion (ppb) with a meanmore » of 4.32 ppb. All water sample types except pond water samples were considered as a single population in interpreting the data. Pond water samples were excluded due to possible concentration of uranium by evaporation. Most of the water samples containing greater than 20 ppb uranium grouped into six clusters that indicate possible areas of interest for further investigation. One cluster is associated with the Pumpkin Buttes District, and two others are near the Kaycee and Mayoworth areas of uranium mineralization. The largest cluster is located on the west side of the Powder River Basin. One cluster is located in the central Big Horn Basin and another is in the Wind River Basin; both are in areas underlain by favorable host units. Uranium concentrations in sediment samples range from 0.08 parts per million (ppm) to 115.50 ppm with a mean of 3.50 ppm. Two clusters of sediment samples over 7 ppm were delineated. The first, containing the two highest-concentration samples, corresponds with the Copper Mountain District. Many of the high uranium concentrations in samples in this cluster may be due to contamination from mining or prospecting activity upstream from the sample sites. The second cluster encompasses a wide area in the Wind River Basin along the southern boundary of the quadrangle.« less

Solubility limits of dibutyl phosphoric acid in uranium-nitric acid solutions

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

Pierce, R.A.

2000-01-04

The Savannah River Site has enriched uranium (EU) solution that has been stored since being purified in its solvent extraction processes. The concentrations in solution are approximately 6 g/L U and 0.1 M nitric acid. Residual tributylphosphate in solution has slowly hydrolyzed to form dibutyl phosphoric acid (HDBP) at concentrations averaging 30--50 mg/L. Dibutyl phosphoric acid, in turn, is in equilibrium with (HDBP){sub 2} and DBP{sup {minus}}. Uranium can form compounds with the dibutylphosphate ion (DBP{sup {minus}}) which have limited solubility, thereby creating a nuclear criticality safety issue. Literature reports and earlier SRTC tests have shown that it is feasiblemore » to precipitate U-DBP solid during the storage and processing of EU solutions. As a result, a series of solubility experiments were run at nitric acid concentrations from 0--4.0 M HNO{sub 3}, uranium at 0--90 g/L, and temperatures from 0--30 C. The data shows temperature and nitric acid concentration dependence consistent with what would be expected. With respect to uranium concentration, U-DBP solubility passes through a minimum between 6 and 12 g/L U at the acid concentrations and temperatures studied. However, the minimum shows a slight shift toward lower uranium concentrations at lower nitric acid concentrations. The shifts in solubility are strongly dependent upon the overall ionic strength of the solution. The data also reveal a shift to higher DBP solubility above 0.5 M HNO{sub 3} for both 6 g/L and 12 g/L uranium solutions. Analysis of U-DBP solids from the tests identified distinct differences between precipitates from less than 0.5 M solutions and those from greater than 4 M acid. Analyses identified UO{sub 2}(DBP){sub 2} as the dominant compound present at low acid concentrations in accordance with literature reports. As the acid concentration increases, the crystalline UO{sub 2}(DBP){sub 2} shows molecular substitutions and an increase in amorphous content.« less

Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel

DOE PAGES

Hames, Amber L.; Tkac, Peter; Paulenova, Alena; ...

2017-01-17

Here, an investigation of molybdate melts containing sodium molybdate (Na 2MoO 4) and molybdenum trioxide (MoO 3) to achieve the separation of uranium from fission products by crystallization has been performed. The separation is based on the difference in solubility of the fission product metal oxides compared to the uranium oxide or molybdate in the molybdate melt. The molybdate melt dissolves uranium dioxide at high temperatures, and upon cooling, uranium precipitates as uranium dioxide or molybdate, whereas the fission product metals remain soluble in the melt. Small-scale experiments using gram quantities of uranium dioxide have been performed to investigate themore » feasibility of UO 2 purification from the fission products. The composition of the uranium precipitate as well as data for partitioning of several fission product surrogates between the uranium precipitate and molybdate melt for various melt compositions are presented and discussed. The fission products Cs, Sr, Ru and Rh all displayed very large distribution ratios. The fission products Zr, Pd, and the lanthanides also displayed good distribution ratios (D > 10). A melt consisting of 20 wt% MoO 3-50 wt% Na 2MoO 4-30 wt% UO 2 heated to 1313 K and cooled to 1123 K for the physical separation of the UO 2 product from the melt, and washed once with Na 2MoO 4 displays optimum conditions for separation of the UO 2 from the fission products.« less

A graphene oxide/amidoxime hydrogel for enhanced uranium capture

PubMed Central

Wang, Feihong; Li, Hongpeng; Liu, Qi; Li, Zhanshuang; Li, Rumin; Zhang, Hongsen; Liu, Lianhe; Emelchenko, G. A.; Wang, Jun

2016-01-01

The efficient development of selective materials for the recovery of uranium from nuclear waste and seawater is necessary for their potential application in nuclear fuel and the mitigation of nuclear pollution. In this work, a graphene oxide/amidoxime hydrogel (AGH) exhibits a promising adsorption performance for uranium from various aqueous solutions, including simulated seawater. We show high adsorption capacities (Qm = 398.4 mg g−1) and high % removals at ppm or ppb levels in aqueous solutions for uranium species. In the presence of high concentrations of competitive ions such as Mg2+, Ca2+, Ba2+ and Sr2+, AGH displays an enhanced selectivity for uranium. For low uranium concentrations in simulated seawater, AGH binds uranium efficiently and selectively. The results presented here reveal that the AGH is a potential adsorbent for remediating nuclear industrial effluent and adsorbing uranium from seawater. PMID:26758649

Elevated Arsenic and Uranium Concentrations in Unregulated Water Sources on the Navajo Nation, USA.

PubMed

Hoover, Joseph; Gonzales, Melissa; Shuey, Chris; Barney, Yolanda; Lewis, Johnnye

2017-01-01

Regional water pollution and use of unregulated water sources can be an important mixed metals exposure pathway for rural populations located in areas with limited water infrastructure and an extensive mining history. Using censored data analysis and mapping techniques we analyzed the joint geospatial distribution of arsenic and uranium in unregulated water sources throughout the Navajo Nation, where over 500 abandoned uranium mine sites are located in the rural southwestern United States. Results indicated that arsenic and uranium concentrations exceeded national drinking water standards in 15.1 % (arsenic) and 12.8 % (uranium) of tested water sources. Unregulated sources in close proximity (i.e., within 6 km) to abandoned uranium mines yielded significantly higher concentrations of arsenic or uranium than more distant sources. The demonstrated regional trends for potential co-exposure to these chemicals have implications for public policy and future research. Specifically, to generate solutions that reduce human exposure to water pollution from unregulated sources in rural areas, the potential for co-exposure to arsenic and uranium requires expanded documentation and examination. Recommendations for prioritizing policy and research decisions related to the documentation of existing health exposures and risk reduction strategies are also provided.

Radium and uranium concentrations and associated hydrogeochemistry in ground water in southwestern Pueblo County, Colorado

USGS Publications Warehouse

Felmlee, J. Karen; Cadigan, Robert Allen

1979-01-01

Radium and uranium concentrations in water from 37 wells tapping the aquifer system of the Dakota Sandstone and Purgatoire Formation in southwestern Pueblo County, Colorado, have a wide range of values and define several areas of high radioactivity in the ground water. Radium ranges from 0.3 to 420 picocuries per liter and has a median value of 8.8, and uranium ranges from 0.02 to 180 micrograms per liter and has a median value of 2.4. Radon concentrations, measured in 32 of the 37 wells, range from less than 100 picocuries per liter to as much as 27,000 and have a median value of 580. Relationships among the radioactive elements and 28 other geochemical parameters were studied by using correlation coefficients and R-mode factor analysis. Five factor groups were determined to represent major influences on water chemistry: (1) short-term solution reactions, (2) oxidation reactions, (3) hydrolysis reactions, (4) uranium distribution, and (5) long-term solution reactions. Uranium concentrations are most strongly influenced by oxidation reactions but also are affected by solution reactions and distribution of uranium in the rocks of the aquifer system. Radon and radium concentrations are mostly controlled by uranium distribution; radium also shows a moderate negative relationship with oxidation. To explain the statistical and spatial relationships among the parameters, a model was developed involving the selective leaching of uranium-bearing phases and metal sulfides which occur in discontinuous zones in sandstone and shale. When reducing conditions prevail, uranium is immobile, but radium can be taken into solution. When faults and associated fractured rocks allow oxidizing conditions to dominate, uranium can be taken into solution; radium can also be taken into solution, or it may become immobilized by coprecipitation with iron and manganese oxides or with barite. Several areas within the study area are discussed in terms of the model.

Physicochemical Characterization of Capstone Depleted Uranium Aerosols I: Uranium Concentration in Aerosols as a Function of Time and Particle Size

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

Parkhurst, MaryAnn; Cheng, Yung-Sung; Kenoyer, Judson L.

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols weremore » evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.« 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.

Occurrence and Distribution of Iron, Manganese, and Selected Trace Elements in Ground Water in the Glacial Aquifer System of the Northern United States

USGS Publications Warehouse

Groschen, George E.; Arnold, Terri L.; Morrow, William S.; Warner, Kelly L.

2009-01-01

Dissolved trace elements, including iron and manganese, are often an important factor in use of ground water for drinking-water supplies in the glacial aquifer system of the United States. The glacial aquifer system underlies most of New England, extends through the Midwest, and underlies portions of the Pacific Northwest and Alaska. Concentrations of dissolved trace elements in ground water can vary over several orders of magnitude across local well networks as well as across regions of the United States. Characterization of this variability is a step toward a regional screening-level assessment of potential human-health implications. Ground-water sampling, from 1991 through 2003, of the National Water-Quality Assessment (NAWQA) Program of the U.S. Geological Survey determined trace element concentrations in water from 847 wells in the glacial aquifer system. Dissolved iron and manganese concentrations were analyzed in those well samples and in water from an additional 743 NAWQA land-use and major-aquifer survey wells. The samples are from monitoring and water-supply wells. Concentrations of antimony, barium, beryllium, cadmium, chromium, cobalt, copper, iron, lead, manganese, molybdenum, nickel, selenium, strontium, thallium, uranium, and zinc vary as much within NAWQA study units (local scale; ranging in size from a few thousand to tens of thousands of square miles) as over the entire glacial aquifer system. Patterns of trace element concentrations in glacial aquifer system ground water were examined by using techniques suitable for a dataset with zero to 80 percent of analytical results reported as below detection. During the period of sampling, the analytical techniques changed, which generally improved the analytical sensitivity. Multiple reporting limits complicated the comparison of detections and concentrations. Regression on Order Statistics was used to model probability distributions and estimate the medians and other quantiles of the trace element concentrations. Strontium and barium were the most frequently detected and usually were present in the highest concentrations. Iron and manganese were the next most commonly detected and next highest in concentrations. Iron concentrations were the most variable with respect to the range of variations (both within local networks and aquifer-wide) and with respect to the disparity between magnitude of concentrations (detections) and the frequency of samples below reporting limits (nondetections). Antimony, beryllium, cadmium, silver, and thallium were detected too infrequently for substantial interpretation of their occurrence or distributions or potential human-health implications. For those elements that were more frequently detected, there are some geographic patterns in their occurrence that primarily reflect climate effects. The highest concentrations of several elements were found in the West-Central glacial framework area (High Plains and northern Plains areas). There are few important patterns for any element in relation to land use, well type, or network type. Shallow land-use (monitor) wells had iron concentrations generally lower than the glacial aquifer system wells overall and much lower than major-aquifer survey wells, which comprise mostly private- and public-supply wells. Unlike those for iron, concentration patterns for manganese were similar among shallow land-use wells and major-aquifer survey wells. An apparent relation between low pH and relatively low concentrations of many elements, except lead, may be more indicative of the relatively low dissolved-solids content in wells in the Northeastern United States that comprise the majority of low pH wells, than of a pH dependent pattern. Iron and manganese have higher concentrations and larger ranges of concentrations especially under more reducing conditions. Dissolved oxygen and well depth were related to iron and manganese concentrations. Redox conditions also affect several trace elements such

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.

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

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.

Potential for U sequestration with select minerals and sediments via base treatment.

PubMed

Emerson, Hilary P; Di Pietro, Silvina; Katsenovich, Yelena; Szecsody, Jim

2018-06-13

Temporary base treatment is a potential remediation technique for heavy metals through adsorption, precipitation, and co-precipitation with minerals. Manipulation of pH with ammonia gas injection may be especially useful for vadose zone environments as it does not require addition of liquids that would increase the flux towards groundwater. In this research, we conducted laboratory batch experiments to evaluate the changes in uranium mobility and mineral dissolution with base treatments including sodium hydroxide, ammonium hydroxide, and ammonia gas. Our data show that partitioning of uranium to the solid phase increases by several orders of magnitude following base treatment in the presence of different minerals and natural sediments from the Hanford site. The presence of dissolved calcium and carbonate play an important role in precipitation and co-precipitation of uranium at elevated pH. In addition, significant incongruent dissolution of bulk mineral phases occurs and likely leads to precipitation of secondary mineral phases. These secondary phases may remove uranium via adsorption, precipitation, and co-precipitation processes and may coat uranium phases with low solubility minerals as the pH returns to natural conditions. Copyright © 2018 Elsevier Ltd. All rights reserved.

Arsenic and uranium in private wells in Connecticut, 2013-15

USGS Publications Warehouse

Flanagan, Sarah M.; Brown, Craig J.

2017-05-03

The occurrence of arsenic and uranium in groundwater at concentrations that exceed drinking-water standards is a concern because of the potential adverse effects on human health. Some early studies of arsenic occurrence in groundwater considered anthropogenic causes, but more recent studies have focused on sources of naturally occurring arsenic to groundwater, such as minerals within aquifer materials that are in contact with groundwater. Arsenic and uranium in groundwater in New England have been shown to have a strong association to the geologic setting and nearby streambed sediment concentrations. In New Hampshire and Massachusetts, arsenic and uranium concentrations greater than human-health benchmarks have shown distinct spatial patterns when related to the bedrock units mapped at the local scale.The Connecticut Department of Public Health (DPH) reported that there are about 322,600 private wells in Connecticut serving approximately 823,000 people, or 23 percent of the State’s population. The State does not require that existing private wells be routinely tested for arsenic, uranium, or other contaminants; consequently, private wells are only sampled at the well owner’s discretion or when they are newly constructed. The U.S. Geological Survey (USGS), in cooperation with the DPH, completed an assessment in 2016 on the distribution of concentrations of arsenic and uranium in groundwater from bedrock in Connecticut. This report presents the major findings for arsenic and uranium concentrations from water samples collected from 2013 to 2015 from private wells.

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.

Radioactive springs geochemical data related to uranium exploration

USGS Publications Warehouse

Cadigan, R.A.; Felmlee, J.K.

1977-01-01

Radioactive mineral springs and wells at 33 localities in the States of Colorado, Utah, Arizona and New Mexico in the United States were sampled and studied to obtain geochemical data which might be used for U exploration. The major source of radioactivity at mineral spring sites is 226Ra. Minor amounts of 228Ra, 238U and 232Th are also present. Ra is presumed to have been selectively removed from possibly quite deep uranium-mineralized rock by hydrothermal solutions and is either precipitated at the surface or added to fresh surface water. In this way, the source rocks influence the geochemistry of the spring waters and precipitates. Characteristics of the spring waters at or near the surface are also affected by variations in total dissolved solids, alkalinity, temperature and co-precipitation. Spring precipitates, both hard and soft, consist of four major types: (1) calcite travertine; (2) iron- and arsenic-rich precipitates; (3) manganese- and barium-rich precipitates; and (4) barite, in some instances accompanied by S, Ra and U, if present in the spring water, are co-precipitated with the barite, Mn-Ba and Fe-As precipitates. Using parameters based on U and Ra concentrations in waters and precipitates springsite areas are tentatively rated for favourability as potential uraniferous areas. ?? 1977.

Stream-water and groundwater quality in and near the Citizen Potawatomi Nation Tribal Jurisdictional Area, Pottawatomie County, Oklahoma, 2012-13

USGS Publications Warehouse

Becker, Carol J.

2014-01-01

Concentrations of the radionuclide uranium ranged from 0.03 to 79.5 µg/L, with a median concentration of 1.9 µg/L in the 30 groundwater samples collected. Two of the groundwater samples collected for this study had uranium concentrations exceeding the MCL of 30 µg/L, with concentrations of 79.5 and 31.1 µg/L. Generally, uranium concentrations were highest in water samples collected from wells completed in the Wellington Formation and the Chase, Council Grove, and Admire Groups in the southern and eastern parts of the study area.

Surface-water hydrology and quality, and macroinvertebrate and smallmouth bass populations in four stream basins in southwestern Wisconsin, 1987-90

USGS Publications Warehouse

Graczyk, David J.; Lillie, Richard A.; Schlesser, Roger A.; Mason, John W.; Lyons, John D.; Kerr, Roger A.; Graczyk, David J.

1993-01-01

Low concentrations of dissolved oxygen constituted the most detrimental water-quality problem affecting smallmouth bass populations. Dissolved-oxygen concentrations were occasionally less than 3 milligrams per liter, a dissolved-oxygen concentration that may be detrimental to early-life stages of smallmouth bass in the streams; however, smallmouth bass were apparently able to withstand these low dissolved-oxygen concentrations and seem to have survived in some situations when dissolved-oxygen concentration decreased to1 milligram per liter.

METHODS OF PREPARATION OF ELEMENT 95

DOEpatents

Seaborg, G.T.; James, R.A.

1962-07-17

A process of making americium by bombarding plutonium or uranium with neutrons or deuterons and aging the mass for decay of the plutonium formed to americium is described. The americium may then be separated by dissolving the mass in aqueous acid and carrier precipitation of the americium, especially on lanthanum or cerous fluoride. (AEC)

Processing fissile material mixtures containing zirconium and/or carbon

DOEpatents

Johnson, Michael Ernest; Maloney, Martin David

2013-07-02

A method of processing spent TRIZO-coated nuclear fuel may include adding fluoride to complex zirconium present in a dissolved TRIZO-coated fuel. Complexing the zirconium with fluoride may reduce or eliminate the potential for zirconium to interfere with the extraction of uranium and/or transuranics from fission materials in the spent nuclear fuel.

Method for oxygen reduction in a uranium-recovery process. [US DOE patent application

DOEpatents

Hurst, F.J.; Brown, G.M.; Posey, F.A.

1981-11-04

An improvement in effecting uranium recovery from phosphoric acid solutions is provided by sparging dissolved oxygen contained in solutions and solvents used in a reductive stripping stage with an effective volume of a nonoxidizing gas before the introduction of the solutions and solvents into the stage. Effective volumes of nonoxidizing gases, selected from the group consisting of argon, carbon dioxide, carbon monoxide, helium, hydrogen, nitrogen, sulfur dioxide, and mixtures thereof, displace oxygen from the solutions and solvents thereby reduce deleterious effects of oxygen such as excessive consumption of elemental or ferrous iron and accumulation of complex iron phosphates or cruds.

URANIUM DECONTAMINATION

DOEpatents

Buckingham, J.S.; Carroll, J.L.

1959-12-22

A process is described for reducing the extractability of ruthenium, zirconium, and niobium values into hexone contained in an aqueous nitric acid uranium-containing solution. The solution is made acid-deficient, heated to between 55 and 70 deg C, and at that temperature a water-soluble inorganic thiosulfate is added. By this, a precipitate is formed which carries the bulk of the ruthenium, and the remainder of the ruthenium as well as the zirconium and niobium are converted to a hexone-nonextractable form. The rutheniumcontaining precipitate can either be removed from the solu tion or it can be dissolved as a hexone-non-extractable compound by the addition of sodium dichromate prior to hexone extraction.

PROCESS FOR THE PURIFICATION OF URANIUM

DOEpatents

Rosenfeld, S.

1959-01-20

A proccss is described for reclaiming uranium values from aqueous solutions containing U, Fe, Ni, Cu, and Cr comprising treating the solution with NH/sub 3/ to precipitate the: U, Fc, and Cr and leaving Cu and Ni in solution as ammonia complex ions. The precipitate is chlorinated with CCl/sub 4/ at an elevated temperature to convert the U, Tc, and Cr into their chlorides. The more volatile FeCl/sub 3/ and CrCl/sub 3/ are separated from the UCl/sub 4/. The process is used when U is treated in a calutron, and composite solutions are produccd which contain dissolved products of stainless steel.

Microbial release of 226Ra2+ from (Ba,Ra)SO4 sludges from uranium mine wastes.

PubMed Central

Fedorak, P M; Westlake, D W; Anders, C; Kratochvil, B; Motkosky, N; Anderson, W B; Huck, P M

1986-01-01

226Ra2+ is removed from uranium mine effluents by coprecipitation with BaSO4. (Ba,Ra)SO4 sludge samples from two Canadian mine sites were found to contain active heterotrophic populations of aerobic, anaerobic, denitrifying, and sulfate-reducing bacteria. Under laboratory conditions, sulfate reduction occurred in batch cultures when carbon sources such as acetate, glucose, glycollate, lactate, or pyruvate were added to samples of (Ba,Ra)SO4 sludge. No external sources of nitrogen or phosphate were required for this activity. Further studies with lactate supplementation showed that once the soluble SO4(2-) in the overlying water was depleted, Ba2+ and 226Ra2+ were dissolved from the (Ba,Ra)SO4 sludge, with the concurrent production of S2-. Levels of dissolved 226Ra2+ reached approximately 400 Bq/liter after 10 weeks of incubation. Results suggest that the ultimate disposal of these sludges must maintain conditions to minimize the activity of the indigenous sulfate-reducing bacteria to ensure that unacceptably high levels of 226Ra2+ are not released to the environment. PMID:3752993

The absorption spectra of the complexes of uranium (VI) with some β-diketones

USGS Publications Warehouse

Feinstein, H.I.

1956-01-01

The absorption spectra of the complexes of uranium (VI) with four β-dike tones were determined under various conditions of pH, concentration of uranium, and alcohol concentration. Under optimum conditions, the maximum molar absorptivity (31,200) is obtained using 2-furoyltrifluoroacetone. This compares with about 4,000 and 19,000 for the thiocyanate and dibenzoylmethane complexes, respectively.

Uranium chemistry in stack solutions and leachates of phosphogypsum disposed at a coastal area in Cyprus.

PubMed

Lysandrou, M; Pashalidis, I

2008-02-01

The effect of the matrix composition (main constituents) on the concentration and chemical behavior of uranium in phosphogypsum stack solutions and leachates has been investigated. Solid and aqueous samples were taken from three different sub-areas of a phosphogypsum stack at a coastal area in Vasilikos (Cyprus). The sub-areas are characterized whether by their acidity (e.g. "aged" and "non-aged" phosphogypsum) or by their salt content, originating from pulping water during wet stacking or (after deposition) from the adjacent sea. Measurements in stack solutions and leachates showed that phosphogypsum characteristics affect both, the concentration and the chemical behavior of uranium in solution. Uranium concentration in solutions of increased salinity is up to three orders of magnitude higher than in solutions of low salinity and this is attributed to the effect of ionic strength on the solubility of phosphogypsum. Modelling showed that uranium in stack solutions is predominantly present in the form of uranium(VI) phosphate complexes (e.g. UO(2)(H(2)PO(4))(2), UO(2)HPO(4)), whereas in leachates uranium(VI) fluoro complexes (e.g. UO(2)F(2), UO(2)F(3)(-)) are predominant in solution. The latter indicates that elution of uranium from phosphogypsum takes places most probably in the form of fluoro complexes. Both, effective elution by saline water and direct migration of uranium to the sea, where it forms very stable uranium(VI) carbonato complexes, indicate that the adjacent sea will be the final receptor of uranium released from Vasilikos phosphogypsum.

