In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions.
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
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
Post, V E A; Vassolo, S I; Tiberghien, C; Baranyikwa, D; Miburo, D
2017-12-31
The potential use of groundwater for potable water supply can be severely compromised by natural contaminants such as uranium. The environmental mobility of uranium depends on a suite of factors including aquifer lithology, redox conditions, complexing agents, and hydrological processes. Uranium concentrations of up to 734μg/L are found in groundwater in northern Burundi, and the objective of the present study was to identify the causes for these elevated concentrations. Based on a comprehensive data set of groundwater chemistry, geology, and hydrological measurements, it was found that the highest dissolved uranium concentrations in groundwater occur near the shores of Lake Tshohoha South and other smaller lakes nearby. A model is proposed in which weathering and evapotranspiration during groundwater recharge, flow and discharge exert the dominant controls on the groundwater chemical composition. Results of PHREEQC simulations quantitatively confirm this conceptual model and show that uranium mobilization followed by evapo-concentration is the most likely explanation for the high dissolved uranium concentrations observed. The uranium source is the granitic sand, which was found to have a mean elemental uranium content of 14ppm, but the exact mobilization process could not be established. Uranium concentrations may further be controlled by adsorption, especially where calcium-uranyl‑carbonate complexes are present. Water and uranium mass balance calculations for Lake Tshohoha South are consistent with the inferred fluxes and show that high‑uranium groundwater represents only a minor fraction of the overall water input to the lake. These findings highlight that the evaporation effects that cause radionuclide concentrations to rise to harmful levels in groundwater discharge areas are not only confined to arid regions, and that this should be considered when selecting suitable locations for water supply wells. Copyright © 2017 Elsevier B.V. All rights reserved.
NASA Astrophysics Data System (ADS)
Roycroft, S. J.; Noel, V.; Boye, K.; Besancon, C.; Weaver, K. L.; Johnson, R. H.; Dam, W. L.; Fendorf, S. E.; Bargar, J.
2016-12-01
Uranium contaminated groundwater in Riverton, Wyoming persists despite anticipated natural attenuation outside of a former uranium ore processing facility. The inability of natural flushing to dilute the uranium below the regulatory threshold indicates that sediments act as secondary sources likely (re)supplying uranium to groundwater. Throughout the contaminated floodplain, uranium rich-evaporites are readily abundant in the upper 2 m of sediments and are spatially coincident with the location of the plume, which suggests a likely link between evaporites and increased uranium levels. Knowledge of where and how uranium is stored within evaporite-associated sediments is required to understand processes controlling the mobility of uranium. We expect that flooding and seasonal changes in hydrologic conditions will affect U phase partitioning, and thus largely control U mobility. The primary questions we are addressing in this project are: What is the relative abundance of uranium incorporated in various mineral complexes throughout the evaporite sediments? How do the factors of depth, location, and seasonality influence the relative incorporation, mobility and speciation of uranium?We have systematically sampled from two soil columns over three dates in Riverton. The sampling dates span before and after a significant flooding event, providing insight into the flood's impact on local uranium mobility. Sequential chemical extractions are used to decipher the reactivity of uranium and approximate U operationally defined within reactants targeting carbonate, silicate, organic, and metal oxide bound or water and exchangeable phases. Extractions throughout the entirety of the sediment cores provide a high-resolution vertical profile of the distribution of uranium in various extracted phases. Throughout the profile, the majority (50-60%) of uranium is bound within carbonate-targeted extracts, a direct effect of the carbonate-rich evaporite sediments. The sum of our analyses provide a dynamic model of uranium incorporation within evaporite sediments holding implications for the fate of uranium throughout contaminated sites across the Colorado River Basin.
Trace elements and Pb isotopes in soils and sediments impacted by uranium mining.
Cuvier, A; Pourcelot, L; Probst, A; Prunier, J; Le Roux, G
2016-10-01
The purpose of this study is to evaluate the contamination in As, Ba, Co, Cu, Mn, Ni, Sr, V, Zn and REE, in a high uranium activity (up to 21,000Bq∙kg(-1)) area, downstream of a former uranium mine. Different geochemical proxies like enrichment factor and fractions from a sequential extraction procedure are used to evaluate the level of contamination, the mobility and the availability of the potential contaminants. Pb isotope ratios are determined in the total samples and in the sequential leachates to identify the sources of the contaminants and to determine the mobility of radiogenic Pb in the context of uranium mining. In spite of the large uranium contamination measured in the soils and the sediments (EF≫40), trace element contamination is low to moderate (2
Nehete, Sachin Vilas; Christensen, Terje; Salbu, Brit; Teien, Hans-Christian
2017-05-05
Humic substances have a tendency to form complexes with metal ions in aquatic medium, impacting the metal mobility, decreasing bioavailability and toxicity. Ultraviolet-B (UV-B) radiation exposure degrades the humic substance, changes their molecular weight distribution and their metal binding capacity in aquatic medium. In this study, we experimented the effect of UV-B radiation on the uranium complexed with fulvic acids and humic acids in a soft water system at different pH, uranium concentrations and radiant exposure. The concentration and distribution of uranium in a complexed form were investigated by asymmetrical flow field-flow fractionation coupled to multi detection technique (AsFlFFF-UV-ICP-MS). The major concentration of uranium present in complexes was primarily associated with average and higher molecular weight fulvic and humic acids components. The concentration of uranium in a complexed form increased with increasing fulvic and humic acid concentrations as well as pH of the solution. The higher molecular weight fraction of uranium was degraded due to the UV-B exposure, transforming about 50% of the uranium-dissolved organic carbon complexes into low molecular weight uranium species in complex form with organic ligands and/or free form. The result also suggests AsFlFFF-UV-ICP-MS to be an important separation and detection technique for understanding the interaction of radionuclides with dissolved organic matter, tracking size distribution changes during degradation of organic complexes for understanding mobility, bioavailability and ecosystem transfer of radionuclides as well as metals. Copyright © 2017 Elsevier B.V. All rights reserved.
SOME GEOCHEMICAL METHODS OF URANIUM EXPLORATION
DOE Office of Scientific and Technical Information (OSTI.GOV)
Illsley, C.T.; Bills, C.W.; Pollock, J.W.
Geochemical research and development projects were carried on to provide basic information which may be applied to exploration or general studies of uranium geology. The applications and limitations of various aspects of geochemistry to uranium geological problems are considerd. Modifications of existing analytical techniques were made and tested in the laboratory and in the field. These include rapid quantitative determination of unranium in water, soil and peat, and of trace amounts of sulfate and phosphate in water. Geochemical anomaly'' has been defined as a significant departure from the average abundance background of an element where the distribution has not beenmore » disturbed by mineralization. The detection and significance of geocthemical anomalies are directly related to the mobility of the element being sought in the zone of weathering. Mobility of uranium is governed by complex physical, chemical, and biological factors. For uranium anomalies in surface materils, the chemicaly factors affecting mobility are the most sigificant. The effects of pH, solubility, coprecipitution, adsorption complexion, or compound formation are discussed in relation to anomalies detected in water, soil, and stream sediments. (auth)« less
Denton, J. S.; Goldstein, S. J.; Paviet, P.; ...
2016-04-10
Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less
Linking AS, SE, V, and MN Behavior to Natural Biostimulated Uranium Cycling
DOE Office of Scientific and Technical Information (OSTI.GOV)
Keimowitz, Alison; Ranville, James; Mailloux, Brian
The project “Linking As, Se, V, and Mn behavior to Natural and Biostimulated Uranium Cycling” successfully investigated Arsenic cycling the Rifle Colorado IFRC. This project trained undergraduate and graduate students at the Colorado School of Mines, Vassar College, and Barnard College. This resulted in both undergraduate theses and a PhD thesis and multiple publications. The science was highly successful and we were able to test the main hypotheses. We have shown that (H1) under reducing conditions that promote uranium immobilization arsenic is readily mobilized, that (H2) thioarsenic species are abundant during this mobilization, and (H3) we have examined arsenic mobilizationmore » for site sediment. At the Rifle IFRC Acetate was added during experiments to immobilize Uranium. These experiments successfully immobilized uranium but unfortunately would mobilize arsenic. We developed robust sampling and analysis methods for thioarsenic species. We showed that the mobilization occurred under sulfate reducing conditions and the majority of the arsenic was in the form of thioarsenic species. Previous studies had predicted the presence of thioarsenic species but this study used robust field and laboratory methods to quantitatively determine the presence of thioarsenic species. During stimulation in wells with high arsenic the primary species were trithioarsenate and dithioarsenate. In wells with low levels of arsenic release thioarsenates were absent or minor components. Fortunately after the injection of acetate ended the aquifer would become less reducing and the arsenic concentrations would decrease to pre-injection levels. In aquifers where organic carbon is being added as a remedial method or as a contaminant the transient mobility of arsenic during sulfidogenesis should be considered especially in sulfate rich aquifers as this could impact downgradient water quality.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fix, N. J.
The U.S. Department of Energy (DOE) is cleaning up and/or monitoring large, dilute plumes contaminated by metals, such as uranium and chromium, whose mobility and solubility change with redox status. Field-scale experiments with acetate as the electron donor have stimulated metal-reducing bacteria to effectively remove uranium [U(VI)] from groundwater at the Uranium Mill Tailings Site in Rifle, Colorado. The Pacific Northwest National Laboratory and a multidisciplinary team of national laboratory and academic collaborators has embarked on a research proposed for the Rifle site, the object of which is to gain a comprehensive and mechanistic understanding of the microbial factors andmore » associated geochemistry controlling uranium mobility so that DOE can confidently remediate uranium plumes as well as support stewardship of uranium-contaminated sites. This Quality Assurance Project Plan provides the quality assurance requirements and processes that will be followed by the Rifle Integrated Field-Scale Subsurface Research Challenge Project.« less
Uranium speciation and stability after reductive immobilization in aquifer sediments
NASA Astrophysics Data System (ADS)
Sharp, Jonathan O.; Lezama-Pacheco, Juan S.; Schofield, Eleanor J.; Junier, Pilar; Ulrich, Kai-Uwe; Chinni, Satya; Veeramani, Harish; Margot-Roquier, Camille; Webb, Samuel M.; Tebo, Bradley M.; Giammar, Daniel E.; Bargar, John R.; Bernier-Latmani, Rizlan
2011-11-01
It has generally been assumed that the bioreduction of hexavalent uranium in groundwater systems will result in the precipitation of immobile uraninite (UO 2). In order to explore the form and stability of uranium immobilized under these conditions, we introduced lactate (15 mM for 3 months) into flow-through columns containing sediments derived from a former uranium-processing site at Old Rifle, CO. This resulted in metal-reducing conditions as evidenced by concurrent uranium uptake and iron release. Despite initial augmentation with Shewanella oneidensis, bacteria belonging to the phylum Firmicutes dominated the biostimulated columns. The immobilization of uranium (˜1 mmol U per kg sediment) enabled analysis by X-ray absorption spectroscopy (XAS). Tetravalent uranium associated with these sediments did not have spectroscopic signatures representative of U-U shells or crystalline UO 2. Analysis by microfocused XAS revealed concentrated micrometer regions of solid U(IV) that had spectroscopic signatures consistent with bulk analyses and a poor proximal correlation (μm scale resolution) between U and Fe. A plausible explanation, supported by biogeochemical conditions and spectral interpretations, is uranium association with phosphoryl moieties found in biomass; hence implicating direct enzymatic uranium reduction. After the immobilization phase, two months of in situ exposure to oxic influent did not result in substantial uranium remobilization. Ex situ flow-through experiments demonstrated more rapid uranium mobilization than observed in column oxidation studies and indicated that sediment-associated U(IV) is more mobile than biogenic UO 2. This work suggests that in situ uranium bioimmobilization studies and subsurface modeling parameters should be expanded to account for non-uraninite U(IV) species associated with biomass.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Denton, J. S.; Goldstein, S. J.; Paviet, P.
Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less
Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J
2010-03-01
Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are <2 x 10(-14), and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.
Biogeochemical Processes Regulating the Mobility of Uranium in Sediments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Belli, Keaton M.; Taillefert, Martial
This book chapters reviews the latest knowledge on the biogeochemical processes regulating the mobility of uranium in sediments. It contains both data from the literature and new data from the authors.
NASA Astrophysics Data System (ADS)
Skalak, K.; Benthem, A. J.; Walton-Day, K. E.; Jolly, G.
2015-12-01
The Grand Canyon region contains a large number of breccia pipes with economically viable uranium, copper, and silver concentrations. Mining in this region has occurred since the late 19th century and has produced ore and waste rock having elevated levels of uranium and other contaminants. Fluvial transport of these contaminants from mine sites is a possibility, as this arid region is susceptible to violent storms and flash flooding which might erode and mobilize ore or waste rock. In order to assess and manage the risks associated with uranium mining, it is important to understand the transport and storage rates of sediment and uranium within the ephemeral streams of this region. We are developing a 1-dimensional sediment transportation model to examine uranium transport and storage through a typical canyon system in this region. Our study site is Hack Canyon Mine, a uranium and copper mine site, which operated in the 1980's and is currently experiencing fluvial erosion of its waste rock repository. The mine is located approximately 40km upstream from the Colorado River and is in a deep, narrow canyon with a small watershed. The stream is ephemeral for the upper half of its length and sediment is primarily mobilized during flash flood events. We collected sediment samples at 110 locations longitudinally through the river system to examine the distribution of uranium in the stream. Samples were sieved to the sand size and below fraction (<2mm) and uranium was measured by gamma-ray spectroscopy. Sediment storage zones were also examined in the upper 8km of the system to determine where uranium is preferentially stored in canyon systems. This information will quantify the downstream transport of constituents associated with the Hack Canyon waste rock and contribute to understanding the risks associated with fluvial mobilization of uranium mine waste.
Localization and toxic effects of cadmium, copper, and uranium in azolla.
Sela, M; Tel-Or, E; Fritz, E; Huttermann, A
1988-09-01
The storage and distribution of copper, cadmium, and uranium and their effects on ionic contents in roots and shoots of Azolla filiculoides has been studied by x-ray microanalysis. The relative content of copper was eightfold higher in the root than in the shoot, suggesting low mobility of this metal in Azolla plant. Cadmium relative content in the shoot was similar to its content in the root, hence its mobility was relatively high. The absence of significant uranium quantities in the shoot and its relative high content in the root suggest the immobility of this metal from Azolla root. Cadmium formed precipitates with phosphate and calcium in xylem cells of the shoot bundle and caused a two- to threefold increase in the content of phosphate in the root. Uranium in roots and cadmium in shoots were associated with calcium. All three treatments caused losses of potassium, chloride, and magnesium from Azolla roots. Accumulation of heavy metals in Azolla and their mobility from the root to the shoot can be correlated with damage caused by the loss of essential nutrients.
van Berk, Wolfgang; Fu, Yunjiao
2017-01-03
Redox conditions are seen as the key to controlling aqueous uranium concentrations (cU (aq) ). Groundwater data collected by a state-wide groundwater quality monitoring study in Mecklenburg-Western Pomerania (Germany) reveal peak cU (aq) up to 75 μg L -1 but low background uranium concentrations (median cU (aq) < 0.5 μg L -1 ). To characterize the hydrogeochemical processes causing such groundwater contamination by peak cU (aq) , we reanalyzed measured redox potentials and total concentrations of aqueous uranium, nitrate, and sulfate species in groundwater together with their distribution across the aquifer depth and performed semigeneric 2D reactive mass transport modeling which is based on chemical thermodynamics. The combined interpretation of modeling results and measured data reveals that high cU (aq) and its depth-specific distribution depending on redox conditions is a result of a nitrate-triggered roll-front mobilization of geogenic uranium in the studied aquifers which are unaffected by nuclear activities. The modeling results show that groundwater recharge containing (fertilizer-derived) nitrate drives the redox shift from originally reducing toward oxidizing environments, when nitrate input has consumed the reducing capacity of the aquifers, which is present as pyrite, degradable organic carbon, and geogenic U(IV) minerals. This redox shift controls the uranium roll-front mobilization and results in high cU (aq) within the redoxcline. Moreover, the modeling results indicate that peak cU (aq) occurring at this redox front increase along with the temporal progress of such redox conversion within the aquifer.
Mobilities of uranium and mercury ions in helium
NASA Technical Reports Server (NTRS)
Johnsen, R.; Biondi, M. A.
1972-01-01
The mobilities of mass-identified U(+) and Hg (+) ions in helium were determined in a drift tube-mass spectrometer. For uranium ions, a reduced mobility value is obtained at 305 K and a standard gas density of 2.69 x 10 to the 19th power/cu cm. The mobility of mercury ions is in agreement with two previous determinations. The effect of fast ion injection in drift mobility measurements is discussed, and a technique to circumvent these problems is described. The results are compared with existing theories of ion mobilities.
Landa, Edward R.; Cravotta, Charles A.; Naftz, David L.; Verplanck, Philip L.; Nordstrom, D. Kirk; Zielinski, Robert A.
2000-01-01
Recent research by the U.S. Geological Survey has characterized contaminant sources and identified important geochemical processes that influence transport of radionuclides from uranium mining and milling wastes. 1) Selective extraction studies indicated that alkaline earth sulfates and hydrous ferric oxides are important hosts of 226Ra in uranium mill tailings. The action of sulfate-reducing and ironreducing bacteria on these phases was shown to enhance release of radium, and this adverse result may temper decisions to dispose of uranium mill tailings in anaerobic environments. 2) Field studies have shown that although surface-applied sewage sludge/wood chip amendments aid in revegetating pyritic spoil, the nitrogen in sludge leachate can enhance pyrite oxidation, acidification of groundwater, and the consequent mobilization of metals and radionuclides. 3) In a U.S. Environmental Protection Agencyfunded study, three permeable reactive barriers consisting of phosphate-rich material, zero-valent iron, or amorphous ferric oxyhydroxide have been installed at an abandoned uranium upgrader facility near Fry Canyon, UT. Preliminary results indicate that each of the permeable reactive barriers is removing the majority of the uranium from the groundwater. 4) Studies on the geochemistry of rare earth elements as analogues for actinides such as uranium and thorium in acid mine drainage environments indicate high mobility under acid-weathering conditions but measurable attenuation associated with iron and aluminum colloid formation. Mass balances from field and laboratory studies are being used to quantify the amount of attenuation. 5) A field study in Colorado demonstrated the use of 234U/238U isotopic ratio measurements to evaluate contamination of shallow groundwater with uranium mill effluent.
Schaller, Jörg; Planer-Friedrich, Britta
2017-05-01
Organic sediments in aquatic ecosystems are well known sinks for nutrients, silicon, and metal(loid)s. Organic matter-consuming organisms like invertebrate shredders, grazers, and bioturbators significantly affect element fixation or remobilization by changing redox conditions or binding properties of organic sediments. Little is known about the effect of filter feeders, like the zebra mussel Dreissena polymorpha, an invasive organism in North American and European freshwater ecosystems. A laboratory batch experiment exposing D. polymorpha (∼1200 organisms per m 2 ) to organic sediment from a site contaminated with arsenic, copper, lead, and uranium revealed a significant uptake and accumulation of arsenic, copper, iron, and especially uranium both into the soft body tissues and the seashell. This is in line with previous observations of metal(loid) accumulation from biomonitoring studies. Regarding its environmental impact, D. polymorpha significantly contributed to mobilization of silicon, iron, phosphorus, arsenic, and copper and to immobilization of uranium (p < 0.001), probably driven by redox conditions, microbial activity within the gut system, or active control of element homeostasis. No net mobilization or immobilization was observed for zinc and lead, because of their low mobility at the prevailing pH of 7.5-8.5. The present results suggest that D. polymorpha can both ameliorate (nutrient mobilization, immobilization of toxicants mobile under oxic conditions) or aggravate negative effects (mobilization of toxicants mobile under reducing conditions) in ecosystems. Relating the results of the present study to observed population densities in natural freshwater ecosystems suggests a significant influence of D. polymorpha on element cycling and needs to be considered in future studies. Copyright © 2017 Elsevier Ltd. All rights reserved.
Localization and Toxic Effects of Cadmium, Copper, and Uranium in Azolla1
Sela, Mordechai; Tel-Or, Elisha; Fritz, Eberhardt; Huttermann, Aloys
1988-01-01
The storage and distribution of copper, cadmium, and uranium and their effects on ionic contents in roots and shoots of Azolla filiculoides has been studied by x-ray microanalysis. The relative content of copper was eightfold higher in the root than in the shoot, suggesting low mobility of this metal in Azolla plant. Cadmium relative content in the shoot was similar to its content in the root, hence its mobility was relatively high. The absence of significant uranium quantities in the shoot and its relative high content in the root suggest the immobility of this metal from Azolla root. Cadmium formed precipitates with phosphate and calcium in xylem cells of the shoot bundle and caused a two- to threefold increase in the content of phosphate in the root. Uranium in roots and cadmium in shoots were associated with calcium. All three treatments caused losses of potassium, chloride, and magnesium from Azolla roots. Accumulation of heavy metals in Azolla and their mobility from the root to the shoot can be correlated with damage caused by the loss of essential nutrients. Images Fig. 1 Fig. 2 Fig. 5 Fig. 7 PMID:16666274
Molecular dynamics simulation of the diffusion of uranium species in clay pores.