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.

Inhibition of poly(ADP-ribose)polymerase-1 and DNA repair by uranium

PubMed Central

Cooper, Karen L.; Dashner, Erica J.; Tsosie, Ranalda; Cho, Young Mi; Lewis, Johnnye

2015-01-01

Uranium has radiological and non-radiological effects within biological systems and there is increasing evidence for genotoxic and carcinogenic properties attributable to uranium through its heavy metal properties. In this study, we report that low concentrations of uranium (as uranyl acetate; <10 μM) is not cytotoxic to human embryonic kidney cells or normal human keratinocytes; however, uranium exacerbates DNA damage and cytotoxicity induced by hydrogen peroxide, suggesting that uranium may inhibit DNA repair processes. Concentrations of uranyl acetate in the low micromolar range inhibited the zinc finger DNA repair protein poly(ADP-ribose) polymerase (PARP)-1 and caused zinc loss from PARP-1 protein. Uranyl acetate exposure also led to zinc loss from the zinc finger DNA repair proteins Xeroderma Pigmentosum, Complementation Group A (XPA) and aprataxin (APTX). In keeping with the observed inhibition of zinc finger function of DNA repair proteins, exposure to uranyl acetate enhanced retention of induced DNA damage. Co-incubation of uranyl acetate with zinc largely overcame the impact of uranium on PARP-1 activity and DNA damage. These findings present evidence that low concentrations of uranium can inhibit DNA repair through disruption of zinc finger domains of specific target DNA repair proteins. This may provide a mechanistic basis to account for the published observations that uranium exposure is associated with DNA repair deficiency in exposed human populations. PMID:26627003

Inhibition of poly(ADP-ribose)polymerase-1 and DNA repair by uranium.

PubMed

Cooper, Karen L; Dashner, Erica J; Tsosie, Ranalda; Cho, Young Mi; Lewis, Johnnye; Hudson, Laurie G

2016-01-15

Uranium has radiological and non-radiological effects within biological systems and there is increasing evidence for genotoxic and carcinogenic properties attributable to uranium through its heavy metal properties. In this study, we report that low concentrations of uranium (as uranyl acetate; <10 μM) is not cytotoxic to human embryonic kidney cells or normal human keratinocytes; however, uranium exacerbates DNA damage and cytotoxicity induced by hydrogen peroxide, suggesting that uranium may inhibit DNA repair processes. Concentrations of uranyl acetate in the low micromolar range inhibited the zinc finger DNA repair protein poly(ADP-ribose) polymerase (PARP)-1 and caused zinc loss from PARP-1 protein. Uranyl acetate exposure also led to zinc loss from the zinc finger DNA repair proteins Xeroderma Pigmentosum, Complementation Group A (XPA) and aprataxin (APTX). In keeping with the observed inhibition of zinc finger function of DNA repair proteins, exposure to uranyl acetate enhanced retention of induced DNA damage. Co-incubation of uranyl acetate with zinc largely overcame the impact of uranium on PARP-1 activity and DNA damage. These findings present evidence that low concentrations of uranium can inhibit DNA repair through disruption of zinc finger domains of specific target DNA repair proteins. This may provide a mechanistic basis to account for the published observations that uranium exposure is associated with DNA repair deficiency in exposed human populations. Copyright © 2015 Elsevier Inc. All rights reserved.

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.

Selective separation of iron from uranium in quantitative determination of traces of uranium by alpha spectrometry in soil/sediment sample.

PubMed

Singhal, R K; Narayanan, Usha; Karpe, Rupali; Kumar, Ajay; Ranade, A; Ramachandran, V

2009-04-01

During this work, controlled redox potential methodology was adopted for the complete separation of traces of uranium from the host matrix of mixed hydroxide of Iron. Precipitates of Fe(+2) and Fe(+3) along with other transuranic elements were obtained from acid leached solution of soil by raising the pH to 9 with 14N ammonia solution. The concentration of the uranium observed in the soil samples was 200-600 ppb, whereas in sediment samples, the concentration range was 61-400 ppb.

Transfer coefficient measurements of uranium to the organs of Wistar rats, as a function of the uranium content in the food.

PubMed

Arruda-Neto, J D; Likhachev, V P; Nogueira, G P; Araujo, G W; Camargo, S P; Cavalcante, G T; Cestari, A C; Craveiro, A M; Deppman, A; Ferreira, J W; Garcia, F; Geraldo, L P; Guzman, F; Helene, O M; Manso, M V; Martins, M N; Mesa, J; Oliveira, M F; Perez, G; Rodriguez, O; Tavares, M V; Vanin, V R

2001-06-01

Groups of animals (Wistar rats) were fed with rations doped with uranyl nitrate at concentrations ranging from 0.5 to 100 ppm. The uranium content in the ashes of the organs was measured by the neutron-fission track counting technique. The most striking result is that the transfer coefficients, as a function of the uranium concentration, exhibit a concave shape with a minimum around 20 ppm-U for all organs. Explanations to interpret this finding are tentatively given.

Specific Conductance and Dissolved-Solids Characteristics for the Green River and Muddy Creek, Wyoming, Water Years 1999-2008

USGS Publications Warehouse

Clark, Melanie L.; Davidson, Seth L.

2009-01-01

Southwestern Wyoming is an area of diverse scenery, wildlife, and natural resources that is actively undergoing energy development. The U.S. Department of the Interior's Wyoming Landscape Conservation Initiative is a long-term science-based effort to assess and enhance aquatic and terrestrial habitats at a landscape scale, while facilitating responsible energy development through local collaboration and partnerships. Water-quality monitoring has been conducted by the U.S. Geological Survey on the Green River near Green River, Wyoming, and Muddy Creek near Baggs, Wyoming. This monitoring, which is being conducted in cooperation with State and other Federal agencies and as part of the Wyoming Landscape Conservation Initiative, is in response to concerns about potentially increased dissolved solids in the Colorado River Basin as a result of energy development. Because of the need to provide real-time dissolved-solids concentrations for the Green River and Muddy Creek on the World Wide Web, the U.S. Geological Survey developed regression equations to estimate dissolved-solids concentrations on the basis of continuous specific conductance using relations between measured specific conductance and dissolved-solids concentrations. Specific conductance and dissolved-solids concentrations were less varied and generally lower for the Green River than for Muddy Creek. The median dissolved-solids concentration for the site on the Green River was 318 milligrams per liter, and the median concentration for the site on Muddy Creek was 943 milligrams per liter. Dissolved-solids concentrations ranged from 187 to 594 milligrams per liter in samples collected from the Green River during water years 1999-2008. Dissolved-solids concentrations ranged from 293 to 2,485 milligrams per liter in samples collected from Muddy Creek during water years 2006-08. The differences in dissolved-solids concentrations in samples collected from the Green River compared to samples collected from Muddy Creek reflect the different basin characteristics. Relations between specific conductance and dissolved-solids concentrations were statistically significant for the Green River (p-value less than 0.001) and Muddy Creek (p-value less than 0.001); therefore, specific conductance can be used to estimate dissolved-solids concentrations. Using continuous specific conductance values to estimate dissolved solids in real-time on the World Wide Web increases the amount and improves the timeliness of data available to water managers for assessing dissolved-solids concentrations in the Colorado River Basin.

SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES

DOEpatents

Maddock, A.G.; Booth, A.H.

1960-09-13

Separation of plutonium present in small amounts from neutron irradiated uranium by making use of the phenomenon of chemisorption is described. Plutonium in the tetravalent state is chemically absorbed on a fluoride in solid form. The steps for the separation comprise dissolving the irradiated uranium in nitric acid, oxidizing the plutonium in the resulting solution to the hexavalent state, adding to the solution a soluble calcium salt which by the common ion effect inhibits dissolution of the fluoride by the solution, passing the solution through a bed or column of subdivided calcium fluoride which has been sintered to about 8OO deg C to remove the chemisorbable fission products, reducing the plutonium in the solution thus obtained to the tetravalent state, and again passing the solution through a similar bed or column of calcium fluoride to selectively absorb the plutonium, which may then be recovered by treating the calcium fluoride with a solution of ammonium oxalate.

A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer

DOE PAGES

Abney, C. W.; Das, S.; Mayes, R. T.; ...

2016-08-01

Development of technology to harvest the uranium dissolved in seawater would enable access to vast quantities of this critical metal for nuclear power generation. Amidoxime polymers are the most promising platform for achieving this separation, yet design of advanced adsorbents is hindered by uncertainty regarding the uranium binding mode. In this work we use XAFS to investigate the uranium coordination environment in an amidoxime-phosphonic acid copolymer adsorbent. In contrast to the binding mode predicted computationally and from small molecule studies, a cooperative chelating model is favoured, attributable to emergent behavior resulting from inclusion of amidoxime in a polymer. Samples exposedmore » to seawater also display a feature consistent with a 2-oxo-bridged transition metal, suggesting formation of an in situ specific binding site. As a result, these findings challenge long held assumptions and provide new opportunities for the design of advanced adsorbent materials.« less

Radium geochemical monitoring in well waters at regional and local scales: an environmental impact indicator-based approach.

PubMed

Lagacé, François; Foucher, Delphine; Surette, Céline; Clarisse, Olivier

2018-04-18

To assess radium ( 226 Ra) as a potential indicator of impact in well waters, we investigated its behavior under natural conditions using a case study approach. 226 Ra geochemistry was investigated in 67 private wells of southeastern New Brunswick, Canada, a region targeted for potential shale gas exploitation. Objectives were to i) establish 226 Ra baseline in groundwater; ii) characterize 226 Ra spatial distribution and temporal variability; iii) characterize 226 Ra partitioning between dissolved phase and particulate forms in well waters; and iv) understand the mechanisms controlling 226 Ra mobility under natural environmental settings. 226 Ra levels were generally low (median = 0.061 pg L -1 , or 2.2 mBq L -1 ), stable over time, and randomly distributed. A principal component analysis revealed that concentrations of 226 Ra were controlled by key water geochemistry factors: the highest levels were observed in waters with high hardness, and/or high concentrations of individual alkaline earth elements (i.e. Mg, Ca, Sr, Ba), high concentrations of Mn and Fe, and low pH. As for partitioning, 226 Ra was essentially observed in the dissolved phase (106 ± 19%) suggesting that the geochemical conditions of groundwater in the studied regions are prone to limit 226 Ra sorption, enhancing its mobility. Overall, this study provided comprehensive knowledge on 226 Ra background distribution at local and regional scales. Moreover, it provided a framework to establish 226 Ra baselines and determine which geochemical conditions to monitor in well waters in order to use this radionuclide as an indicator of environmental impact caused by anthropogenic activities (e.g. unconventional shale gas exploitation, uranium mining, or nuclear generating power plants). Copyright © 2018 Elsevier Ltd. All rights reserved.

Kinetics of dissolution of UO2 in nitric acid solutions: A multiparametric study of the non-catalysed reaction

NASA Astrophysics Data System (ADS)

Cordara, T.; Szenknect, S.; Claparede, L.; Podor, R.; Mesbah, A.; Lavalette, C.; Dacheux, N.

2017-12-01

UO2 pellets were prepared by densification of oxides obtained from the conversion of the oxalate precursor. Then characterized in order to perform a multiparametric study of the dissolution in nitric acid medium. In this frame, for each sample, the densification rate, the grain size and the specific surface area of the prepared pellets were determined prior to the final dissolution experiments. By varying the concentration of the nitric acid solution and temperature, three different and successive steps were identified during the dissolution. Under the less aggressive conditions considered, a first transient step corresponding to the dissolution of the most reactive phases was observed at the solid/solution interface. Then, for all the tested conditions, a steady state step was established during which the normalised dissolution rate was found to be constant. It was followed by a third step characterized by a strong and continuous increase of the normalised dissolution rate. The duration of the steady state, also called "induction period", was found to vary drastically as a function of the HNO3 concentration and temperature. However, independently of the conditions, this steady state step stopped at almost similar dissolved material weight loss and dissolved uranium concentration. During the induction period, no important evolution of the topology of the solid/liquid interface was evidenced authorizing the use of the starting reactive specific surface area to evaluate the normalised dissolution rates thus the chemical durability of the sintered pellets. From the multiparametric study of UO2 dissolution proposed, oxidation of U(IV) to U(VI) by nitrate ions at the solid/liquid interface constitutes the limiting step in the overall dissolution mechanism associated to this induction period.

Groundwater uranium and cancer incidence in South Carolina

PubMed Central

Wagner, Sara E.; Burch, James B.; Bottai, Matteo; Puett, Robin; Porter, Dwayne; Bolick-Aldrich, Susan; Temples, Tom; Wilkerson, Rebecca C.; Vena, John E.; Hébert, James R.

2012-01-01

Objective This ecologic study tested the hypothesis that census tracts with elevated groundwater uranium and more frequent groundwater use have increased cancer incidence. Methods Data sources included: incident total, leukemia, prostate, breast, colorectal, lung, kidney, and bladder cancers (1996–2005, SC Central Cancer Registry); demographic and groundwater use (1990 US Census); and groundwater uranium concentrations (n = 4,600, from existing federal and state databases). Kriging was used to predict average uranium concentrations within tracts. The relationship between uranium and standardized cancer incidence ratios was modeled among tracts with substantial groundwater use via linear or semiparametric regression, with and without stratification by the proportion of African Americans in each area. Results A total of 134,685 cancer cases were evaluated. Tracts with ≥50% groundwater use and uranium concentrations in the upper quartile had increased risks for colorectal, breast, kidney, prostate, and total cancer compared to referent tracts. Some of these relationships were more likely to be observed among tracts populated primarily by African Americans. Conclusion SC regions with elevated groundwater uranium and more groundwater use may have an increased incidence of certain cancers, although additional research is needed since the design precluded adjustment for race or other predictive factors at the individual level. PMID:21080052

Effect of uranium(VI) speciation on simultaneous microbial reduction of uranium(VI) and iron(III).

PubMed

Stewart, Brandy D; Amos, Richard T; Fendorf, Scott

2011-01-01

Uranium is a pollutant of concern to both human and ecosystem health. Uranium's redox state often dictates whether it will reside in the aqueous or solid phase and thus plays an integral role in the mobility of uranium within the environment. In anaerobic environments, the more oxidized and mobile form of uranium (UO2(2+) and associated species) may be reduced, directly or indirectly, by microorganisms to U(IV) with subsequent precipitation of UO. However, various factors within soils and sediments, such as U(VI) speciation and the presence of competitive electron acceptors, may limit biological reduction of U(VI). Here we examine simultaneous dissimilatory reduction of Fe(III) and U(VI) in batch systems containing dissolved uranyl acetate and ferrihydrite-coated sand. Varying amounts of calcium were added to induce changes in aqueous U(VI) speciation. The amount of uranium removed from solution during 100 h of incubation with S. putrefaciens was 77% in absence of Ca or ferrihydrite, but only 24% (with ferrihydrite) and 14% (without ferrihydrite) were removed for systems with 0.8 mM Ca. Dissimilatory reduction of Fe(III) and U(VI) proceed through different enzyme pathways within one type of organism. We quantified the rate coefficients for simultaneous dissimilatory reduction of Fe(III) and U(VI) in systems varying in Ca concecentration (0-0.8 mM). The mathematical construct, implemented with the reactive transport code MIN3P, reveals predominant factors controlling rates and extent of uranium reduction in complex geochemical systems.

Salt transport extraction of transuranium elements from LWR fuel

DOEpatents

Pierce, R.D.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R.; Miller, W.E.

1992-11-03

A process is described for separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl[sub 2] and a Cu--Mg alloy containing not less than about 25% by weight Mg at a temperature in the range of from about 750 C to about 850 C to precipitate uranium metal and some of the noble metal fission products leaving the Cu--Mg alloy having transuranium actinide metals and rare earth fission product metals and some of the noble metal fission products dissolved therein. The CaCl[sub 2] having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO[sub 2]. The Ca metal and CaCl[sub 2] is recycled to reduce additional oxide fuel. The Cu--Mg alloy having transuranium metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with a transport salt including MgCl[sub 2] to transfer Mg values from the transport salt to the Cu--Mg alloy while transuranium actinide and rare earth fission product metals transfer from the Cu--Mg alloy to the transport salt. Then the transport salt is mixed with a Mg--Zn alloy to transfer Mg values from the alloy to the transport salt while the transuranium actinide and rare earth fission product values dissolved in the salt are reduced and transferred to the Mg--Zn alloy. 2 figs.

Salt transport extraction of transuranium elements from lwr fuel

DOEpatents

Pierce, R. Dean; Ackerman, John P.; Battles, James E.; Johnson, Terry R.; Miller, William E.

1992-01-01

A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl.sub.2 and a Cu--Mg alloy containing not less than about 25% by weight Mg at a temperature in the range of from about 750.degree. C. to about 850.degree. C. to precipitate uranium metal and some of the noble metal fission products leaving the Cu--Mg alloy having transuranium actinide metals and rare earth fission product metals and some of the noble metal fission products dissolved therein. The CaCl.sub.2 having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO.sub.2. The Ca metal and CaCl.sub.2 is recycled to reduce additional oxide fuel. The Cu--Mg alloy having transuranium metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with a transport salt including Mg Cl.sub.2 to transfer Mg values from the transport salt to the Cu--Mg alloy while transuranium actinide and rare earth fission product metals transfer from the Cu--Mg alloy to the transport salt. Then the transport salt is mixed with a Mg--Zn alloy to transfer Mg values from the alloy to the transport salt while the transuranium actinide and rare earth fission product values dissolved in the salt are reduced and transferred to the Mg--Zn alloy.

Isotopic Analysis of Uranium in NIST SRM Glass by Femtosecond Laser Ablation

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

Duffin, Andrew M.; Hart, Garret L.; Hanlen, Richard C.

We employed femtosecond Laser Ablation Multicollector Inductively Coupled Mass Spectrometry for the 11 determination of uranium isotope ratios in a series of standard reference material glasses (NIST 610, 612, 614, and 12 616). This uranium concentration in this series of SRM glasses is a combination of isotopically natural uranium in 13 the materials used to make the glass matrix and isotopically depleted uranium added to increase the uranium 14 elemental concentration across the series. Results for NIST 610 are in excellent agreement with literature values. 15 However, other than atom percent 235U, little information is available for the remaining glasses.more » We present atom 16 percent and isotope ratios for 234U, 235U, 236U, and 238U for all four glasses. Our results show deviations from the 17 certificate values for the atom percent 235U, indicating the need for further examination of the uranium isotopes in 18 NIST 610-616. Our results are fully consistent with a two isotopic component mixing between the depleted 19 uranium spike and natural uranium in the bulk glass.« less

An experimental and modeling study of grain-scale uranium desorption from field-contaminated sediments and the potential influence of microporosity on mass-transfer

NASA Astrophysics Data System (ADS)

Stoliker, D.; Liu, C.; Kent, D. B.; Zachara, J. M.

2012-12-01

The aquifer below the 300-Area of the Hanford site (Richland, WA, USA) is plagued by a persistent plume of dissolved uranium (U(VI)) in excess of the Environmental Protection Agency drinking water maximum contamination level even after the removal of highly contaminated sediments. The aquifer sediments in the seasonally saturated lower vadose zone act as both a source and sink for uranium during stage changes in the nearby Columbia River. Diffusion limitation of uranium mass-transfer within these sediments has been cited as a potential cause of the plume's persistence. Equilibrium U(VI) sorption is a strong function of variable chemical conditions, especially carbonate, hydrogen, and uranyl ion activities. Field-contaminated sediments from the site require up to 1,000 hours to reach equilibrium in static batch reactors. Increases in U(VI) concentrations over longer time-scales result from changes in chemical conditions, which drive reactions with sediments that favor U(VI) desorption. Grain-scale U(VI) sorption/desorption rates are slow, likely owing to diffusion of U(VI) and other solutes through intra-granular pore domains. In order to improve understanding of the impact of intra-granular diffusion and chemical reactions controlling grain-scale U(VI) release, experiments were conducted on individual particle size fractions of a <8 mm composite of field-contaminated, lower vadose zone sediments. For each size fraction, equilibrium U(VI) sorption/desorption in static batch reactors was well-described by surface complexation models over a range of chemical conditions applicable to the field site. Desorption rates from individual size fractions in flow-through batch reactors, examined under a single set of constant chemical conditions with multiple stop-flow events, were similar for all size fractions <2 mm. Kinetic U(VI) desorption in flow-through batch reactors was modeled using a multi-rate surface complexation approach, where sorption/desorption rates were assumed to be proportional to the displacement from equilibrium and multiple diffusion domains were described with a two-parameter lognormal distribution of mass-transfer rate coefficients. Parameters describing mass transfer were the same for all size fractions <2 mm but differed for the largest (2-8 mm) size fraction. The evolution of pH, along with dissolved cation and carbonate concentrations, was modeled using equilibrium cation exchange, rate-limited calcite dissolution, aerobic respiration, and silica dissolution. Desorption and chemical reaction models calibrated with individual size fractions predicted U(VI) and chemical composition as a function of time for the bulk sediment sample. Volumes of pores less than 2.4 nm, quantified using nitrogen adsorption-desorption isotherms, were the same for all size fractions < 2 mm, nearly double that of the 2-8 mm size fraction. Similarity in the observed pore volumes and multi-rate mass-transfer parameters across all size fractions <2 mm suggest the importance of pores in this size class in controlling slow grain-scale U(VI) desorption rates. Models like these provide a means for testing the influence of grain-scale mass-transfer on the persistence of U(VI) plume at the site.

Isotope hydrology of the Chalk River Laboratories site, Ontario, Canada

USGS Publications Warehouse

Peterman, Zell; Neymark, Leonid; King-Sharp, K.J.; Gascoyne, Mel

2016-01-01

This paper presents results of hydrochemical and isotopic analyses of groundwater (fracture water) and porewater, and physical property and water content measurements of bedrock core at the Chalk River Laboratories (CRL) site in Ontario. Density and water contents were determined and water-loss porosity values were calculated for core samples. Average and standard deviations of density and water-loss porosity of 50 core samples from four boreholes are 2.73 ± 12 g/cc and 1.32 ± 1.24 percent. Respective median values are 2.68 and 0.83 indicating a positive skewness in the distributions. Groundwater samples from four deep boreholes were analyzed for strontium (87Sr/86Sr) and uranium (234U/238U) isotope ratios. Oxygen and hydrogen isotope analyses and selected solute concentrations determined by CRL are included for comparison. Groundwater from borehole CRG-1 in a zone between approximately +60 and −240 m elevation is relatively depleted in δ18O and δ2H perhaps reflecting a slug of water recharged during colder climatic conditions. Porewater was extracted from core samples by centrifugation and analyzed for major dissolved ions and for strontium and uranium isotopes. On average, the extracted water contains 15 times larger concentration of solutes than the groundwater. 234U/238U and correlation of 87Sr/86Sr with Rb/Sr values indicate that the porewater may be substantially older than the groundwater. Results of this study show that the Precambrian gneisses at Chalk River are similar in physical properties and hydrochemical aspects to crystalline rocks being considered for the construction of nuclear waste repositories in other regions.

Non-enzymatic U(VI) interactions with biogenic mackinawite

NASA Astrophysics Data System (ADS)

Veeramani, H.; Qafoku, N. P.; Kukkadapu, R. K.; Murayama, M.; Hochella, M. F.

2011-12-01

Reductive immobilization of hexavalent uranium [U(VI)] by stimulation of dissimilatory metal and/or sulfate reducing bacteria (DMRB or DSRB) has been extensively researched as a remediation strategy for subsurface U(VI) contamination. These bacteria derive energy by reducing oxidized metals as terminal electron acceptors, often utilizing organic substrates as electron donors. Thus, when evaluating the potential for in-situ uranium remediation in heterogeneous subsurface media, it is important to understand how the presence of alternative electron acceptors such as Fe(III) and sulfate affect U(VI) remediation and the long term behavior and reactivity of reduced uranium. Iron, an abundant subsurface element, represents a substantial sink for electrons from DMRB, and the reduction of Fe(III) leads to the formation of dissolved Fe(II) or to reactive biogenic Fe(II)- and mixed Fe(II)/Fe(III)- mineral phases. Consequently, abiotic U(VI) reduction by reactive forms of biogenic Fe(II) minerals could be a potentially important process for uranium immobilization. In our study, the DMRB Shewanella putrefaciens CN32 was used to synthesize a biogenic Fe(II)-bearing sulfide mineral: mackinawite, that has been characterized by XRD, SEM, HRTEM and Mössbauer spectroscopy. Batch experiments involving treated biogenic mackinawite and uranium (50:1 molar ratio) were carried out at room temperature under strict anoxic conditions. Following complete removal of uranium from solution, the biogenic mackinawite was analyzed by a suite of analytical techniques including XAS, HRTEM and Mössbauer spectroscopy to determine the speciation of uranium and investigate concomitant Fe(II)-phase transformation. Determining the speciation of uranium is critical to success of a remediation strategy. The present work elucidates non-enzymatic/abiotic molecular scale redox interactions between biogenic mackinawite and uranium.

Water-quality assessment of the Rio Grande Valley, Colorado, New Mexico, and Texas : shallow ground-water quality and land use in the Albuquerque area, central New Mexico, 1993

USGS Publications Warehouse

Anderholm, Scott K.

1997-01-01

This report describes the quality of shallow ground water and the relations between land use and the quality of that shallow ground water in an urban area in and adjacent to Albuquerque, New Mexico. Water samples were collected from 24 shallow wells. Samples were analyzed for selected common constituents, nutrients, trace elements, radionuclides, volatile organic compounds, and pesticides. The study area, which is in the Albuquerque Basin in central New Mexico, was limited to the Rio Grande flood plain; depth to water in this area generally is less than 25 feet. The amount and composition of recharge to the shallow ground-water system are important factors that affect shallow ground-water composition in this area. Important sources of recharge that affect shallow ground-water quality in the area include infiltration of surface water, which is used in agricultural land-use areas to irrigate crops, and infiltration of septic-system effluent in residential areas. Agricultural land use represents about 28 percent of the area, and residential land use represents about 35 percent of the total study area. In most of the study area, agricultural land use is interspersed with residential land use and neither is the dominant land use in the area. Land use in the study area historically has been changing from agricultural to urban. The composition of shallow ground water in the study area varies considerably. The dissolved solids concentration in shallow ground water in the study area ranges from 272 to 1,650 milligrams per liter, although the relative percentages of selected cations and anions do not vary substantially. Calcium generally is the dominant cation and bicarbonate generally is the dominant anion. Concentrations of nutrients generally were less than 1 milligram per liter. The concentration of many trace elements in shallow ground water was below or slightly above 1 microgram per liter and there was little variation in the concentrations. Barium, iron, manganese, molybdenum, and uranium were the only trace elements analyzed for that had median concentrations greater than 5 micrograms per liter. Volatile organic compounds were detected in 5 of 24 samples. Cis-1,2-dichloroethene and 1,1-dichloroethane were the most commonly detected volatile organic compounds (detected in two samples each). Pesticides were detected in 8 of 24 samples. Prometon was the most commonly detected pesticide (detected in 5 of 24 samples). Concentrations of volatile organic compounds and pesticides detected were much smaller than any U.S. Environmental Protection Agency standards that have been established. Infiltration of surface water and the evaporation or transpiration of this water, which partially is the result of past and present agricultural land use, seem to affect the concentrations of common constituents in shallow ground water in the study area. The small excess chloride in shallow ground water relative to surface water that has been affected by evaporation or transpiration could be due to mixing of shallow ground water with small amounts of precipitation/bulk deposition or septic-system effluent. Infiltration of septic-system effluent (residential land use) has affected the shallow ground-water composition in parts of the study area on the basis of the small dissolved oxygen concentrations, large dissolved organic carbon concentrations, and excess chloride. Despite the loading of nitrogen to the shallow ground-water system as the result of infiltration of septic-system effluent, the small nitrogen concentrations in shallow ground water probably are due to the small dissolved oxygen concentrations and relatively large dissolved organic carbon concentrations. The small concentrations and lack of variation of most trace elements indicate that land use has not substantially affected the concentration

Hydrological and Geochemical Influences on the Dissolved Silica Concentrations in Natural Water in a Steep Headwater Catchment

NASA Astrophysics Data System (ADS)

Asano, Y.; Uchida, T.; Ohte, N.

2002-12-01

Dissolved silica has been used as a useful indicator of a chemical weathering in many geochemical studies in natural environment. Previous hydrological studies indicated that various hydrological processes affect the dissolution and precipitation of silica in hillslope and transport of this silica to stream; however, information is still limited to link this knowledge to understand geochemical processes. The observations of dissolved silica concentration in groundwater, spring and stream water was conducted at the unchannelled hillslope in the Tanakami Mountains of central Japan; (1) to clarify the effects of preferential flowpaths including lateral and vertical flow in soil layer and flow through bedrock fracture in the variation of dissolved silica concentration in runoff and groundwater, and (2) to isolate the effects of mixing of water from geochemically diverse water sources on the dissolved silica concentration. The mean dissolved silica concentrations in soil water at 40 cm depth and transient groundwater formed in upslope area were relatively constant independent of the variation in the new water ratio. The mean dissolved silica concentrations were similar regardless of the sampling depth in soil although the mean residence times of water increase with depth. These results indicated that dissolved silica concentrations in soil water and transient groundwater were defined almost independent of contact time of water with minerals. While the mean dissolved silica concentration in perennial groundwater, which was recharged by infiltrating water through soil and water emerging from bedrock in a area near to spring, was more than twice that of transient groundwater and the variation was relatively large. The mean dissolved silica concentration increased significantly at downslope from perennial groundwater, spring to the stream and the spring and stream concentrations also showed large variation. The dissolved silica concentrations of those perennial groundwater, the spring and the stream was controlled by the mixing of water from soil and bedrock. Our results demonstrated that in most areas of this headwater catchment, the preferential flowpaths give only small effect on dissolved silica concentrations. While in a small area (less than 10% of the longitudinal axis of the hollow near the spring), the dissolved silica concentration were controlled by the mixing of water from geochemically diverse water sources.

Analysis of the 2H-evaporator scale samples (HTF-17-56, -57)

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

Hay, M.; Coleman, C.; Diprete, D.

Savannah River National Laboratory analyzed scale samples from both the wall and cone sections of the 242-16H Evaporator prior to chemical cleaning. The samples were analyzed for uranium and plutonium isotopes required for a Nuclear Criticality Safety Assessment of the scale removal process. The analysis of the scale samples found the material to contain crystalline nitrated cancrinite and clarkeite. Samples from both the wall and cone contain depleted uranium. Uranium concentrations of 16.8 wt% 4.76 wt% were measured in the wall and cone samples, respectively. The ratio of plutonium isotopes in both samples is ~85% Pu-239 and ~15% Pu-238 bymore » mass and shows approximately the same 3.5 times higher concentration in the wall sample versus the cone sample as observed in the uranium concentrations. The mercury concentrations measured in the scale samples were higher than previously reported values. The wall sample contains 19.4 wt% mercury and the cone scale sample 11.4 wt% mercury. The results from the current scales samples show reasonable agreement with previous 242-16H Evaporator scale sample analysis; however, the uranium concentration in the current wall sample is substantially higher than previous measurements.« 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

ACTUAL WASTE TESTING OF GYCOLATE IMPACTS ON THE SRS TANK FARM

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

Martino, C.

2014-05-28

Glycolic acid is being studied as a replacement for formic acid in the Defense Waste Processing Facility (DWPF) feed preparation process. After implementation, the recycle stream from DWPF back to the high-level waste Tank Farm will contain soluble sodium glycolate. Most of the potential impacts of glycolate in the Tank Farm were addressed via a literature review and simulant testing, but several outstanding issues remained. This report documents the actual-waste tests to determine the impacts of glycolate on storage and evaporation of Savannah River Site high-level waste. The objectives of this study are to address the following: Determine the extentmore » to which sludge constituents (Pu, U, Fe, etc.) dissolve (the solubility of sludge constituents) in the glycolate-containing 2H-evaporator feed. Determine the impact of glycolate on the sorption of fissile (Pu, U, etc.) components onto sodium aluminosilicate solids. The first objective was accomplished through actual-waste testing using Tank 43H and 38H supernatant and Tank 51H sludge at Tank Farm storage conditions. The second objective was accomplished by contacting actual 2H-evaporator scale with the products from the testing for the first objective. There is no anticipated impact of up to 10 g/L of glycolate in DWPF recycle to the Tank Farm on tank waste component solubilities as investigated in this test. Most components were not influenced by glycolate during solubility tests, including major components such as aluminum, sodium, and most salt anions. There was potentially a slight increase in soluble iron with added glycolate, but the soluble iron concentration remained so low (on the order of 10 mg/L) as to not impact the iron to fissile ratio in sludge. Uranium and plutonium appear to have been supersaturated in 2H-evaporator feed solution mixture used for this testing. As a result, there was a reduction of soluble uranium and plutonium as a function of time. The change in soluble uranium concentration was independent of added glycolate concentration. The change in soluble plutonium content was dependent on the added glycolate concentration, with higher levels of glycolate (5 g/L and 10 g/L) appearing to suppress the plutonium solubility. The inclusion of glycolate did not change the dissolution of or sorption onto actual-waste 2H-evaporator pot scale to an extent that will impact Tank Farm storage and concentration. The effects that were noted involved dissolution of components from evaporator scale and precipitation of components onto evaporator scale that were independent of the level of added glycolate.« less

Uranium Anodic Dissolution under Slightly Alkaline Conditions Progress Report Full-Scale Demonstration with DU Foil

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

Gelis, A.; Brown, M. A.; Wiedmeyer, S.

2014-02-18

Argonne National Laboratory (Argonne) is developing an alternative method for digesting irradiated low enriched uranium (LEU) foil targets to produce 99Mo in neutral/alkaline media. This method consists of the electrolytic dissolution of irradiated uranium foil in sodium bicarbonate solution, followed by precipitation of base-insoluble fission and activation products, and uranyl-carbonate species with CaO. The addition of CaO is vital for the effective anion exchange separation of 99MoO 4 2- from the fission products, since most of the interfering anions (e.g., CO 3 2-) are removed from the solution, while molybdate remains in solution. An anion exchange is used to retainmore » and to purify the 99Mo from the filtrate. The electrochemical dissolver has been designed and fabricated in 304 stainless-steel (SS), and tested for the dissolution of a full-size depleted uranium (DU) target, wrapped in Al foil. Future work will include testing with low-burn-up DU foil at Argonne and later with high-burn-up LEU foils at Oak Ridge National Laboratory.« less

Construction of the Syngonium podophyllum-Pseudomonas sp. XNN8 Symbiotic Purification System and Investigation of Its Capability of Remediating Uranium Wastewater.

PubMed

Deng, Qin-Wen; Wang, Yong-Dong; Ding, De-Xin; Hu, Nan; Sun, Jing; He, Jia-Dong; Xu, Fei

2017-02-01

The endophyte Pseudomonas sp. XNN8 was separated from Typha orientalis which can secrete indole-3-acetic acid and 1-aminocyclopropane-1-carboxylate deaminase and siderophores and has strong resistance to uranium it was then colonized in the Syngonium podophyllum; and the S. podophyllum-Pseudomonas sp. XNN8 symbiotic purification system (SPPSPS) for uranium-containing wastewater was constructed. Afterwards, the hydroponic experiments to remove uranium from uranium-containing wastewater by the SPPSPS were conducted. After 24 days of treatment, the uranium concentrations of the wastewater samples with uranium concentrations between 0.5 and 5.0 mg/L were lowered to below 0.05 mg/L. Furthermore, the uranium in the plants was assayed using Fourier transform infrared spectroscopy (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. The Pseudomonas sp. XNN8 was found to generate substantial organic groups in the roots of the Syngonium podophyllum, which could improve the complexing capability of S. podophyllum for uranium. The uranium in the roots of S. podophyllum was found to be the uranyl phosphate (47.4 %) and uranyl acetate (52.6 %).

Water-quality assessment of the Rio Grande Valley, Colorado, New Mexico and Texas; ground-water quality in the Rio Grande flood plain, Cochiti Lake, New Mexico, to El Paso, Texas, 1995

USGS Publications Warehouse

Bexfield, L.M.; Anderholm, S.K.

1997-01-01

From March to May of 1995, water samples were collected from 30 wells located in the flood plain of the Rio Grande between Cochiti Lake, New Mexico, and El Paso, Texas. These samples were analyzed for a broad host of constituents, including field parameters, major constituents, nutrients, dissolved organic carbon, trace elements, radiochemicals, pesticides, and volatile organic compounds. The main purpose of this study was to observe the quality of ground water in this part of the Rio Grande Valley study unit of the U.S. Geological Survey National Water-Quality Assessment program. The sampling effort was limited to the basin- fill aquifer beneath the above-defined reach of the Rio Grande flood plain because of the relative homogeneity of the hydrogeology, the large amount of ground-water use for public supply, and the potential for land-use activities to affect the quality of ground water. Most of the wells sampled for the study are used for domestic purposes, including drinking water. Depths to the tops of the sampling intervals in the 30 wells ranged from 10 to 345 feet below land surface, and the median was 161.5 feet; the sampling intervals in most of the wells spanned about 10 feet or less. Quality-control data were collected at three of the wells. A significant amount of variation was found in the chemical composition of ground water sampled throughout the study area, but the water generally was found to be of suitable chemical quality for use as drinking water, according to current enforceable standards established by the U.S. Environmental Protection Agency (EPA). Nutrients generally were measured at concentrations near or below their method reporting limits. The most dominant nutrient species was nitrite plus nitrate, at a maximum concentration of 1.9 milligrams per liter (as N). Only eight of the trace elements analyzed for had median concentrations greater than their respective minimum reporting levels. Water from one well exceeded the lifetime health advisory established by the EPA for molybdenum; water from a different well exceeded the proposed EPA maximum contaminant level for uranium. Gross alpha and gross beta particle activities generally appeared to strongly correlate with quantities of uranium and potassium, respectively, detected in ground water. However, water from one well exceeded the EPA maximum contaminant level for gross alpha particle activity and may exceed the EPA maximum contaminant level for beta particle and photon activity, although current data on gross beta particle activities are not conclusive on this point. Radon concentrations did not appear to directly correlate with uranium concentrations. The herbicide prometon was the only synthetic organic compound detected in ground water in the study area, and was detected in only one well, at a concentration of 0.038 microgram per liter. This well is shallow and is not used for drinking water. With the exception of the one detection of prometon, no strong evidence was found of effects on ground-water quality from human activities. Therefore, most of the water sampled probably recharged at the margins of the alluvial basins or recharged through the flood plain before human development began. With respect to major constituents, the concentrations of dissolved solids ranged from 209 to 3,380 milligrams per liter, and the median concentration was 409.5 milligrams per liter. There is evidence that the overall chemical composition of ground water in the study area may be affected by several processes, including cation exchange, feldspar weathering, calcite dissolution and precipitation, dissolution of volcanic glass, and microbial activity. Several chemical constituents in ground water showed relatively distinct spatial patterns that appear to be related to one or more of these processes.

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.

Concentrations of dissolved oxygen in the lower Puyallup and White rivers, Washington, August and September 2000 and 2001

USGS Publications Warehouse

Ebbert, J.C.

2002-01-01

The U.S. Geological Survey, Washington State Department of Ecology, and Puyallup Tribe of Indians conducted a study in August and September 2001 to assess factors affecting concentrations of dissolved oxygen in the lower Puyallup and White Rivers, Washington. The study was initiated because observed concentrations of dissolved oxygen in the lower Puyallup River fell to levels ranging from less than 1 milligram per liter (mg/L) to about 6 mg/L on several occasions in September 2000. The water quality standard for the concentration of dissolved oxygen in the Puyallup River is 8 mg/L.This study concluded that inundation of the sensors with sediment was the most likely cause of the low concentrations of dissolved oxygen observed in September 2000. The conclusion was based on (1) knowledge gained when a dissolved-oxygen sensor became covered with sediment in August 2001, (2) the fact that, with few exceptions, concentrations of dissolved oxygen in the lower Puyallup and White Rivers did not fall below 8 mg/L in August and September 2001, and (3) an analysis of other mechanisms affecting concentrations of dissolved oxygen.The analysis of other mechanisms indicated that they are unlikely to cause steep declines in concentrations of dissolved oxygen like those observed in September 2000. Five-day biochemical oxygen demand ranged from 0.22 to 1.78 mg/L (mean of 0.55 mg/L), and river water takes only about 24 hours to flow through the study reach. Photosynthesis and respiration cause concentrations of dissolved oxygen in the lower Puyallup River to fluctuate as much as about 1 mg/L over a 24-hour period in August and September. Release of water from Lake Tapps for the purpose of hydropower generation often lowered concentrations of dissolved oxygen downstream in the White River by about 1 mg/L. The effect was smaller farther downstream in the Puyallup River at river mile 5.8, but was still observable as a slight decrease in concentrations of dissolved oxygen caused by photosynthesis and respiration. The upper limit on oxygen demand caused by the scour of anoxic bed sediment and subsequent oxidation of reduced iron and manganese is less than 1 mg/L. The actual demand, if any, is probably negligible.In August and September 2001, concentrations of dissolved oxygen in the lower Puyallup River did not fall below the water-quality standard of 8 mg/L, except at high tide when the saline water from Commencement Bay reached the monitor at river mile 2.9. The minimum concentration of dissolved oxygen (7.6 mg/L) observed at river mile 2.9 coincided with the maximum value of specific conductance. Because the dissolved-oxygen standard for marine water is 6.0 mg/L, the standard was not violated at river mile 2.9. The concentration of dissolved oxygen at river mile 1.8 in the White River dropped below the water-quality standard on two occasions in August 2001. The minimum concentration of 7.8 mg/L occurred on August 23, and a concentration of 7.9 mg/L was recorded on August 13. Because there was some uncertainty in the monitoring record for those days, it cannot be stated with certainty that the actual concentration of dissolved oxygen in the river dropped below 8 mg/L. However, at other times when the quality of the monitoring record was good, concentrations as low as 8.2 mg/L were observed at river mile 1.8 in the White River.

Immobilization of uranium into magnetite from aqueous solution by electrodepositing approach.

PubMed

Lu, Bing-Qing; Li, Mi; Zhang, Xiao-Wen; Huang, Chun-Mei; Wu, Xiao-Yan; Fang, Qi

2018-02-05

Immobilization of uranium into magnetite (Fe 3 O 4 ), which was generated from metallic iron by electrochemical method, was proposed to rapidly remove uranium from aqueous solution. The effects of electrochemical parameters such as electrode materials, voltage, electrode gap, reaction time and pH value on the crystallization of Fe 3 O 4 and uranium removal efficiencies were investigated. More than 90% uranium in the solution was precipitated with Fe 3 O 4 under laboratory conditions when uranium concentration range from 0.5mg/L to 10mg/L. The Fe 3 O 4 crystallization mechanism and immobilization of uranium was proved by XPS, XRD, TEM, FTIR and VSM methods. The results indicated that the cationic (including Fe 2+ , Fe 3+ and U(VI)) migrate to cathode side under the electric field and the uranium was incorporated or adsorbed by Fe 3 O 4 which was generated at cathode while the pH ranges between 2-7. The uranium-containing precipitate of Fe 3 O 4 can exist stably at the acid concentration below 60g/L. Furthermore, the precipitate may be used as valuable resources for uranium or iron recycling, which resulted in no secondary pollution in the removal of uranium from aqueous solution. Copyright © 2017. Published by Elsevier B.V.

Development of practical decontamination process for the removal of uranium from gravel.

PubMed

Kim, Ilgook; Kim, Gye-Nam; Kim, Seung-Soo; Choi, Jong-Won

2018-01-01

In this study, a practical decontamination process was developed to remove uranium from gravel using a soil washing method. The effects of critical parameters including particle size, H 2 SO 4 concentration, temperature, and reaction time on uranium removal were evaluated. The optimal condition for two-stage washing of gravel was found to be particle size of 1-2 mm, 1.0 M H 2 SO 4 , temperature of 60°C, and reaction time of 3 h, which satisfied the required uranium concentration for self-disposal. Furthermore, most of the extracted uranium was removed from the waste solution by precipitation, implying that the treated solution can be reused as washing solution. These results clearly demonstrated that our proposed process can be indeed a practical technique to decontaminate uranium-polluted gravel.

Dibutyl Phosphoric Acid Solubility in High-Acid, Uranium-Bearing Solutions at SRS

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

Pierce, R.A.