Liu, Xiao-yu; Wang, Lu-hua; Zheng, Zhong; Kang, Ming-liang; Li, Chun; Liu, Chun-li
2013-01-15
Molecular dynamics simulations were carried out to investigate the diffusive behavior of aqueous uranium species in montmorillonite pores. Three uranium species (UO(2)(2+), UO(2)CO(3), UO(2)(CO(3))(2)(2-)) were confirmed in both the adsorbed and diffuse layers. UO(2)(CO(3))(3)(4-) was neglected in the subsequent analysis due to its scare occurrence. The species-based diffusion coefficients in montmorillonite pores were then calculated, and compared with the water mobility and their diffusivity in aqueous solution/feldspar nanosized fractures. Three factors were considered that affected the diffusive behavior of the uranium species: the mobility of water, the self-diffusion coefficient of the aqueous species, and the electrostatic forces between the negatively charged surface and charged molecules. The mobility of U species in the adsorbed layer decreased in the following sequence: UO(2)(2+)>UO(2)CO(3)>UO(2)(CO(3))(2)(2-). In the diffuse layer, we obtained the highest diffusion coefficient for UO(2)(CO(3))(2)(2-) with the value of 5.48×10(-10) m(2) s(-1), which was faster than UO(2)(2+). For these two charged species, the influence of electrostatic forces on the diffusion of solutes in the diffuse layer is overwhelming, whereas the influence of self-diffusion and water mobility is minor. Our study demonstrated that the negatively charged uranyl carbonate complex must be addressed in the safety assessment of potential radioactive waste disposal systems. Copyright © 2012 Elsevier B.V. All rights reserved.
The new nuclear west: Uranium milling as community on Colorado's western slope
NASA Astrophysics Data System (ADS)
Tidwell, Abraham S. D.
In mid-2007, Energy Fuels, a Toronto-based uranium mining and milling company, announced their intent to build Piñon Ridge, the first new conventional uranium mill in the United States in 30 years. The prospect of a return to uranium milling has mobilized community support to bring back an industry some see as both familiar and capable of supporting and growing their communities. Using transcripts generated during the Colorado Department of Public Health and Environment's public meetings and hearings during 2010 and 2012, this study examines how proponents of the mill frame the socioeconomic advantages of bringing the industry back. Applying Kinsella's bounded constitutive model of communication, this study shows that the community and the uranium mill are bound in a "sorge-enframing" duality where the care generated by each binds the other to the recalcitrant nature of the uranium industry and preconceived notions of socioeconomic development, respectively.
Ion Mobility Spectrometer Field Test
DOE Office of Scientific and Technical Information (OSTI.GOV)
Smith, Nicholas; McLain, Derek; Steeb, Jennifer
The Morpho Saffran Itemizer 4DX Ion Mobility Spectrometer previously used to detect uranium signatures in FY16 was used at the former New Brunswick Facility, a past uranium facility located on site at Argonne National Laboratory. This facility was chosen in an attempt to detect safeguards relevant signatures and has a history of processing uranium at various enrichments, chemical forms, and purities; various chemicals such as nitric acid, uranium fluorides, phosphates and metals are present at various levels. Several laboratories were sampled for signatures of nuclear activities around the laboratory. All of the surfaces that were surveyed were below background levelsmore » of the radioanalytical instrumentation and determined to be radiologically clean.« less
Recent developments in uranium exploration using the U.S. geological survey's mobile helium detector
Reimer, G.M.; Denton, E.H.; Friedman, I.; Otton, J.K.
1979-01-01
A mobile mass spectrometer to measure He concentrations has been developed by the U.S. Geological Survey. This instrument has been tested in areas of known uranium deposits, and He anomalies have been found in both soil gas and water. A gas sample is collected in a hypodermic syringe, injected into the spectrometer, and analyzed for He. Over 100 analyses a day can be performed with a sensitivity of 10 parts per billion (ppb). One detailed study conducted in Weld County, Colorado, shows that values for He in soil gas can be contoured to outline an anomalous area and that the anomaly is displaced from the deposit in the direction of groundwater flow. Other studies include the Schwartzwalder uranium mine, Jefferson County, Colorado, where He anomalies may be related to geologic structure; near Ambrosia Lake, New Mexico, where the location of He anomalies are related to groundwater movement; and tests for diurnal effects showing only slight variations probably related to soil-moisture content. ?? 1979.
Uranium mobility across annual growth rings in three deciduous tree species
DOE Office of Scientific and Technical Information (OSTI.GOV)
McHugh, Kelly C.; Widom, Elisabeth; Spitz, Henry B.
Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is potentially dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236U) in growth rings of allmore » three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination.« less
Uranium mobility across annual growth rings in three deciduous tree species.
McHugh, Kelly C; Widom, Elisabeth; Spitz, Henry B; Wiles, Gregory C; Glover, Sam E
2018-02-01
Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236 U) in growth rings of all three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination. Copyright © 2017 Elsevier Ltd. All rights reserved.
Sitte, Jana; Akob, Denise M; Kaufmann, Christian; Finster, Kai; Banerjee, Dipanjan; Burkhardt, Eva-Maria; Kostka, Joel E; Scheinost, Andreas C; Büchel, Georg; Küsel, Kirsten
2010-05-01
Sulfate-reducing bacteria (SRB) can affect metal mobility either directly by reductive transformation of metal ions, e.g., uranium, into their insoluble forms or indirectly by formation of metal sulfides. This study evaluated in situ and biostimulated activity of SRB in groundwater-influenced soils from a creek bank contaminated with heavy metals and radionuclides within the former uranium mining district of Ronneburg, Germany. In situ activity of SRB, measured by the (35)SO(4)(2-) radiotracer method, was restricted to reduced soil horizons with rates of < or =142 +/- 20 nmol cm(-3) day(-1). Concentrations of heavy metals were enriched in the solid phase of the reduced horizons, whereas pore water concentrations were low. X-ray absorption near-edge structure (XANES) measurements demonstrated that approximately 80% of uranium was present as reduced uranium but appeared to occur as a sorbed complex. Soil-based dsrAB clone libraries were dominated by sequences affiliated with members of the Desulfobacterales but also the Desulfovibrionales, Syntrophobacteraceae, and Clostridiales. [(13)C]acetate- and [(13)C]lactate-biostimulated soil microcosms were dominated by sulfate and Fe(III) reduction. These processes were associated with enrichment of SRB and Geobacteraceae; enriched SRB were closely related to organisms detected in soils by using the dsrAB marker. Concentrations of soluble nickel, cobalt, and occasionally zinc declined < or =100% during anoxic soil incubations. In contrast to results in other studies, soluble uranium increased in carbon-amended treatments, reaching < or =1,407 nM in solution. Our results suggest that (i) ongoing sulfate reduction in contaminated soil resulted in in situ metal attenuation and (ii) the fate of uranium mobility is not predictable and may lead to downstream contamination of adjacent ecosystems.
Sitte, Jana; Akob, Denise M.; Kaufmann, Christian; Finster, Kai; Banerjee, Dipanjan; Burkhardt, Eva-Maria; Kostka, Joel E.; Scheinost, Andreas C.; Büchel, Georg; Küsel, Kirsten
2010-01-01
Sulfate-reducing bacteria (SRB) can affect metal mobility either directly by reductive transformation of metal ions, e.g., uranium, into their insoluble forms or indirectly by formation of metal sulfides. This study evaluated in situ and biostimulated activity of SRB in groundwater-influenced soils from a creek bank contaminated with heavy metals and radionuclides within the former uranium mining district of Ronneburg, Germany. In situ activity of SRB, measured by the 35SO42− radiotracer method, was restricted to reduced soil horizons with rates of ≤142 ± 20 nmol cm−3 day−1. Concentrations of heavy metals were enriched in the solid phase of the reduced horizons, whereas pore water concentrations were low. X-ray absorption near-edge structure (XANES) measurements demonstrated that ∼80% of uranium was present as reduced uranium but appeared to occur as a sorbed complex. Soil-based dsrAB clone libraries were dominated by sequences affiliated with members of the Desulfobacterales but also the Desulfovibrionales, Syntrophobacteraceae, and Clostridiales. [13C]acetate- and [13C]lactate-biostimulated soil microcosms were dominated by sulfate and Fe(III) reduction. These processes were associated with enrichment of SRB and Geobacteraceae; enriched SRB were closely related to organisms detected in soils by using the dsrAB marker. Concentrations of soluble nickel, cobalt, and occasionally zinc declined ≤100% during anoxic soil incubations. In contrast to results in other studies, soluble uranium increased in carbon-amended treatments, reaching ≤1,407 nM in solution. Our results suggest that (i) ongoing sulfate reduction in contaminated soil resulted in in situ metal attenuation and (ii) the fate of uranium mobility is not predictable and may lead to downstream contamination of adjacent ecosystems. PMID:20363796
Effects of Uranium Oxides on Some of the Algae Native to Eglin Air Force Base, Florida.
1982-06-01
Chlorella , and Selenastrum were not identified from the collections after microscopic examination. 4. MOBILITY OF DEPLETED URANIUM BY DISSOLUTION IN NATURAL...processes. A similar finding nas been previously reported for Chlorella regularis (Sakaguchi, Horikoshi, and Nakajima, 1978). In addition, uranium
Johnson, Raymond H.; Tutu, Hlanganani; Brown, Adrian; Figueroa, Linda; Wolkersdorfer, Christian
2013-01-01
Geochemical changes that can occur down gradient from uranium in situ recovery (ISR) sites are important for various stakeholders to understand when evaluating potential effects on surrounding groundwater quality. If down gradient solid-phase material consists of sandstone with iron hydroxide coatings (no pyrite or organic carbon), sorption of uranium on iron hydroxides can control uranium mobility. Using one-dimensional reactive transport models with PHREEQC, two different geochemical databases, and various geochemical parameters, the uncertainties in uranium sorption on iron hydroxides are evaluated, because these oxidized zones create a greater risk for future uranium transport than fully reduced zones where uranium generally precipitates.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Silver, L T; Williams, I S; Woodhead, J A
1980-10-01
Some of the principal findings of the study on the Lawler Peak Granite are: the granite is dated precisely by this work at 1411 +- 3 m.y., confirming its synchroneity with a great regional terrane of granites. Uranium is presently 8-10 times crustal abundance and thorium 2-3 times in this granite. Uranium is found to be enriched in at least eight, possibly ten, primary igneous mineral species over the whole-rock values. Individual mineral species show distinct levels in, and characteristics ranges of, uranium concentration. It appears that in a uraniferous granite such as this, conventional accuracy mineral suites probably cannotmore » account for most of the uranium in the rock, and more rare, high U-concentration phases also are present and are significant uranium hosts. It appears that at least two different geological episodes have contributed to the disturbance of the U-Th-Pb isotope systems. Studies of various sites for transient dispersal of uranium, thorium, and radiogenic lead isotopes indicate a non-uniform dispersal of these components. It appears that the bulk rock has lost at least 24 percent of its original uranium endowment, accepting limited or no radiogenic lead or thorium migration from the sample.« less
Landa, E.R.
2003-01-01
Specific extraction studies in our laboratory have shown that iron and manganese oxide- and alkaline earth sulfate minerals are important hosts of radium in uranium mill tailings. Iron- and sulfate-reducing bacteria may enhance the release of radium (and its analog barium) from uranium mill tailings, oil field pipe scale [a major technologically enhanced naturally occurring radioactive material (TENORM) waste], and jarosite (a common mineral in sulfuric acid processed-tailings). These research findings are reviewed and discussed in the context of nuclear waste forms (such as barium sulfate matrices), radioactive waste management practices, and geochemical environments in the Earth's surficial and shallow subsurface regions.
Studies of the mobility of uranium and thorium in Nevada Test Site tuff
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wollenberg, H.A.; Flexser, S.; Smith, A.R.
1991-06-01
Hydro-geochemical processes must be understood if the movement of radionuclides away from a breached radioactive waste canister is to be modeled and predicted. In this respect, occurrences of uranium and thorium in hydrothermal systems are under investigation in tuff and in rhyolitic tuff that was heated to simulate the effects of introduction of radioactive waste. In these studies, high-resolution gamma spectrometry and fission-track radiography are coupled with observations of alteration mineralogy and thermal history to deduce the evidence of, or potential for movement of, U and Th in response to the thermal environment. Observations to date suggest that U wasmore » mobile in the vicinity of the heater but that localized reducing environments provided by Fe-Ti-Mn-oxide minerals concentrated U and thus attenuated its migration.« less
Uranium transport in the Walker River Basin, California and Nevada
Benson, L.V.; Leach, D.L.
1979-01-01
During the summer of 1976 waters from tributaries, rivers, springs and wells were sampled in the Walker River Basin. Snow and sediments from selected sites were also sampled. All samples were analyzed for uranium and other elements. The resulting data provide an understanding of the transport of uranium within a closed hydrologic basin as well as providing a basis for the design of geochemical reconnaissance studies for the Basin and Range Province of the Western United States. Spring and tributary data are useful in locating areas containing anomalous concentrations of uranium. However, agricultural practices obscure the presence of known uranium deposits and render impossible the detection of other known deposits. Uranium is extremely mobile in stream waters and does not appear to sorb or precipitate. Uranium has a long residence time (2500 years) in the open waters of Walker Lake; however, once it crosses the sediment-water interface, it is reduced to the U(IV) state and is lost from solution. Over the past two million years the amount of uranium transported to the terminal point of the Walker River system may have been on the order of 4 ?? 108 kg. This suggests that closed basin termini are sites for significant uranium accumulations and are, therefore, potential sites of uranium ore deposits. ?? 1979.
Edmands, J D; Brabander, D J; Coleman, D S
2001-08-01
In a preliminary study, the uptake and the mobility of uranium (U) by black oak trees (Quercus velutina) were assessed by measuring the isotopic composition of tree rings in two mature oak trees in a heavy metal contaminated bog in Concord, MA. The bog is adjacent to a nuclear industrial facility that has been processing depleted uranium (DU) since 1959. Over the past 40 years, DU has been leaking from an onsite holding basin and cooling pond down gradient to the bog where the oaks are located. Because DU has no source outside the nuclear industry, contamination from the industrial facility is readily discernable from uptake of natural U by measuring isotopic compositions. Isotope ratio analysis confirms the occurrence of DU in bark, sapwood and heartwood tree rings dating back to 1937, pre-dating the introduction of DU at the site by at least 20 years. Isotope dilution analysis indicates high concentrations of U (>3 ppb) in sapwood that drop rapidly to relatively constant concentrations (0.3-0.4 ppb) in heartwood. These data indicate that once incorporated into tree cells, U is mobile, possibly by diffusion through the tree wood. Concentrations of U in sapwood are approximately equal to average U concentrations in groundwater onsite over the past 10 years, suggesting that oak trees can be used as present-day bioindicators of U-contaminated groundwater. We suggest that regional sampling of oak bark and sapwood is a reasonable, inexpensive alternative to drilling wells to monitor shallow groundwater U contamination.
Innovative mathematical modeling in environmental remediation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yeh, Gour T.; National Central Univ.; Univ. of Central Florida
2013-05-01
There are two different ways to model reactive transport: ad hoc and innovative reaction-based approaches. The former, such as the Kd simplification of adsorption, has been widely employed by practitioners, while the latter has been mainly used in scientific communities for elucidating mechanisms of biogeochemical transport processes. It is believed that innovative mechanistic-based models could serve as protocols for environmental remediation as well. This paper reviews the development of a mechanistically coupled fluid flow, thermal transport, hydrologic transport, and reactive biogeochemical model and example-applications to environmental remediation problems. Theoretical bases are sufficiently described. Four example problems previously carried out aremore » used to demonstrate how numerical experimentation can be used to evaluate the feasibility of different remediation approaches. The first one involved the application of a 56-species uranium tailing problem to the Melton Branch Subwatershed at Oak Ridge National Laboratory (ORNL) using the parallel version of the model. Simulations were made to demonstrate the potential mobilization of uranium and other chelating agents in the proposed waste disposal site. The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium. The third example simulated laboratory experiments involving extremely high concentrations of uranium, technetium, aluminum, nitrate, and toxic metals (e.g.,Ni, Cr, Co).The fourth example modeled microbially-mediated immobilization of uranium in an unconfined aquifer using acetate amendment in a field-scale experiment. The purposes of these modeling studies were to simulate various mechanisms of mobilization and immobilization of radioactive wastes and to illustrate how to apply reactive transport models for environmental remediation.The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium.« less
Distribution and potential health risk of groundwater uranium in Korea.
Shin, Woosik; Oh, Jungsun; Choung, Sungwook; Cho, Byong-Wook; Lee, Kwang-Sik; Yun, Uk; Woo, Nam-Chil; Kim, Hyun Koo
2016-11-01
Chronic exposure even to extremely low specific radioactivity of natural uranium in groundwater results in kidney problems and potential toxicity in bones. This study was conducted to assess the potential health risk via intake of the groundwater containing uranium, based on the determination of the uranium occurrence in groundwater. The groundwater was investigated from a total of 4140 wells in Korea. Most of the groundwater samples showed neutral pH and (sub-)oxic condition that was influenced by the mixing with shallow groundwater due to long-screened (open) wells. High uranium contents exceeding the WHO guideline level of 30 μg L(-1) were observed in the 160 wells located mainly in the plutonic bedrock regions. The statistical analysis suggested that the uranium component was present in groundwater by desorption and re-dissolution processes. Predominant uranium phases were estimated to uranyl carbonates under the Korean groundwater circumstances. These mobile forms of uranium and oxic condition facilitate the increase of potential health risk downgradient. In particular, long-term intake of groundwater containing >200 μg U L(-1) may induce internal exposure to radiation as well as the effects of chemical toxicity. These high uranium concentrations were found in twenty four sampling wells of rural areas in this study, and they were mainly used for drinking. Therefore, the high-level uranium wells and neighboring areas must be properly managed and monitored to reduce the exposure risk for the residents by drinking groundwater. Copyright © 2016 Elsevier Ltd. All rights reserved.
Grossmann, Kay; Arnold, Thuro; Steudtner, Robin; Weiss, Stefan; Bernhard, Gert
2009-08-01
Low-temperature alteration reactions on uranium phases may lead to the mobilization of uranium and thereby poses a potential threat to humans living close to uranium-contaminated sites. In this study, the surface alteration of uraninite (UO(2)) and uranium tetrachloride (UCl(4)) in air atmosphere was studied by confocal laser scanning microscopy (CLSM) and laser-induced fluorescence spectroscopy using an excitation wavelength of 408 nm. It was found that within minutes the oxidation state on the surface of the uraninite and the uranium tetrachloride changed. During the surface alteration process U(IV) atoms on the uraninite and uranium tetrachloride surface became stepwise oxidized by a one-electron step at first to U(V) and then further to U(VI). These observed changes in the oxidation states of the uraninite surface were microscopically visualized and spectroscopically identified on the basis of their fluorescence emission signal. A fluorescence signal in the wavelength range of 415-475 nm was indicative for metastable uranium(V), and a fluorescence signal in the range of 480-560 nm was identified as uranium(VI). In addition, the oxidation process of tetravalent uranium in aqueous solution at pH 0.3 was visualized by CLSM and U(V) was fluorescence spectroscopically identified. The combination of microscopy and fluorescence spectroscopy provided a very convincing visualization of the brief presence of U(V) as a metastable reaction intermediate and of the simultaneous coexistence of the three states U(IV), U(V), and U(VI). These results have a significant importance for fundamental uranium redox chemistry and should contribute to a better understanding of the geochemical behavior of uranium in nature.
Bioremediation of Uranium-Contaminated Groundwater using Engineered Injection and Extraction
NASA Astrophysics Data System (ADS)
Greene, J. A.; Neupauer, R.; Ye, M.; Kasprzyk, J. R.; Mays, D. C.; Curtis, G. P.
2017-12-01
During in-situ remediation of contaminated groundwater, a treatment chemical is injected into the contaminated groundwater to react with and degrade the contaminant, with reactions occurring where the treatment chemical contacts the contaminant. Traditional in-situ groundwater remediation relies on background groundwater flow for spreading of treatment chemicals into contaminant plumes. Engineered Injection and Extraction (EIE), in which time-varying induced flow fields are used to actively spread the treatment chemical into the contaminant plume, has been developed to increase contact between the contaminant and treatment chemical, thereby enhancing contaminant degradation. EIE has been investigated for contaminants that degrade through irreversible bimolecular reaction with a treatment chemical, but has not been investigated for a contaminant governed by reversible reactions. Uranium primarily occurs in its aqueous, mobile form, U(VI), in the environment but can be bioreduced to its sparingly soluble, immobile form, U(IV), by iron reducing bacteria stimulated by an acetate amendment. In this study, we investigate the ability of EIE to facilitate and sustain favorable conditions to immobilize uranium during remediation, and to prevent re-mobilization of uranium into the aqueous phase after active remediation has ended. Simulations in this investigation are conducted using a semi-synthetic model based on physical and chemical conditions at the Naturita Uranium Mill Tailings Remedial Action (UMTRA) site in southwestern Colorado and the Old Rifle UMTRA site in western Colorado. The EIE design is optimized for the synthetic model using the Borg multi-objective evolutionary algorithm.
Uranium association with iron-bearing phases in mill tailings from Gunnar, Canada.