1998-10-02

The Savannah River Site has enriched uranium (EU) solution which has been stored for almost 10 years since being purified in the second uranium cycle of the H area solvent extraction process. The concentrations in solution are approximately 6 g/L U and about 0.1 M nitric acid. Residual tributylphosphate in the solutions has slowly hydrolyzed to form dibutyl phosphoric acid (HDBP) at concentrations averaging 50 mg/L. Uranium is known to form compounds with the dibutylphosphate ion (DBP) which have limited solubility. The potential to form uranium-DBP solids raises a nuclear criticality safety issue. Prior SRTC tests (WSRC-TR-98-00188) showed that U-DBPmore » solids precipitate at concentrations potentially attainable during the storage of enriched uranium solutions. Furthermore, evaporation of the existing EUS solution without additional acidification could result in the precipitation of U-DBP solids if the DBP concentration in the resulting solution exceeds 110 mg/L at ambient temperature. The same potential exists for evaporation of unwashed 1CU solutions. As a follow-up to the earlier studies, SRTC studied the solubility limits for solutions containing acid concentrations above 0.5M HNO3. The data obtained in these tests reveals a shift to higher levels of DBP solubility above 0.5M HNO3 for both 6 g/L and 12 g/L uranium solutions. Analysis of U-DBP solids from the tests identified a mixture of different molecular structures for the solids created. The analysis distinguished UO2(DBP)2 as the dominant compound present at low acid concentrations. As the acid concentration increases, the crystalline UO2(DBP)2 shows molecular substitutions and an increase in amorphous content. Further analysis by methods not available at SRS will be needed to better identify the specific compounds present. This data indicates that acidification prior to evaporation can be used to increase the margin of safety for the storage of the EUS solutions. Subsequent experimentation evaluated options for absorbing HDBP from solution using either activated carbon or anion exchange resin. The activated carbon outperformed the anion exchange resin. Activated carbon absorbs DBP rapidly and has demonstrated the capability of absorbing 15 mg of DBP per gram of activated carbon. Analytical results also show that activated carbon absorbs uranium up to 17 mg per gram of carbon. It is speculated that the uranium absorbed is part of a soluble U-DBP complex that has been absorbed. Additional testing must still be performed to 1) establish absorption limits for uranium for anion exchange resin, 2) evaluate desorption characteristics of uranium and DBP, and 3) study the possibility of re-using the absorbent.« less

Numerical simulation of migration behavior of uranium ore dust particles in the human respiratory tract

NASA Astrophysics Data System (ADS)

Ye, Yong-jun; Yin, An-song; Li, Zhi; Lei, Bo; Ding, De-xin

2017-04-01

There is a certain concentration of radioactive dust particles in the air of workplace of underground uranium mines. Some small diameter particles will pass through the masks and enter the respiratory tract which will cause radiation damage to the human body. In order to study deposition regularity of uranium dust in the human respiratory tract, in this paper, we firstly use the RNG turbulence model to simulate the gas flow field in the human respiratory tract Z0 ∼ Z3 level under different respiratory intensity. Then we use DPM discrete phase model to simulate the concentration, particle size distribution, deposition rate and deposition share of uranium dust particles after being filtered through the masks in the human respiratory tract Z0 to Z3 bronchus. According to the simulation results, we have got the following conclusions: the particles’ number concentration of uranium dust after being filtered through the mask in the human respiratory tract basically decreases with the increasing of particle size under different respiratory intensities on the environment of uranium mine. In addition, the intensity of respiration and the mass concentration of particles have an important influence on the deposition rate and the deposition of particles in the respiratory tract.

Simulations of Ground-Water Flow and Particle Pathline Analysis in the Zone of Contribution of a Public-Supply Well in Modesto, Eastern San Joaquin Valley, California

USGS Publications Warehouse

Burow, Karen R.; Jurgens, Bryant C.; Kauffman, Leon J.; Phillips, Steven P.; Dalgish, Barbara A.; Shelton, Jennifer L.

2008-01-01

Shallow ground water in the eastern San Joaquin Valley is affected by high nitrate and uranium concentrations and frequent detections of pesticides and volatile organic compounds (VOC), as a result of ground-water development and intensive agricultural and urban land use. A single public-supply well was selected for intensive study to evaluate the dominant processes affecting the vulnerability of public-supply wells in the Modesto area. A network of 23 monitoring wells was installed, and water and sediment samples were collected within the approximate zone of contribution of the public-supply well, to support a detailed analysis of physical and chemical conditions and processes affecting the water chemistry in the well. A three-dimensional, steady-state local ground-water-flow and transport model was developed to evaluate the age of ground water reaching the well and to evaluate the vulnerability of the well to nonpoint source input of nitrate and uranium. Particle tracking was used to compute pathlines and advective travel times in the ground-water flow model. The simulated ages of particles reaching the public-supply well ranged from 9 to 30,000 years, with a median of 54 years. The age of the ground water contributed to the public-supply well increased with depth below the water table. Measured nitrate concentrations, derived primarily from agricultural fertilizer, were highest (17 milligrams per liter) in shallow ground water and decreased with depth to background concentrations of less than 2 milligrams per liter in the deepest wells. Because the movement of water is predominantly downward as a result of ground-water development, and because geochemical conditions are generally oxic, high nitrate concentrations in shallow ground water are expected to continue moving downward without significant attenuation. Simulated long-term nitrate concentrations indicate that concentrations have peaked and will decrease in the public-supply well during the next 100 years because of the low nitrate concentrations in recharge beneath the urban area and the increasing proportion of urban-derived ground water reaching the well. The apparent lag time between peak input concentrations and peak concentrations in the well is about 20 to 30 years. Measured uranium concentrations were also highest (45 micrograms per liter) in shallow ground water, and decreased with depth to background concentrations of about 0.5 microgram per liter. Naturally-occurring uranium adsorbed to aquifer sediments is mobilized by oxygen-rich, high-alkalinity water. Alkalinity increased in shallow ground water in response to agricultural development. As ground-water pumping increased in the 1940s and 1950s, this alkaline water moved downward through the ground-water flow system, mobilizing the uranium adsorbed to aquifer sediments. Ground water with high alkalinity and high uranium concentrations is expected to continue to move deeper in the system, resulting in increased uranium concentrations with depth in ground water. Because alkalinity (and correspondingly uranium) concentrations were high in shallow ground water beneath both the urban and the agricultural land, long-term uranium concentrations in the public-supply well are expected to increase as the proportion of uranium-affected water contributed to the well increases. Assuming that the alkalinity near the water table remains the same, the simulation of long-term alkalinity in the public-supply well indicates that uranium concentrations in the public-supply well will likely approach the maximum contaminant level; however, the time to reach this level is more than 100 years because of the significant proportion of old, unaffected water at depth that is contributed to the public-supply well.

Seasonality of diel cycles of dissolved trace-metal concentrations in a Rocky Mountain stream

USGS Publications Warehouse

Nimick, D.A.; Cleasby, T.E.; McCleskey, R. Blaine

2005-01-01

Substantial diel (24-h) cycles in dissolved (0.1-??m filtration) metal concentrations were observed during summer low flow, winter low flow, and snowmelt runoff in Prickly Pear Creek, Montana. During seven diel sampling episodes lasting 34-61.5 h, dissolved Mn and Zn concentrations increased from afternoon minimum values to maximum values shortly after sunrise. Dissolved As concentrations exhibited the inverse timing. The magnitude of diel concentration increases varied in the range 17-152% for Mn and 70-500% for Zn. Diel increases of As concentrations (17-55%) were less variable. The timing of minimum and maximum values of diel streamflow cycles was inconsistent among sampling episodes and had little relation to the timing of metal concentration cycles, suggesting that geochemical rather than hydrological processes are the primary control of diel metal cycles. Diel cycles of dissolved metal concentrations should be assumed to occur at any time of year in any stream with dissolved metals and neutral to alkaline pH. ?? Springer-Verlag 2005.

Microbially catalyzed nitrate-dependent metal/radionuclide oxidation in shallow subsurface sediments

NASA Astrophysics Data System (ADS)

Weber, K.; Healy, O.; Spanbauer, T. L.; Snow, D. D.

2011-12-01

Anaerobic, microbially catalyzed nitrate-dependent metal/radionuclide oxidation has been demonstrated in a variety of sediments, soils, and groundwater. To date, studies evaluating U bio-oxidation and mobilization have primarily focused on anthropogenically U contaminated sites. In the Platte River Basin U originating from weathering of uranium-rich igneous rocks in the Rocky Mountains was deposited in shallow alluvial sediments as insoluble reduced uranium minerals. These reduced U minerals are subject to reoxidation by available oxidants, such nitrate, in situ. Soluble uranium (U) from natural sources is a recognized contaminant in public water supplies throughout the state of Nebraska and Colorado. Here we evaluate the potential of anaerobic, nitrate-dependent microbially catalyzed metal/radionuclide oxidation in subsurface sediments near Alda, NE. Subsurface sediments and groundwater (20-64ft.) were collected from a shallow aquifer containing nitrate (from fertilizer) and natural iron and uranium. The reduction potential revealed a reduced environment and was confirmed by the presence of Fe(II) and U(IV) in sediments. Although sediments were reduced, nitrate persisted in the groundwater. Nitrate concentrations decreased, 38 mg/L to 30 mg/L, with increasing concentrations of Fe(II) and U(IV). Dissolved U, primarily as U(VI), increased with depth, 30.3 μg/L to 302 μg/L. Analysis of sequentially extracted U(VI) and U(IV) revealed that virtually all U in sediments existed as U(IV). The presence of U(IV) is consistent with reduced Fe (Fe(II)) and low reduction potential. The increase in aqueous U concentrations with depth suggests active U cycling may occur at this site. Tetravalent U (U(IV)) phases are stable in reduced environments, however the input of an oxidant such as oxygen or nitrate into these systems would result in oxidation. Thus co-occurrence of nitrate suggests that nitrate could be used by bacteria as a U(IV) oxidant. Most probable number enumeration of nitrate-dependent U(IV) oxidizing microorganisms demonstrated an abundant community ranging from 1.61x104 to 2.74x104 cells g-1 sediment. Enrichments initiated verified microbial U reduction and U oxidation coupled to nitrate reduction. Sediment slurries were serially diluted and incubated over a period of eight weeks and compared to uninoculated controls. Oxidation (0-4,554 μg/L) and reduction (0-55 μg/L) of U exceeded uninoculated controls further providing evidence of a U biogeochemical cycling in these subsurface sediments. The oxidation of U(IV) could contribute to U mobilization in the groundwater and result in decreased water quality. Not only could nitrate serve as an oxidant, but Fe(III) could also contribute to U mobilization. Nitrate-dependent Fe(II) oxidation is an environmentally ubiquitous process facilitated by a diversity of microorganisms. Additional research is necessary in order to establish a role of biogenic Fe(III) oxides in U geochemical cycling at this site. These microbially mediated processes could also have a confounding effect on uranium mobility in subsurface environments.

Data from synoptic water-quality studies on the Colorado River in the Grand Canyon, Arizona, November 1990 and June 1991

USGS Publications Warehouse

Taylor, Howard E.; Peart, D.B.; Antweiler, Ronald C.; Brinton, T.I.; Campbell, W.L.; Barbarino, J.R.; Roth, D.A.; Hart, R.J.; Averett, R.C.

1996-01-01

Two water-quality synoptic studies were made on the Colorado River in the Grand Canyon, Arizona. Field measurements and the collection of water samples for laboratory analysis were made at 10 mainstem and 6 tributary sites every 6 hours for a 48-hour period on November 5-6, 1990, and again on June 18-20, 1991. Field measurements included discharge, alkalinity, water temperature, light penetration, pH, specific conductance, and dissolved oxygen. Water samples were collected for the laboratory analysis of major and minor ions (calcium, magnesium, sodium, potassium, strontium, chloride, sulfate, silica as SiO2), trace elements (aluminum, arsenic, boron, barium, beryllium, cadmium, cobalt, chromium, copper, iron, lead, lithium, manganese, molybdenum, nickel, selenium, thallium, uranium, vanadium and zinc), and nutrients (phosphate, nitrate, ammonium, nitrite, total dissolved nitrogen, total dissolved phosphorus and dissolved organic carbon). Biological measurements included drift (benthic invertebrates and detrital material), and benthic invertebrates from the river bottom.

Dissolution of Used Nuclear Fuel Using a TBP/N-Paraffin Solvent

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

Rudisill, T. S.; Shehee, T. C.; Jones, D. H.

2017-10-02

The dissolution of unirradiated used nuclear fuel (UNF) pellets pretreated for tritium removal was demonstrated using a tributly phosphate (TBP) solvent. Dissolution of pretreated fuel in TBP could potentially combine dissolution with two cycle of solvent extraction required for separating the actinides and lanthanides from other fission products. Dissolutions were performed using UNF surrogates prepared from both uranyl nitrate and uranium trioxide produced from the pretreatment process by adding selected actinide and stable fission product elements. In laboratory-scale experiments, the U dissolution efficiency ranged from 80-99+% for both the nitrate and oxide surrogate fuels. On average, 80% of the Pumore » and 50% of the Np and Am in the nitrate surrogate dissolved; however, little of the transuranic elements dissolved in the oxide form. The majority of the 3+ lanthanide elements dissolved. Only small amounts of Sr (0-1.6%) and Mo (0.1-1.7%) and essentially no Cs, Ru, Zr, or Pd dissolved.« less

Study of oxidative stress related responses induced in Arabidopsis thaliana following mixed exposure to uranium and cadmium.

PubMed

Vanhoudt, Nathalie; Vandenhove, Hildegarde; Horemans, Nele; Wannijn, Jean; Bujanic, Andelko; Vangronsveld, Jaco; Cuypers, Ann

2010-01-01

In this study, toxicity effects in plants of uranium in a binary pollution condition were investigated by studying biological responses and unraveling oxidative stress related mechanisms in Arabidopsis thaliana seedlings, grown on hydroponics and exposed for 3 days to 10 μM uranium in combination with 5 μM cadmium. While uranium mostly accumulated in the roots with very low root-to-shoot transport, cadmium was taken up less by the roots but showed higher translocation to the shoots. Under mixed exposure, cadmium influenced uranium uptake highly but not the other way round resulting in a doubled uranium concentration in the roots. Under our mixed exposure conditions, it is clear that micronutrient concentrations in the roots are strongly influenced by addition of cadmium as a second stressor, while leaf macronutrient concentrations are mostly influenced by uranium. Oxidative stress related responses are highly affected by cadmium while uranium influence is more limited. Hereby, an important role was attributed to the ascorbate redox balance together with glutathione as both metabolites, but more explicitly for ascorbate, increased their reduced form, indicating an important defense and regulatory function. While for roots, based on an increase in FSD1 gene expression, oxidative stress was suggested to be superoxide induced, in leaves on the other hand, hydrogen peroxide related genes were mostly altered. Copyright © 2010 Elsevier Masson SAS. All rights reserved.

National Uranium Resource Evaluation Program. Hydrogeochemical and stream sediment reconnaissance basic data for Beeville NTMS Quadrangle, Texas. Uranium resource evaluation project

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

Not Available

Results of a reconnaissance geochemical survey of the Beeville Quadrangle, Texas are reported. Field and laboratory data are presented for 373 groundwater and 364 stream sediment samples. Statistical and areal distributions of uranium and possible uranium-related variables are displayed. A generalized geologic map of the survey area is provided, and pertinent geologic factors which may be of significance in evaluating the potential for uranium mineralization are briefly discussed. The groundwater data indicate that the northwestern corner of the quadrangle is the most favorable for potential uranium mineralization. Favorability is indicated by high uranium concentrations; high arsenic, molybdenum, and vanadium concentrations;more » and proximity and similar geologic setting to the mines of the Karnes County mining district. Other areas that appear favorable are an area in Bee and Refugio Counties and the northeastern part of the quadrangle. Both areas have water chemistry similar to the Karnes County area, but the northeastern area does not have high concentrations of pathfinder elements. The stream sediment data indicate that the northeastern corner of the quadrangle is the most favorable for potential mineralization, but agricultural practices and mineralogy of the outcropping Beaumont Formation may indicate a false anomaly. The northwestern corner of the quadrangle is considered favorable because of its proximity to the known uranium deposits, but the data do not seem to support this.« less

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

Influence of Calcium on Microbial Reduction of Solid Phase Uranium (VI)

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

Liu, Chongxuan; Jeon, Byong-Hun; Zachara, John M.

2007-06-27

The effect of calcium on microbial reduction of a solid phase U(VI), sodium boltwoodite (NaUO2SiO3OH ∙1.5H2O), was evaluated in a culture of a dissimilatory metal-reducing bacterium (DMRB), Shewanella oneidensis strain MR-1. Batch experiments were performed in a non-growth bicarbonate medium with lactate as electron donor at pH 7 buffered with PIPES. Calcium increased both the rate and extent of Na-boltwoodite dissolution by increasing its solubility through the formation of a ternary aqueous calcium-uranyl-carbonate species. The ternary species, however, decreased the rates of microbial reduction of aqueous U(VI). Laser-induced fluorescence spectroscopy (LIFS) and transmission electron microscopy (TEM) revealed that microbial reductionmore » of solid phase U(VI) is a sequentially coupled process of Na-boltwoodite dissolution, U(VI) aqueous speciation, and microbial reduction of dissolved U(VI) to U(IV) that accumulated on bacterial surfaces/periplasm. The overall rates of microbial reduction of solid phase U(VI) can be described by the coupled rates of dissolution and microbial reduction that were both influenced by calcium. The results demonstrated that dissolved U(VI) concentration during microbial reduction was a complex function of solid phase U(VI) dissolution kinetics, aqueous U(VI) speciation, and microbial activity.« less

Investigations Into the Reusability of Amidoxime-Based Polymeric Uranium Adsorbents

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

Kuo, Li-Jung; Gill, Gary A.; Strivens, Jonathan E.

Significant advancements in amidoxime-based polymeric adsorbents to extract uranium from seawater are achieved in recent years. The success of uranium adsorbent development can help provide a sustainable supply of fuel for nuclear reactors. To bring down the production cost of this new technology, in addition to the development of novel adsorbents with high uranium capacity and manufacture cost, the development of adsorbent re-using technique is critical because it can further reduce the cost of the adsorbent manufacture. In our last report, the use of high concentrations of bicarbonate solution (3M KHCO3) was identified as a cost-effective, environmental friendly method tomore » strip uranium from amidoxime-based polymeric adsorbents. This study aims to further improve the method for high recovery of uranium capacity in re-uses and to evaluate the performance of adsorbents after multiple re-use cycles. Adsorption of dissolved organic matter (DOM) on the uranium adsorbents during seawater exposure can hinder the uranium adsorption and slow down the adsorption rate. An additional NaOH rinse (0.5 M NaOH, room temperature) was applied after the 3 M KHCO3 elution to remove natural organic matter from adsorbents. The combination of 3 M KHCO3 elution and 0.5 M NaOH rinse significantly improves the recovery of uranium adsorption capacity in the re-used adsorbents. In the first re-use, most ORNL adsorbents tested achieve ~100% recovery by using 3 M KHCO3 elution + 0.5 M NaOH rinse approach, in comparison to 54% recovery when only 3 M KHCO3 elution was applied. A significant drop in capacity was observed when the adsorbents went through more than one re-use. FTIR spectra revealed that degradation of amidoxime ligands occurs during seawater exposure, and is more significant the longer the exposure time. Significantly elevated ratios of Ca/U and Mg/U in re-used adsorbents support the decrease in abundance of amidoxime ligands and increase carboxylate group from FT-IR analysis. The impact of the length of seawater exposure cycle in adsorbent re-use was evaluated by comparing the adsorption capacity for a common adsorbent formulation (ORNL AI8 formulation) under different exposure cycle (28 days and 42 days). Adsorbents with a 28 days seawater exposure cycle had higher recovery of uranium capacity than adsorbent with 42 days of seawater exposure. Under different cumulative seawater exposure time, the adsorbent with 28 days seawater exposure cycle also had less amidoxime ligands degradation than the adsorbent with 42 days seawater exposure cycle. These observations support the negative impact of prolonged seawater exposure on amidoxime ligands stability. Recovery of uranium capacity in re-uses also varies across different adsorbent formulations. Among three different ORNL adsorbents tested (AI8, AF8, AF1-DMSO), AI8 had the best recovery in each re-use, followed by AF8 and then AF1-DMSO. This demonstrates that continuing efforts on developing new adsorbents with high capacity and stability is critical. The overall performance of adsorbents in multiple re-use cycles can be evaluated by calculation total harvestable uranium, the summation of adsorbed uranium from each seawater exposure cycle. In this assessment, the ORNL AI8 braid with 28 days seawater exposure cycle can reach total harvestable uranium 10g Uranium/kg adsorbent in ~140 days; while the same type of braid but with 42 days seawater exposure cycle reach the same level in ~170 days. Notably, the performance of total harvestable uranium also varies among different adsorbent formulations (AI8 > AF1-DMSO > AF8). Short seawater exposure cycle is associated with high re-use frequency. The development of low-cost offshore adsorbent deployment/extraction is essential for high frequency reuse operation. This study also highlights the importance to examine the re-use performance of newly developed uranium adsorbents for selection of optimal adsorbents for ocean deployment.« less

Impact of dissolved oxygen concentration on some key parameters and production of rhG-CSF in batch fermentation.

PubMed

Krishna Rao, Dasari V; Ramu, Chatadi T; Rao, Joginapally V; Narasu, Mangamoori L; Bhujanga Rao, Adibhatla Kali S

2008-09-01

The impact of different levels of agitation speed, carbondioxide and dissolved oxygen concentration on the key parameters and production of rhG-CSF in Escherichia coli BL21(DE3)PLysS were studied. Lower carbondioxide concentrations as well as higher agitation speeds and dissolved oxygen concentrations led to reduction in the acetate concentrations, and enhanced the cell growth, but inhibited plasmid stability and rhG-CSF expression. Similarly, higher carbondioxide concentrations and lower agitation speeds as well as dissolved oxygen concentrations led to enhanced acetate concentrations, but inhibited the cell growth and protein expression. To address the bottlenecks, a two-stage agitation control strategy (strategy-1) and two-stage dissolved oxygen control strategy (strategy-2) were employed to establish the physiological and metabolic conditions, so as to improve the expression of rhG-CSF. By adopting strategy-1 the yields were improved 1.4-fold over constant speed of 550 rpm, 1.1-fold over constant dissolved oxygen of 45%, respectively. Similarly, using strategy-2 the yields were improved 1.6-fold over constant speed of 550 rpm, 1.3-fold over constant dissolved oxygen of 45%, respectively.

Trends in nitrate and dissolved-solids concentrations in ground water, Carson Valley, Douglas County, Nevada, 1985-2001

USGS Publications Warehouse

Rosen, Michael R.

2003-01-01

Analysis of trends in nitrate and total dissolved-solids concentrations over time in Carson Valley, Nevada, indicates that 56 percent of 27 monitoring wells that have long-term records of nitrate concentrations show increasing trends, 11 percent show decreasing trends, and 33 percent have not changed. Total dissolved-solids concentrations have increased in 52 percent of these wells and are stable in 48 percent. None of these wells show decreasing trends in total dissolved-solids concentrations. The wells showing increasing trends in nitrate and total dissolved-solids concentrations were always in areas that use septic waste-disposal systems. Therefore, the primary cause of these increases is likely the increase in septic-tank usage over the past 40 years.

Water-Quality Data for Selected National Park Units within the Southern Colorado Plateau Network, Arizona, Utah, Colorado, and New Mexico, Water Years 2005 and 2006

USGS Publications Warehouse

Macy, Jamie P.; Monroe, Stephen A.