Othmane, Guillaume; Allard, Thierry; Morin, Guillaume; Sélo, Madeleine; Brest, Jessica; Llorens, Isabelle; Chen, Ning; Bargar, John R; Fayek, Mostafa; Calas, Georges
2013-11-19
The speciation of uranium was studied in the mill tailings of the Gunnar uranium mine (Saskatchewan, Canada), which operated in the 1950s and 1960s. The nature, quantification, and spatial distribution of uranium-bearing phases were investigated by chemical and mineralogical analyses, fission track mapping, electron microscopy, and X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopies at the U LIII-edge and Fe K-edge. In addition to uranium-containing phases from the ore, uranium is mostly associated with iron-bearing minerals in all tailing sites. XANES and EXAFS data and transmission electron microscopy analyses of the samples with the highest uranium concentrations (∼400-700 mg kg(-1) of U) demonstrate that uranium primarily occurs as monomeric uranyl ions (UO2(2+)), forming inner-sphere surface complexes bound to ferrihydrite (50-70% of the total U) and to a lesser extent to chlorite (30-40% of the total U). Thus, the stability and mobility of uranium at the Gunnar site are mainly influenced by sorption/desorption processes. In this context, acidic pH or alkaline pH with the presence of UO2(2+)- and/or Fe(3+)-complexing agents (e.g., carbonate) could potentially solubilize U in the tailings pore waters.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moore, Robert C.; Szecsody, James; Rigali, Mark J.
We have performed an initial evaluation and testing program to assess the effectiveness of a hydroxyapatite (Ca10(PO4)6(OH)2) permeable reactive barrier and source area treatment to decrease uranium mobility at the Department of Energy (DOE) former Old Rifle uranium mill processing site in Rifle, western Colorado. Uranium ore was processed at the site from the 1940s to the 1970s. The mill facilities at the site as well as the uranium mill tailings previously stored there have all been removed. Groundwater in the alluvial aquifer beneath the site still contains elevated concentrations of uranium, and is currently used for field tests tomore » study uranium behavior in groundwater and investigate potential uranium remediation technologies. The technology investigated in this work is based on in situ formation of apatite in sediment to create a subsurface apatite PRB and also for source area treatment. The process is based on injecting a solution containing calcium citrate and sodium into the subsurface for constructing the PRB within the uranium plume. As the indigenous sediment micro-organisms biodegrade the injected citrate, the calcium is released and reacts with the phosphate to form hydroxyapatite (precipitate). This paper reports on proof-of-principle column tests with Old Rifle sediment and synthetic groundwater.« less
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.
Uranium vacancy mobility at the Σ5 symmetric tilt and Σ5 twist grain boundaries in UO₂
Uberuaga, Blas Pedro; Andersson, David A.
2015-10-01
Ionic transport at grain boundaries in oxides dictates a number of important phenomena, from ionic conductivity to sintering to creep. For nuclear fuels, it also influences fission gas bubble nucleation and growth. Here, using a combination of atomistic calculations and object kinetic Monte Carlo (okMC) simulations, we examine the kinetic pathways associated with uranium vacancies at two model grain boundaries in UO 2. The barriers for vacancy motion were calculated using the nudged elastic band method at all uranium sites at each grain boundary and were used as the basis of the okMC simulations. For both boundaries considered – amore » simple tilt and a simple twist boundary – the mobility of uranium vacancies is significantly higher than in the bulk. For the tilt boundary, there is clearly preferred migration along the tilt axis as opposed to in the perpendicular direction while, for the twist boundary, migration is essentially isotropic within the boundary plane. These results show that cation defect mobility in fluorite-structured materials is enhanced at certain types of grain boundaries and is dependent on the boundary structure with the tilt boundary exhibiting higher rates of migration than the twist boundary.« less
Uranium mobility during interaction of rhyolitic glass with alkaline solutions: dissolution of glass
Zielinski, Robert A.
1977-01-01
This report concerns investigations designed to identify the important physical and chemical parameters influencing the rate of release of uranium from glass shards of rhyolitic air-fall ash. Oxidizing, silica undersaturated, alkaline solutions are eluted through a column of rhyolitic glass shards at a carefully controlled temperature, pressure, and flow rate. The solutions are monitored for the concentration of uranium and selected additional elements (Si, K, Li, F), and the glass is recovered and examined for physical and/or chemical evidence of attack. The flushing mode is designed to mimic leaching of glass shards by intermittent, near-surface waters with which the glass is not in equilibrium. Reported rates are applicable only to the experimental conditions (120?C, 7,000 psi), but it is assumed that the reaction mechanisms and the relative importance of rate-influencing parameters remain unchanged, at reduced temperature and pressure. Results of the above experiment indicate that silica and uranium are released from glass shards at comparable rates, while lithium and potassium are released faster and fluorine slower than either Si or U. Rates of release of silica and uranium correlate positively with the surface area of the shards. Rhyolitic shards release uranium at faster rates than rhyodacitic shards of comparable surface area. Changes in the shards resulting from experimental treatment and observed in the original glass separates from an Oligocene ash (compared to a Pleistocene ash) include; surface pitting, increased surface area, devitrification rinds (<1l micron wide) and reduced lithium contents. Future investigations will study the effect of temperature, pressure, solution composition, and flow rate on the relative mobility of U, Si, Li, F, and K.
Innovative mathematical modeling in environmental remediation.
Yeh, Gour-Tsyh; Gwo, Jin-Ping; Siegel, Malcolm D; Li, Ming-Hsu; Fang, Yilin; Zhang, Fan; Luo, Wensui; Yabusaki, Steve B
2013-05-01
There are two different ways to model reactive transport: ad hoc and innovative reaction-based approaches. The former, such as the Kd simplification of adsorption, has been widely employed by practitioners, while the latter has been mainly used in scientific communities for elucidating mechanisms of biogeochemical transport processes. It is believed that innovative mechanistic-based models could serve as protocols for environmental remediation as well. This paper reviews the development of a mechanistically coupled fluid flow, thermal transport, hydrologic transport, and reactive biogeochemical model and example-applications to environmental remediation problems. Theoretical bases are sufficiently described. Four example problems previously carried out are used to demonstrate how numerical experimentation can be used to evaluate the feasibility of different remediation approaches. The first one involved the application of a 56-species uranium tailing problem to the Melton Branch Subwatershed at Oak Ridge National Laboratory (ORNL) using the parallel version of the model. Simulations were made to demonstrate the potential mobilization of uranium and other chelating agents in the proposed waste disposal site. The second problem simulated laboratory-scale system to investigate the role of natural attenuation in potential off-site migration of uranium from uranium mill tailings after restoration. It showed inadequacy of using a single Kd even for a homogeneous medium. The third example simulated laboratory experiments involving extremely high concentrations of uranium, technetium, aluminum, nitrate, and toxic metals (e.g., Ni, Cr, Co). The fourth example modeled microbially-mediated immobilization of uranium in an unconfined aquifer using acetate amendment in a field-scale experiment. The purposes of these modeling studies were to simulate various mechanisms of mobilization and immobilization of radioactive wastes and to illustrate how to apply reactive transport models for environmental remediation. Copyright © 2011 Elsevier Ltd. All rights reserved.
Uranium redox transition pathways in acetate-amended sediments
Bargar, John R.; Williams, Kenneth H.; Campbell, Kate M.; Long, Philip E.; Stubbs, Joanne E.; Suvorova, Elenal I.; Lezama-Pacheco, Juan S.; Alessi, Daniel S.; Stylo, Malgorzata; Webb, Samuel M.; Davis, James A.; Giammar, Daniel E.; Blue, Lisa Y.; Bernier-Latmani, Rizlan
2013-01-01
Redox transitions of uranium [from U(VI) to U(IV)] in low-temperature sediments govern the mobility of uranium in the environment and the accumulation of uranium in ore bodies, and inform our understanding of Earth’s geochemical history. The molecular-scale mechanistic pathways of these transitions determine the U(IV) products formed, thus influencing uranium isotope fractionation, reoxidation, and transport in sediments. Studies that improve our understanding of these pathways have the potential to substantially advance process understanding across a number of earth sciences disciplines. Detailed mechanistic information regarding uranium redox transitions in field sediments is largely nonexistent, owing to the difficulty of directly observing molecular-scale processes in the subsurface and the compositional/physical complexity of subsurface systems. Here, we present results from an in situ study of uranium redox transitions occurring in aquifer sediments under sulfate-reducing conditions. Based on molecular-scale spectroscopic, pore-scale geochemical, and macroscale aqueous evidence, we propose a biotic–abiotic transition pathway in which biomass-hosted mackinawite (FeS) is an electron source to reduce U(VI) to U(IV), which subsequently reacts with biomass to produce monomeric U(IV) species. A species resembling nanoscale uraninite is also present, implying the operation of at least two redox transition pathways. The presence of multiple pathways in low-temperature sediments unifies apparently contrasting prior observations and helps to explain sustained uranium reduction under disparate biogeochemical conditions. These findings have direct implications for our understanding of uranium bioremediation, ore formation, and global geochemical processes.
Effect of uranium(VI) speciation on simultaneous microbial reduction of uranium(VI) and iron(III).
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.
Microbial transformations of uranium in wastes and implication on its mobility
DOE Office of Scientific and Technical Information (OSTI.GOV)
Suzuki,Y.; Nankawa, T.; Ozaki, T.
2008-09-14
Uranium exists in several chemical forms in mining and mill tailings and in nuclear and weapons production wastes. Under appropriate conditions, microorganisms can affect the stability and mobility of U in wastes by altering the chemical speciation, solubility and sorption properties and thus could increase or decrease the concentrations of U in solution and the bioavailability. Dissolution or immobilization of U is brought about by direct enzymatic action or indirect nonenzymatic action of microorganisms. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of U have been extensively investigated, we have only limited information on the mechanismsmore » of microbial transformations of various chemical forms of U in the presence of electron donors and acceptors.« less
A phase-field simulation of uranium dendrite growth on the cathode in the electrorefining process
NASA Astrophysics Data System (ADS)
Shibuta, Yasushi; Unoura, Seiji; Sato, Takumi; Shibata, Hiroki; Kurata, Masaki; Suzuki, Toshio
2011-07-01
The uranium dendrite growth on the cathode during the pyroprocessing of uranium is investigated using a novel phase-field model, in which electrodeposition of uranium and zirconium from the molten-salt is taken into account. The threshold concentration of zirconium in the molten salt demarcating the dendritic and planar growth is then estimated as a function of the current density. Moreover, the growth process of both the dendritic and planar electrodeposits has been demonstrated by way of varying the mobility of the phase field, which consists of the effect of attachment kinetics and diffusion.
Oxidative Uranium Release from Anoxic Sediments under Diffusion-Limited Conditions.
Bone, Sharon E; Cahill, Melanie R; Jones, Morris E; Fendorf, Scott; Davis, James; Williams, Kenneth H; Bargar, John R
2017-10-03
Uranium (U) contamination occurs as a result of mining and ore processing; often in alluvial aquifers that contain organic-rich, reduced sediments that accumulate tetravalent U, U(IV). Uranium(IV) is sparingly soluble, but may be mobilized upon exposure to nitrate (NO 3 - ) and oxygen (O 2 ), which become elevated in groundwater due to seasonal fluctuations in the water table. The extent to which oxidative U mobilization can occur depends upon the transport properties of the sediments, the rate of U(IV) oxidation, and the availability of inorganic reductants and organic electron donors that consume oxidants. We investigated the processes governing U release upon exposure of reduced sediments to artificial groundwater containing O 2 or NO 3 - under diffusion-limited conditions. Little U was mobilized during the 85-day reaction, despite rapid diffusion of groundwater within the sediments and the presence of nonuraninite U(IV) species. The production of ferrous iron and sulfide in conjunction with rapid oxidant consumption suggested that the sediments harbored large concentrations of bioavailable organic carbon that fueled anaerobic microbial respiration and stabilized U(IV). Our results suggest that seasonal influxes of O 2 and NO 3 - may cause only localized mobilization of U without leading to export of U from the reducing sediments when ample organic carbon is present.
Merroun, Mohamed L; Nedelkova, Marta; Ojeda, Jesus J; Reitz, Thomas; Fernández, Margarita López; Arias, José M; Romero-González, María; Selenska-Pobell, Sonja
2011-12-15
This work describes the mechanisms of uranium biomineralization at acidic conditions by Bacillus sphaericus JG-7B and Sphingomonas sp. S15-S1 both recovered from extreme environments. The U-bacterial interaction experiments were performed at low pH values (2.0-4.5) where the uranium aqueous speciation is dominated by highly mobile uranyl ions. X-ray absorption spectroscopy (XAS) showed that the cells of the studied strains precipitated uranium at pH 3.0 and 4.5 as a uranium phosphate mineral phase belonging to the meta-autunite group. Transmission electron microscopic (TEM) analyses showed strain-specific localization of the uranium precipitates. In the case of B. sphaericus JG-7B, the U(VI) precipitate was bound to the cell wall. Whereas for Sphingomonas sp. S15-S1, the U(VI) precipitates were observed both on the cell surface and intracellularly. The observed U(VI) biomineralization was associated with the activity of indigenous acid phosphatase detected at these pH values in the absence of an organic phosphate substrate. The biomineralization of uranium was not observed at pH 2.0, and U(VI) formed complexes with organophosphate ligands from the cells. This study increases the number of bacterial strains that have been demonstrated to precipitate uranium phosphates at acidic conditions via the activity of acid phosphatase. Copyright © 2011 Elsevier B.V. All rights reserved.
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.
Yang, Yu; Saiers, James E; Xu, Na; Minasian, Stefan G; Tyliszczak, Tolek; Kozimor, Stosh A; Shuh, David K; Barnett, Mark O
2012-06-05
The risk stemming from human exposure to actinides via the groundwater track has motivated numerous studies on the transport of radionuclides within geologic environments; however, the effects of waterborne organic matter on radionuclide mobility are still poorly understood. In this study, we compared the abilities of three humic acids (HAs) (obtained through sequential extraction of a peat soil) to cotransport hexavalent uranium (U) within water-saturated sand columns. Relative breakthrough concentrations of U measured upon elution of 18 pore volumes increased from undetectable levels (<0.001) in an experiment without HAs to 0.17 to 0.55 in experiments with HAs. The strength of the HA effect on U mobility was positively correlated with the hydrophobicity of organic matter and NMR-detected content of alkyl carbon, which indicates the possible importance of hydrophobic organic matter in facilitating U transport. Carbon and uranium elemental maps collected with a scanning transmission X-ray microscope (STXM) revealed uneven microscale distribution of U. Such molecular- and column-scale data provide evidence for a critical role of hydrophobic organic matter in the association and cotransport of U by HAs. Therefore, evaluations of radionuclide transport within subsurface environments should consider the chemical characteristics of waterborne organic substances, especially hydrophobic organic matter.
NASA Astrophysics Data System (ADS)
Calas, G.; Angiboust, S.; Fayek, M.; Camacho, A.; Allard, T.; Agrinier, P.
2009-12-01
The Peña Blanca molybdenum-uranium field (Chihuahua, Mexico) exhibits over 100 airborne anomalies hosted in tertiary ignimbritic ash-flow tuffs (44 Ma) overlying the Pozos conglomerate and a sequence of Cretaceous carbonate rocks. Uranium occurrences are associated with breccia zones at the intersection of two or more fault systems. Periodic reactivation of these structures associated with Basin and Range and Rio Grande tectonic events resulted in the mobilization of U and other elements by meteoric fluids heated by geothermal activity. Trace element geochemistry (U, Th, REE) provides evidence for local mobilization of uranium under oxidizing conditions. In addition, O- and H-isotope geochemistry of kaolinite, smectite, opal and calcite suggests that argillic alteration proceeded at shallow depth with meteoric water at 25-75 °C. Focussed along breccia zones, fluids precipitated several generations of pyrite and uraninite together with kaolinite, as in the Nopal 1 mine, indicating that mineralization and hydrothermal alteration of volcanic tuffs are contemporaneous. Low δ34S values (~ -24.5 ‰) of pyrites intimately associated with uraninite suggest that the reducing conditions at the origin of the U-mineralization arise from biological activity. Later, the uplift of Sierra Pena Blanca resulted in oxidation and remobilization of uranium, as confirmed by the spatial distribution of radiation-induced defect centers in kaolinites. These data show that tectonism and biogenic reducing conditions can play a major role in the formation and remobilization of uranium in epithermal deposits. By comparison with the other uranium deposits at Sierra Pena Blanca and nearby Sierra de Gomez, Nopal 1 deposit is one of the few deposits having retained a reduced uranium mineralization.
Uranium fate in wetland mesocosms: Effects of plants at two iron loadings with different pH values
Small-scale continuous flow wetland mesocosms (~0.8 L) were used to evaluate how plant roots under different iron loadings affect uranium (U) mobility. When significant concentrations of ferrous iron (Fe) were present at circumneutral pH values, U concentrations in root exposed ...
DOE Office of Scientific and Technical Information (OSTI.GOV)
Long, M.P.; Carbaugh, E.H.; Fairrow, N.L.
1994-11-01
Workers at two Department of Energy facilities, the Pantex Plant in Texas and the Hanford Site in Washington, are potentially exposed to class Y depleted or natural uranium. Since trace amounts of uranium are naturally present in urine excretion, site bioassay programs must be able to discern occupational exposure from naturally occurring uranium exposure. In 1985 Hanford established a 0.2-{mu}g/d environmental screening level for elemental uranium in urine; the protocol was based on log-normal probability analysis of unexposed workers. A second study of background uranium levels commenced in 1990, and experiences in the field indicated that there seemed to bemore » an excessive number of urine samples with uranium above the screening level and that the environmental screening level should be reviewed. Due to unforeseen problems, that second study was terminated before the complete data could be obtained. Natural uranium in rock (by weight, 99.27% {sup 288}U, 0.72% {sup 235}U, and 0.006% {sup 234}U) has approximately equal activity concentrations of {sup 238}U and {sup 234}U. Earlier studies, summarized by the U.S. Environmental Protection Agency in 51 FR 32068, have indicated that {sup 234}U (via {sup 234}Th) has a greater environmental mobility than {sup 238}U and may well have a higher concentration in ground water. By assuming that the {sup 238}U-to {sup 234}U ratio in the urine of nonoccupationally exposed persons should reflect the ratio of environmental levels, significant occupational exposure to depleted uranium would shift that ratio in favor of {sup 238}U, allowing use of the ratio as a co-indicator of occupational exposure in addition to the isotope-specific screening levels. This approach has been adopted by Pantex. The Pacific Northwest Laboratory is studying the feasibility of applying this method to the natural and recycled uranium mixtures encountered at Hanford. The Hanford data included in this report represent work-in-progress.« less
The Nopal 1 Uranium Deposit: an Overview
NASA Astrophysics Data System (ADS)
Calas, G.; Allard, T.; Galoisy, L.
2007-05-01
The Nopal 1 natural analogue is located in the Pena Blanca uranium district, about 50 kms north of Chihuahua City, Mexico. The deposit is hosted in tertiary ignimbritic ash-flow tuffs, dated at 44 Ma (Nopal and Colorados formations), and overlying the Pozos conglomerate formation and a sequence of Cretaceous carbonate rocks. The deposit is exposed at the ground surface and consists of a near vertical zone extending over about 100 m with a diameter of 40 m. An interesting characteristic is that the primary mineralization has been exposed above the water table, as a result of the uplift of the Sierra Pena Blanca, and subsequently oxidized with a remobilization of hexavalent uranium. The primary mineralization has been explained by various genetic models. It is associated to an extensive hydrothermal alteration of the volcanic tuffs, locally associated to pyrite and preserved by an intense silicification. Several kaolinite parageneses occur in fissure fillings and feldspar pseudomorphs, within the mineralized breccia pipe and the barren surrounding rhyolitic tuffs. Smectites are mainly developed in the underlying weakly welded tuffs. Several radiation-induced defect centers have been found in these kaolinites providing a unique picture of the dynamics of uranium mobilization (see Allard et al., this session). Another evidence of this mobilization is given by the spectroscopy of uranium-bearing opals, which show characteristic fluorescence spectra of uranyl groups sorbed at the surface of silica. By comparison with the other uranium deposits of the Sierra Pena Blanca and the nearby Sierra de Gomez, the Nopal 1 deposit is original, as it is one of the few deposits hving retained a reduced uranium mineralization.
Uranium concentrations in groundwater, northeastern Washington
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.
Sepulveda-Medina, Paola; Katsenovich, Yelena; Musaramthota, Vishal; Lee, Michelle; Lee, Brady; Dua, Rupak; Lagos, Leonel
2015-06-01
Past disposal practices at nuclear production facilities have led to the release of liquid waste into the environment creating multiple radionuclide plumes. Microorganisms are known for the ability to interact with radionuclides and impact their mobility in soils and sediments. Gram-positive Arthrobacter sp. are one of the most common bacterial groups in soils and are found in large numbers in subsurface environments contaminated with radionuclides. This study experimentally analyzed changes on the bacteria surface at the nanoscale level after uranium exposure and evaluated the effect of aqueous bicarbonate ions on U(VI) toxicity of a low uranium-tolerant Arthrobacter oxydans strain G968 by investigating changes in adhesion forces and cell dimensions via atomic force microscopy (AFM). Experiments were extended to assess cell viability by the Live/Dead BacLight Bacterial Viability Kit (Molecular Probes) and quantitatively illustrate the effect of uranium exposure in the presence of varying concentrations of bicarbonate ions. AFM and viability studies showed that samples containing bicarbonate were able to withstand uranium toxicity and remained viable. Samples containing no bicarbonate exhibited deformed surfaces and a low height profile, which, in conjunction with viability studies, indicated that the cells were not viable. Copyright © 2015 Institut Pasteur. All rights reserved.
NASA Astrophysics Data System (ADS)
Dangelmayr, Martin A.; Reimus, Paul W.; Johnson, Raymond H.; Clay, James T.; Stone, James J.
2018-06-01
This research assesses the ability of a GC SCM to simulate uranium transport under variable geochemical conditions typically encountered at uranium in-situ recovery (ISR) sites. Sediment was taken from a monitoring well at the SRH site at depths 192 and 193 m below ground and characterized by XRD, XRF, TOC, and BET. Duplicate column studies on the different sediment depths, were flushed with synthesized restoration waters at two different alkalinities (160 mg/l CaCO3 and 360 mg/l CaCO3) to study the effect of alkalinity on uranium mobility. Uranium breakthrough occurred 25% - 30% earlier in columns with 360 mg/l CaCO3 over columns fed with 160 mg/l CaCO3 influent water. A parameter estimation program (PEST) was coupled to PHREEQC to derive site densities from experimental data. Significant parameter fittings were produced for all models, demonstrating that the GC SCM approach can model the impact of carbonate on uranium in flow systems. Derived site densities for the two sediment depths were between 141 and 178 μmol-sites/kg-soil, demonstrating similar sorption capacities despite heterogeneity in sediment mineralogy. Model sensitivity to alkalinity and pH was shown to be moderate compared to fitted site densities, when calcite saturation was allowed to equilibrate. Calcite kinetics emerged as a potential source of error when fitting parameters in flow conditions. Fitted results were compared to data from previous batch and column studies completed on sediments from the Smith-Ranch Highland (SRH) site, to assess variability in derived parameters. Parameters from batch experiments were lower by a factor of 1.1 to 3.4 compared to column studies completed on the same sediments. The difference was attributed to errors in solid-solution ratios and the impact of calcite dissolution in batch experiments. Column studies conducted at two different laboratories showed almost an order of magnitude difference in fitted site densities suggesting that experimental methodology may play a bigger role in column sorption behavior than actual sediment heterogeneity. Our results demonstrate the necessity for ISR sites to remove residual pCO2 and equilibrate restoration water with background geochemistry to reduce uranium mobility. In addition, the observed variability between fitted parameters on the same sediments highlights the need to provide standardized guidelines and methodology for regulators and industry when the GC SCM approach is used for ISR risk assessments.
Dangelmayr, Martin A; Reimus, Paul W; Johnson, Raymond H; Clay, James T; Stone, James J
2018-06-01
This research assesses the ability of a GC SCM to simulate uranium transport under variable geochemical conditions typically encountered at uranium in-situ recovery (ISR) sites. Sediment was taken from a monitoring well at the SRH site at depths 192 and 193 m below ground and characterized by XRD, XRF, TOC, and BET. Duplicate column studies on the different sediment depths, were flushed with synthesized restoration waters at two different alkalinities (160 mg/l CaCO 3 and 360 mg/l CaCO 3 ) to study the effect of alkalinity on uranium mobility. Uranium breakthrough occurred 25% - 30% earlier in columns with 360 mg/l CaCO 3 over columns fed with 160 mg/l CaCO 3 influent water. A parameter estimation program (PEST) was coupled to PHREEQC to derive site densities from experimental data. Significant parameter fittings were produced for all models, demonstrating that the GC SCM approach can model the impact of carbonate on uranium in flow systems. Derived site densities for the two sediment depths were between 141 and 178 μmol-sites/kg-soil, demonstrating similar sorption capacities despite heterogeneity in sediment mineralogy. Model sensitivity to alkalinity and pH was shown to be moderate compared to fitted site densities, when calcite saturation was allowed to equilibrate. Calcite kinetics emerged as a potential source of error when fitting parameters in flow conditions. Fitted results were compared to data from previous batch and column studies completed on sediments from the Smith-Ranch Highland (SRH) site, to assess variability in derived parameters. Parameters from batch experiments were lower by a factor of 1.1 to 3.4 compared to column studies completed on the same sediments. The difference was attributed to errors in solid-solution ratios and the impact of calcite dissolution in batch experiments. Column studies conducted at two different laboratories showed almost an order of magnitude difference in fitted site densities suggesting that experimental methodology may play a bigger role in column sorption behavior than actual sediment heterogeneity. Our results demonstrate the necessity for ISR sites to remove residual pCO2 and equilibrate restoration water with background geochemistry to reduce uranium mobility. In addition, the observed variability between fitted parameters on the same sediments highlights the need to provide standardized guidelines and methodology for regulators and industry when the GC SCM approach is used for ISR risk assessments. Copyright © 2018 Elsevier B.V. All rights reserved.
Uranium fate in wetland mesocosms: Effects of plants at two ...
Small-scale continuous flow wetland mesocosms (~0.8 L) were used to evaluate how plant roots under different iron loadings affect uranium (U) mobility. When significant concentrations of ferrous iron (Fe) were present at circumneutral pH values, U concentrations in root exposed sediments were an order of magnitude greater than concentrations in root excluded sediments. Micro X-ray absorption near-edge structure (µ-XANES) spectroscopy indicated that U was associated with the plant roots primarily as U(VI) or U(V), with limited evidence of U(IV). Micro X-ray fluorescence (µ-XRF) of plant roots suggested that for high iron loading at circumneutral pH, U was co-located with Fe, perhaps co-precipitated with root Fe plaques, while for low iron loading at a pH of ~4 the correlation between U and Fe was not significant, consistent with previous observations of U associated with organic matter. Quantitative PCR analyses indicated that the root exposed sediments also contained elevated numbers of Geobacter spp., which are likely associated with enhanced iron cycling, but may also reduce mobile U(VI) to less mobile U(IV) species. There are significant uncertainties regarding the environmental fate of uranium (U) and efforts to minimize U exposures require understanding of its mobility in environmental systems. Much research has focused on sequestering U as solids within groundwater aquifers, where localized risks can be controlled.1 Subsurface sequestration limits t
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
NASA Astrophysics Data System (ADS)
Dam, W. L.; Johnson, R. H.; Campbell, S.; Bone, S. E.; Noel, V.; Bargar, J.
2015-12-01
Understanding uranium mobility in subsurface environments is not trivial. Obtaining sufficient data to accurately represent soil and aquifer characteristics can require unique approaches that evolve with added site knowledge. At Riverton, the primary source of uranium mill tailings remaining from ore processing was removed but contaminant plumes have persisted longer than predicted by groundwater modeling. What are the primary mechanisms controlling plume persistence? DOE is conducting new characterization studies to assist our understanding of underlying biogeochemical and hydrogeological mechanisms affecting secondary sources. A variety of field sampling techniques are being sequentially employed including augering, trenching, pore water sampling, and installing multi-level wells. In August 2012, vadose zone soil samples from 34 locations and groundwater from 103 boreholes were collected with Geoprobe ® direct push rods. Lower than expected uranium concentrations in composited shallow soils indicated the need for more focused and deeper samples. In May 2014, soil samples containing evaporites were collected along the bank of the Little Wind River; elevated uranium concentrations in evaporite minerals correlated with plume configurations and reflect contaminated groundwater discharge at the river. In September 2014, hand anger samples collected by the river and oxbow lake also indicated the presence of organic rich zones containing elevated uranium (>50 mg/kg). Subsequent samples collected from five backhoe trenches in May 2015 revealed a highly heterogeneous vadose zone composed of clay, silt, sand and cobbles containing evaporites and organic rich zones which may interact with groundwater plumes.Plans for August 2015 include sonic drilling to obtain continuous cores from the surface down to the base of the surficial aquifer with multi-level monitoring wells constructed in each borehole to assess vertical variation in groundwater chemistry. Temporary well-points will be installed adjacent to the river to assess geochemical and flow controls in the area of plume stagnation. Analyses include critical element speciation (C, S, Fe, and U), microbes, isotopes, diffusivity and flow characteristics. These activities support a dramatically improved understanding of plume persistence.
Federal Register 2010, 2011, 2012, 2013, 2014
2011-09-30
... and Extend the NRC Long-Term Surveillance Boundary With Respect to Materials License SUA-1139 AGENCY... concentration limits and to extend the NRC Long-Term Surveillance Boundary at its Highland Uranium Mine and Mill... wells and at the proposed POC well. The amendment also proposes to expand the Long-Term Surveillance...
Reactivity of Uranium and Ferrous Iron with Natural Iron Oxyhydroxides.
Stewart, Brandy D; Cismasu, A Cristina; Williams, Kenneth H; Peyton, Brent M; Nico, Peter S
2015-09-01
Determining key reaction pathways involving uranium and iron oxyhydroxides under oxic and anoxic conditions is essential for understanding uranium mobility as well as other iron oxyhydroxide mediated processes, particularly near redox boundaries where redox conditions change rapidly in time and space. Here we examine the reactivity of a ferrihydrite-rich sediment from a surface seep adjacent to a redox boundary at the Rifle, Colorado field site. Iron(II)-sediment incubation experiments indicate that the natural ferrihydrite fraction of the sediment is not susceptible to reductive transformation under conditions that trigger significant mineralogical transformations of synthetic ferrihydrite. No measurable Fe(II)-promoted transformation was observed when the Rifle sediment was exposed to 30 mM Fe(II) for up to 2 weeks. Incubation of the Rifle sediment with 3 mM Fe(II) and 0.2 mM U(VI) for 15 days shows no measurable incorporation of U(VI) into the mineral structure or reduction of U(VI) to U(IV). Results indicate a significantly decreased reactivity of naturally occurring Fe oxyhydroxides as compared to synthetic minerals, likely due to the association of impurities (e.g., Si, organic matter), with implications for the mobility and bioavailability of uranium and other associated species in field environments.
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
U-Sries Disequilibra in Soils, Pena Blanca Natural Analog, Chihuahua, Mexico
DOE Office of Scientific and Technical Information (OSTI.GOV)
D. French; E. Anthony; P. Goodell
2006-03-16
The Nopal I uranium deposit located in the Sierra Pena Blanca, Mexico. The deposit was mined in the early 1980s, and ore was stockpiled close by. This stockpile area was cleared and is now referred to as the Prior High Grade Stockpile (PHGS). Some of the high-grade boulders from the site rolled downhill when it was cleared in the 1990s. For this study soil samples were collected from the alluvium surrounding and underlying one of these boulders. A bulk sample of the boulder was also collected. Because the Prior High Grade Stockpile had no ore prior to the 1980s amore » maximum residence time for the boulder is about 25 years, this also means that the soil was at background as well. The purpose of this study is to characterize the transport of uranium series radionuclides from ore to the soil. Transport is characterized by determining the activities of individual radionuclides and daughter to parent ratios. Isotopes of the uranium series decay chain detected include {sup 210}Pb, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 214}Pb, and {sup 214}Bi. Peak areas for each isotope are determined using gamma-ray spectroscopy with a Canberra Ge (Li) detector and GENIE 2000 software. The boulder sample is close to secular equilibrium when compared to the standard BL-5 (Beaver Lodge Uraninite from Canada). Results for the soils, however, indicate that some daughter/parent pairs are in secular disequilibrium. These daughter/parent (D/P) ratios include {sup 230}Th/{sup 234}U, which is greater than unity, {sup 226}Ra/{sup 230}Th, which is also greater than unity, and {sup 210}Pb/{sup 214}Bi, which is less than unity. The gamma-ray spectrum for organic material lacks {sup 230}Th peaks, but contains {sup 234}U and {sup 226}Ra, indicating that plants preferentially incorporate {sup 226}Ra. Our results, combined with previous studies require multistage history of mobilization of the uranium series radionuclides. Earlier studies at the ore zone could limit the time span for mobilization only to a few thousand years. The contribution of this study is that the short residence time of the ore at the Prior High Grade Stockpile requires a time span for mobilization of 20-30 years.« less
Aftermath of Uranium Ore Processing on Floodplains: Lasting Effects of Uranium on Soil and Microbes
NASA Astrophysics Data System (ADS)
Tang, H.; Boye, K.; Bargar, J.; Fendorf, S. E.
2016-12-01
A former uranium ore processing site located between the Wind River and the Little Wind River near the city of Riverton, Wyoming, has generated a uranium plume in the groundwater within the floodplain. Uranium is toxic and poses a threat to human health. Thus, controlling and containing the spread of uranium will benefit the human population. The primary source of uranium was removed from the processing site, but a uranium plume still exists in the groundwater. Uranium in its reduced form is relatively insoluble in water and therefore is retained in organic rich, anoxic layers in the subsurface. However, with the aid of microbes uranium becomes soluble in water which could expose people and the environment to this toxin, if it enters the groundwater and ultimately the river. In order to better understand the mechanisms controlling uranium behavior in the floodplains, we examined sediments from three sediment cores (soil surface to aquifer). We determined the soil elemental concentrations and measured microbial activity through the use of several instruments (e.g. Elemental Analyzer, X-ray Fluorescence, MicroResp System). Through the data collected, we aim to obtain a better understanding of how the interaction of geochemical factors and microbial metabolism affect uranium mobility. This knowledge will inform models used to predict uranium behavior in response to land use or climate change in floodplain environments.
Uranium extraction by complexation with siderophores
NASA Astrophysics Data System (ADS)
Bahamonde Castro, Cristina
One of the major concerns of energy production is the environmental impact associated with the extraction of natural resources. Nuclear energy fuel is obtained from uranium, an abundant and naturally occurring element in the environment, but the currently used techniques for uranium extraction leave either a significant fingerprint (open pit mines) or a chemical residue that alters the pH of the environment (acid or alkali leaching). It is therefore clear that a new and greener approach to uranium extraction is needed. Bioleaching is one potential alternative. In bioleaching, complexants naturally produced from fungi or bacteria may be used to extract the uranium. In the following research, the siderophore enterobactin, which is naturally produced by bacteria to extract and solubilize iron from the environment, is evaluated to determine its potential for complexing with uranium. To determine whether enterobactin could be used for uranium extraction, its acid dissociation and its binding strength with the metal of interest must be determined. Due to the complexity of working with radioactive materials, lanthanides were used as analogs for uranium. In addition, polyprotic acids were used as structural and chemical analogs for the siderophore during method development. To evaluate the acid dissociation of enterobactin and the subsequent binding constants with lanthanides, three different analytical techniques were studied including: potentiometric titration, UltraViolet Visible (UV-Vis) spectrophotometry and Isothermal Titration Calorimetry (ITC). After evaluation of three techniques, a combination of ITC and potentiometric titrations was deemed to be the most viable way for studying the siderophore of interest. The results obtained from these studies corroborate the ideal pH range for enterobactin complexation to the lanthanide of interest and pave the way for determining the strength of complexation relative to other naturally occurring metals. Ultimately, this fundamental research enhances our current understanding of heavy metal complexation to naturally occurring complexants, which may enhance the metals mobility in the environment or potentially be used as a greener alternative in uranium extraction or remediation.
Wan, Jiamin; Tokunaga, Tetsu K; Kim, Yongman; Brodie, Eoin; Daly, Rebecca; Hazen, Terry C; Firestone, Mary K
2008-10-15
Bioreduction-based strategies for remediating uranium (U)-contaminated sediments face the challenge of maintaining the reduced status of U for long times. Because groundwater influxes continuously bring in oxidizing terminal electron acceptors (O2, NO3(-)), it is necessary to continue supplying organic carbon (OC) to maintain the reducing environment after U bioreduction is achieved. We tested the influence of OC supply rates on mobility of previously microbial reduced uranium U(IV) in contaminated sediments. We found that high degrees of U mobilization occurred when OC supply rates were high, and when the sediment still contained abundant Fe(III). Although 900 days with low levels of OC supply minimized U mobilization, the sediment redox potential increased with time as did extractable U(VI) fractions. Molecular analyses of total microbial activity demonstrated a positive correlation with OC supply and analyses of Geobacteraceae activity (RT-qPCR of 16S rRNA) indicated continued activity even when the effluent Fe(II) became undetectable. These data support our hypothesis on the mechanisms responsible for remobilization of U under reducing conditions; that microbial respiration caused increased (bi)carbonate concentration and formation of stable uranyl carbonate complexes, thereby shifted U(IV)/U(VI) equilibrium to more reducing potentials. The data also suggested that low OC concentrations could not sustain the reducing condition of the sediment for much longer time. Bioreduced U(IV) is not sustainable in an oxidizing environment for a very long time.
DOE Office of Scientific and Technical Information (OSTI.GOV)
McDiarmid, Melissa A.; Gaitens, Joanna M.; Hines,
Background: A small group of Gulf War I veterans wounded in depleted uranium (DU) friendly-fire incidents have been monitored for health changes in a clinical surveillance program at the Veterans Affairs Medical Center, Baltimore since 1994. Methods: During the spring of 2015, an in-patient clinical surveillance protocol was performed on 36 members of the cohort, including exposure monitoring for total and isotopic uranium concentrations in urine and a comprehensive assessment of health outcomes. Results: On-going mobilization of U from embedded fragments is evidenced by elevated urine U concentrations. The DU isotopic signature is observed principally in participants possessing embedded fragments.more » Those with only an inhalation exposure have lower urine U concentration and a natural isotopic signature. Conclusions: At 25 years since first exposure to DU, an aging cohort of military veterans continues to show no U-related health effects in known target organs of U toxicity. As U body burden continues to accrue from in-situ mobilization from metal fragment depots, and increases with exposure duration, critical tissue-specific U concentration thresholds may be reached, thus recommending on-going surveillance of this veteran cohort. - Highlights: • Gulf War I veterans wounded with depleted uranium are monitored for health changes. • In 2015 in-patient clinical surveillance was performed on 36 members of the cohort. • Mobilization of U from embedded fragments is evidenced by elevated U in urine. • This cohort of continues to show no U-related health effects.« less
Reactivity of iron-rich phyllosilicates with uranium and chromium through redox transition zones
DOE Office of Scientific and Technical Information (OSTI.GOV)
Burgos, William D.
This project performed thermodynamic, kinetic, and mineral structural studies on the reactivity of phyllosilicate Fe(II/III) with metal-reducing bacteria, and with two important poly-valent DOE contaminants (chromium and uranium) that show high mobility in their oxidized state. We focused on Fe-bearing phyllosilicates because these are important components of the reactive, fines fraction of Hanford, Oak Ridge, and Idaho National Laboratory sediments. Iron-bearing phyllosilicates strongly influence the redox state and mobility of Cr and U because of their limited hydraulic conductivity, high specific surface area, and redox reactivity. This was a collaborative project between Penn State (W.D. Burgos – PI), Miami Universitymore » (H. Dong – Co-PI), and Argonne National Laboratory (K. Kemner and M. Boyanov – Co-PIs). Penn State and Miami University were funded together but separately from ANL. This report summarizes research findings and publications produced by Penn State and Miami University.« less
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
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
Zielinski, R.A.; Lindsey, D.A.; Rosholt, J.N.
1980-01-01
The distribution and mobility of uranium in a diagenetically altered, 8 Ma old tuff in the Keg Mountain area, Utah, are modelled in this study. The modelling represents an improvement over similar earlier studies in that it: (1) considers a large number of samples (76) collected with good geologic control and exhibiting a wide range of alteration; (2) includes radiometric data for Th, K and RaeU (radium equivalent uranium) as well as U; (3) considers mineralogic and trace-element data for the same samples; and (4) analyzes the mineral and chemical covariation by multivariate statistical methods. The variation of U in the tuff is controlled mainly by its primary abundance in glass and by the relative abundance of non-uraniferous detritus and uraniferous accessory minerals. Alteration of glass to zeolite, even though extensive, caused no large or systematic change in the bulk concentration of U in the tuff. Some redistribution of U during diagenesis is indicated by association of U with minor alteration products such as opal and hydrous Fe-Mn oxide minerals. Isotopic studies indicate that the zeolitized tuff has been open to migration of U decay products during the last 0.8 Ma. The tuff of Keg Mountain has not lost a statistically detectable fraction of its original U, even though it has a high (??? 9 ppm) trace U content and has been extensively altered to zeolite. Similar studies in a variety of geological environments are required in order to identify the particular combination of conditions most favorable for liberation and migration of U from tuffs. ?? 1980.
Uranium decay daughters from isolated mines: Accumulation and sources.
Cuvier, A; Panza, F; Pourcelot, L; Foissard, B; Cagnat, X; Prunier, J; van Beek, P; Souhaut, M; Le Roux, G
2015-11-01
This study combines in situ gamma spectrometry performed at different scales, in order to accurately locate the contamination pools, to identify the concerned radionuclides and to determine the distribution of the contaminants from soil to bearing phase scale. The potential mobility of several radionuclides is also evaluated using sequential extraction. Using this procedure, an accumulation area located downstream of a former French uranium mine and concentrating a significant fraction of radioactivity is highlighted. We report disequilibria in the U-decay chains, which are likely related to the processes implemented on the mining area. Coupling of mineralogical analyzes with sequential extraction allow us to highlight the presence of barium sulfate, which may be the carrier of the Ra-226 activities found in the residual phase (Ba(Ra)SO4). In contrast, uranium is essentially in the reducible fraction and potentially trapped in clay-iron coatings located on the surface of minerals. Copyright © 2015 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Truex, Michael J.; Szecsody, James E.; Qafoku, Nikolla
2014-09-01
Historically, uranium was disposed in waste solutions of varying waste chemistry at the Hanford Site Central Plateau. The character of how uranium was distributed in the vadose zone during disposal, how it has continued to migrate through the vadose zone, and the magnitude of potential impacts on groundwater are strongly influenced by geochemical reactions in the vadose zone. These geochemical reactions can be significantly influenced by the disposed-waste chemistry near the disposal location. This report provides conceptual models and supporting information to describe uranium fate and transport in the vadose zone for both acidic and alkaline wastes discharged at amore » substantial number of waste sites in the Hanford Site Central Plateau. The conceptual models include consideration of how co-disposed acidic or alkaline fluids influence uranium mobility in terms of induced dissolution/precipitation reactions and changes in uranium sorption with a focus on the conditions near the disposal site. This information, when combined with the extensive information describing uranium fate and transport at near background pH conditions, enables focused characterization to support effective fate and transport estimates for uranium in the subsurface.« less
Understanding Uranium Behavior in a Reduced Aquifer
NASA Astrophysics Data System (ADS)
Janot, N.; Lezama-Pacheco, J. S.; Williams, K. H.; Bernier-Latmani, R.; Long, P. E.; Davis, J. A.; Fox, P. M.; Yang, L.; Giammar, D.; Cerrato, J. M.; Bargar, J.