2006-01-01

The National Park Service initiated a Level 1 Water-Quality Inventory program to provide water-quality data to park managers so informed natural resource management decisions could be made. Level 1 water-quality data were collected by the U.S. Geological Survey Arizona Water Science Center at 57 sites in 13 National Park units located in the Southern Colorado Plateau Inventory and Monitoring network in water years 2005 and 2006. These data describe the current water-quality at selected sites within the park units and provide information for monitoring future trends. Water samples were collected three times at each type of site including wells, springs, seeps, tinajas, rivers, a lake, and an irrigation ditch. Field measurements were taken at each site and they included pH, specific conductance, temperature, barometric pressure, dissolved oxygen, alkalinity, turbidity, and discharge rates where applicable. Water samples collected were sent to the U.S. Geological Survey National Water Quality Laboratory and analyzed for major ions, trace elements, and nutrients. The National Water Quality Laboratory also analyzed selected samples for mercury and petroleum hydrocarbons. Additional samples at selected sites were collected and analyzed for cyanide, radiochemistry, and suspended sediment by U.S. Geological Survey contract labs. Fecal-indicator bacteria (Escherichia coli) were sampled for at selected sites as another indicator of water quality. Quality control for this study was achieved through proper training of field personnel, use of standard U.S. Geological Survey field and laboratory protocols, collection of sample blanks and replicates, and a thorough review of the water-quality analyses. Measured field pH ranged from 6.0 to 8.8, within normal range for springs and rivers, at most sites. Concentrations of dissolved solids ranged from 48 to 8,680 mg/L and the majority of samples had concentrations of dissolved solids below 900 mg/L. Trace-element concentrations at most sites were at or near the laboratory reporting levels. The highest overall trace-element concentrations were found at U.S. Highway 160 Spring near Park Entrance to Mesa Verde National Park. Concentrations of uranium in samples at all sites ranged from below the detection limit to 55.7 ?g/L. Water samples from selected sites were analyzed for total petroleum hydrocarbons and concentrations of total petroleum hydrocarbons were at or above the laboratory detection limit in samples at six National Park units. Ten sites were sampled for Escherichia coli and positive counts were found at 9 out of the ten sites, the highest colony counts were found at Chinle Creek at Chinle, AZ in Canyon de Chelly National Monument. Measured concentrations of dissolved ammonia, nitrite, and nitrate were at or near laboratory reporting levels at most sites; nitrate concentrations ranged from below the reporting limit (0.047 mg/L) to 9.77 mg/L. Samples that were analyzed for mercury had concentrations below or at the laboratory reporting level. Concentrations of cyanide were less than the laboratory reporting level for all samples except two, Spruce Tree House Spring in Mesa Verde National Park and Pine Tree Canyon Tinaja in Canyon de Chelly National Monument, which had average concentrations of .042 and .011 ?g/L respectively. Gross alpha/beta radioactivity counts were below the U.S. Environmental Protection Agency maximum contaminant level except for samples from Casa Chiquita Well Middle at Chaco Culture National Historical Park which averaged 35 pCi/L. Suspended-sediment concentrations were variable and ranged from 10 to 150,000 mg/L.

Bacterial diversity and composition of an alkaline uranium mine tailings-water interface.

PubMed

Khan, Nurul H; Bondici, Viorica F; Medihala, Prabhakara G; Lawrence, John R; Wolfaardt, Gideon M; Warner, Jeff; Korber, Darren R

2013-10-01

The microbial diversity and biogeochemical potential associated with a northern Saskatchewan uranium mine water-tailings interface was examined using culture-dependent and -independent techniques. Morphologically-distinct colonies from uranium mine water-tailings and a reference lake (MC) obtained using selective and non-selective media were selected for 16S rRNA gene sequencing and identification, revealing that culturable organisms from the uranium tailings interface were dominated by Firmicutes and Betaproteobacteria; whereas, MC organisms mainly consisted of Bacteroidetes and Gammaproteobacteria. Ion Torrent (IT) 16S rRNA metagenomic analysis carried out on extracted DNA from tailings and MC interfaces demonstrated the dominance of Firmicutes in both of the systems. Overall, the tailings-water interface environment harbored a distinct bacterial community relative to the MC, reflective of the ambient conditions (i.e., total dissolved solids, pH, salinity, conductivity, heavy metals) dominating the uranium tailings system. Significant correlations among the physicochemical data and the major bacterial groups present in the tailings and MC were also observed. Presence of sulfate reducing bacteria demonstrated by culture-dependent analyses and the dominance of Desulfosporosinus spp. indicated by Ion Torrent analyses within the tailings-water interface suggests the existence of anaerobic microenvironments along with the potential for reductive metabolic processes.

Effects of uranium mining, Puerco River, New Mexico

USGS Publications Warehouse

Lopes, Thomas J.

1991-01-01

Effluent from uranium-mine dewatering and acidic water released by a tailings-pond dike failure increased radionuclide activities in streamflow in the Puerco River in New Mexico and Arizona. Median dissolved gross-alpha activity in the streamflow was 1,130 picocuries per liter from 1975 to 1986 when mine discharges ceased and 6.2 picocuries per liter from 1986 to 1989. From 1975 to July 1979, major ions in streamflow at the Puerco River at Gallup streamflow-gaging station were sodium, bicarbonate, and sulfate. On July 16, 1979, the day of the tailing spill, major ions in streamflow were magnesium, calcium, and sulfate. From 1979 to 1984, major ions in streamflow had a greater proportion of calcium and sulfate than prior to the spill, indicating flushing of residual tailings solution. Geochemical modeling of mine effluent indicates that uranium was unlikely to precipitate from effluent between the mines and Gallup or when mixed with wastewater downstream from Gallup. Geochemical modeling of acidic-tailings solution indicates that uranium was in solution as far downstream as Gallup. When the acidic-tailings solution mixed with 10- to 40-percent wastewater, uranium may have precipitated from solution as carnotite [K2(UO2)2(VO4)2] and tyuyamunite [Ca(UO2)2(VO4)2].

Assessment of nonpoint source chemical loading potential to watersheds containing uranium waste dumps and human health hazards associated with uranium exploration and mining, Red, White, and Fry Canyons, southeastern Utah, 2007

USGS Publications Warehouse

Beisner, Kimberly R.; Marston, Thomas M.; Naftz, David L.; Snyder, Terry; Freeman, Michael L.

2010-01-01

During May, June, and July 2007, 58 solid-phase samples were collected from abandoned uranium mine waste dumps, background sites, and adjacent streambeds in Red, White, and Fry Canyons in southeastern Utah. The objectives of this sampling program were to (1) assess the nonpoint-source chemical loading potential to ephemeral and perennial drainage basins from uranium waste dumps and (2) assess potential effects on human health due to recreational activities on and around uranium waste dumps on Bureau of Land Management property. Uranium waste-dump samples were collected using solid-phase sampling protocols. After collection, solid-phase samples were homogenized and extracted in the laboratory using a leaching procedure. Filtered (0.45 micron) water samples were obtained from the field leaching procedure and were analyzed for major and trace elements at the Inductively Coupled Plasma-Mass Spectrometry Metals Analysis Laboratory at the University of Utah. A subset of the solid-phase samples also were digested with strong acids and analyzed for major ions and trace elements at the U.S. Geological Survey Geologic Division Laboratory in Denver, Colorado. For the initial ranking of chemical loading potential for uranium waste dumps, results of leachate analyses were compared with existing aquatic-life and drinking-water-quality standards. To assess potential effects on human health, solid-phase digestion values for uranium were compared to soil screening levels (SSL) computed using the computer model RESRAD 6.5 for a probable concentration of radium. One or more chemical constituents exceeded aquatic life and drinking-water-quality standards in approximately 64 percent (29/45) of the leachate samples extracted from uranium waste dumps. Most of the uranium waste dump sites with elevated trace-element concentrations in leachates were located in Red Canyon. Approximately 69 percent (31/45) of the strong acid digestible soil concentration values were greater than a calculated SSL. Uranium waste dump sites with elevated leachate and total digestible concentrations may need to be further investigated to determine the most appropriate remediation method.

Uranium content and leachable fraction of fluorspars

USGS Publications Warehouse

Landa, E.R.; Councell, T.B.

2000-01-01

Much attention in the radiological health community has recently focused on the management and regulation of naturally occurring radioactive materials. Although uranium-bearing minerals are present in a variety of fluorspar deposits, their potential consideration as naturally occurring radioactive materials has received only limited recognition. The uranium content of 28 samples of acid- and cryolite-grade (>97% CaF2) fluorspar from the National Defense Stockpile was found to range from 120 to 24,200 ??g kg-1, with a mean of 2,145 ??g kg-1. As a point of comparison, the average concentration of uranium in the upper crust of the earth is about 2,500 ??g kg-1. Leachability of this uranium was assessed by means of the Toxicity Characteristic Leaching Procedure (TCLP). The TCLP extractable fraction ranged from 1 to 98%, with a mean of 24% of the total uranium. The typically low concentrations of uranium seen in these materials probably reflects the removal of uranium-bearing mineral phases during the beneficiation of the crude fluorspar ore to achieve industrial specifications. Future NORM studies should examine crude fluorspar ores and flotation tailings.

Implementation of ICP-MS protocols for uranium urinary measurements in worker monitoring.

PubMed

Baglan, N; Cossonnet, C; Trompier, F; Ritt, J; Bérard, P

1999-10-01

The uranium concentration in human urine spiked with natural uranium and rat urine containing metabolized depleted uranium was determined by ICP-MS. The use of ICP-MS was investigated without any chemical treatment or after the different stages of a purification protocol currently carried out for routine monitoring. In the case of spiked urine, the measured uranium concentrations were consistent with those certified by an intercomparison network in radiotoxicological analysis (PROCORAD) and with those obtained by alpha spectrometry in the case of the urine containing metabolized uranium. The quantitative information which could be obtained in the different protocols investigated shows the extent to which ICP-MS provides greater flexibility for setting up appropriate monitoring approaches in radiation protection routines and accidental situations. This is due to the combination of high sensitivity and the accuracy with which traces of uranium in urine can be determined in a shorter time period. Moreover, it has been shown that ICP-MS measurement can be used to quantify the 235U isotope, which is useful for characterizing the nature of the uranium compound, but difficult to perform using alpha spectrometry.

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.

Bacterial leaching of waste uranium materials.

PubMed

Barbic, F F; Bracilović, D M; Krajincanić, B V; Lucić, J L

1976-01-01

The effect of ferrobacteria and thiobacteria on the leaching of waste uranium materials from which 70-80% of uranium was previously leached by classical chemical hydrometallurgical procedure has been investigated. The bacteria used are found in the ore and the mine water of Zletovska River locality, Yugoslavia. Parameters of biological leaching were examined in the laboratory. Leaching conditions were changed with the aim of increasing the amount of uranium leached. The effect of pyrite added to the waste materials before the beginning of leaching has also been examined. Uranium leaching is directly proportional to the composition and number of ferrobacteria and thiobacteria, and increased by almost twice the value obtained from the same starting materials without using bacteria. Increased sulphuric acid concentrations stimulate considerably the rate of leaching. Uranium leaching is increased up to 20% while sulphuric acid consumption is simultaneously decreased by the addition of pyrite. Uranium concentrations in starting waste materials used for leaching were extremely low (0.0278 and 0.372% U) but about 60% recovery of uranium was obtained, with relatively low consumption of sulphuric acid.

Preparation and biosorption evaluation of Bacillus subtilis/alginate–chitosan microcapsule

PubMed Central

Tong, Ke

2017-01-01

The aim of this study was to assess the effect of alginate–chitosan microcapsule on viability characteristics of Bacillus subtilis and the ability of B. subtilis/alginate–chitosan microcapsule to remove uranium ion from aqueous solution. The effects of particle size, chitosan molecular weight and inoculum density on viability characteristics were studied using alginate–chitosan microcapsule-immobilized B. subtilis experiments. In addition, the effects of pH, immobilized spherule dosage, temperature, initial uranium ion concentration and contact time on removal of uranium ion were studied using batch adsorption experiments. The results showed that alginate–chitosan microcapsule significantly improved the viability characteristics of B. subtilis and that B. subtilis/alginate–chitosan microcapsule strongly promoted uranium ion absorption. Moreover, the optimum values of pH was 6; immobilized spherule dosage was 3.5; temperature was 20°C; initial uranium ion concentration was 150 mg/L; contact time was 3 h of uranium ion absorption and the maximum adsorption capacity of uranium ion was 376.64 mg/g. PMID:28223783

Bioaccumulation and Toxicity of Uranium, Arsenic and Nickel to Juveniles and Adults Hyalella azteca in Spiked Sediment Bioassays.

PubMed

Goulet, Richard R; Thompson, Patsy-A

2018-05-26

Uranium mining and milling release arsenic (As), nickel (Ni) and uranium (U) to receiving waters, which accumulate in sediments. The objective of this study was to investigate if As, Ni and U concentrations in tissue residue of Hyalella azteca, overlying water, sediment pore water and solids could predict juvenile and adult survival and growth in similar conditions to lake sediments downstream of Uranium mines and mills. We conducted 14 day, static sediment toxicity tests spiked with uranium, arsenic and nickel salts. For uranium, we spiked uranyl nitrate with sodium bicarbonate to limit U precipitation once in contact with circumneutral sediment. LC 50 for As, Ni and U of juveniles and adults based on measured concentrations in sediments were 1.8 and 2.2 µmol As/g dw, 6.3 and 13.4 µmol Ni/g dw and 0.2 and 0.9 µmol U/g dw, respectively. Adult survival and growth linearly decreased with increasing bioaccumulation. For juveniles, metal accumulation linearly predicted survival. We calculated lethal body concentrations (LBC 50 ) for juveniles and adults of 70 and 485 nmol As/g dw, 246 and 832 nmol Ni/g dw and 1.7 and 4.4 nmol U/g dw, respectively. The concentrations of As, Ni and U in tissue residue leading to a 20% decrease in growth were 427 nmol As/g, 755 nmol Ni/g and 5 nmol U/g. Overall, this study showed that Uranium was the most toxic element followed by As and Ni, that juveniles were more sensitive to the three metals tested than adults and that threshold body concentrations can support assessment of benthic invertebrate community impairment. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

Comparison of the Kinetic Rate Law Parameters for the Dissolution of Natural and Synthetic Autunite in the Presence of Aqueous Bicarbonate Ions

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

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn M.

2013-08-02

Bicarbonate is one of the most significant components within the uranium geochemical cycle. In aqueous solutions, bicarbonate forms strong complexes with uranium. As such, aqueous bicarbonate may significantly increase the rate of uranium release from uranium minerals. Quantifying the relationship of aqueous bicarbonate concentration to the rate of uranium release during dissolution is critical to understanding the long-term fate of uranium within the environment. Single-pass flow-through (SPTF) experiments were conducted to estimate the rate of uranium release from Na meta-autunite as a function of bicarbonate (0.0005-0.003 M) under the pH range of 6-11 and a temperature range of 5-60oC. Consistentmore » with the results of previous investigation, the rate of uranium release exhibited minimal dependency on temperature; but were strongly dependent on pH. Increasing aqueous bicarbonate concentrations afforded comparable increases in the rate of release of uranium. Most notably under low pH conditions the aqueous bicarbonate resulted in up to 370 fold increases in the rate of uranium release in relative to the rate of uranium release in the absence of bicarbonate. However, the effect of aqueous bicarbonate on the release of uranium was significantly less under higher pH conditions. It is postulated that at high pH values, surface sites are saturated with carbonate, thus the addition of more bicarbonate would have less effect on uranium release.« less

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.

High resolution analysis of uranium and thorium concentration as well as U-series isotope distributions in a Neanderthal tooth from Payre (Ardèche, France) using laser ablation ICP-MS

NASA Astrophysics Data System (ADS)

Grün, Rainer; Aubert, Maxime; Joannes-Boyau, Renaud; Moncel, Marie-Hélène

2008-11-01

We have mapped U ( 238U) and Th ( 232Th) elemental concentrations as well as U-series isotope distributions in a Neanderthal tooth from the Middle Palaeolithic site of Payre using laser ablation ICP-MS. The U-concentrations in an enamel section varied between 1 and 1500 ppb. The U-concentration maps show that U-migration through the external enamel surface is minute, the bulk of the uranium having migrated internally via the dentine into the enamel. The uranium migration and uptake is critically dependent on the mineralogical structure of the enamel. Increased U-concentrations are observed along lineaments, some of which are associated with cracks, and others may be related to intra-prismatic zones or structural weaknesses reaching from the dentine into the enamel. The uranium concentrations in the dentine vary between about 25,000 and 45,000 ppb. Our systematic mapping of U-concentration and U-series isotopes provides insight into the time domain of U-accumulation. Most of the uranium was accumulated in an early stage of burial, with some much later overprints. None of the uranium concentration and U-series profiles across the root of the tooth complied with a single stage diffusion-adsorption (D-A) model that is used for quality control in U-series dating of bones and teeth. Nevertheless, in the domains that yielded the oldest apparent U-series age estimates, U-leaching could be excluded. This means that the oldest apparent U-series ages of around 200 ka represent a minimum age for this Neanderthal specimen. This is in good agreement with independent age assessments (200-230 ka) for the archaeological layer, in which it was found. The Th elemental concentrations in the dental tissues were generally low (between about 1 and 20 ppb), and show little relationship with the nature of the tissue.

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

Investigation of uranium binding forms in selected German mineral waters.

PubMed

Osman, Alfatih A A; Geipel, Gerhard; Bernhard, Gert; Worch, Eckhard

2013-12-01

Cryogenic time-resolved laser-induced fluorescence spectroscopy was successfully used to identify uranium binding forms in selected German mineral waters of extremely low uranium concentrations (<2.0 μg/L). The measurements were performed at a low temperature of 153 K. The spectroscopic data showed a prevalence of aquatic species Ca2UO2(CO3)3 in all investigated waters, while other uranyl-carbonate complexes, viz, UO2CO3(aq) and UO2(CO3)2 (2-), only existed as minor species. The pH value, alkalinity (CO3 (2-)), and the main water inorganic constituents, specifically the Ca(2+) concentration, showed a clear influence on uranium speciation. Speciation modeling was performed using the most recent thermodynamic data for aqueous complexes of uranium. The modeling results for the main uranium binding form in the investigated waters indicated a good agreement with the spectroscopy measurements.

Hydrogeochemical and stream sediment reconnaissance basic data for Palestine NTMS Quadrangle, Texas

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

Not Available

1979-05-04

Results of a reconnaissance geochemical survey of the Palestine Quadrangle are reported. Field and laboratory data are presented for 714 groundwater and 577 stream sediment samples. Statistical and areal distributions of uranium and possible uranium-related variables are displayed. A generalized geologic map of the survey area is provided, and pertinent geologic factors which may be of significance in evaluating the potential for uranium mineralization are briefly discussed. Groundwater data indicate that uranium concentrations above the 85th percentile occur primarily in the Caddell, Wellborn, and Manning Formations of the Jackson Group; and the Yegua Formation of the Claiborne Group. Saline watermore » trends are also prominent in these formations. Stream sediment data indicate that uranium values above the 85th percentile correlate with high concentrations of cerium, niobium, thorium, titanium, yttrium, and zirconium. This elemental suite probably indicates that uranium is associated with resistate and/or heavy minerals.« less

Depleted Uranium Program: Repository and Chemical Analysis of Biological Samples

DTIC Science & Technology

2010-11-01

Chemical Samples • Chemical Pathology and Analytical Assessment of U and DU in: • Tissues • Urine • Whole blood • Semen • Embedded fragments...preparation for determination of total uranium and isotopic uranium ratios  Semen – Total Uranium – dry ashed by concentrated nitric acid in muffle...Total uranium and DU measurements in blood 0.0 50.0 100.0 150.0 200.0 250.0 ng U in s am pl e Sample Number Semen Measured U Theortical U Uranium

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.

Depleted uranium analysis in blood by inductively coupled plasma mass spectrometry

USGS Publications Warehouse

Todorov, T.I.; Xu, H.; Ejnik, J.W.; Mullick, F.G.; Squibb, K.; McDiarmid, M.A.; Centeno, J.A.

2009-01-01

In this study we report depleted uranium (DU) analysis in whole blood samples. Internal exposure to DU causes increased uranium levels as well as change in the uranium isotopic composition in blood specimen. For identification of DU exposure we used the 235U/238U ratio in blood samples, which ranges from 0.00725 for natural uranium to 0.002 for depleted uranium. Uranium quantification and isotopic composition analysis were performed by inductively coupled plasma mass spectrometry. For method validation we used eight spiked blood samples with known uranium concentrations and isotopic composition. The detection limit for quantification was determined to be 4 ng L-1 uranium in whole blood. The data reproduced within 1-5% RSD and an accuracy of 1-4%. In order to achieve a 235U/238U ratio range of 0.00698-0.00752% with 99.7% confidence limit a minimum whole blood uranium concentration of 60 ng L??1 was required. An additional 10 samples from a cohort of veterans exposed to DU in Gulf War I were analyzed with no knowledge of their medical history. The measured 235U/ 238U ratios in the blood samples were used to identify the presence or absence of DU exposure within this patient group. ?? 2009 The Royal Society of Chemistry.

Effects of uranium concentration on microbial community structure and functional potential.

PubMed

Sutcliffe, Brodie; Chariton, Anthony A; Harford, Andrew J; Hose, Grant C; Greenfield, Paul; Elbourne, Liam D H; Oytam, Yalchin; Stephenson, Sarah; Midgley, David J; Paulsen, Ian T

2017-08-01

Located in the Northern Territory of Australia, Ranger uranium mine is directly adjacent to the UNESCO World Heritage listed Kakadu National Park, with rehabilitation targets needed to ensure the site can be incorporated into the park following the mine's closure in 2026. This study aimed to understand the impact of uranium concentration on microbial communities, in order to identify and describe potential breakpoints in microbial ecosystem services. This is the first study to report in situ deployment of uranium-spiked sediments along a concentration gradient (0-4000 mg U kg -1 ), with the study design maximising the advantages of both field surveys and laboratory manipulative studies. Changes to microbial communities were characterised through the use of amplicon and shotgun metagenomic next-generation sequencing. Significant changes to taxonomic and functional community assembly occurred at a concentration of 1500 mg U kg -1 sediment and above. At uranium concentrations of ≥ 1500 mg U kg -1 , genes associated with methanogenic consortia and processes increased in relative abundance, while numerous significant changes were also seen in the relative abundances of genes involved in nitrogen cycling. Such alterations in carbon and nitrogen cycling pathways suggest that taxonomic and functional changes to microbial communities may result in changes in ecosystem processes and resilience. © 2017 Society for Applied Microbiology and John Wiley & Sons Ltd.