2012-12-01
Uranium contamination of groundwater is a concern at several US Department of Energy sites, such Old Rifle, CO. Uranium transport in the environment is mainly controlled by its oxidation state, since oxidized U(VI) is relatively mobile, whereas U(IV) is relatively insoluble. Bio-remediation of contaminated aquifers aims at immobilizing uranium in a reduced form. Previous laboratory and field studies have shown that adding electron donor (lactate, acetate, ethanol) to groundwater stimulates the activity of metal- and sulfate-reducing bacteria, which promotes U(VI) reduction in contaminated aquifers. However, obtaining information on chemical and physical forms of U, Fe and S species for sediments biostimulated in the field, as well as kinetic parameters such as U(VI) reduction rate, is challenging due to the low concentration of uranium in the aquifers (typically < 10 ppm) and the expense of collecting large number of cores. An in-situ technique has been developed for studying uranium, iron and sulfur reduction dynamics during such bioremediation episodes. This technique uses in-well columns to obtain direct access to chemical and physical forms of U(IV) produced in the aquifer, evolving microbial communities, and trace and major ion groundwater constituents. While several studies have explored bioreduction of uranium under sulfate-reducing conditions, less attention has been paid to the initial iron-reducing phase, noted as being of particular importance to uranium removal. The aim of this work was to assess the formation of U(IV) during the early stages of a bio-remediation experiment at the Old Rifle site, CO, from early iron-reducing conditions to the transition to sulfate-reducing conditions. Several in-well chromatographic columns packed with sediment were deployed and were sampled at different days after the start of bio-reduction. X-ray absorption spectroscopy and X-ray microscopy were used to obtain information on Fe, S and U speciation and distribution. Chemical extractions of the reduced sediments have also been performed, to determine the rate of Fe(II) and U(IV) accumulation.
Characterization of uranium redox state in organic-rich Eocene sediments.
Cumberland, Susan A; Etschmann, Barbara; Brugger, Joël; Douglas, Grant; Evans, Katy; Fisher, Louise; Kappen, Peter; Moreau, John W
2018-03-01
The presence of organic matter (OM) has a profound impact on uranium (U) redox cycling, either limiting or promoting the mobility of U via binding, reduction, or complexation. To understand the interactions between OM and U, we characterised U oxidation state and speciation in nine OM-rich sediment cores (18 samples), plus a lignite sample from the Mulga Rock polymetallic deposit in Western Australia. Uranium was unevenly dispersed within the analysed samples with 84% of the total U occurring in samples containing >21 wt % OM. Analyses of U speciation, including x-ray absorption spectroscopy and bicarbonate extractions, revealed that U existed predominately (∼71%) as U(VI), despite the low pH (4.5) and nominally reducing conditions within the sediments. Furthermore, low extractability by water, but high extractability by a bi-carbonate solution, indicated a strong association of U with particulate OM. The unexpectedly high proportion of U(VI) relative to U(IV) within the OM-rich sediments implies that OM itself does not readily reduce U, and the reduction of U is not a requirement for immobilizing uranium in OM-rich deposits. The fact that OM can play a significant role in limiting the mobility and reduction of U(VI) in sediments is important for both U-mining and remediation. Copyright © 2017 Elsevier Ltd. All rights reserved.
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.
Uranium reduction and resistance to reoxidation under iron-reducing and sulfate-reducing conditions.
Boonchayaanant, Benjaporn; Nayak, Dipti; Du, Xin; Criddle, Craig S
2009-10-01
Oxidation and mobilization of microbially-generated U(IV) is of great concern for in situ uranium bioremediation. This study investigated the reoxidation of uranium by oxygen and nitrate in a sulfate-reducing enrichment and an iron-reducing enrichment derived from sediment and groundwater from the Field Research Center in Oak Ridge, Tennessee. Both enrichments were capable of reducing U(VI) rapidly. 16S rRNA gene clone libraries of the two enrichments revealed that Desulfovibrio spp. are dominant in the sulfate-reducing enrichment, and Clostridium spp. are dominant in the iron-reducing enrichment. In both the sulfate-reducing enrichment and the iron-reducing enrichment, oxygen reoxidized the previously reduced uranium but to a lesser extent in the iron-reducing enrichment. Moreover, in the iron-reducing enrichment, the reoxidized U(VI) was eventually re-reduced to its previous level. In both, the sulfate-reducing enrichment and the iron-reducing enrichment, uranium reoxidation did not occur in the presence of nitrate. The results indicate that the Clostridium-dominated iron-reducing communities created conditions that were more favorable for uranium stability with respect to reoxidation despite the fact that fewer electron equivalents were added to these systems. The likely reason is that more of the added electrons are present in a form that can reduce oxygen to water and U(VI) back to U(IV).
Laser fluorometric analysis of plants for uranium exploration
Harms, T.F.; Ward, F.N.; Erdman, J.A.
1981-01-01
A preliminary test of biogeochemical exploration for locating uranium occurrences in the Marfa Basin, Texas, was conducted in 1978. Only 6 of 74 plant samples (mostly catclaw mimosa, Mimosa biuncifera) contained uranium in amounts above the detection limit (0.4 ppm in the ash) of the conventional fluorometric method. The samples were then analyzed using a Scintrex UA-3 uranium analyzer* * Use of trade names in this paper is for descriptive purposes only and does not constitute endorsement by the U.S. Geological Survey. - an instrument designed for direct analysis of uranium in water, and which can be conveniently used in a mobile field laboratory. The detection limit for uranium in plant ash (0.05 ppm) by this method is almost an order of magnitude lower than with the fluorometric conventional method. Only 1 of the 74 samples contained uranium below the detection limit of the new method. Accuracy and precision were determined to be satisfactory. Samples of plants growing on mineralized soils and nonmineralized soils show a 15-fold difference in uranium content; whereas the soils themselves (analyzed by delayed neutron activation analysis) show only a 4-fold difference. The method involves acid digestion of ashed tissue, extraction of uranium into ethyl acetate, destruction of the ethyl acetate, dissolution of the residue in 0.005% nitric acid, and measurement. ?? 1981.
In-situ evidence for uranium immobilization and remobilization
Senko, John M.; Istok, Jonathan D.; Suflita, Joseph M.; Krumholz, Lee R.
2002-01-01
The in-situ microbial reduction and immobilization of uranium was assessed as a means of preventing the migration of this element in the terrestrial subsurface. Uranium immobilization (putatively identified as reduction) and microbial respiratory activities were evaluated in the presence of exogenous electron donors and acceptors with field push−pull tests using wells installed in an anoxic aquifer contaminated with landfill leachate. Uranium(VI) amended at 1.5 μM was reduced to less than 1 nM in groundwater in less than 8 d during all field experiments. Amendments of 0.5 mM sulfate or 5 mM nitrate slowed U(VI) immobilization and allowed for the recovery of 10% and 54% of the injected element, respectively, as compared to 4% in the unamended treatment. Laboratory incubations confirmed the field tests and showed that the majority of the U(VI) immobilized was due to microbial reduction. In these tests, nitrate treatment (7.5 mM) inhibited U(VI) reduction, and nitrite was transiently produced. Further push−pull tests were performed in which either 1 or 5 mM nitrate was added with 1.0 μM U(VI) to sediments that already contained immobilized uranium. After an initial loss of the amendments, the concentration of soluble U(VI) increased and eventually exceeded the injected concentration, indicating that previously immobilized uranium was remobilized as nitrate was reduced. Laboratory experiments using heat-inactivated sediment slurries suggested that the intermediates of dissimilatory nitrate reduction (denitrification or dissimilatory nitrate reduction to ammonia), nitrite, nitrous oxide, and nitric oxide were all capable of oxidizing and mobilizing U(IV). These findings indicate that in-situ subsurface U(VI) immobilization can be expected to take place under anaerobic conditions, but the permanence of the approach can be impaired by disimilatory nitrate reduction intermediates that can mobilize previously reduced uranium.
Zielinski, Robert A.; Otton, James K.; Schumann, R. Randall; Wirt, Laurie
2008-01-01
Geochemical sampling of 82 stream waters and 87 stream sediments within mountainous areas immediately west of Denver, Colorado, was conducted by the U.S. Geological Survey in October 1994. The primary purpose was to evaluate regionally the effects of geology and past mining on the concentration and distribution of uranium. The study area contains uranium- and thorium-rich bedrock, numerous noneconomic occurrences of uranium minerals, and several uranium deposits of variable size and production history. During the sampling period, local streams had low discharge and were more susceptible to uranium-bearing acid drainage originating from historical mines of base- and precious-metal sulfides. Results indicated that the spatial distribution of Precambrian granites and metamorphic rocks strongly influences the concentration of uranium in stream sediments. Within-stream transport increases the dispersion of uranium- and thorium rich mineral grains derived primarily from granitic source rocks. Dissolved uranium occurs predominantly as uranyl carbonate complexes, and concentrations ranged from less than 1 to 65 micrograms per liter. Most values were less than 5 micrograms per liter, which is less than the current drinking water standard of 30 micrograms per liter and much less than locally applied aquatic-life toxicity standards of several hundred micrograms per liter. In local streams that are affected by uranium-bearing acid mine drainage, dissolved uranium is moderated by dilution and sorptive uptake by stream sediments. Sorbents include mineral alteration products and chemical precipitates of iron- and aluminum-oxyhydroxides, which form where acid drainage enters streams and is neutralized. Suspended uranium is relatively abundant in some stream segments affected by nearby acid drainage, which likely represents mobilization of these chemical precipitates. The 234U/238U activity ratio of acid drainage (0.95-1.0) is distinct from that of local surface waters (more than 1.05), and this distinctive isotopic composition may be preserved in iron-oxyhydroxide precipitates of acid drainage origin. The study area includes a particularly large vein-type uranium deposit (Schwartzwalder mine) with past uranium production. Stream water and sediment collected downstream from the mine's surface operations have locally anomalous concentrations of uranium. Fine-grained sediments downstream from the mine contain rare minute particles (10-20 micrometers) of uraninite, which is unstable in a stream environment and thus probably of recent origin related to mining. Additional rare particles of very fine grained (less than 5 micrometer) barite likely entered the stream as discharge from settling ponds in which barite precipitation was formerly used to scavenge dissolved radium from mine effluent.
NASA Astrophysics Data System (ADS)
Huang, Ke; Keiser, Dennis D.; Sohn, Yongho
2013-02-01
U-Mo alloys are being developed as low enrichment uranium fuels under the Reduced Enrichment for Research and Test Reactor (RERTR) Program. In order to understand the fundamental diffusion behavior of this system, solid-to-solid pure U vs Mo diffusion couples were assembled and annealed at 923 K, 973 K, 1073 K, 1173 K, and 1273 K (650 °C, 700 °C, 800 °C, 900 °C, and 1000 °C) for various times. The interdiffusion microstructures and concentration profiles were examined via scanning electron microscopy and electron probe microanalysis, respectively. As the Mo concentration increased from 2 to 26 at. pct, the interdiffusion coefficient decreased, while the activation energy increased. A Kirkendall marker plane was clearly identified in each diffusion couple and utilized to determine intrinsic diffusion coefficients. Uranium intrinsically diffused 5-10 times faster than Mo. Molar excess Gibbs free energy of U-Mo alloy was applied to calculate the thermodynamic factor using ideal, regular, and subregular solution models. Based on the intrinsic diffusion coefficients and thermodynamic factors, Manning's formalism was used to calculate the tracer diffusion coefficients, atomic mobilities, and vacancy wind parameters of U and Mo at the marker composition. The tracer diffusion coefficients and atomic mobilities of U were about five times larger than those of Mo, and the vacancy wind effect increased the intrinsic flux of U by approximately 30 pct.
Potential aquifer vulnerability in regions down-gradient from uranium in situ recovery (ISR) sites.
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.
Leachability of uranium and other elements from freshly erupted volcanic ash
Smith, D.B.; Zielinski, R.A.; Rose, W.I.
1982-01-01
A study of leaching of freshly erupted basaltic and dacitic air-fall ash and bomb fragment samples, unaffected by rain, shows that glass dissolution is the dominant process by which uranium is initially mobilized from air-fall volcanic ash. Si, Li, and V are also preferentially mobilized by glass dissolution. Gaseous transfer followed by fixation of soluble uranium species on volcanic-ash particles is not an important process affecting uranium mobility. Gaseous transfer, however, may be important in forming water-soluble phases, adsorbed to ash surfaces, enriched in the economically and environmentally important elements Zn, Cu, Cd, Pb, B, F, and Ba. Quick removal of these adsorbed elements by the first exposure of freshly erupted ash to rain and surface water may pose short-term hazards to certain forms of aquatic and terrestrial life. Such rapid release of material may also represent the first step in transportation of economically important elements to environments favorable for precipitation into deposits of commercial interest. Ash samples collected from the active Guatemalan volcanoes Fuego and Pacaya (high-Al basalts) and Santiaguito (hornblende-hypersthene dacite); bomb fragments from Augustine volcano (andesite-dacite), Alaska, and Heimaey (basalt), Vestmann Islands, Iceland; and fragments of "rhyolitic" pumice from various historic eruptions were subjected to three successive leaches with a constant water-to-ash weight ratio of 4:1. The volcanic material was successively leached by: (1) distilled-deionized water (pH = 5.0-5.5) at room temperature for 24 h, which removes water-soluble gases and salts adsorbed on ash surfaces during eruption; (2) dilute HCl solution (pH = 3.5-4.0) at room temperature for 24 h, which continues the attack initiated by the water and also attacks acid-soluble sulfides and oxides; (3) a solution 0.05 M in both Na,CO, and NaHCO, (pH = 9.9) at 80°C for one week, which preferentially dissolves volcanic glass. The first two leaches mimic interaction of ash with rain produced in the vicinity of an active eruption. The third leach accelerates the effect of prolonged contact of volcanic ash with alkaline ground water present during ash diagenesis.
U-Pb dating of uranium deposits in collapse breccia pipes of the Grand Canyon region
Ludwig, K. R.; Simmons, K.R.
1992-01-01
Two major periods of uranium mineralization are indicated by U-Pb isotope dating of uranium ores from collapse breccia pipes in the Grand Canyon region, northern Arizona. The Hack 2 and 3, Kanab North, and EZ 1 and 2 orebodies apparently formed in the interval of 200 ?? 20 Ma, similar to ages inferred for strata-bound, Late Triassic-hosted uranium deposits in southern Utah and northern Arizona. Samples from the Grand Canyon and Pine Nut pipes, however, indicate a distinctly older age of about 260 Ma. The clustering in ages for a variety of uranium deposits at about the age of the lower part of the Chinle Formation (Late Triassic) suggests that uranium in these deposits may have been derived by leaching from volcanic ash in the Chinle and mobilized by ground-water movement. Pb isotope ratios of galenas in mineralized pipes are more radiogenic than those of sulfides from either uranium-poor pipes or occurrences away from pipes. Fluids which passed through the pipes had interacted with the Proterozoic basement, possibly through the vertical fractures which influenced the location and evolution of the pipes themselves. -from Authors
Bioreduction of U(VI)-Phthalate to a Polymeric U(IV)-Phthalate Colloid
DOE Office of Scientific and Technical Information (OSTI.GOV)
Vazquez, G.; Dodge, C; Francis, A
2009-01-01
Phthalic acid, a ubiquitous organic ligand, formed soluble mono- and biligand complexes with a uranyl ion that was then reduced to a U(IV)-phthalate by a Clostridium species under anaerobic conditions. We confirmed the reduction of the hexavalent uranium to the tetravalent oxidation state by UV-vis absorption and X-ray absorption near edge structure spectroscopy. Sequential micro- and ultrafiltration of the solution revealed that the bioreduced uranium was present as a colloid with particles between 0.03 and 0.45 {mu}m. Analysis with extended X-ray absorption fine structure revealed the association of the reduced uranium with the phthalic acid as a repeating biligand 1:2more » U(IV):phthalic acid polymer. This is the first report of the formation of a U(IV) complexed to two phthalic acid molecules in the form of a polymeric colloid. Although it was proposed that the bioreduction and the precipitation of uranium might be an invaluable strategy to immobilize uranium in contaminated environments, our results suggest that the organic ligands present there might hinder the precipitation of the bioreduced uranium under anaerobic conditions and, thereby, enhance its environmental mobility as uranium organic complexes or colloids.« less
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
Effect of Co-Contaminants Uranium and Nitrate on Iodine Remediation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Szecsody, James E.; Lee, Brady D.; Lawter, Amanda R.
The objective of this study is to evaluate the significance of co-contaminants on the migration and transformation of iodine species in the Hanford subsurface environment. These impacts are relevant because remedies that target individual contaminants like iodine, may not only impact the fate and transport of other contaminants in the subsurface, but also inhibit the effectiveness of a targeted remedy. For example, iodine (as iodate) co-precipitates with calcite, and has been identified as a potential remedy because it immobilizes iodine. Since uranium also co-precipitates with calcite in field sediments, the presence of uranium may also inhibit iodine co-precipitation. Another potentiallymore » significant impact from co-existing contaminants is iodine and nitrate. The presence of nitrate has been shown to promote biogeochemical reduction of iodate to iodide, thereby increasing iodine species subsurface mobility (as iodide exhibits less sorption). Hence, this study reports on both laboratory batch and column experiments that investigated a) the change in iodate uptake mass and rate of uptake into precipitating calcite due to the presence of differing amounts of uranium, b) the amount of change of the iodate bio-reduction rate due to the presence of differing nitrate concentrations, and c) whether nitrite can reduce iodate in the presence of microbes and/or minerals acting as catalysts.« less
Method for mobilization of hazardous metal ions in soils
Dugan, Patrick R.; Pfister, Robert M.
1995-01-01
A microbial process for removing heavy metals such as bismuth, cadmium, lead, thorium, uranium and other transuranics from soils and sediments, utilizing indigenous, or isolates of indigenous, microorganisms and reducing agents, such as cysteine or sodium thioglycollate, or complexing agents such as the amino acid glycine, to effect the mobilization or release of the metals from the soil particles.
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.
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
Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn
2018-05-02
Uranium is a key contaminant of concern in the groundwater at U.S. Department of Energy (DOE) facilities within the United States and is a potential source of groundwater contamination and a risk to human health and the environment through discharges to surface water. Dissolved inorganic carbon (bicarbonate/carbonate) has a high affinity for complexing with uranium that is present as sorbed or unique uranium-bearing mineral phases within the sedimentary matrix. This process can result in the formation of soluble uranyl carbonate aqueous species, which are mobile under circumneutral pH conditions. This study was conducted to quantify the rate of release of uranium from the autunite mineral, (Ca[(UO 2 )(PO 4 )] 2 •3H 2 O), that was formed during polyphosphate injection to remediate uranium; the dissolution of uranium was studied as a function of the aqueous bicarbonate concentration, ranging from 25 to 100 mM. Experiments were carried out in the pH range from 7 to 11 in the temperature range of 23-90 °C via single-pass flow-through testing. Consistent with the results of previous studies (Gudavalli et al., 2013a, 2013b), the rate of uranium release from autunite exhibited minimal dependency on temperature, but was strongly dependent on pH and increasing concentrations of bicarbonate in the solution. Data obtained during these experiments were compared with results of previous experiments conducted using a low-concentration range of bicarbonate solutions (0.5-3.0 mM). An 8- to 30-fold increase in the rate of uranium release was observed in the presence of high bicarbonate concentrations at pH 7-8 compared to low bicarbonate values, while at pH 9-11, there was only a 5-fold increase in uranium rate of release with an increase in bicarbonate concentrations. The rate of uranium release was calculated to be between 5.18 × 10 -8 and 1.69 × 10 -7 mol m -2 s -1 . The activation energy values at high and low bicarbonate concentrations were similar, with ratio values in the range of 0.6-1.0. Copyright © 2018 Elsevier Ltd. All rights reserved.
Uranium in groundwater - A synopsis based on a large hydrogeochemical data set.