Status and understanding of groundwater quality in the Monterey-Salinas Shallow Aquifer Study Unit, 2012–13: California GAMA Priority Basin Project

USGS Publications Warehouse

Burton, Carmen; Wright, Michael

2018-05-30

Groundwater quality in the approximately 7,820-square-kilometer (km2) Monterey-Salinas Shallow Aquifer (MS-SA) study unit was investigated from October 2012 to May 2013 as part of the second phase of the Priority Basin Project of the Groundwater Ambient Monitoring and Assessment (GAMA) Program. The study unit is in the central coast region of California in the counties of Santa Cruz, Monterey, and San Luis Obispo. The GAMA Priority Basin Project is being conducted by the California State Water Resources Control Board in cooperation with the U.S. Geological Survey and the Lawrence Livermore National Laboratory.The MS-SA study was designed to provide a statistically robust assessment of untreated-groundwater quality in the shallow aquifer systems. The assessment was based on water-quality samples collected by the U.S. Geological Survey from 100 groundwater sites and 70 household tap sites, along with ancillary data such as land use and well-construction information. The shallow aquifer systems were defined by the depth interval of wells associated with domestic supply. The MS-SA study unit consisted of four study areas—Santa Cruz (210 km2), Pajaro Valley (360 km2), Salinas Valley (2,000 km2), and Highlands (5,250 km2).This study had two primary components: the status assessment and the understanding assessment. The first primary component of this study—the status assessment—assessed the quality of the groundwater resource indicated by data from samples analyzed for volatile organic compounds (VOCs), pesticides, and naturally present inorganic constituents, such as major ions and trace elements. The status assessment is intended to characterize the quality of groundwater resources in the shallow aquifer system of the MS-SA study unit, not the treated drinking water delivered to consumers by water purveyors. As opposed to the public wells, however, water from private wells, which often tap the shallow aquifer, is usually consumed without any treatment. The second component of this study—the understanding assessment—identified the natural and human factors that potentially affect groundwater quality by evaluating land-use characteristics, measures of location, geologic factors, groundwater age, and geochemical conditions of the shallow aquifer. An additional component of this study was a comparison of MS-SA water-quality results to those of the GAMA Monterey Bay and Salinas Valley Groundwater Basins study unit. This study unit covered much of the same areal extent as the MS-SA, but assessed the deeper, public drinking-water aquifer system.Relative concentrations (sample concentration divided by the benchmark concentration) were used to evaluate concentrations of constituents in groundwater samples relative to water-quality benchmarks for those constituents that have Federal or California benchmarks, such as maximum contaminant levels. For organic and special-interest constituents, relative concentrations were classified as high, greater than 1.0; moderate, greater than 0.1 and less than or equal to 1.0; or low, less than or equal to 0.1. For inorganic constituents, relative concentrations were classified as high, greater than 1.0; moderate, greater than 0.5 and less than or equal to 1.0; or low, less than or equal to 0.5. A relative concentration greater than 1.0 indicates that the concentration was greater than a benchmark. Aquifer-scale proportions were used to quantify regional-scale groundwater quality. The aquifer-scale proportions are the areal percentages of the shallow aquifer system where relative concentrations for a given constituent or class of constituents were high, moderate, or low.Inorganic constituents were measured at high and moderate relative concentrations more frequently than organic constituents. In the MS-SA study unit, inorganic constituents with benchmarks were detected at high relative concentrations in 51 percent of the study unit. The greatest proportions of high relative concentrations of trace elements and radioactive constituents were in the Highlands and Santa Cruz study areas, whereas high relative concentrations of nutrients were most often detected in the Salinas Valley and Pajaro Valley study areas and salinity indicators were most often detected in the Highlands and Salinas Valley study areas. The trace elements detected at high relative concentrations were arsenic, boron, iron, manganese, molybdenum, selenium, and strontium. The radioactive constituents detected at high relative concentrations were adjusted gross alpha radioactivity and uranium. The nutrient detected at high relative concentrations was nitrate plus nitrite. The salinity indicators detected at high relative concentrations were chloride, sulfate, and total dissolved solids.Organic constituents (VOCs and pesticides) were not detected at high relative concentrations in any of the study areas. The fumigant 1,2-dichloropropane was detected at moderate relative concentrations. The VOC chloroform and the pesticide simazine were the only organic constituents detected in more than 10 percent of samples. The constituents of special interest NDMA (N-nitrosodimethylamine) and perchlorate were detected at high relative concentrations in the MS-SA study unit.Selected constituents were evaluated with explanatory factors to identify potential sources or processes that could explain their presence and distribution. Trace elements and radioactive constituents came from natural sources and were not elevated by anthropogenic sources or processes, except for selenium and the radioactive constituent uranium. Arsenic, manganese, iron, selenium, and uranium concentrations were all influenced by oxidation-reduction conditions.Unlike other trace elements and radioactive constituents, uranium and selenium can be affected by agricultural practices. Uranium and selenium can be released from aquifer sediments as a result of irrigation recharge water interacting with bicarbonate systems.Nitrate can be strongly affected by anthropogenic sources. Nitrate concentrations were significantly higher in modern groundwater, indicating recent inputs of nitrate to the shallow aquifer system. Nitrate was positively correlated with agricultural land use, indicating that irrigation-return water could be leaching nitrogen fertilizer and naturally present nitrate to elevate nitrate concentrations in shallow groundwater.The salinity indicators total dissolved solids, chloride, and sulfate all had natural sources in the MS-SA study unit, primarily marine sediments. Concentrations of the constituents were elevated as a result of evaporative concentration of irrigation water or precipitation. Sulfate concentrations were significantly correlated to agricultural land use, indicating that agricultural land-use practices are a contributing source of sulfate to groundwater.The samples with most of the detections of VOCs were from sites in the Pajaro Valley and northern part of the Salinas Valley. Most of the samples with pesticide detections were from sites in the Salinas Valley study area. The herbicide simazine was positively correlated to the percentage of agricultural land use, and its concentrations were higher in modern groundwater than in pre-modern groundwater.Perchlorate, similar to nitrate, has natural and anthropogenic sources. Correlations of perchlorate to dissolved oxygen, nitrate, and percentage of agricultural land use indicated that the irrigation-return water could be leaching naturally present perchlorate, as well as perchlorate from historical applications of Chilean nitrate fertilizer, to increase perchlorate concentrations in groundwater.The quality of the water in the shallow aquifer system from this study was compared with the quality of water in the public drinking-water aquifer in a previous GAMA (MS-PA) study in the same area. The shallow system was more oxic and had more sites with modern groundwater than the public drinking-water aquifer, which was more anoxic and had sites with more pre-modern groundwater. Arsenic and selenium were found at high relative concentrations in a greater proportion of the shallow system. Manganese and iron were found at high relative concentrations in a greater proportion of the public drinking-water aquifer. Uranium was found at higher relative concentrations in a greater proportion of the shallow system. Concentrations of arsenic, iron, manganese, and molybdenum are not likely to change much as groundwater percolates from the shallow system to the public drinking-water aquifer because there are no anthropogenic sources affecting these constituents. Uranium and selenium concentrations in the public drinking-water aquifer could be affected by the higher concentrations in the shallow system because of irrigation-return water, however.Nitrate and salinity indicators had concentrations that were much higher in the shallow system than the deeper public drinking-water aquifer. High concentrations of these constituents in the shallow system could lead to increased concentrations in the public drinking-water aquifer in parts of the study units because of land-use practices, such as irrigated agriculture.Organic constituents were detected more frequently in the public drinking-water aquifer than in the shallow system, possibly because more of the sites sampled in the public drinking-water aquifer were in urban areas compared to the sites sampled for the shallow system or because sources of contamination have decreased as a result of changes in use at the land surface.

Analyzing the impact of reactive transport on the repository performance of TRISO fuel

NASA Astrophysics Data System (ADS)

Schmidt, Gregory

One of the largest determiners of the amount of electricity generated by current nuclear reactors is the efficiency of the thermodynamic cycle used for power generation. Current light water reactors (LWR) have an efficiency of 35% or less for the conversion of heat energy generated by the reactor to electrical energy. If this efficiency could be improved, more power could be generated from equivalent volumes of nuclear fuel. One method of improving this efficiency is to use a coolant flow that operates at a much higher temperature for electricity production. A reactor design that is currently proposed to take advantage of this efficiency is a graphite-moderated, helium-cooled reactor known as a High Temperature Gas Reactor (HTGR). There are significant differences between current LWR's and the proposed HTGR's but most especially in the composition of the nuclear fuel. For LWR's, the fuel elements consist of pellets of uranium dioxide or plutonium dioxide that are placed in long tubes made of zirconium metal alloys. For HTGR's, the fuel, known as TRISO (TRIstructural-ISOtropic) fuel, consists of an inner sphere of fissile material, a layer of dense pyrolytic carbon (PyC), a ceramic layer of silicon carbide (SiC) and a final dense outer layer of PyC. These TRISO particles are then compacted with graphite into fuel rods that are then placed in channels in graphite blocks. The blocks are then arranged in an annular fashion to form a reactor core. However, this new fuel form has unanswered questions on the environmental post-burn-up behavior. The key question for current once-through fuel operations is how these large irradiated graphite blocks with spent fuel inside will behave in a repository environment. Data in the literature to answer this question is lacking, but nevertheless this is an important question that must be answered before wide-spread adoption of HTGR's could be considered. This research has focused on answering the question of how the large quantity of graphite surrounding the spent HTGR fuel will impact the release of aqueous uranium from the TRISO fuel. In order to answer this question, the sorption and partitioning behavior of uranium to graphite under a variety of conditions was investigated. Key systematic variables that were analyzed include solution pH, dissolved carbonate concentration, uranium metal concentration and ionic strength. The kinetics and desorption characteristics of uranium/graphite partitioning were studied as well. The graphite used in these experiments was also characterized by a variety of techniques and conclusions are drawn about the relevant surface chemistry of graphite. This data was then used to generate a model for the reactive transport of uranium in a graphite matrix. This model was implemented with the software code CXTFIT and validated through the use of column studies mirroring the predicted system.

Ba, B, and U element partitioning in magnesian calcite skeletons of Octocorallia corals

NASA Astrophysics Data System (ADS)

Yoshimura, T.; Suzuki, A.; Iwasaki, N.

2015-01-01

Barium, boron and uranium element partitioning and oxygen and carbon isotope fractionation of high-Mg calcite skeletons of Octocorallia corals were investigated. The dissolved Ba concentration in seawater and the coral Ba/Ca ratio showed a clear positive correlation. The empirically derived barium partition coefficient is comparable to previous data for not only calcitic corals but also intermediate- to deep-water-dwelling scleractinian corals whose skeletons are composed of aragonite. Octocorallia corals are geologically important producers of biominerals, and they provide long-term records (up to hundreds of years) of environmental conditions in the deep ocean. Our data suggest that Ba/Ca ratios in Octocorallia corals may be a useful proxy for nutrients in intermediate and deep waters. The Ba/Ca ratio, a possible proxy for pH or carbonate ion concentration in seawater, showed the largest correlation with δ13C among the examined parameters. This result implies that the pH of the extracytoplasmic calcifying fluid (ECF) simultaneously influences δ18O, δ13C, and Ba/Ca by influencing the relative contributions of dissolved carbon sources in the ECF. Positive correlations of Ba/Ca with δ18 and δ13C suggest that δ18 and δ13C are enriched in light isotopes when conditions are less alkaline, suggesting a potential role of biological alkalinity pumping becomes more favorable with decreasing calcifying fluid pH. Substantial inter- and intra-specimen variations in Ba/Ca suggest that physicochemical factors do not exert a dominant systematic control on U incorporation.

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.

Target and method for the production of fission product molybdenum-99

DOEpatents

Vandegrift, George F.; Vissers, Donald R.; Marshall, Simon L.; Varma, Ravi

1989-01-01

A target for the reduction of fission product Mo-99 is prepared from uranium of low U-235 enrichment by coating a structural support member with a preparatory coating of a substantially oxide-free substrate metal. Uranium metal is electrodeposited from a molten halide electrolytic bath onto a substrate metal. The electrodeposition is performed at a predetermined direct current rate or by using pulsed plating techniques which permit relaxation of accumulated uranium ion concentrations within the melt. Layers of as much as to 600 mg/cm.sup.2 of uranium can be prepared to provide a sufficient density to produce acceptable concentrations of fission product Mo-99.

Long-term accumulation of uranium in bones of Wistar rats as a function of intake dosages.

PubMed

Arruda-Neto, J D T; Guevara, M V Manso; Nogueira, G P; Saiki, M; Cestari, A C; Shtejer, K; Deppman, A; Pereira Filho, J W; Garcia, F; Geraldo, L P; Gouveia, A N; Guzmán, F; Mesa, J; Rodriguez, O; Semmler, R; Vanin, V R

2004-01-01

Groups of Wistar rats were fed with ration doped with uranyl nitrate at concentration A ranging from 0.5 to 100 ppm, starting after the weaning period and lasting until the postpuberty period when the animals were sacrificed. Uranium in the ashes of bones was determined by neutron activation analysis. It was found that the uranium concentration in the bones, as a function of A, exhibits a change in its slope at approximately 20 ppm-a probable consequence of the malfunctioning of kidneys. The uranium transfer coefficient was obtained and an analytical expression was fitted into the data, thus allowing extrapolation down to low doses. Internal and localized doses were calculated. Absorbed doses exceeded the critical dose, even for the lowest uranium dosage.

Water-Quality Assessment of the Rio Grande Valley, Colorado, New Mexico, and Texas--Surface-Water Quality, Shallow Ground-Water Quality, and Factors Affecting Water Quality in the Rincon Valley, South-Central New Mexico, 1994-95

USGS Publications Warehouse

Anderholm, Scott K.

2002-01-01

As part of the National Water-Quality Assessment Program, surface-water and ground-water samples were collected in 1994 and 1995 for analysis of common constituents, nutrients, dissolved organic carbon, trace elements, radioactivity, volatile organic compounds, and pesticides to characterize surface- water quality and shallow ground-water quality and to determine factors affecting water quality in the Rincon Valley, south-central New Mexico. Samples of surface water were collected from three sites on the Rio Grande and from sites on three agricultural drains in the Rincon Valley in January 1994 and 1995, April 1994, and October 1994. Ground-water samples were collected in late April and early May 1994 from 30 shallow wells that were installed during the investigation. Dissolved-solids concentrations in surface water ranged from 434 to 1,510 milligrams per liter (mg/L). Dissolved-solids concentrations were smallest in water from the Rio Grande below Caballo Dam and largest in the drains. Nitrite plus nitrate concentrations ranged from less than 0.05 to 3.3 mg/L as nitrogen, and ammonia concentrations ranged from less than 0.015 to 0.33 mg/L as nitrogen in surface-water samples. Trace-element concentrations in surface water were significantly smaller than the acute-fisheries standards. One or more pesticides were detected in 34 of 37 surface-water samples. DCPA (dacthal) and metolachlor were the most commonly detected pesticides. No standards have been established for the pesticides analyzed for in this study. Dissolved-solids concentrations in shallow ground water ranged from 481 to 3,630 mg/L. All but 2 of 30 samples exceeded the secondary maximum contaminant level for dissolved solids of 500 mg/L. Water from about 73 percent of the wells sampled exceeded the secondary maximum contaminant level of 250 mg/L for sulfate, and water from about 7 percent of the wells sampled exceeded the secondary maximum contaminant level of 250 mg/L for chloride. Nitrite plus nitrate concentrations ranged from less than 0.05 to 33 mg/L as nitrogen in shallow ground water. Water from about 17 percent of the well samples exceeded the maximum contaminant level of 10 mg/L as nitrogen for nitrite plus nitrate. Trace-element concentrations in shallow ground water generally were small (1 to 10 micrograms per liter). The proposed maximum contaminant level of 20 micrograms per liter for uranium was exceeded in about 13 percent of the samples. The secondary maximum contaminant level of 300 micrograms per liter for iron was exceeded in about 17 percent of the samples and of 50 micrograms per liter for manganese was exceeded in about 83 percent of the samples. Samples from about 23 percent of the wells exceeded the maximum contaminant level of 15 picocuries per liter for gross alpha activity. One or more pesticides were detected in water from 12 of 30 wells sampled. The pesticides or pesticide metabolites diazinon, metolachlor, napropamide, p,p'-DDE, and prometon were detected in one or more samples. Metolachlor and prometon were the most commonly detected pesticides. Health advisories for the pesticides detected in shallow ground water (no maximum contaminant levels have been established for the pesticides detected) are 10 to 300 times larger than the concentrations detected. Infiltration, evaporation, and transpiration of irrigation water are important factors affecting the concentrations of common constituents in shallow ground water in the Rincon Valley. Dissolution and precipitation of minerals and mixing of shallow ground water and inflow of ground water from adjacent areas also affect the composition of shallow ground water and water in the drains. Relatively large nitrite plus nitrate concentrations in several shallow ground-water samples indicate leaching of fertilizers in some areas of th

Uranium and other natural radionuclides in drinking water and risk of leukemia: a case-cohort study in Finland.

PubMed

Auvinen, Anssi; Kurttio, Päivi; Pekkanen, Juha; Pukkala, Eero; Ilus, Taina; Salonen, Laina

2002-11-01

We assessed the effect of natural uranium and other radionuclides in drinking water on risk of leukemia. The subjects (n = 144,627) in the base cohort had lived outside the municipal tapwater system during 1967-1980. A subcohort was formed as a stratified random sample of the base cohort and subjects using drinking water from drilled wells prior to 1981 were identified. A case-cohort design was used comparing exposure among cases with leukemia (n = 35) with a stratified random sample (n = 274) from the subcohort. Activity concentrations of uranium, radium-226, and radon in the drinking water were analyzed using radiochemical and alpha-spectrometric methods. The median activity concentration of uranium in well water was 0.08 Bq/L for the leukemia cases and 0.06 Bq/L for the reference group, radon concentrations 80 and 130 Bq/L, respectively, and radium-226 concentrations 0.01 Bq/L for both groups. The hazard ratio of leukemia for uranium was 0.91 (95% confidence interval 0.73-1.13) per Bq/L. for radon 0.79 per Bq/L (95% CI 0.27-2.29), and for radium-226 0.80 (95% CI 0.46-1.39) per Bq/L. Our results do not indicate an increased risk of leukemia from ingestion of natural uranium or other radionuclides through drinking water at these exposure levels.

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

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

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

Volumetric determination of uranium using titanous sulfate as reductant before oxidimetric titration

USGS Publications Warehouse

Wahlberg, James S.; Skinner, Dwight L.; Rader, Lewis F.

1956-01-01

A new method for determining uranium in samples containing 0.05 percent or more U3O8, using titanous sulfate as reducing agent, is much shorter, faster, and has fewer interferences than conventional methods using reductor columns. The sample is dissolved with sulfuric, nitric, perchloric, and hydrofluoric acids. Elements that would otherwise form insoluble fluorides are kept in solution by complexing the fluoride ion with boric acid. A precipitation is made with cupferron to remove interfering elements. The solution is filtered to remove the precipitated cupferrates instead of extracting them with chloroform as is usually done. Filtration is preferred to extraction because any niobium that may be in solution forms an insoluble cupferrate that may be removed by filtering but is very difficult to extract with chloroform. Excess cupferron is destroyed by oxidizing with nitric and perchloric acids, and evaporating to dense fumes of sulfuric acid. The uranium is reduced to U(IV) by the addition of titanous sulfate, with cupric sulfate used as an indicator of the completeness of the reduction. Metallic copper is formed when all the uranium is reduced. The reduced copper is then reoxidized by the addition of mercuric perchlorate, an excess of ferric sulfate added, and the solution titrated immediately with standard ceric sulfate with ferroin as an indicator. Precision of the method compared favorable with methods in common use, both for uranium ores and for most types of uranium-rich materials.

Data Validation Package December 2015 Groundwater Sampling at the Ambrosia Lake, New Mexico, Disposal Site March 2016

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

Tsosie, Bernadette; Johnson, Dick

The Long-Term Surveillance Plan for the Ambrosia Lake, New Mexico, Disposal Site does not require groundwater monitoring because groundwater in the uppermost aquifer is of limited use, and supplemental standards have been applied to the aquifer. However, at the request of the New Mexico Environment Department, the U.S. Department of Energy conducts annual monitoring at three locations: monitoring wells 0409, 0675, and 0678. Sampling and analyses were conducted as specified in the Sampling and Analysis Plan for US. Department of Energy Office of Legacy Management Sites (LMS/PRO/S04351, continually updated). Monitoring Well 0409 was not sampled during this event because itmore » was dry. Water levels were measured at each sampled well. One duplicate sample was collected from location 0675. Groundwater samples from the two sampled wells were analyzed for the constituents listed in Table 1. Time-concentration graphs for selected analytes are included in this report. At well 0675, the duplicate results for total dissolved solids and for most metals (magnesium, molybdenum, potassium, selenium, sodium, and uranium) were outside acceptance criteria, which may indicate non-homogeneous conditions at this location. November 2014 results for molybdenum and uranium at well 0675 also were outside acceptance criteria. The well condition will be evaluated prior to the next sampling event.« less

Chemical and biological quality of streams at the Indiana Dunes National Lakeshore, Indiana, 1978-80

USGS Publications Warehouse

Hardy, M.A.

1984-01-01

Wetland drainage contributed significant amounts of organic materials to streams and at times increased concentrations of dissolved sulfate and iron. Dissolved-iron concentrations correlated with dissolved-organic-carbon concentrations in yellow-brown water of Kintzele and Derby ditches.

Correlation between electron spin resonance spectra and oil yield in eastern oil shales

USGS Publications Warehouse

Choudhury, M.; Rheams, K.F.; Harrell, J.W.

1986-01-01

Organic free radical spin concentrations were measured in 60 raw oil shale samples from north Alabama and south Tennessee and compared with Fischer assays and uranium concentrations. No correlation was found between spin concentration and oil yield for the complete set of samples. However, for a 13 sample set taken from a single core hole, a linear correlation was obtained. No correlation between spin concentration and uranium concentration was found. ?? 1986.

Long-term ecological effects of exposure to uranium

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

Hanson, W.C.; Miera, F.R. Jr.

1976-03-01

The consequences of releasing natural and depleted uranium to terrestrial ecosystems during development and testing of depleted uranium munitions were investigated. At Eglin Air Force Base, Florida, soil at various distances from armor plate target butts struck by depleted uranium penetrators was sampled. The upper 5 cm of soil at the target bases contained an average of 800 ppM of depleted uranium, about 30 times as much as soil at 5- to 10-cm depth, indicating some vertical movement of depleted uranium. Samples collected beyond about 20 m from the targets showed near-background natural uranium levels, about 1.3 +- 0.3 ..mu..g/gmore » or ppM. Two explosives-testing areas at the Los Alamos Scientific Laboratory (LASL) were selected because of their use history. E-F Site soil averaged 2400 ppM of uranium in the upper 5 cm and 1600 ppM at 5-10 cm. Lower Slobovia Site soil from two subplots averaged about 2.5 and 0.6 percent of the E-F Site concentrations. Important uranium concentration differences with depth and distance from detonation points were ascribed to the different explosive tests conducted in each area. E-F Site vegetation samples contained about 320 ppM of uranium in November 1974 and about 125 ppM in June 1975. Small mammals trapped in the study areas in November contained a maximum of 210 ppM of uranium in the gastrointestinal tract contents, 24 ppM in the pelt, and 4 ppM in the remaining carcass. In June, maximum concentrations were 110, 50, and 2 ppM in similar samples and 6 ppM in lungs. These data emphasized the importance of resuspension of respirable particles in the upper few millimeters of soil as a contamination mechanism for several components of the LASL ecosystem.« less

Isotopic Tracers for Delineating Non-Point Source Pollutants in Surface Water

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

Davisson, M L

2001-03-01

This study tested whether isotope measurements of surface water and dissolved constituents in surface water could be used as tracers of non-point source pollution. Oxygen-18 was used as a water tracer, while carbon-14, carbon-13, and deuterium were tested as tracers of DOC. Carbon-14 and carbon-13 were also used as tracers of dissolved inorganic carbon, and chlorine-36 and uranium isotopes were tested as tracers of other dissolved salts. In addition, large databases of water quality measurements were assembled for the Missouri River at St. Louis and the Sacramento-San Joaquin Delta in California to enhance interpretive results of the isotope measurements. Muchmore » of the water quality data has been under-interpreted and provides a valuable resource to investigative research, for which this report exploits and integrates with the isotope measurements.« less

Radium and radon in ground water in the Chickies Quartzite, southeastern Pennsylvania

USGS Publications Warehouse

Senior, L.A.; Vogel, K.L.

1995-01-01

The Chickies Quartzite, a Lower Cambrian-age formation compromised of quartzite and slate overlying a basal conglomerate, forms a narrow ridges and crops out discontinuously over 112 square miles in the Piedmont physiographic province of southeastern Pennsylvania. The formation is a low-yielding, fractured- rock, water-table aquifer recharged primarily by local precipitation. It is the sole source of water supply for thousands of domestic users. Ground water in the Chickies Quartzite generally is soft and acidic. During 1986-88, the U.S. Geological Survey sampled water from 160 wells that penetrate the Chickies Quartzite to determine the magnitude and distribution of radium-226 (Ra-226), radium-228 (Ra-228), and radon-222 (Rn-222) activities in ground water in the formation and to characterize the geochemical environmental associated with elevated activities of radium (Ra). In addition, 28 wells penetrating adjacent geologic units and 1 well in the Hardyston Quartzite were sampled to determine relative background Ra and RN-222 activities in ground water. Analyses included determination of activities of dissolved Ra-226, Ra-228, and RN-222, and concentrations of dissolved uranium (U), dissolved organic carbon (DOC), and major and minor dissolved inorganic ions. Rock samples were analyzed for U and thorium (Th) and geophysical logs were run to determine sources of Ra and RN-222 in the Chickies Quartzite. Activities of up to 41 pCi/L (picocuries per liter) for Ra-226, 160 pCi/L for Ra-228, and 32,300 pCi/L for RN-222 were measured in ground water in the Chickies Quartzite. Forty-seven percent of the samples contained Ra-226 and Ra-228 activities greater than 5 pCi/L. Median activities measured were 1.2 pCi/L for Ra-226, 2.6 pCi/L for Ra-228, 4.2 pCi/L for combined Ra-226 and Ra-228, and 2,400 pCi/L for RN-222 Ra-228 activity exceeded Ra-226 activity in about 92 percent of 100 water samples; the median Ra-228/Ra226 activity ratio was 2.4. Ra-228/Ra-226 activity ratios commonly were greater in ground water than calculated Th/U ratios in rock samples, suggesting perferential leaching of Ra-228 from aquifer solids. Of ground water in the adjacent geologic units, the highest activities (up to 2.9 pCi/L for Ra-226, 12 pCi/L for Ra-228, and 25,300 pCi/L for RN-222) were measured in ground water in the Harpers Phyllite and Antietam Quartzite. Nonparametric (Spearman rho test) statistical correlations show that the activity of dissolved Ra is inversely related to pH and directly related to concentrations of total dissolved solids, DOC, barium, and sulfate. Low pH decreases absorption of Ra onto the aquifer matrix. The other factors may favor Ra mobility by enhancing complexation or increasing solubility. RN-222 activity does not correlate with and is not supported by the activity of its parent, Ra-226, in solution. Ra-226 activity correlates positively, but weakly, with U concentrations. Ra-226 does not appear to be supported by its parent, U-238, in solution. Observed distributions of Ra-228, Ra-226, and RN-222 activities in ground water in different lithologies of the Chickies Quartzite reflect different geochemical controls on absorption and distribution of parent thorium-232 (Th-232) and uranium-238 (U-238) in the formation. Radium activities were greatest in acidic ground water in the conglomerate and quartzite (median pH of 5.0 and 5.2, respectively) and least in the more neutral water in the slate (median pH of 6.4). For ground water in the conglomerate, quartzite, and slate, respectively, median activities measured were 1.3, 1.5, and .02 pCi/L for Ra-226; and 3.7, 2.5, and 1.0 pCi/L for Ra-228. Natural-gamma-ray geophysical logs and results of rock analyses indicate that the conglomerate may contain more Th and U than the quartzite and that the conglomerate may be more enriched in Th with respect to U than the quartzite; Th and U distribution in both lithogies is variable. Median RN-222 activities in gro

Uranium in sediments, mussels (Mytilus sp.) and seawater of the Krka river estuary.

PubMed

Cuculić, Vlado; Cukrov, Neven; Barisić, Delko; Mlakar, Marina

2006-01-01

The response of an aquatic environment to the decrease of phosphate discharges from a technologically improved transhipment terminal, situated at the Croatian Adriatic coast in the port of Sibenik, has been assessed based on uranium activity and concentration in sediment, seawater and mussels Mytilus sp. The highest 238U activities (485+/-16Bqkg(-1) dry weight) were found in the sediment sample collected from the sampling site closest to the terminal. The maximum concentrations in the sediment samples are above the natural ranges and clearly indicate the harbour activities' influence. The 238U/226Ra activity ratios in sediment samples demonstrate the decreasing trend of phosphate ore input. Mussel samples showed levels of 238U activities in the range from 12.1+/-2.9 to 19.4+/-7.2 Bqkg(-1) dry weight, thus being slightly higher than in normally consumed mussels. Only the seawater, taken just above the bottom sediment at the sampling site closest to the terminal, shows a slightly higher uranium concentration (3.1+/-0.2 microgL(-1)) when compared to the samples taken in upper seawater layers (2.1+/-0.2 microgL(-1)) but is in the range of the concentration level of uranium in natural seawater. Since the transhipment terminal in the port of Sibenik was modernised in 1988, discharge of phosphate ore into the seawater was drastically reduced and, consequently, uranium concentration levels in seawater have decreased. However, enhanced uranium activity levels are still found in deeper sediment layer samples and in mussel.

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.

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.

METHOD OF RECOVERING TRANSURANIC ELEMENTS OF AN ATOMIC NUMBER BELOW 95

DOEpatents

Seaborg, G.T.; James, R.A.

1959-12-15

The concentration of neptanium or plutonium by two carrier precipitation steps with identical carriers but using (after dissolution of the first carrier in nitric acid) a reduced quantity of carrier for the second precipitation is discussed. Carriers suitable are uranium(IV) hypophosphate, uranium(IV) pyrophosphate, uranium(IV) oxalate, thorium oxalate, thorium citrate, thorium tartrate, thorium sulfide, and uranium(IV) sulfide.

Drought effects on water quality in the South Platte River Basin, Colorado

USGS Publications Warehouse

Sprague, Lori A.

2005-01-01

Twenty-three stream sites representing a range of forested, agricultural, and urban land uses were sampled in the South Platte River Basin of Colorado from July through September 2002 to characterize water quality during drought conditions. With a few exceptions, dissolved ammonia, Kjeldahl nitrogen, total phosphorus, and dissolved orthophosphate concentrations were similar to seasonal historical levels in all land use areas during the drought. At some agricultural sites, decreased dilution of irrigation return flow may have contributed to higher concentrations of some nutrient species, increased primary productivity, and higher dissolved oxygen concentrations. At some urban sites, decreased dilution of base flow and wastewater treatment plant effluent may have contributed to higher dissolved nitrite-plus-nitrate concentrations, increased primary productivity, and higher dissolved oxygen concentrations. Total pesticide concentrations in urban and agricultural areas were not consistently higher or lower during the drought. At most forested sites, decreased dilution of ground water-derived calcium bicarbonate type base flow likely led to elevated pH and specific-conductance values. Water temperatures at many of the forested sites also were higher, contributing to lower dissolved oxygen concentrations during the drought.

Uranium in Kosovo's drinking water.

PubMed

Berisha, Fatlume; Goessler, Walter

2013-11-01

The results of this paper are an initiation to capture the drinking water and/or groundwater elemental situation in the youngest European country, Kosovo. We aim to present a clear picture of the natural uranium concentration in drinking water and/or groundwater as it is distributed to the population of Kosovo. Nine hundred and fifty-one (951) drinking water samples were analyzed by inductively coupled plasma mass spectrometry (ICPMS). The results are the first countrywide interpretation of the uranium concentration in drinking water and/or groundwater, directly following the Kosovo war of 1999. More than 98% of the samples had uranium concentrations above 0.01 μg L(-1), which was also our limit of quantification. Concentrations up to 166 μg L(-1) were found with a mean of 5 μg L(-1) and median 1.6 μg L(-1) were found. Two point six percent (2.6%) of the analyzed samples exceeded the World Health Organization maximum acceptable concentration of 30 μg L(-1), and 44.2% of the samples exceeded the 2 μg L(-1) German maximum acceptable concentrations recommended for infant food preparations. Copyright © 2013 Elsevier Ltd. All rights reserved.

Tetravalent uranium extraction by HDEHP in kerosene from phosphate medium

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

Daoud, J.A.; Zeid, M.M.; Aly, H.F.

1997-03-01

The extraction of U(IV) by di-2-ethylhexyl phosphoric acid (HDEHP) in kerosene from phosphoric acid was measured spectrophotometrically. The effect of extractant, phosphoric acid, uranium, Fe(II) and Fe(III) concentrations on the extraction process were separately investigated. The effect of different reagents and temperature on the stripping of U(IV) were also tested. The results obtained showed that the extraction increases with the increase in HDEHP and Fe(III) concentrations while it decreases with the increase in phosphoric acid, uranium and Fe(II) concentration. The use of high phosphoric acid concentration as strip solutions at low temperature was found to give good stripping results. 11more » refs., 8 figs., 2 tabs.« less

Dynamic leaching studies of 48 MWd/kgU UO2 commercial spent nuclear fuel under oxic conditions

NASA Astrophysics Data System (ADS)

Serrano-Purroy, D.; Casas, I.; González-Robles, E.; Glatz, J. P.; Wegen, D. H.; Clarens, F.; Giménez, J.; de Pablo, J.; Martínez-Esparza, A.

2013-03-01

The leaching of a high-burn-up spent nuclear fuel (48 MWd/KgU) has been studied in a carbonate-containing solution and under oxic conditions using a Continuously Stirred Tank Flow-Through Reactor (CSTR). Two samples of the fuel, one prepared from the centre of the pellet (labelled CORE) and another one from the fuel pellet periphery, enriched with the so-called High Burn-Up Structure (HBS, labelled OUT) have been used.For uranium and actinides, the results showed that U, Np, Am and Cm gave very similar normalized dissolution rates, while Pu showed slower dissolution rates for both samples. In addition, dissolution rates were consistently two to four times lower for OUT sample compared to CORE sample.Considering the fission products release the main results are that Y, Tc, La and Nd dissolved very similar to uranium; while Cs, Sr, Mo and Rb have up to 10 times higher dissolution rates. Rh, Ru and Zr seemed to have lower dissolution rates than uranium. The lowest dissolution rates were found for OUT sample.Three different contributions were detected on uranium release, modelled and attributed to oxidation layer, fines and matrix release.

Isotopic tracking of Hanford 300 area derived uranium in the Columbia River.

PubMed

Christensen, John N; Dresel, P Evan; Conrad, Mark E; Patton, Gregory W; DePaolo, Donald J

2010-12-01

Our objectives in this study are to quantify the discharge rate of uranium (U) to the Columbia River from the Hanford Site's 300 Area and to follow that U downriver to constrain its fate. Uranium from the Hanford Site has variable isotopic composition due to nuclear industrial processes carried out at the site. This characteristic makes it possible to use high-precision isotopic measurements of U in environmental samples to identify even trace levels of contaminant U, determine its sources, and estimate discharge rates. Our data on river water samples indicate that as much as 3.2 kg/day can enter the Columbia River from the 300 Area, which is only a small fraction of the total load of dissolved natural background U carried by the Columbia River. This very low level of Hanford-derived U can be discerned, despite dilution to <1% of natural background U, 400 km downstream from the Hanford Site. These results indicate that isotopic methods can allow the amounts of U from the 300 Area of the Hanford Site entering the Columbia River to be measured accurately to ascertain whether they are an environmental concern or insignificant relative to natural uranium background in the Columbia River.

Determination of Depleted Uranium in Environmental Bio-monitor Samples and Soil from Target sites in Western Balkan Region

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

Sahoo, Sarata K.; Enomoto, Hiroko; Tokonami, Shinji

2008-08-07

Lichen and Moss are widely used to assess the atmospheric pollution by heavy metals and radionuclides. In this paper, we report results of uranium and its isotope ratios using mass spectrometric measurements (followed by chemical separation procedure) for mosses, lichens and soil samples from a depleted uranium (DU) target site in western Balkan region. Samples were collected in 2003 from Han Pijesak (Republika Srpska in Bosnia and Hercegovina). Inductively coupled plasma mass spectrometry (ICP-MS) measurements show the presence of high concentration of uranium in some samples. Concentration of uranium in moss samples ranged from 5.2-755.43 Bq/Kg. We have determined {supmore » 235}U/{sup 238}U isotope ratio using thermal ionization mass spectrometry (TIMS) from the samples with high uranium content and the ratios are in the range of 0.002097-0.002380. TIMS measurement confirms presence of DU in some samples. However, we have not noticed any traces of DU in samples containing lesser amount of uranium or from any samples from the living environment of same area.« less

Assessing the concentration, speciation, and toxicity of dissolved metals during mixing of acid-mine drainage and ambient river water downstream of the Elizabeth Copper Mine, Vermont, USA

USGS Publications Warehouse

Balistrieri, L.S.; Seal, R.R.; Piatak, N.M.; Paul, B.

2007-01-01

The authors determine the composition of a river that is impacted by acid-mine drainage, evaluate dominant physical and geochemical processes controlling the composition, and assess dissolved metal speciation and toxicity using a combination of laboratory, field and modeling studies. Values of pH increase from 3.3 to 7.6 and the sum of dissolved base metal (Cd + Co + Cu + Ni + Pb + Zn) concentrations decreases from 6270 to 100 ??g/L in the dynamic mixing and reaction zone that is downstream of the river's confluence with acid-mine drainage. Mixing diagrams and PHREEQC calculations indicate that mixing and dilution affect the concentrations of all dissolved elements in the reach, and are the dominant processes controlling dissolved Ca, K, Li, Mn and SO4 concentrations. Additionally, dissolved Al and Fe concentrations decrease due to mineral precipitation (gibbsite, schwertmannite and ferrihydrite), whereas dissolved concentrations of Cd, Co, Cu, Ni, Pb and Zn decrease due to adsorption onto newly formed Fe precipitates. The uptake of dissolved metals by aquatic organisms is dependent on the aqueous speciation of the metals and kinetics of complexation reactions between metals, ligands and solid surfaces. Dissolved speciation of Cd, Cu, Ni and Zn in the mixing and reaction zone is assessed using the diffusive gradients in thin films (DGT) technique and results of speciation calculations using the Biotic Ligand Model (BLM). Data from open and restricted pore DGT units indicate that almost all dissolved metal species are inorganic and that aqueous labile or DGT available metal concentrations are generally equal to total dissolved concentrations in the mixing zone. Exceptions occur when labile metal concentrations are underestimated due to competition between H+ and metal ions for Chelex-100 binding sites in the DGT units at low pH values. Calculations using the BLM indicate that dissolved Cd and Zn species in the mixing and reaction zone are predominantly inorganic, which is consistent with the DGT results. Although the DGT method indicates that the majority of aqueous Cu species are inorganic, BLM calculations indicate that dissolved Cu is inorganic at pH 5.5. Integrated dissolved labile concentrations of Cd, Cu and Zn in the mixing and reaction zone are compared to calculated acute toxicity concentrations (LC50 values) for fathead minnows (Pimephales promelas) (Cd, Cu and Zn) and water fleas (Ceriodaphnia dubia) (Cd and Cu) using the BLM, and to national recommended water quality criteria [i.e., criteria maximum concentration (CMC) and criterion continuous concentration (CCC)]. Observed labile concentrations of Cd and Zn are below LC50 values and CMC for Cd, but above CCC and CMC for Zn at sites <30 m downstream of the confluence. In contrast, labile Cu concentrations exceed LC50 values for the organisms as well as CCC and CMC at sites <30 m downstream of the confluence. These results suggest that environmental conditions at sites closest to the confluence of the river and acid-mine drainage should not support healthy aquatic organisms. ?? 2007 Elsevier Ltd. All rights reserved.

Recovery of fissile materials from nuclear wastes

DOEpatents

Forsberg, Charles W.

1999-01-01

A process for recovering fissile materials such as uranium, and plutonium, and rare earth elements, from complex waste feed material, and converting the remaining wastes into a waste glass suitable for storage or disposal. The waste feed is mixed with a dissolution glass formed of lead oxide and boron oxide resulting in oxidation, dehalogenation, and dissolution of metal oxides. Carbon is added to remove lead oxide, and a boron oxide fusion melt is produced. The fusion melt is essentially devoid of organic materials and halogens, and is easily and rapidly dissolved in nitric acid. After dissolution, uranium, plutonium and rare earth elements are separated from the acid and recovered by processes such as PUREX or ion exchange. The remaining acid waste stream is vitrified to produce a waste glass suitable for storage or disposal. Potential waste feed materials include plutonium scrap and residue, miscellaneous spent nuclear fuel, and uranium fissile wastes. The initial feed materials may contain mixtures of metals, ceramics, amorphous solids, halides, organic material and other carbon-containing material.

CONTINUOUS CHELATION-EXTRACTION PROCESS FOR THE SEPARATION AND PURIFICATION OF METALS

DOEpatents

Thomas, J.R.; Hicks, T.E.; Rubin, B.; Crandall, H.W.

1959-12-01

A continuous process is presented for separating metal values and groups of metal values from each other. A complex mixture. e.g., neutron-irradiated uranium, can be resolved into component parts. In the present process the values are dissolved in an acidic solution and adjusted to the proper oxidation state. Thenceforth the solution is contacted with an extractant phase comprising a fluorinated beta -diketone in an organic solvent under centain pH conditions whereupon plutonium and zirconium are extracted. Plutonium is extracted from the foregoing extract with reducing aqueous solutions or under specified acidic conditions and can be recovered from the aqueous solution. Zirconium is then removed with an oxalic acid aqueous phase. The uranium is recovered from the residual original solution using hexone and hexone-diketone extractants leaving residual fission products in the original solution. The uranium is extracted from the hexone solution with dilute nitric acid. Improved separations and purifications are achieved using recycled scrub solutions and the "self-salting" effect of uranyl ions.

TRANSURANIC ELEMENT, COMPOSITION THEREOF, AND METHODS FOR PRODUCING SEPARATING AND PURIFYING SAME

DOEpatents

Wahl, A.C.

1961-09-19

A process of separating plutonium from fission products contained in an aqueous solution is described. Plutonium, in the tri- or tetravalent state, and the fission products are coprecipitated on lanthanum fluoride, lanthanum oxalate, cerous fluoride, cerous phosphate, ceric iodate, zirconyl phosphate, thorium iodate, or thorium fluoride. The precipitate is dissolved in acid, and the plutonium is oxidized to the hexavalent state. The fission products are selectively precipitated on a carrier of the above group but different from that used for the coprecipitation. The plutonium in the solution, after removal of the fission product precipitate, is reduced to at least the tetravalent state and precipitated on lanthanum fluoride, lanthanum phosphate, lanthanum oxalate, lanthanum hydroxide, cerous fluoride, cerous phosphate, cerous oxalate, cerous hydroxide, ceric iodate, zirconyl phosphate, zirconyl iodate, zirconium hydroxide, thorium fluoride, thorium oxalate, thorium iodate, thorium peroxide, uranium iodate, uranium oxalate, or uranium peroxide, again using a different carrier than that used for the precipitation of the fission products.

An evaluation of health risk to the public as a consequence of in situ uranium mining in Wyoming, USA

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

Ruedig, Elizabeth; Johnson, Thomas E.

In the United States there is considerable public concern regarding the health effects of in situ recovery uranium mining. These concerns focus principally on exposure to contaminants mobilized in groundwater by the mining process. However, the risk arising as a result of mining must be viewed in light of the presence of naturally occurring uranium ore and other constituents which comprise a latent hazard. The United States Environmental Protection Agency recently proposed new guidelines for successful restoration of an in situ uranium mine by limiting concentrations of thirteen groundwater constituents: arsenic, barium, cadmium, chromium, lead, mercury, selenium, silver, nitrate (asmore » nitrogen), molybdenum, radium, total uranium, and gross α activity. We investigated the changes occurring to these constituents at an ISR uranium mine in Wyoming, USA by comparing groundwater quality at baseline measurement to that at stability (post-restoration) testing. Of the groundwater constituents considered, only uranium and radium-226 showed significant (p < 0.05) deviation from site-wide baseline conditions in matched-wells. Uranium concentrations increased by a factor of 5.6 (95% CI 3.6–8.9 times greater) while radium-226 decreased by a factor of about one half (95% CI 0.42–0.75 times less). Change in risk was calculated using the RESRAD (onsite) code for an individual exposed as a resident-farmer; total radiation dose to a resident farmer decreased from pre-to post-mining by about 5.2 mSv y –1. As a result, higher concentrations of uranium correspond to increased biomarkers of nephrotoxicity, however the clinical significance of this increase is unclear.« less

Adsorption property of Br-PADAP-impregnated multiwall carbon nanotubes towards uranium and its performance in the selective separation and determination of uranium in different environmental samples.

PubMed

Khamirchi, Ramzanali; Hosseini-Bandegharaei, Ahmad; Alahabadi, Ahmad; Sivamani, Selvaraju; Rahmani-Sani, Abolfazl; Shahryari, Taher; Anastopoulos, Ioannis; Miri, Mohammad; Tran, Hai Nguyen

2018-04-15

A newer efficient U(VI) ion adsorbent was synthesized by impregnating Br-PADAP [2-(5-Bromo-2-pyridylazo)-5-(diethylamino)phenol] onto multiwall carbon nanotubes (MWCNTs). The effects of various operation conditions on uranium adsorption (i.e., pH contact time, temperature, and initial uranium concentration) were systematically evaluated using batch experiments. The results indicated that the uranium adsorption on modified MWNCTs (5.571 × 10 -3 g/mg × min) reached faster equilibrium than that on pristine MWNCTs (4.832 × 10 -3 g/mg × min), reflecting the involvement of appropriate functional groups of Br-PADAP on the chelating ion-exchange mechanism of U(VI) adsorption. Modified MWNCTs (83.4mg/g) exhibited significantly higher maximum Langmuir adsorption capacity than pristine MWNCTs (15.1mg/g). Approximately 99% of uranium adsorbed onto modified MWNCTs can be desorbed by 2.5mL of 1M HNO 3 solution. Therefore, Br-PADAP-modified MWNCTs can server as a promising adsorbent for efficient uranium adsorption applications in water treatment. Subsequently, the proposed solid-phase extraction (using a mini-column packed with Br-PADAP/MWCNT) was successfully utilized for analysing trace uranium levels by the ICP-AES method in different environmental samples with a pre-concentration factor of 300-fold. The coexistence of other ions demonstrated an insignificant interference on the separative pre-concentration of uranium. the detection limit was recognized as 0.14μg/L, and the relative standard deviation was approximately 3.3% (n = 7). Copyright © 2017 Elsevier Inc. All rights reserved.