Riedel, Thomas; Kübeck, Christine
2018-02-01
Most of the knowledge on the occurrence of Uranium (U) in groundwater comes from in-situ manipulation experiments in the field, computational modelling studies or from laboratory analyses where individual processes of U mobilization were studied in isolation. Because of Uranium's vital redox chemistry it interacts, often simultaneously, with many other element cycles (e.g., sulfur, carbon, iron, and manganese) making it difficult to predict U concentrations in natural environments. For the present study a large data set was analyzed to predict the occurrence of U in groundwater from basic hydrochemistry. The data set consists of more than 8000 chemical groundwater analyses (including Uranium concentrations) from more than 2000 sampling locations. A strong relation between U concentrations and electric conductivity as well as alkalinity was observed, suggesting that weathering of geogenic source material and desorption from mineral surfaces is the principle mechanism of U release. Except for aquifers with strongly reducing conditions this process leads to a slow but continuous accumulation of U in groundwater in most cases. Importantly, the occurrence of U is modulated by the prevailing redox conditions in an aquifer. Uranium concentrations were moderate under oxic conditions and highest under manganese and nitrate-reducing conditions (heterotrophic as wells as autotrophic nitrate reduction). Only in iron- and sulfate-reducing groundwater the probability of U concentrations above 1 μg l -1 was virtually zero, as these ground waters act as U sinks. The combination of mineral weathering (especially carbonates) with mobilization of U under manganese and nitrate reducing conditions results in the highest risk of detecting U. In contrast, a low risk is associated with low pH (<7) and low mineralization of groundwater, which is the case in granitic catchments, for example. Our results further provide evidence, that agricultural practices such as liming, use of fertilizers and irrigation influence the occurrence of U in groundwater in multiple ways. Accurate management of aquifers underlying farmland will therefore become more and more important in the future. In summary, we find that the vulnerability of an aquifer to elevated U concentrations cannot be explained by a single factor. This complicates efforts to target elevated U concentrations in groundwaters that are abstracted for drinking water production. Copyright © 2017 Elsevier Ltd. All rights reserved.
Method for mobilization of hazardous metal ions in soils
Dugan, P.R.; Pfister, R.M.
1995-06-27
A microbial process is revealed for removing heavy metals such as bismuth, cadmium, lead, thorium, uranium and other transuranics from soils and sediments. The method utilizes indigenous, or isolates of indigenous, microorganisms and reducing agents, such as cysteine or sodium thioglycollate, or complexing agents such as the amino acid glycine, to effect the mobilization or release of the metals from the soil particles. 5 figs.
Uranium Isotope Ratios in Modern and Precambrian Soils
NASA Astrophysics Data System (ADS)
DeCorte, B.; Planavsky, N.; Wang, X.; Auerbach, D. J.; Knudsen, A. C.
2015-12-01
Uranium isotopes (δ238U values) are an emerging paleoredox proxy that can help to better understand the redox evolution of Earth's surface environment. Recently, uranium isotopes have been used to reconstruct ocean and atmospheric redox conditions (Montoya-Pino et al., 2010; Brennecka et al., 2011; Kendall et al., 2013; Dahl et al., 2014). However, to date, there have not been studies on paleosols, despite that paleosols are, arguably better suited to directly tracking the redox conditions of the atmosphere. Sedimentary δ238U variability requires the formation of the soluble, oxidized form of U, U(VI). The formation of U(VI) is generally thought to require oxygen levels orders of magnitude higher than prebiotic levels. Without significant U mobility, it would have been impossible to develop isotopically distinct pools of uranium in ancient Earth environments. Conversely, an active U redox cycle leads to significant variability in δ238U values. Here we present a temporally and geographically expansive uranium isotope record from paleosols and modern soils to better constrain atmospheric oxygen levels during the Precambrian. Preliminary U isotope measurements of paleosols are unfractionated (relative to igneous rocks), possibly because of limited fractionation during oxidation (e.g., {Wang, 2015 #478}) or insufficient atmospheric oxygen levels to oxidize U(IV)-bearing minerals in the bedrock. Further U isotope measurements of paleosols with comparison to modern soils will resolve this issue.
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.
NASA Astrophysics Data System (ADS)
Denton, J.; Goldstein, S. J.; Paviet, P.; Nunn, A. J.; Amato, R. S.; Hinrichs, K. A.
2015-12-01
In this study we utilize U-series disequilibria measurements to investigate mineral fluid interactions and the role fractures play in the geochemical evolution of an analogue for a high level nuclear waste repository, the Nopal I uranium ore deposit. Samples of fracture-fill materials have been collected from a vertical drill core and surface fractures. High uranium concentrations in these materials (12-7700 ppm) indicate U mobility and transport from the deposit in the past. U concentrations generally decrease with horizontal distance away from the ore deposit but show no trend with depth. Isotopic activity ratios indicate a complicated geochemical evolution in terms of the timing and extent of actinide mobility, possibly due to changing environmental (redox) conditions over the history of the deposit. 234U/238U activity ratios are generally distinct from secular equilibrium and indicate some degree of open system U behavior during the past 1.2 Ma. However, calculated closed system 238U-234U-230Th model ages are generally >313 ka and >183 ka for the surface fracture and drill core samples respectively, suggesting closed system behavior for U and Th over this most recent time period. Whole rock isochrons drawn for the drill core samples show that at two of three depths fractures have remained closed with respect to U and Th mobility for >200 ka. However, open system behavior for U in the last 350 ka is suggested at 67 m depth. 231Pa/235U activity ratios within error of unity suggest closed system behavior for U and Pa for at least the past 185 ka. 226Ra/230Th activity ratios are typically <1 (0.7-1.2), suggesting recent (<8 ka) radium loss and mobility due to ongoing fluid flow in the fractures. Overall, the mainly closed system behavior of U-Th-Pa over the past ~200 ka provides one indicator of the geochemical immobility of these actinides over long time-scales for potential nuclear waste repositories sited in fractured, unsaturated tuff.
Natural uranium and thorium isotopes in sediment cores off Malaysian ports
NASA Astrophysics Data System (ADS)
Yusoff, Abdul Hafidz; Sabuti, Asnor Azrin; Mohamed, Che Abd Rahim
2015-06-01
Sediment cores collected from three Malaysian marine ports, namely, Kota Kinabalu, Labuan and Klang were analyzed to determine the radioactivities of 234U, 238U, 230Th, 232Th and total organic carbon (TOC) content. The objectives of this study were to determine the factors that control the activity of uranium isotopes and identify the possible origin of uranium and thorium in these areas. The activities of 234U and 238U show high positive correlation with TOC at the middle of sediment core from Kota Kinabalu port. This result suggests that activity of uranium at Kota Kinabalu port was influenced by organic carbon. The 234U/238U value at the upper layer of Kota Kinabalu port was ≥1.14 while the ratio value at Labuan and Klang port was ≤ 1.14. These results suggest a reduction process occurred at Kota Kinabalu port where mobile U(VI) was converted to immobile U(IV) by organic carbon. Therefore, it can be concluded that the major input of uranium at Kota Kinabalu port is by sorptive uptake of authigenic uranium from the water column whereas the major inputs of uranium to Labuan and Klang port are of detrital origin. The ratio of 230Th/232Th was used to estimate the origin of thorium. Low ratio value (lt; 1.5) at Labuan and Klang ports support the suggestion that thorium from both areas were come from detrital input while the high ratio (> 1.5) of 230Th/232Th at Kota Kinabalu port suggest the anthropogenic input of 230Th to this area. The source of 230Th is probably from phosphate fertilizers used in the oil-palm cultivation in Kota Kinabalu that is adjacent to the Kota Kinabalu port.
Geochemical control on uranium(IV) mobility in a mining-impacted wetland.
Wang, Yuheng; Bagnoud, Alexandre; Suvorova, Elena; McGivney, Eric; Chesaux, Lydie; Phrommavanh, Vannapha; Descostes, Michael; Bernier-Latmani, Rizlan
2014-09-02
Wetlands often act as sinks for uranium and other trace elements. Our previous work at a mining-impacted wetland in France showed that a labile noncrystalline U(IV) species consisting of U(IV) bound to Al-P-Fe-Si aggregates was predominant in the soil at locations exhibiting a U-containing clay-rich layer within the top 30 cm. Additionally, in the porewater, the association of U(IV) with Fe(II) and organic matter colloids significantly increased U(IV) mobility in the wetland. In the present study, within the same wetland, we further demonstrate that the speciation of U at a location not impacted by the clay-rich layer is a different noncrystalline U(IV) species, consisting of U(IV) bound to organic matter in soil. We also show that the clay-poor location includes an abundant sulfate supply and active microbial sulfate reduction that induce substantial pyrite (FeS2) precipitation. As a result, Fe(II) concentrations in the porewater are much lower than those at clay-impacted zones. U porewater concentrations (0.02-0.26 μM) are also considerably lower than those at the clay-impacted locations (0.21-3.4 μM) resulting in minimal U mobility. In both cases, soil-associated U represents more than 99% of U in the wetland. We conclude that the low U mobility reported at clay-poor locations is due to the limited association of Fe(II) with organic matter colloids in porewater and/or higher stability of the noncrystalline U(IV) species in soil at those locations.
Field Testing of Downgradient Uranium Mobility at an In-Situ Recovery Uranium Mine
NASA Astrophysics Data System (ADS)
Reimus, P. W.; Clay, J. T.; Rearick, M.; Perkins, G.; Brown, S. T.; Basu, A.; Chamberlain, K.
2015-12-01
In-situ recovery (ISR) mining of uranium involves the injection of O2 and CO2 (or NaHCO3) into saturated roll-front deposits to oxidize and solubilize the uranium, which is then removed by ion exchange at the surface and processed into U3O8. While ISR is economical and environmentally-friendly relative to conventional mining, one of the challenges of extracting uranium by this process is that it leaves behind a geochemically-altered aquifer that is exceedingly difficult to restore to pre-mining geochemical conditions, a regulatory objective. In this research, we evaluated the ability of the aquifer downgradient of an ISR mining area to attenuate the transport of uranium and other problem constituents that are mobilized by the mining process. Such an evaluation can help inform both regulators and the mining industry as to how much restoration of the mined ore zone is necessary to achieve regulatory compliance at various distances downgradient of the mining zone even if complete restoration of the ore zone proves to be difficult or impossible. Three single-well push-pull tests and one cross-well test were conducted in which water from an unrestored, previously-mined ore zone was injected into an unmined ore zone that served as a geochemical proxy for the downgradient aquifer. In all tests, non-reactive tracers were injected with the previously-mined ore zone water to allow the transport of uranium and other constituents to be compared to that of the nonreactive species. In the single-well tests, it was shown that the recovery of uranium relative to the nonreactive tracers ranged from 12-25%, suggesting significant attenuation capacity of the aquifer. In the cross-well test, selenate, molybdate and metavanadate were injected with the unrestored water to provide information on the transport of these potentially-problematic anionic constituents. In addition to the species-specific transport information, this test provided valuable constraints on redox conditions within the system, as redox couples involving these species collectively bracket the predicted transition redox potential for the U(VI)/U(IV) couple. Reduction should provide much longer-lasting immobilization of constituents than adsorption, especially given the inherent reducing characteristics of roll-front systems.
Sorption and bioreduction of hexavalent uranium at a military facility by the Chesapeake Bay.
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).
NASA Astrophysics Data System (ADS)
Mercadier, Julien; Cuney, Michel; Cathelineau, Michel; Lacorde, Mathieu
2011-02-01
Proterozoic basement-hosted unconformity-related uranium deposits of the Athabasca Basin (Saskatchewan, Canada) were affected by significant uranium redistribution along oxidation-reduction redox fronts related to cold and late meteoric fluid infiltration. These redox fronts exhibit the same mineralogical and geochemical features as the well-studied uranium roll-front deposits in siliclastic rocks. The primary hydrothermal uranium mineralisation (1.6-1.3 Ga) of basement-hosted deposits is strongly reworked to new disseminated ores comprising three distinctly coloured zones: a white-green zone corresponding to the previous clay-rich alteration halo contemporaneous with hydrothermal ores, a uranium front corresponding to the uranium deposition zone of the redox front (brownish zone, rich in goethite) and a hematite-rich red zone marking the front progression. The three zones directly reflect the mineralogical zonation related to uranium oxides (pitchblende), sulphides, iron minerals (hematite and goethite) and alumino-phosphate-sulphate (APS) minerals. The zoning can be explained by processes of dissolution-precipitation along a redox interface and was produced by the infiltration of cold (<50°C) meteoric fluids to the hydrothermally altered areas. U, Fe, Ca, Pb, S, REE, V, Y, W, Mo and Se were the main mobile elements in this process, and their distribution within the three zones was, for most of them, directly dependent on their redox potential. The elements concentrated in the redox fronts were sourced by the alteration of previously crystallised hydrothermal minerals, such as uranium oxides and light rare earth element (LREE)-rich APS. The uranium oxides from the redox front are characterised by LREE-enriched patterns, which differ from those of unconformity-related ores and clearly demonstrate their distinct conditions of formation. Uranium redox front formation is thought to be linked to fluid circulation episodes initiated during the 400-300 Ma period during uplift and erosion of the Athabasca Basin when it was near the Equator and to have been still active during the last million years. A major kaolinisation event was caused by changes in the fluid circulation regime, reworking the primary uranium redox fronts and causing the redistribution of elements originally concentrated in the uranium-enriched meteoric-related redox fronts.
Uranium (VI) transport in saturated heterogeneous media: Influence of kaolinite and humic acid.
Chen, Chong; Zhao, Kang; Shang, Jianying; Liu, Chongxuan; Wang, Jin; Yan, Zhifeng; Liu, Kesi; Wu, Wenliang
2018-05-07
Natural aquifers typically exhibit a variety of structural heterogeneities. However, the effect of mineral colloids and natural organic matter on the transport behavior of uranium (U) in saturated heterogeneous media are not totally understood. In this study, heterogeneous column experiments were conducted, and the constructed columns contained a fast-flow domain (FFD) and a slow-flow domain (SFD). The effect of kaolinite, humic acid (HA), and kaolinite/HA mixture on U(VI) retention and release in saturated heterogeneous media was examined. Media heterogeneity significantly influenced U fate and transport behavior in saturated subsurface environment. The presence of kaolinite, HA, and kaolinite/HA enhanced the mobility of U in heterogeneous media, and the mobility of U was the highest in the presence of kaolinite/HA and the lowest in the presence of kaolinite. In the presence of kaolinite, there was no difference in the amount of U released from the FFD and SFD. However, in the presence of HA and kaolinite/HA, a higher amount of U was released from the FFD. The findings in this study showed that medium structure and mineral colloids, as well as natural organic matter in the aqueous phase had significant effects on U transport and fate in subsurface environment. Copyright © 2018 Elsevier Ltd. All rights reserved.
Landa, Edward R.
2004-01-01
Uranium mill tailings (UMT) are a high volume, low specific activity radioactive waste typically disposed in surface impoundments. This review focuses on research on UMT and related earth materials during the past decade relevant to the assessment of: (1) mineral hosts of radionuclides; (2) the use of soil analogs in predicting long-term fate of radionuclides; (3) microbial and diagenetic processes that may alter radionuclide mobility in the surficial environment; (4) waste-management technologies to limit radionuclide migration; and (5) the impact of UMT on biota.
Effects of nitrate on the stability of uranium in a bioreduced region of the subsurface.
Wu, Wei-Min; Carley, Jack; Green, Stefan J; Luo, Jian; Kelly, Shelly D; Van Nostrand, Joy; Lowe, Kenneth; Mehlhorn, Tonia; Carroll, Sue; Boonchayanant, Benjaporn; Löfller, Frank E; Watson, David; Kemner, Kenneth M; Zhou, Jizhong; Kitanidis, Peter K; Kostka, Joel E; Jardine, Philip M; Criddle, Craig S
2010-07-01
The effects of nitrate on the stability of reduced, immobilized uranium were evaluated in field experiments at a U.S. Department of Energy site in Oak Ridge, TN. Nitrate (2.0 mM) was injected into a reduced region of the subsurface containing high levels of previously immobilized U(IV). The nitrate was reduced to nitrite, ammonium, and nitrogen gas; sulfide levels decreased; and Fe(II) levels increased then deceased. Uranium remobilization occurred concomitant with nitrite formation, suggesting nitrate-dependent, iron-accelerated oxidation of U(IV). Bromide tracer results indicated changes in subsurface flowpaths likely due to gas formation and/or precipitate. Desorption-adsorption of uranium by the iron-rich sediment impacted uranium mobilization and sequestration. After rereduction of the subsurface through ethanol additions, background groundwater containing high levels of nitrate was allowed to enter the reduced test zone. Aqueous uranium concentrations increased then decreased. Clone library analyses of sediment samples revealed the presence of denitrifying bacteria that can oxidize elemental sulfur, H(2)S, Fe(II), and U(IV) (e.g., Thiobacillus spp.), and a decrease in relative abundance of bacteria that can reduce Fe(III) and sulfate. XANES analyses of sediment samples confirmed changes in uranium oxidation state. Addition of ethanol restored reduced conditions and triggered a short-term increase in Fe(II) and aqueous uranium, likely due to reductive dissolution of Fe(III) oxides and release of sorbed U(VI). After two months of intermittent ethanol addition, sulfide levels increased, and aqueous uranium concentrations gradually decreased to <0.1 microM.
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.
NASA Astrophysics Data System (ADS)
Carpenter, J.; Hyun, S.; Hayes, K. F.
2010-12-01
Uranium (U) originating from mining operations for weapon manufacturing and nuclear energy production is a significant radionuclide contaminant in groundwater local to uranium mining, uranium milling, and uranium mill tailing (UMT) storage sites. In the USA, the Department of Energy (DOE) is currently overseeing approximately 24 Uranium Mill Tailing Remediation Action (UMTRA) sites which have collectively processed over 27 million tons of uranium ore1,2. In-Situ microbial bio-reduction of the highly mobile U6+ ion into the dramatically less mobile U4+ ion has been demonstrated as an effective remedial process to inhibit uranium migration in the aqueous phase3. The resistance of this process to oxidization and possible remobilization of U when bioremediation stops (and oxidants such as oxygen from the air or nitrate in water diffuse into the formation) in the long term is not known. UMTRA site studies3 have shown that iron sulfide solids are produced by sulfate reducing bacteria (SRB) during U bioremediation, and some forms of these iron sulfide solids are known to be effective oxidant scavengers, potentially protecting against re-oxidation and thus remobilization of U. This work is investigating the role of iron sulfide solids in the long-term immobilization of reduced U compounds after bioremediation is completed in groundwater local to UMTRA sites. Re-oxidation tests are being performed in packed media columns loaded with both FeS and U solids. High quality mackinawite (FeS), and uraninite (UO2) have been synthesized in our laboratory via a wet chemistry approach. These synthetic materials are expected to mimic the naturally occurring and biogenic materials present in biologically stimulated UMTRA sites. In order to establish the initial conditions of the prepared experimental columns and to compare synthetic and biogenic FeS and UO2, these synthesized materials have been characterized with synchrotron radiation at the Stanford Synchrotron Radiation Lightsource using synchrotron x-ray powder diffraction (SXRD) and extended x-ray absorption fine structure (EXAFS). SXRD data were collected and analyzed with profile fitting to determine lattice parameters and crystallite size for comparison with published values for both biogenic and synthetic materials. This is particularly of interest for UO2, as there is very little information on particle size and lattice parameters for synthetic UO2 in the literature. Profile fitting of the SXRD data for FeS gives lattice parameters of a = b = 3.668 and a mean crystallite size of 5 to 8 nm. Both of these values are in good agreement with published values. For fresh UO2, lattice parameters were determined as a = b = c = 5.4 nm for both freshly synthesized and aged (3 months) UO2 and particle size was determined to be 3.5 nm for fresh UO2 and 5.83 nm for aged UO2. This suggests a growth mechanism for crystallites over time, and an inferred decrease in reactivity.
Uranium fate in wetland mesocosms: Effects of plants at two iron loadings with different pH values.
Koster van Groos, Paul G; Kaplan, Daniel I; Chang, Hyun-Shik; Seaman, John C; Li, Dien; Peacock, Aaron D; Scheckel, Kirk G; Jaffé, Peter R
2016-11-01
Small-scale continuous flow wetland mesocosms (∼0.8 L) were used to evaluate how plant roots under different iron loadings affect uranium (U) mobility. When significant concentrations of ferrous iron (Fe) were present at circumneutral pH values, U concentrations in root exposed sediments were an order of magnitude greater than concentrations in root excluded sediments. Micro X-ray absorption near-edge structure (μ-XANES) spectroscopy indicated that U was associated with the plant roots primarily as U(VI) or U(V), with limited evidence of U(IV). Micro X-ray fluorescence (μ-XRF) of plant roots suggested that for high iron loading at circumneutral pH, U was co-located with Fe, perhaps co-precipitated with root Fe plaques, while for low iron loading at a pH of ∼4 the correlation between U and Fe was not significant, consistent with previous observations of U associated with organic matter. Quantitative PCR analyses indicated that the root exposed sediments also contained elevated numbers of Geobacter spp., which are likely associated with enhanced iron cycling, but may also reduce mobile U(VI) to less mobile U(IV) species. Copyright © 2016 Elsevier Ltd. All rights reserved.
Alpine, Andrea E.
2010-01-01
On July 21, 2009, U.S. Secretary of the Interior Ken Salazar proposed a two-year withdrawal of about 1 million acres of Federal land near the Grand Canyon from future mineral entry. These lands are contained in three parcels: two parcels on U.S. Bureau of Land Management land to the north of the Grand Canyon (North and East Segregation Areas) and one on the Kaibab National Forest south of the Grand Canyon (South Segregation Area). The purpose of the two-year withdrawal is to examine the potential effects of restricting these areas from new mine development for the next 20 years. This proposed withdrawal initiated a period of study during which the effects of the withdrawal must be evaluated. At the direction of the Secretary, the U.S. Geological Survey began a series of short-term studies designed to develop additional information about the possible effects of uranium mining on the natural resources of the region. Dissolved uranium and other major, minor, and trace elements occur naturally in groundwater as the result of precipitation infiltrating from the surface to water-bearing zones and, presumably, to underlying regional aquifers. Discharges from these aquifers occur as seeps and springs throughout the region and provide valuable habitat and water sources for plants and animals. Uranium mining within the watershed may increase the amount of radioactive materials and heavy metals in the surface water and groundwater flowing into Grand Canyon National Park and the Colorado River, and deep mining activities may increase mobilization of uranium through the rock strata into the aquifers. In addition, waste rock and ore from mined areas may be transported away from the mines by wind and runoff.
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
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
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.
Potential for U sequestration with select minerals and sediments via base treatment.
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.
Molten uranium dioxide structure and dynamics
Skinner, L. B.; Parise, J. B.; Benmore, C. J.; ...
2014-11-21
Uranium dioxide (UO 2) is the major nuclear fuel component of fission power reactors. A key concern during severe accidents is the melting and leakage of radioactive UO 2 as it corrodes through its zirconium cladding and steel containment. Yet, the very high temperatures (>3140 kelvin) and chemical reactivity of molten UO 2 have prevented structural studies. In this work, we combine laser heating, sample levitation, and synchrotron x-rays to obtain pair distribution function measurements of hot solid and molten UO 2. The hot solid shows a substantial increase in oxygen disorder around the lambda transition (2670 K) but negligiblemore » U-O coordination change. On melting, the average U-O coordination drops from 8 to 6.7 ± 0.5. Molecular dynamics models refined to this structure predict higher U-U mobility than 8-coordinated melts.« less
Uranium- and thorium-bearing pegmatites of the United States
DOE Office of Scientific and Technical Information (OSTI.GOV)
Adams, J.W.; Arengi, J.T.; Parrish, I.S.
1980-04-01
This report is part of the National Uranium Resource Evaluation (NURE) Program designed to identify criteria favorable for the occurrence of the world's significant uranium deposits. This project deals specifically with uranium- and thorium-bearing pegmatites in the United States and, in particular, their distribution and origin. From an extensive literature survey and field examination of 44 pegmatite localities in the United States and Canada, the authors have compiled an index to about 300 uranium- and thorium-bearing pegmatites in the United States, maps giving location of these deposits, and an annotated bibliography to some of the most pertinent literature on themore » geology of pegmatites. Pegmatites form from late-state magma differentiates rich in volatile constituents with an attendant aqueous vapor phase. It is the presence of an aqueous phase which results in the development of the variable grain size which characterizes pegmatites. All pegmatites occur in areas of tectonic mobility involving crustal material usually along plate margins. Those pegmatites containing radioactive mineral species show, essentially, a similar distribution to those without radioactive minerals. Criteria such as tectonic setting, magma composition, host rock, and elemental indicators among others, all serve to help delineate areas more favorable for uranium- and thorium-bearing pegmatites. The most useful guide remains the radioactivity exhibited by uranium- and thorium-bearing pegmatites. Although pegmatites are frequently noted as favorable hosts for radioactive minerals, the general paucity and sporadic distribution of these minerals and inherent mining and milling difficulties negate the resource potential of pegmatites for uranium and thorium.« less
NASA Astrophysics Data System (ADS)
Wang, Qing; Cheng, Tao; Wu, Yang
2014-12-01
Mineral colloids and humic substances often co-exist in subsurface environment and substantially influence uranium (U) transport. However, the combined effects of mineral colloids and humic substances on U transport are not clear. This study is aimed at quantifying U transport and elucidating geochemical processes that control U transport when both mineral colloids and humic acid (HA) are present. U-spiked solutions/suspensions were injected into water-saturated sand columns, and U and colloid concentrations in column effluent were monitored. We found that HA promoted U transport via (i) formation of aqueous U-HA complexes, and (ii) competition against aqueous U for surface sites on transport media. Illite colloids had no influence on U transport at pH 5 in the absence of HA due to low mobility of the colloids. At pH 9, U desorbed from mobile illite and the presence of illite decreased U transport. At pH 5, high U transport occurred when both illite colloids and HA were present, which was attributed to enhanced U adsorption to illite colloids via formation of ternary illite-HA-U surface complexes, and enhanced illite transport due to HA attachment to illite and transport media. This study demonstrates that the combined effects of mineral colloids and HA on contaminant transport is different from simple addition of the individual effect.
Uranium Biomineralization By Natural Microbial Phosphatase Activities in the Subsurface
DOE Office of Scientific and Technical Information (OSTI.GOV)
Taillefert, Martial
This project investigated the geochemical and microbial processes associated with the biomineralization of radionuclides in subsurface soils. During this study, it was determined that microbial communities from the Oak Ridge Field Research subsurface are able to express phosphatase activities that hydrolyze exogenous organophosphate compounds and result in the non-reductive bioimmobilization of U(VI) phosphate minerals in both aerobic and anaerobic conditions. The changes of the microbial community structure associated with the biomineralization of U(VI) was determined to identify the main organisms involved in the biomineralization process, and the complete genome of two isolates was sequenced. In addition, it was determined thatmore » both phytate, the main source of natural organophosphate compounds in natural environments, and polyphosphate accumulated in cells could also be hydrolyzed by native microbial population to liberate enough orthophosphate and precipitate uranium phosphate minerals. Finally, the minerals produced during this process are stable in low pH conditions or environments where the production of dissolved inorganic carbon is moderate. These findings suggest that the biomineralization of U(VI) phosphate minerals is an attractive bioremediation strategy to uranium bioreduction in low pH uranium-contaminated environments. These efforts support the goals of the SBR long-term performance measure by providing key information on "biological processes influencing the form and mobility of DOE contaminants in the subsurface".« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean - Francois
2010-12-10
The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity.more » Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.« less
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.
Oliver, Ian W; Graham, Margaret C; MacKenzie, Angus B; Ellam, Robert M; Farmer, John G
2008-12-15
The mobility and bioavailability of depleted uranium (DU) in soils at a UK Ministry of Defence (UK MoD) weapons testing range were investigated. Soil and vegetation were collected near a test-firing position and at eight points along a transect line extending approximately 200 m down-slope, perpendicular to the firing line, toward a small stream. Earthworms and porewaters were subsequently separated from the soils and both total filtered porewater (<0.2 microm) and discrete size fractions (0.2 microm-100 kDa, 100-30 kDa, 30-3 kDa, and <3 kDa)obtainedvia centrifugal ultrafiltration were examined. Uranium concentrations were determined by inductively coupled plasma optical emission spectrometry (ICP-OES) for soils and ICP-mass spectrometry (MS) for earthworms and porewaters, while 235U:238U atom ratios were determined by multicollector (MC)-ICP-MS. Comparison of the porewater and earthworm isotopic values with those of the soil solids indicated that DU released into the environment during weapons test-firing operations was more labile and more bioavailable than naturally occurring U in the soils at the testing range. Importantly, DU was shown to be present in soil porewater even at a distance of approximately 185 m from the test-firing position and, along the extent of the transect was apparently associated with organic colloids.
Liu, Bo; Peng, Tongjiang; Sun, Hongjuan
2017-06-01
Pollution by the release of heavy metals from tailings constitutes a potential threat to the environment. To characterize the processes governing the release of Mn, Sr, Pb, and U from the uranium mill tailings, a dynamic leaching test was applied for different size of uranium mill tailings samples. Inductively coupled plasma atomic emission spectroscopy (ICP-AES) and inductively coupled plasma mass spectrometry (ICP-MS) were performed to determine the content of Mn, Sr, Pb, and U in the leachates. The release of mobile Mn, Sr, Pb, and U fraction was slow, being faster in the initial stage and then attained a near steady-state condition. The experimental results demonstrate that the release of Mn, Sr, Pb, and U from uranium mill tailings with different size fractions is controlled by a variety of mechanisms. Surface wash-off is the release mechanism for Mn. The main release mechanism of Sr and Pb is the dissolution in the initial leaching stage. For U, a mixed process of wash-off and diffusion is the controlling mechanism.
Formation and Geological Sequestration of Uranium Nanoparticles in Deep Granitic Aquifer
Suzuki, Yohey; Mukai, Hiroki; Ishimura, Toyoho; Yokoyama, Takaomi D.; Sakata, Shuhei; Hirata, Takafumi; Iwatsuki, Teruki; Mizuno, Takashi
2016-01-01
The stimulation of bacterial activities that convert hexavalent uranium, U(VI), to tetravalent uranium, U(IV), appears to be feasible for cost-effective remediation of contaminated aquifers. However, U(VI) reduction typically results in the precipitation of U(IV) particles less than 5 nanometers in diameter, except for environmental conditions enriched with iron. Because these tiny particles are mobile and susceptible to oxidative dissolution after the termination of nutrient injection, in situ bioremediation remains to be impractical. Here we show that U(IV) nanoparticles of coffinite (U(SiO4)1−x(OH)4x) formed in fracture-filling calcium carbonate in a granitic aquifer. In situ U-Pb isotope dating demonstrates that U(IV) nanoparticles have been sequestered in the calcium carbonate for at least 1 million years. As the microbiologically induced precipitation of calcium carbonate in aquifer systems worldwide is extremely common, we anticipate simultaneous stimulation of microbial activities for precipitation reactions of calcium carbonate and U(IV) nanoparticles, which leads to long-term sequestration of uranium and other radionuclides in contaminated aquifers and deep geological repositories. PMID:26948389
Formation and Geological Sequestration of Uranium Nanoparticles in Deep Granitic Aquifer.
Suzuki, Yohey; Mukai, Hiroki; Ishimura, Toyoho; Yokoyama, Takaomi D; Sakata, Shuhei; Hirata, Takafumi; Iwatsuki, Teruki; Mizuno, Takashi
2016-03-07
The stimulation of bacterial activities that convert hexavalent uranium, U(VI), to tetravalent uranium, U(IV), appears to be feasible for cost-effective remediation of contaminated aquifers. However, U(VI) reduction typically results in the precipitation of U(IV) particles less than 5 nanometers in diameter, except for environmental conditions enriched with iron. Because these tiny particles are mobile and susceptible to oxidative dissolution after the termination of nutrient injection, in situ bioremediation remains to be impractical. Here we show that U(IV) nanoparticles of coffinite (U(SiO4)1-x(OH)4x) formed in fracture-filling calcium carbonate in a granitic aquifer. In situ U-Pb isotope dating demonstrates that U(IV) nanoparticles have been sequestered in the calcium carbonate for at least 1 million years. As the microbiologically induced precipitation of calcium carbonate in aquifer systems worldwide is extremely common, we anticipate simultaneous stimulation of microbial activities for precipitation reactions of calcium carbonate and U(IV) nanoparticles, which leads to long-term sequestration of uranium and other radionuclides in contaminated aquifers and deep geological repositories.
238U and 235U isotope fractionation upon oxidation of uranium-bearing rocks by fracture waters
NASA Astrophysics Data System (ADS)
Chernyshev, I. V.; Golubev, V. N.; Chugaev, A. V.; Mandzhieva, G. V.
2016-10-01
The variations in 238U/235U values accompanying mobilization of U by fracture waters from uranium-bearing rocks, in which U occurs as a fine impregnation of oxides and silicates, were studied by the high-precision (±0.07‰) MC-ICP-MS method. Transition of U into the aqueous phase in the oxidized state U(VI) is accompanied by its isotope fractionation with enrichment of dissolved U(VI) in the heavy isotope 238U up to 0.32‰ in relation to the composition of the solid phases. According to the sign, this effect is consistent with the tendency of the behavior of 238U and 235U upon interaction of river waters with rocks of the catchment areas [11] and with the effect observed during oxidation of uraninite by the oxygen-bearing NaHCO3 solution [12].
Molecular Dynamics Simulation of Thermodynamic Properties in Uranium Dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wang, Xiangyu; Wu, Bin; Gao, Fei
2014-03-01
In the present study, we investigated the thermodynamic properties of uranium dioxide (UO2) by molecular dynamics (MD) simulations. As for solid UO2, the lattice parameter, density, and enthalpy obtained by MD simulations were in good agreement with existing experimental data and previous theoretical predictions. The calculated thermal conductivities matched the experiment results at the midtemperature range but were underestimated at very low and very high temperatures. The calculation results of mean square displacement represented the stability of uranium at all temperatures and the high mobility of oxygen toward 3000 K. By fitting the diffusivity constant of oxygen with the Vogel-Fulcher-Tammanmore » law, we noticed a secondary phase transition near 2006.4 K, which can be identified as a ‘‘strong’’ to ‘‘fragile’’ supercooled liquid or glass phase transition in UO2. By fitting the oxygen diffusion constant with the Arrhenius equation, activation energies of 2.0 and 2.7 eV that we obtained were fairly close to the recommended values of 2.3 to 2.6 eV. Xiangyu Wang, Bin Wu, Fei Gao, Xin Li, Xin Sun, Mohammed A. Khaleel, Ademola V. Akinlalu and Li Liu« less
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.
Drill-back studies examine fractured, heated rock
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wollenberg, H.A.; Flexser, S.; Myer, L.R.
1990-01-01
To investigate the effects of heating on the mineralogical, geochemical, and mechanical properties of rock by high-level radioactive waste, cores are being examined from holes penetrating locations where electric heaters simulated the presence of a waste canister, and from holes penetration natural hydrothermal systems. Results to date indicate the localized mobility and deposition of uranium in an open fracture in heated granitic rock, the mobility of U in a breccia zone in an active hydrothermal system in tuff, and the presence of U in relatively high concentration in fracture-lining material in tuff. Mechanical -- property studies indicate that differences inmore » compressional- and shear-wave parameters between heated and less heated rock can be attributed to differences in the density of microcracks. Emphasis has shifted from initial studies of granitic rock at Stripa, Sweden to current investigations of welded tuff at the Nevada Test Site. 7 refs., 8 figs.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Szecsody, James E.; Truex, Michael J.; Zhong, Lirong
2010-01-04
This laboratory-scale investigation is focused on decreasing mobility of uranium in subsurface contaminated sediments in the vadose zone by in situ geochemical manipulation at low water content. This geochemical manipulation of the sediment surface phases included reduction, pH change (acidic and alkaline), and additions of chemicals (phosphate, ferric iron) to form specific precipitates. Reactants were advected into 1-D columns packed with Hanford 200 area U-contaminated sediment as a reactive gas (for CO2, NH3, H2S, SO2), with a 0.1% water content mist (for NaOH, Fe(III), HCl, PO4) and with a 1% water content foam (for PO4). Uranium is present in themore » sediment in multiple phases that include (in decreasing mobility): aqueous U(VI) complexes, adsorbed U, reduced U(IV) precipitates, rind-carbonates, total carbonates, oxides, silicates, phosphates, and in vanadate minerals. Geochemical changes were evaluated in the ability to change the mixture of surface U phases to less mobile forms, as defined by a series of liquid extractions that dissolve progressively less soluble phases. Although liquid extractions provide some useful information as to the generalized uranium surface phases (and are considered operational definitions of extracted phases), positive identification (by x-ray diffraction, electron microprobe, other techniques) was also used to positively identify U phases and effects of treatment. Some of the changes in U mobility directly involve U phases, whereas other changes result in precipitate coatings on U surface phases. The long-term implication of the U surface phase changes to alter U mass mobility in the vadose zone was then investigated using simulations of 1-D infiltration and downward migration of six U phases to the water table. In terms of the short-term decrease in U mobility (in decreasing order), NH3, NaOH mist, CO2, HCl mist, and Fe(III) mist showed 20% to 35% change in U surface phases. Phosphate addition (mist or foam advected) showed inconsistent change in aqueous and adsorbed U, but significant coating (likely phosphates) on U-carbonates. The two reductive gas treatments (H2S and SO2) showed little change. For long-term decrease in U reduction, mineral phases created that had low solubility (phosphates, silicates) were desired, so NH3, phosphates (mist and foam delivered), and NaOH mist showed the greatest formation of these minerals. In addition, simulations showed the greatest decrease in U mass transport time to reach groundwater (and concentration) for these silicate/phosphate minerals. Advection of reactive gasses was the easiest to implement at the laboratory scale (and presumably field scale). Both mist and foam advection show promise and need further development, but current implementation move reactants shorter distances relative to reactive gasses. Overall, the ammonia and carbon dioxide gas had the greatest overall geochemical performance and ability to implement at field scale. Corresponding mist-delivered technologies (NaOH mist for ammonia and HCl mist for carbon dioxide) performed as well or better geochemically, but are not as easily upscaled. Phosphate delivery by mist was rated slightly higher than by foam delivery simply due to the complexity of foam injection and unknown effect of U mobility by the presence of the surfactant.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bai, Xian-Ming; Zhang, Yongfeng; Tonks, Michael R.
2015-02-01
Strong thermal gradients in low-thermal-conductivity ceramics may drive extended defects, such as grain boundaries and voids, to migrate in preferential directions. In this work, molecular dynamics simulations are conducted to study thermal gradient driven grain boundary migration and to verify a previously proposed thermal gradient driving force equation, using uranium dioxide as a model system. It is found that a thermal gradient drives grain boundaries to migrate up the gradient and the migration velocity increases under a constant gradient owing to the increase in mobility with temperature. Different grain boundaries migrate at very different rates due to their different intrinsicmore » mobilities. The extracted mobilities from the thermal gradient driven simulations are compared with those calculated from two other well-established methods and good agreement between the three different methods is found, demonstrating that the theoretical equation of the thermal gradient driving force is valid, although a correction of one input parameter should be made. The discrepancy in the grain boundary mobilities between modeling and experiments is also discussed.« less
Hinkle, S.R.; Kauffman, L.J.; Thomas, M.A.; Brown, C.J.; McCarthy, K.A.; Eberts, S.M.; Rosen, Michael R.; Katz, B.G.
2009-01-01
Flow-model particle-tracking results and geochemical data from seven study areas across the United States were analyzed using three statistical methods to test the hypothesis that these variables can successfully be used to assess public supply well vulnerability to arsenic and uranium. Principal components analysis indicated that arsenic and uranium concentrations were associated with particle-tracking variables that simulate time of travel and water fluxes through aquifer systems and also through specific redox and pH zones within aquifers. Time-of-travel variables are important because many geochemical reactions are kinetically limited, and geochemical zonation can account for different modes of mobilization and fate. Spearman correlation analysis established statistical significance for correlations of arsenic and uranium concentrations with variables derived using the particle-tracking routines. Correlations between uranium concentrations and particle-tracking variables were generally strongest for variables computed for distinct redox zones. Classification tree analysis on arsenic concentrations yielded a quantitative categorical model using time-of-travel variables and solid-phase-arsenic concentrations. The classification tree model accuracy on the learning data subset was 70%, and on the testing data subset, 79%, demonstrating one application in which particle-tracking variables can be used predictively in a quantitative screening-level assessment of public supply well vulnerability. Ground-water management actions that are based on avoidance of young ground water, reflecting the premise that young ground water is more vulnerable to anthropogenic contaminants than is old ground water, may inadvertently lead to increased vulnerability to natural contaminants due to the tendency for concentrations of many natural contaminants to increase with increasing ground-water residence time.
NASA Astrophysics Data System (ADS)
Joseph, C. N.; Waugh, W.; Glenn, E.
2015-12-01
The U.S. Department of Energy (DOE) is responsible for long-term stewardship of disposal cells for uranium mill tailings throughout the United States. Rock-armored disposal cell covers create favorable habitat for deep-rooted plants by reducing soil evaporation, increasing soil water storage, and trapping windblown dust, thereby providing water and nutrients for plant germination and establishment. DOE is studying the tradeoffs of potential detrimental and beneficial effects of plants growing on disposal cell covers to develop a rational and consistent vegetation management policy. Plant roots often extend vertically through disposal cell covers into underlying tailings, therefore, uptake of tailings contaminants and dissemination through animals foraging on stems and leaves is a possible exposure pathway. The literature shows that plant uptake of contaminants in uranium mill tailings occurs, but levels can vary widely depending on plant species, tailings and soil chemistry, and cover soil hydrology. Our empirical field study measured concentrations of uranium, radium, thorium, molybdenum, selenium, manganese, lead, and arsenic in above ground tissues harvested from plants growing on disposal cells near Native American communities in western states that represent a range of climates, cover designs, cover soil types, and vegetation types. For risk screening, contaminant levels in above ground tissues harvested from plants on disposal cells were compared to Maximum Tolerance Levels (MTLs) set for livestock by the National Research Council, and to tissue levels in the same plant species growing in reference areas near disposal cells. Although tailings were covered with uncontaminated soils, for 14 of 46 comparisons, levels of uranium and other contaminants were higher in plants growing on disposal cells compared to reference area plants, indicating possible mobilization of these elements from the tailing into plant tissues. However, with one exception, all plant levels were well below MTLs. Selenium, the only element that exceeded its MTL, likely originated in local seleniferous soil found both at reference areas and in disposal cell covers, and not in the underlying tailings. Our screening risk assessment suggests that allowing plants to grow on disposal cells appears to be safe.