An evaluation of health risk to the public as a consequence of in situ uranium mining in Wyoming, USA

DOE PAGES

Ruedig, Elizabeth; Johnson, Thomas E.

2015-08-30

In the United States there is considerable public concern regarding the health effects of in situ recovery uranium mining. These concerns focus principally on exposure to contaminants mobilized in groundwater by the mining process. However, the risk arising as a result of mining must be viewed in light of the presence of naturally occurring uranium ore and other constituents which comprise a latent hazard. The United States Environmental Protection Agency recently proposed new guidelines for successful restoration of an in situ uranium mine by limiting concentrations of thirteen groundwater constituents: arsenic, barium, cadmium, chromium, lead, mercury, selenium, silver, nitrate (asmore » nitrogen), molybdenum, radium, total uranium, and gross α activity. We investigated the changes occurring to these constituents at an ISR uranium mine in Wyoming, USA by comparing groundwater quality at baseline measurement to that at stability (post-restoration) testing. Of the groundwater constituents considered, only uranium and radium-226 showed significant (p < 0.05) deviation from site-wide baseline conditions in matched-wells. Uranium concentrations increased by a factor of 5.6 (95% CI 3.6–8.9 times greater) while radium-226 decreased by a factor of about one half (95% CI 0.42–0.75 times less). Change in risk was calculated using the RESRAD (onsite) code for an individual exposed as a resident-farmer; total radiation dose to a resident farmer decreased from pre-to post-mining by about 5.2 mSv y –1. As a result, higher concentrations of uranium correspond to increased biomarkers of nephrotoxicity, however the clinical significance of this increase is unclear.« less

An evaluation of health risk to the public as a consequence of in situ uranium mining in Wyoming, USA.

PubMed

Ruedig, Elizabeth; Johnson, Thomas E

2015-12-01

In the United States there is considerable public concern regarding the health effects of in situ recovery uranium mining. These concerns focus principally on exposure to contaminants mobilized in groundwater by the mining process. However, the risk arising as a result of mining must be viewed in light of the presence of naturally occurring uranium ore and other constituents which comprise a latent hazard. The United States Environmental Protection Agency recently proposed new guidelines for successful restoration of an in situ uranium mine by limiting concentrations of thirteen groundwater constituents: arsenic, barium, cadmium, chromium, lead, mercury, selenium, silver, nitrate (as nitrogen), molybdenum, radium, total uranium, and gross α activity. We investigated the changes occurring to these constituents at an ISR uranium mine in Wyoming, USA by comparing groundwater quality at baseline measurement to that at stability (post-restoration) testing. Of the groundwater constituents considered, only uranium and radium-226 showed significant (p < 0.05) deviation from site-wide baseline conditions in matched-wells. Uranium concentrations increased by a factor of 5.6 (95% CI 3.6-8.9 times greater) while radium-226 decreased by a factor of about one half (95% CI 0.42-0.75 times less). Change in risk was calculated using the RESRAD (onsite) code for an individual exposed as a resident-farmer; total radiation dose to a resident farmer decreased from pre-to post-mining by about 5.2 mSv y(-1). Higher concentrations of uranium correspond to increased biomarkers of nephrotoxicity, however the clinical significance of this increase is unclear. Published by Elsevier Ltd.

Solvent wash solution

DOEpatents

Neace, J.C.

1984-03-13

A process is claimed for removing diluent degradation products from a solvent extraction solution, which has been used to recover uranium and plutonium from spent nuclear fuel. A wash solution and the solvent extraction solution are combined. The wash solution contains (a) water and (b) up to about, and including, 50 vol % of at least one-polar water-miscible organic solvent based on the total volume of the water and the highly-polar organic solvent. The wash solution also preferably contains at least one inorganic salt. The diluent degradation products dissolve in the highly-polar organic solvent and the organic solvent extraction solvent do not dissolve in the highly-polar organic solvent. The highly-polar organic solvent and the extraction solvent are separated.

Solvent wash solution

DOEpatents

Neace, James C.

1986-01-01

Process for removing diluent degradation products from a solvent extraction solution, which has been used to recover uranium and plutonium from spent nuclear fuel. A wash solution and the solvent extraction solution are combined. The wash solution contains (a) water and (b) up to about, and including, 50 volume percent of at least one-polar water-miscible organic solvent based on the total volume of the water and the highly-polar organic solvent. The wash solution also preferably contains at least one inorganic salt. The diluent degradation products dissolve in the highly-polar organic solvent and the organic solvent extraction solvent do not dissolve in the highly-polar organic solvent. The highly-polar organic solvent and the extraction solvent are separated.

Reconnaissance for radioactive deposits in eastern Alaska, 1952

USGS Publications Warehouse

Nelson, Arthur Edward; West, Walter S.; Matzko, John J.

1954-01-01

Reconnaissance for radioactive deposits was conducted in selected areas of eastern Alaska during 1952. Examination of copper, silver, and molybdenum occurrences and of a reported nickel prospect in the Slana-Nabesna and Chisana districts in the eastern Alaska Range revealed a maximum radioactivity of about 0.003 percent equivalent uranium. No appreciable radioactivity anomolies were indicated by aerial and foot traverses in the area. Reconnaissance for possible lode concentrations of uranium minerals in the vicinity of reported fluoride occurrences in the Hope Creek and Miller House-Circle Hot Springs areas of the Circle quadrangle and in the Fortymile district found a maximum of 0.055 percent equivalent uranium in a float fragment of ferruginous breccia in the Hope Creek area; analysis of samples obtained in the vicinity of the other fluoride occurrences showed a maximum of only 0.005 percent equivalent uranium. No uraniferous loads were discovered in the Koyukuk-Chandalar region, nor was the source of the monazite, previously reported in the placer concentrates from the Chandalar mining district, located. The source of the uranotheorianite in the placers at Gold Bench on the South Fork of the Koyukuk River was not found during a brief reconaissance, but a placer concentrate was obtained that contains 0.18 percent equivalent uranium. This concentrate is about ten times more radioactive than concentrates previously available from the area.

Effects of depleted uranium on the health and survival of Ceriodaphnia dubia and Hyalella azteca

USGS Publications Warehouse

Kuhne, W.W.; Caldwell, C.A.; Gould, W.R.; Fresquez, P.R.; Finger, S.

2002-01-01

Depleted uranium (DU) has been used as a substitute for the fissionable enriched uranium component of atomic weapons tested at Los Alamos National Laboratory (LANL) (Los Alamos, NM, USA) since the early 1950s, resulting in considerable concentrations of DU in the soils within the test sites. Although the movement of DU into major aquatic systems has been shown to be minimal, there are many small-order ephemeral streams and areas of standing water in canyons throughout LANL that may be affected by inputs of DU via runoff, erosion, and leaching. Ninety-six-hour acute and 7-d chronic toxicity assays were conducted to measure the toxicity of DU on survival and reproduction of Ceriodaphnia dubia. A 14-d water-only assay was conducted to measure survival and growth of Hyalella azteca. The estimated median lethal concentration (LC50) to produce 50% mortality of the test population for the 96-h Ceriodaphnia dubia assay was 10.50 mg/L. Reproductive effects occurred at a lowest-observable-effect concentration ???3.91 mg/L with a no-observable-effect concentration of 1.97 mg/L. The estimated 14-d LC50 for the Hyalella azteca assay was 1.52 mg/L No significant relationship was detected between growth and DU concentrations. Concentrations at which toxicity effects were observed in this study for both invertebrates exceeded concentrations of total uranium observed in runoff from LANL lands. Thus, it is likely that current runoff levels of uranium do not pose a threat to these types of aquatic invertebrates.

Assessment of nonpoint source chemical loading potential to watersheds containing uranium waste dumps associated with uranium exploration and mining, San Rafael Swell, Utah

USGS Publications Warehouse

Freeman, Michael L.; Naftz, David L.; Snyder, Terry; Johnson, Greg

2008-01-01

During July and August of 2006, 117 solid-phase samples were collected from abandoned uranium waste dumps, geologic background sites, and adjacent streambeds in the San Rafael Swell, in southeastern Utah. The objective of this sampling program was to assess the nonpoint source chemical loading potential to ephemeral and perennial watersheds from uranium waste dumps on Bureau of Land Management property. Uranium waste dump samples were collected using solid-phase sampling protocols. After collection, solid-phase samples were homogenized and extracted in the laboratory using a field leaching procedure. Filtered (0.45 micron) water samples were obtained from the field leaching procedure and were analyzed for Ag, As, Ba, Be, Cd, Cr, Cu, Fe, Mn, Mo, Ni, Pb, Sb, Se, U, V, and Zn at the Inductively Coupled Plasma-Mass Spectrometry Metals Analysis Laboratory at the University of Utah, Salt Lake City, Utah and for Hg at the U.S. Geological Survey National Water Quality Laboratory, Denver, Colorado. For the initial ranking of chemical loading potential of suspect uranium waste dumps, leachate analyses were compared with existing aquatic life and drinking-water-quality standards and the ratio of samples that exceeded standards to the total number of samples was determined for each element having a water-quality standard for aquatic life and drinking-water. Approximately 56 percent (48/85) of the leachate samples extracted from uranium waste dumps had one or more chemical constituents that exceeded aquatic life and drinking-water-quality standards. Most of the uranium waste dump sites with elevated trace-element concentrations in leachates were along Reds Canyon Road between Tomsich Butte and Family Butte. Twelve of the uranium waste dump sites with elevated trace-element concentrations in leachates contained three or more constituents that exceeded drinking-water-quality standards. Eighteen of the uranium waste dump sites had three or more constituents that exceeded trace-element concentrations for aquatic life water-quality standards. The proximity of the uranium waste dumps in the Tomsich Butte area near Muddy Creek, coupled with the elevated concentration of trace elements, increases the offsite impact potential to water resources. Future assessment and remediation priority of these areas may be done by using GIS-based risk-mapping techniques, such as Sensitive Catchment Integrated Mapping and Analysis Project.

Perils of categorical thinking: "Oxic/anoxic" conceptual model in environmental remediation

USGS Publications Warehouse

Bradley, Paul M.

2012-01-01

Given ambient atmospheric oxygen concentrations of about 21 percent (by volume), the lower limit for reliable quantitation of dissolved oxygen concentrations in groundwater samples is in the range of 0.1–0.5 mg/L. Frameworks for assessing in situ redox condition are often applied using a simple two-category (oxic/anoxic) model of oxygen condition. The "oxic" category defines the environmental range in which dissolved oxygen concentrations are clearly expected to impact contaminant biodegradation, either by supporting aerobic biodegradation of electron-donor contaminants like petroleum hydrocarbons or by inhibiting anaerobic biodegradation of electron-acceptor contaminants like chloroethenes. The tendency to label the second category "anoxic" leads to an invalid assumption that oxygen is insignificant when, in fact, the dissolved oxygen concentration is less than detection but otherwise unknown. Expressing dissolved oxygen concentrations as numbers of molecules per volume, dissolved oxygen concentrations that fall below the 0.1 mg/L field detection limit range from 1 to 1017 molecules/L. In light of recent demonstrations of substantial oxygen-linked biodegradation of chloroethene contaminants at dissolved oxygen concentrations well below the 0.1–0.5 mg/L field detection limit, characterizing "less than detection" oxygen concentrations as "insignificant" is invalid.

Target and method for the production of fission product molybdenum-99

DOEpatents

Vandegrift, G.F.; Vissers, D.R.; Marshall, S.L.; Varma, R.

1987-10-26

A target for the reduction of fission product Mo-99 is prepared from uranium of low U-235 enrichment by coating a structural support member with a preparatory coating of a substantially oxide-free substrate metal. Uranium metal is electrodeposited from a molten halide electrolytic bath onto a substrate metal. The electrodeposition is performed at a predetermined direct current rate or by using pulsed plating techniques which permit relaxation of accumulated uranium ion concentrations within the melt. Layers of as much as to 600 mg/cm/sup 2/ of uranium can be prepared to provide a sufficient density to produce acceptable concentrations of fission product Mo-99. 2 figs.

Application of neodymium isotope ratio measurements for the origin assessment of uranium ore concentrates.

PubMed

Krajkó, Judit; Varga, Zsolt; Yalcintas, Ezgi; Wallenius, Maria; Mayer, Klaus

2014-11-01

A novel procedure has been developed for the measurement of (143)Nd/(144)Nd isotope ratio in various uranium-bearing materials, such as uranium ores and ore concentrates (UOC) in order to evaluate the usefulness and applicability of variations of (143)Nd/(144)Nd isotope ratio for provenance assessment in nuclear forensics. Neodymium was separated and pre-concentrated by extraction chromatography and then the isotope ratios were measured by multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). The method was validated by the measurement of standard reference materials (La Jolla, JB-2 and BCR-2) and the applicability of the procedure was demonstrated by the analysis of uranium samples of world-wide origin. The investigated samples show distinct (143)Nd/(144)Nd ratio depending on the ore type, deposit age and Sm/Nd ratio. Together with other characteristics of the material in question, the Nd isotope ratio is a promising signature for nuclear forensics and suggests being indicative of the source material, the uranium ore. Copyright © 2014 The Authors. Published by Elsevier B.V. All rights reserved.

Macroporous monoliths for trace metal extraction from seawater

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

Yue, Yanfeng; Mayes, Richard; Gill, Gary A.

2015-05-29

The viability of seawater-based uranium recovery depends on the uranium adsorption rate and capacity, since the concentration of uranium in the oceans is relatively low (3.3 μgL⁻¹). An important consideration for a fast adsorption is to maximize the adsorption properties of adsorbents such as surface areas and pore structures, which can greatly improve the kinetics of uranium extraction and the adsorption capacity simultaneously. Following this consideration, macroporous monolith adsorbents were prepared from the copolymerization of acrylonitrile (AN) and N, N’-methylenebis(acrylamide) (MBAAm) based on a cryogel method using both hydrophobic and hydrophilic monomers. The monolithic sorbents were tested with simulated seawatermore » containing a high uranyl concentration (–6 ppm) and the uranium adsorption results showed that the adsorption capacities are strongly influenced by the ratio of monomer to the crosslinker, i.e., the density of the amidoxime groups. The preliminary seawater testing indicates the high salinity content of seawater does not hinder the adsorption of uranium.« less

Macroporous monoliths for trace metal extraction from seawater

DOE PAGES

Yue, Yanfeng; Mayes, Richard T.; Gill, Gary; ...

2015-05-29

The viability of seawater-based uranium recovery depends on the uranium adsorption rate and capacity, since the concentration of uranium in the oceans is relatively low (3.3 gL -1). An important consideration for a fast adsorption is to maximize the adsorption properties of adsorbents such as surface areas and pore structures, which can greatly improve the kinetics of uranium extraction and the adsorption capacity simultaneously. Following this consideration, macroporous monolith adsorbents were prepared from the copolymerization of acrylonitrile (AN) and N,N -methylenebis(acrylamide) (MBAAm) based on a cryogel method using both hydrophobic and hydrophilic monomers. The monolithic sorbents were tested with simulatedmore » seawater containing a high uranyl concentration (–6 ppm) and the uranium adsorption results showed that the adsorption capacities are strongly influenced by the ratio of monomer to the crosslinker, i.e., the density of the amidoxime groups. Furthermore, the preliminary seawater testing indicates the high salinity content of seawater does not hinder the adsorption of uranium.« less

Assessment of age-dependent uranium intake due to drinking water in Hyderabad, India.

PubMed

Balbudhe, A Y; Srivastava, S K; Vishwaprasad, K; Srivastava, G K; Tripathi, R M; Puranik, V D

2012-03-01

A study has been done to assess the uranium intake through drinking water. The area of study is twin cities of Hyderabad and Secunderabad, India. Uranium concentration in water samples was analysed by laser-induced fluorimetry. The associated age-dependent uranium intake was estimated by taking the prescribed water intake values. The concentration of uranium varies from below detectable level (minimum detectable level = 0.20 ± 0.02 μg l(-1)) to 2.50 ± 0.18 μg l(-1), with the geometric mean (GM) of 0.67 μg l(-1) in tap water, whereas in ground water, the range is 0.60 ± 0.05 to 82 ± 7.1 µg l(-1) with GM of 10.07 µg l(-1). The daily intake of uranium by drinking water pathway through tap water for various age groups is found to vary from 0.14 to 9.50 µg d(-1) with mean of 1.55 µg d(-1).

Effects of clay minerals and organic matter in formulated sediments on the bioavailability of sediment-associated uranium to the freshwater midge, Chironomus dilutus.

PubMed

Crawford, Sarah E; Liber, Karsten

2015-11-01

It is well established that bioavailability influences metal toxicity in aquatic ecosystems. However, the factors and mechanisms that influence uranium (U) bioavailability and toxicity in sediment have not been thoroughly evaluated, despite evidence that suggests different sediment components can influence the sorption and interaction of some metals. Given that dissolved U is generally accepted as being the primary bioavailable fraction of U, it is hypothesized that adsorption and interaction of U with different sediment components will influence the bioavailability of U in sediment. We investigated the effects of key sediment physicochemical properties on the bioavailability of U to a model freshwater benthic invertebrate, Chironomus dilutus. Several 10-day spiked sediment bioaccumulation experiments were performed, exposing C. dilutus larvae to a variety of formulated sediments spiked with different concentrations of U (5, 50 and/or 200 mg U/kg d.w.). Mean accumulation of U in C. dilutus larvae decreased significantly from 1195 to 10 mg U/kg d.w. as kaolin clay content increased from 0% to 60% in sediment spiked with 50 mg U/kg d.w. Similarly, higher organic matter content also resulted in a significant reduction of U bioaccumulation in C. dilutus larvae, indicating a reduction in U bioavailability. Concentrations of U in both the overlying water and sediment pore water displayed a strong positive relationship to U bioaccumulation in C. dilutus larvae (r(2) = 0.77, p<0.001 and r(2) = 0.57, p < 0.001, respectively) for all experiments, while total U concentrations in the sediment had a poor relationship to U bioaccumulation (r(2) = 0.10, p = 0.028). Results from this research confirm that sediment clay and organic matter content play a significant role in altering U bioavailability, which is important in informing risk assessments of U contaminated sites and in the development of site-specific sediment quality guidelines for U. Copyright © 2015 Elsevier B.V. All rights reserved.

Uranium and plutonium in anoxic marine sediments of the Santiago River mouth (Eastern Pacific, Mexico).

PubMed

Almazán-Torres, María Guadalupe; Ordóñez-Regil, Eduardo; Ruiz-Fernández, Ana Carolina

2016-11-01

The uranium (U) and plutonium (Pu) content with depth in a sediment core collected in the continental shelf off the mouth of the Santiago River in the Mexican Pacific was studied to evaluate the contamination effects of the effluent of the Santiago-Lerma River as it moves into the sea. The large mass of terrestrial detritus delivered by the river influences the physicochemical and geochemical processes in the seafloor. Abnormal concentrations of U and Pu in sediments were examined as indicative of the effects of anoxic conditions. One of the indicators of pollution of seawater is the bacterial activity of the shallow seabed layer; and among the prevailing bacteria, the magnetotactic ones induce the formation of euhedral and framboidal shapes (pyrite). These pyrite entities are by-products of anoxic environments loaded with decomposing detrital material and are very abundant in the surface layers of the sediment core analyzed. The pyrite formation is the result of a biochemical reaction between iron and organic sulphur reduced by bacteria, and the pyrite entities precipitate to the seafloor. In the same upper zone of the profile, 238 U is readily immobilized, while 234 U is oxidized and dissolved in seawater by the effect of hot atom chemistry. This may cause the activity ratio (AR) 234 U/ 238 U disequilibrium (near 0.41). Furthermore, in the shallow layer of the sediment core, an abnormally high concentration of 239+240 Pu was detected. In this upper layer, the activity concentrations found were 3.19 Bq kg -1 for 238 U, 1.32 kg -1 for 234 U and 2.78 Bq kg -1 for 239+240 Pu. In the lower fractions of the sediment core, normal values of AR 234 U/ 238 U (≈1) were found, with traces of 239+240 Pu. Copyright © 2016 Elsevier Ltd. All rights reserved.

Removal of uranium from soil samples for ICP-OES analysis of RCRA metals

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

Wero, M.; Lederer-Cano, A.; Billy, C.

1995-12-01

Soil samples containing high levels of uranium present unique analytical problems when analyzed for toxic metals (Ag, As, Ba, Cd, Cr, Cu, Ni, Pb, Se and Tl) because of the spectral interference of uranium in the ICP-OES emission spectrometer. Methods to remove uranium from the digestates of soil samples, known to be high in uranium, have been developed that reduce the initial uranium concentration (1-3%) to less than 500 ppm. UTEVA ion exchange columns, used as an ICP-OES analytical pre-treatment, reduces uranium to acceptable levels, permitting good analytical results of the RCRA metals by ICP-OES.

Dissolved-solids transport in surface water of the Muddy Creek Basin, Utah

USGS Publications Warehouse

Gerner, Steven J.

2008-01-01

Muddy Creek is located in the southeastern part of central Utah and is a tributary of the Dirty Devil River, which, in turn, is a tributary of the Colorado River. Dissolved solids transported from the Muddy Creek Basin may be stored in the lower Dirty Devil River Basin, but are eventually discharged to the Colorado River and impact downstream water users. This study used selected dissolved-solids measurements made by various local, State, and Federal agencies from the 1970s through 2006, and additional dissolved-solids data that were collected by the U.S. Geological Survey during April 2004 through November 2006, to compute dissolved-solids loads, determine the distribution of dissolved-solids concentrations, and identify trends in dissolved-solids concentration in surface water of the Muddy Creek Basin. The dissolved-solids concentration values measured in water samples collected from Muddy Creek during April 2004 through October 2006 ranged from 385 milligrams per liter (mg/L) to 5,950 mg/L. The highest dissolved-solids concentration values measured in the study area were in water samples collected at sites in South Salt Wash (27,000 mg/L) and Salt Wash (4,940 to 6,780 mg/L). The mean annual dissolved-solids load in Muddy Creek for the periods October 1976 to September 1980 and October 2005 to September 2006 was smallest at a site near the headwaters (9,670 tons per year [tons/yr]) and largest at a site at the mouth (68,700 tons/yr). For this period, the mean annual yield of dissolved solids from the Muddy Creek Basin was 44 tons per square mile. During October 2005 to September 2006, direct runoff transported as much as 45 percent of the annual dissolved-solids load at the mouth of Muddy Creek. A storm that occurred during October 5?7, 2006 resulted in a peak streamflow at the mouth of Muddy Creek of 7,150 cubic feet per second (ft3/s) and the transport of an estimated 35,000 tons of dissolved solids, which is about 51 percent of the average annual dissolved-solids load at the mouth of Muddy Creek. A significant downward trend in dissolved-solids concentrations from 1973 to 2006 was determined for Muddy Creek at a site just downstream of that portion of the basin containing agricultural land. Dissolved-solids concentrations decreased about 2.1 percent per year; however, the rate of change was a decrease of 1.8 percent per year when dissolved-solids concentrations were adjusted for flow.