NASA Astrophysics Data System (ADS)
Uvarova, Yulia A.; Kyser, T. Kurt; Geagea, Majdi Lahd; Chipley, Don
2014-12-01
Variations in 238U/235U and 234U/238U ratios were measured in uranium minerals from a spectrum of uranium deposit types, as well as diagenetic phosphates in uranium-rich basins and peraluminous rhyolites and associated autunite mineralisation from Macusani Meseta, Peru. Mean δ238U values of uranium minerals relative to NBL CRM 112-A are 0.02‰ for metasomatic deposits, 0.16‰ for intrusive, 0.18‰ for calcrete, 0.18‰ for volcanic, 0.29‰ for quartz-pebble conglomerate, 0.29‰ for sandstone-hosted, 0.44‰ for unconformity-type, and 0.56‰ for vein, with a total range in δ238U values from -0.30‰ to 1.52‰. Uranium mineralisation associated with igneous systems, including low-temperature calcretes that are sourced from U-rich minerals in igneous systems, have low δ238U values of ca. 0.1‰, near those of their igneous sources, whereas uranium minerals in basin-hosted deposits have higher and more variable values. High-grade unconformity-related deposits have δ238U values around 0.2‰, whereas lower grade unconformity-type deposits in the Athabasca, Kombolgie and Otish basins have higher δ238U values. The δ234U values for most samples are around 0‰, in secular equilibrium, but some samples have δ234U values much lower or higher than 0‰ associated with addition or removal of 234U during the past 2.5 Ma. These δ238U and δ234U values suggest that there are at least two different mechanisms responsible for 238U/235U and 234U/238U variations. The 234U/238U disequilibria ratios indicate recent fluid interaction with the uranium minerals and preferential migration of 234U. Fractionation between 235U and 238U is a result of nuclear-field effects with enrichment of 238U in the reduced insoluble species (mostly UO2) and 235U in oxidised mobile species as uranyl ion, UO22+, and its complexes. Therefore, isotopic fractionation effects should be reflected in 238U/235U ratios in uranium ore minerals formed either by reduction of uranium to UO2 or chemical precipitation in the form of U6+ minerals. The δ238U values of uranium ore minerals from a variety of deposits are controlled by the isotopic signature of the uranium source, the efficiency of uranium reduction in the case of UO2 systems, and the degree to which uranium was previously removed from the fluid, with less influence from temperature of ore formation and later alteration of the ore. Uranium isotopes are potentially superb tracers of redox in natural systems.
Impact of homogeneous strain on uranium vacancy diffusion in uranium dioxide
Goyal, Anuj; Phillpot, Simon R.; Subramanian, Gopinath; ...
2015-03-03
We present a detailed mechanism of, and the effect of homogeneous strains on, the migration of uranium vacancies in UO 2. Vacancy migration pathways and barriers are identified using density functional theory and the effect of uniform strain fields are accounted for using the dipole tensor approach. We report complex migration pathways and noncubic symmetry associated with the uranium vacancy in UO 2 and show that these complexities need to be carefully accounted for to predict the correct diffusion behavior of uranium vacancies. We show that under homogeneous strain fields, only the dipole tensor of the saddle with respect tomore » the minimum is required to correctly predict the change in the energy barrier between the strained and the unstrained case. Diffusivities are computed using kinetic Monte Carlo simulations for both neutral and fully charged state of uranium single and divacancies. We calculate the effect of strain on migration barriers in the temperature range 800–1800 K for both vacancy types. Homogeneous strains as small as 2% have a considerable effect on diffusivity of both single and divacancies of uranium, with the effect of strain being more pronounced for single vacancies than divacancies. In contrast, the response of a given defect to strain is less sensitive to changes in the charge state of the defect. Further, strain leads to anisotropies in the mobility of the vacancy and the degree of anisotropy is very sensitive to the nature of the applied strain field for strain of equal magnitude. Our results indicate that the influence of strain on vacancy diffusivity will be significantly greater when single vacancies dominate the defect structure, such as sintering, while the effects will be much less substantial under irradiation conditions where divacancies dominate.« less
Modeling the effectiveness of U(VI) biomineralization in dual-porosity porous media
NASA Astrophysics Data System (ADS)
Rotter, B. E.; Barry, D. A.; Gerhard, J. I.; Small, J. S.
2011-05-01
SummaryUranium contamination is a serious environmental concern worldwide. Recent attention has focused on the in situ immobilization of uranium by stimulation of dissimilatory metal-reducing bacteria (DMRB). The objective of this work was to investigate the effectiveness of this approach in heterogeneous and structured porous media, since such media may significantly affect the geochemical and microbial processes taking place in contaminated sites, impacting remediation efficiency during biostimulation. A biogeochemical reactive transport model was developed for uranium remediation by immobile-region-resident DMRB in two-region porous media. Simulations were used to investigate the parameter sensitivities of the system over wide-ranging geochemical, microbial and groundwater transport conditions. The results suggest that optimal biomineralization is generally likely to occur when the regional mass transfer timescale is less than one-thirtieth the value of the volumetric flux timescale, and/or the organic carbon fermentation timescale is less than one-thirtieth the value of the advective timescale, and/or the mobile region porosity ranges between equal to and four times the immobile region porosity. Simulations including U(VI) surface complexation to Fe oxides additionally suggest that, while systems exhibiting U(VI) surface complexation may be successfully remediated, they are likely to display different degrees of remediation efficiency over varying microbial efficiency, mobile-immobile mass transfer, and porosity ratios. Such information may aid experimental and field designs, allowing for optimized remediation in dual-porosity (two-region) biostimulated DMRB U(VI) remediation schemes.
Determination of the oxidation states of metals and metalloids: An analytical review
NASA Astrophysics Data System (ADS)
Vodyanitskii, Yu. N.
2013-12-01
The hazard of many heavy metals/metalloids in the soil depends on their oxidation state. The problem of determining the oxidation state has been solved due to the use of synchrotron radiation methods with the analysis of the X-ray absorption near-edge structure (XANES). The determination of the oxidation state is of special importance for some hazardous heavy elements (arsenic, antimony, selenium, chromium, uranium, and vanadium). The mobility and hazard of each of these elements depend on its oxidation state. The mobilities are higher at lower oxidation states of As, Cr, V, and Se and at higher oxidation states of Sb and U. The determination of the oxidation state of arsenic has allowed revealing its fixation features in the rhizosphere of hydrophytes. The known oxidation states of chromium and uranium are used for the retention of these elements on geochemical barriers. Different oxidation states have been established for vanadium displacing iron in goethite. The determination of the oxidation state of manganese in the rhizosphere and the photosynthetic apparatus of plants is of special importance for agricultural chemists.
NASA Astrophysics Data System (ADS)
Prikryl, James D.; Pickett, David A.; Murphy, William M.; Pearcy, English C.
1997-04-01
Oxidation of pyrite at the Nopal I uranium deposit, Peña Blanca district, Chihuahua, Mexico has resulted in the formation of Fe-oxides/hydroxides. Anomalous U concentrations (i.e. several hundred to several thousand ppm) measured in goethite, hematite, and amorphous Fe-oxyhydroxides in a major fracture that crosscuts the deposit and the absence of U minerals in the fracture suggest that U was retained during secondary mineral growth or sorbed on mineral surfaces. Mobilization and transport of U away from the deposit is suggested by decreasing U concentrations in fracture-infilling materials and in goethite and hematite with distance from the deposit. Greater than unity {234U}/{238U} activity ratios measured in fracture-infilling materials indicate relatively recent ( < 1 Ma) U uptake from fluids that carried excess 234U. Systematic decreases in {234U}/{238U} activity ratios of fracture materials with distance from the deposit suggest a multistage mobilization process, such as remobilization of U from 234U-enriched infill minerals or differential or diminished transport of U-bearing solutions containing excess 234U.
Use of an ion mobility spectrometer for detecting uranium compounds
DOE Office of Scientific and Technical Information (OSTI.GOV)
McLain, Derek R.; Steeb, Jennifer L.; Smith, Nicholas A.
The safeguards community currently lacks a method to rapidly determine the chemical form of radioactive and non-radioactive compounds in real time during inspection activities. Chemical speciation identification can provide important information on both the types of materials that are collected during environmental sampling and can inform inspectors as to where to focus efforts during inspections or complementary access visits. Ion Mobility Spectrometry (IMS) is an established field technique for the detection of explosives, narcotics, and other organic compounds. More recently, electrospray ionization (ESI) has been used to introduce inorganic compounds to IMS instruments for analysis. These techniques have shown themore » ability to supply chemical information about the compounds being analyzed. Although these laboratory based instruments use a liquid-based injection system, there is evidence in the literature of unaltered and intact pharmaceutical tablets being volatilized and ionized in open atmosphere using heat and a Ni-63 source. Lastly, this work determined that a commercial-off-the-shelf (COTS) IMS could be used for the identification of solid uranium compounds directly after sampling using a COTS sample swipe.« less
Use of an ion mobility spectrometer for detecting uranium compounds
McLain, Derek R.; Steeb, Jennifer L.; Smith, Nicholas A.
2018-03-09
The safeguards community currently lacks a method to rapidly determine the chemical form of radioactive and non-radioactive compounds in real time during inspection activities. Chemical speciation identification can provide important information on both the types of materials that are collected during environmental sampling and can inform inspectors as to where to focus efforts during inspections or complementary access visits. Ion Mobility Spectrometry (IMS) is an established field technique for the detection of explosives, narcotics, and other organic compounds. More recently, electrospray ionization (ESI) has been used to introduce inorganic compounds to IMS instruments for analysis. These techniques have shown themore » ability to supply chemical information about the compounds being analyzed. Although these laboratory based instruments use a liquid-based injection system, there is evidence in the literature of unaltered and intact pharmaceutical tablets being volatilized and ionized in open atmosphere using heat and a Ni-63 source. Lastly, this work determined that a commercial-off-the-shelf (COTS) IMS could be used for the identification of solid uranium compounds directly after sampling using a COTS sample swipe.« less
XANES and EXAFS investigation of uranium incorporation on nZVI in the presence of phosphate.
Qiu, Muqing; Wang, Min; Zhao, Qingzhou; Hu, Baowei; Zhu, Yuling
2018-06-01
Effect of phosphate on the reduction of U(VI) on nZVI was determined by batch, XPS, XANES and EXAFS techniques. The batch experiments showed that nZVI was quite effective for the removal of uranium under the anaerobic conditions, whereas the addition of phosphate enhanced uranium removal over wide pH range. At low pH, the reduction of U(VI) to U(IV) significantly decreased with increasing phosphate concentration by XPS and XANES analysis. According to EXAFS analysis, the occurrence of UU shell at 10 mg/L phosphate and pH 4.0 was similar to that of U (IV) O 2 (s), whereas the UP and UFe shells were observed at 50 mg/L phosphate, revealing that reductive co-precipitate (U (IV) O 2 (s)) and precipitation of uranyl-phosphate were observed at low and high phosphate, respectively. The findings are crucial for the prediction of the effect of phosphate on the speciation and binding of uranium by nZVI at low pH, which is significant in controlling the mobility of U(VI) in contaminated environments. Copyright © 2018 Elsevier Ltd. All rights reserved.
Factoring uncertainty into restoration modeling of in-situ leach uranium mines
Johnson, Raymond H.; Friedel, Michael J.
2009-01-01
Postmining restoration is one of the greatest concerns for uranium in-situ leach (ISL) mining operations. The ISL-affected aquifer needs to be returned to conditions specified in the mining permit (either premining or other specified conditions). When uranium ISL operations are completed, postmining restoration is usually achieved by injecting reducing agents into the mined zone. The objective of this process is to restore the aquifer to premining conditions by reducing the solubility of uranium and other metals in the ground water. Reactive transport modeling is a potentially useful method for simulating the effectiveness of proposed restoration techniques. While reactive transport models can be useful, they are a simplification of reality that introduces uncertainty through the model conceptualization, parameterization, and calibration processes. For this reason, quantifying the uncertainty in simulated temporal and spatial hydrogeochemistry is important for postremedial risk evaluation of metal concentrations and mobility. Quantifying the range of uncertainty in key predictions (such as uranium concentrations at a specific location) can be achieved using forward Monte Carlo or other inverse modeling techniques (trial-and-error parameter sensitivity, calibration constrained Monte Carlo). These techniques provide simulated values of metal concentrations at specified locations that can be presented as nonlinear uncertainty limits or probability density functions. Decisionmakers can use these results to better evaluate environmental risk as future metal concentrations with a limited range of possibilities, based on a scientific evaluation of uncertainty.
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
Summary of Uranium Solubility Studies in Concrete Waste Forms and Vadose Zone Environments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Golovich, Elizabeth C.; Wellman, Dawn M.; Serne, R. Jeffrey
2011-09-30
One of the methods being considered for safely disposing of Category 3 low-level radioactive wastes is to encase the waste in concrete. Concrete encasement would contain and isolate the waste packages from the hydrologic environment and act as an intrusion barrier. The current plan for waste isolation consists of stacking low-level waste packages on a trench floor, surrounding the stacks with reinforced steel, and encasing these packages in concrete. These concrete-encased waste stacks are expected to vary in size with maximum dimensions of 6.4 m long, 2.7 m wide, and 4 m high. The waste stacks are expected to havemore » a surrounding minimum thickness of 15 cm of concrete encasement. These concrete-encased waste packages are expected to withstand environmental exposure (solar radiation, temperature variations, and precipitation) until an interim soil cover or permanent closure cover is installed and to remain largely intact thereafter. Any failure of concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. This report presents the results of investigations elucidating the uranium mineral phases controlling the long-term fate of uranium within concrete waste forms and the solubility of these phases in concrete pore waters and alkaline, circum-neutral vadose zone environments.« less
Microbial biogeochemistry of uranium mill tailings
Landa, Edward R.
2005-01-01
Uranium mill tailings (UMT) are the crushed ore residues from the extraction of uranium (U) from ores. Among the radioactive wastes associated with the nuclear fuel cycle, UMT are unique in terms of their volume and their limited isolation from the surficial environment. For this latter reason, their management and long-term fate has many interfaces with environmental microbial communities and processes. The interactions of microorganisms with UMT have been shown to be diverse and with significant consequences for radionuclide mobility and bioremediation. These radionuclides are associated with the U-decay series. The addition of organic carbon and phosphate is required to initiate the reduction of the U present in the groundwater down gradient of the mills. Investigations on sediment and water from the U-contaminated aquifer, indicates that the addition of a carbon source stimulates the rate of U removal by microbial reduction. Moreover, most attention with respect to passive or engineered removal of U from groundwaters focuses on iron-reducing and sulfate-reducing bacteria.
Uranium (VI) exhibits little adsorption onto sediment minerals in acidic, alkaline or high ionic-strength aqueous media that often occur in U mining or contaminated sites, which makes U(VI) very mobile and difficult to sequester. In this work, magnetic mesoporous silica nanoparti...
Reitz, Thomas; Rossberg, Andre; Barkleit, Astrid; Selenska-Pobell, Sonja; Merroun, Mohamed L.
2014-01-01
Interactions of a facultative anaerobic bacterial isolate named Paenibacillus sp. JG-TB8 with U(VI) were studied under oxic and anoxic conditions in order to assess the influence of the oxygen-dependent cell metabolism on microbial uranium mobilization and immobilization. We demonstrated that aerobically and anaerobically grown cells of Paenibacillus sp. JG-TB8 accumulate uranium from aqueous solutions under acidic conditions (pH 2 to 6), under oxic and anoxic conditions. A combination of spectroscopic and microscopic methods revealed that the speciation of U(VI) associated with the cells of the strain depend on the pH as well as on the aeration conditions. At pH 2 and pH 3, uranium was exclusively bound by organic phosphate groups provided by cellular components, independently on the aeration conditions. At higher pH values, a part (pH 4.5) or the total amount (pH 6) of the dissolved uranium was precipitated under oxic conditions in a meta-autunite-like uranyl phosphate mineral phase without supplying an additional organic phosphate substrate. In contrast to that, under anoxic conditions no mineral formation was observed at pH 4.5 and pH 6, which was clearly assigned to decreased orthophosphate release by the cells. This in turn was caused by a suppression of the indigenous phosphatase activity of the strain. The results demonstrate that changes in the metabolism of facultative anaerobic microorganisms caused by the presence or absence of oxygen can decisively influence U(VI) biomineralization. PMID:25157416
Radiation attenuation on labyrinth design bunker using Iridium-192 source
NASA Astrophysics Data System (ADS)
Ismail, Mohamad Pauzi bin; Sani, Suhairy bin; Masenwat, Noor Azreen bin; Mohd, Shukri; Sayuti, Shaharudin; Ahmad, Mohamad Ridzuan Bin; Mahmud, Mohamad Haniza bin; Isa, Nasharuddin bin
2017-01-01
Gamma rays are better absorbed by materials with high atomic numbers and high density. Steel, lead, depleted uranium, concrete, water or sand can be used as gamma shielding. Lead and steel are normally used for making doors of the bunker and to reduce radiation scatter. Depleted uranium is used for gamma container. Water is used in nuclear reactor as neutron and gamma absorber. Sand is used for mobile hot cell. However concrete is the most common and cheap material for gamma radiation bunker. In this research, concrete made from hematite aggregates was used to make chevron blocks for a temporary construction of labyrinth bunker. This paper explains and discusses the gamma attenuation around labyrinth bunker with concrete containing hematite aggregates.
Spectroscopic confirmation of uranium(VI)-carbonato adsorption complexes on hematite
Bargar, John R.; Reitmeyer, Rebecca; Davis, James A.
1999-01-01
Evaluating societal risks posed by uranium contamination from waste management facilities, mining sites, and heavy industry requires knowledge about uranium transport in groundwater, often the most significant pathway of exposure to humans. It has been proposed that uranium mobility in aquifers may be controlled by adsorption of U(VI)−carbonato complexes on oxide minerals. The existence of such complexes has not been demonstrated, and little is known about their compositions and reaction stoichiometries. We have used attenuated total reflectance Fourier transform infrared (ATR-FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopies to probe the existence, structures, and compositions of ≡FeOsurface−U(VI)−carbonato complexes on hematite throughout the pH range of uranyl uptake under conditions relevant to aquifers. U(VI)−carbonato complexes were found to be the predominant adsorbed U(VI) species at all pH values examined, a much wider pH range than previously postulated based on analogy to aqueous U(VI)−carbonato complexes, which are trace constituents at pH < 6. This result indicates the inadequacy of the common modeling assumption that the compositions and predominance of adsorbed species can be inferred from aqueous species. By extension, adsorbed carbonato complexes may be of major importance to the groundwater transport of similar actinide contaminants such as neptunium and plutonium.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Truex, Michael J.; Szecsody, James E.; Zhong, Lirong
Uranium is present in the vadose zone at the Hanford Central Plateau and is of concern for protection of groundwater. The Deep Vadose Zone Treatability Test Plan for the Hanford Central Plateau identified gas-phase treatment and geochemical manipulation as potentially effective treatment approaches for uranium and technetium in the Hanford Central Plateau vadose zone. Based on laboratory evaluation, use of ammonia vapor was selected as the most promising uranium treatment candidate for further development and field testing. While laboratory tests have shown that ammonia treatment effectively reduces the mobility of uranium, additional information is needed to enable deployment of thismore » technology for remediation. Of importance for field applications are aspects of the technology associated with effective distribution of ammonia to a targeted treatment zone, understanding the fate of injected ammonia and its impact on subsurface conditions, and identifying effective monitoring approaches. In addition, information is needed to select equipment and operational parameters for a field design. As part of development efforts for the ammonia technology for remediation of vadose zone uranium contamination, field scale-up issues were identified and have been addressed through a series of laboratory and modeling efforts. This report presents a conceptual description for field application of the ammonia treatment process, engineering calculations to support treatment design, ammonia transport information, field application monitoring approaches, and a discussion of processes affecting the fate of ammonia in the subsurface. The report compiles this information from previous publications and from recent research and development activities. The intent of this report is to provide technical information about these scale-up elements to support the design and operation of a field test for the ammonia treatment technology.« less
NASA Astrophysics Data System (ADS)
Schaller, Jörg; Planer-Friedrich, Britta
2017-04-01
Organic sediments in aquatic ecosystems are well known sinks for nutrients, silicon, and metal(loid)s. Organic matter-decomposing organisms like invertebrate shredders, grazers, bioturbators, and filter feeder are key-species for the carbon and energy turnover within the decomposer community. We could show that invertebrate shredders and grazer affect element fixation or remobilization by changing binding properties of organic sediments and the attached biofilm. Bioturbators affect element fixation or remobilization by changing redox conditions within the uppermost sediment layer. Last but not least filter feeders, like the zebra mussel Dreissena polymorpha, an invasive organism in North American and European freshwater ecosystems significantly contributed to element mobilization of silicon, iron, phosphorus, arsenic, and copper and to immobilization of uranium (p<0.001), probably driven by redox conditions, microbial activity within the gut system, or active control of element homeostasis. Except of the filter feeder D. polymorpha, the invertebrates are able to minimize the accumulation of non-nutrient elements due to specific strategies, which is an important strategy for species living in systems tending to element accumulation. However, D. polymorpha revealed a significant uptake and accumulation of arsenic, copper, iron, and especially uranium both into the soft body tissues and the seashell. This accumulation by D. polymorpha is in line with previous observations of metal(loid) accumulation from biomonitoring studies. In summary, higher trophic level strongly contributes to element fixation or remobilization in aquatic systems.
Microbial Metabolic Response to Carbon Sources in a Uranium Contaminated Floodplain
NASA Astrophysics Data System (ADS)
Barragan, L.; Boye, K.; Bargar, J.; Fendorf, S. E.
2016-12-01
In Riverton, Wyoming, uranium (U) from a former ore processing plant, contaminated the groundwater and accumulated in Naturally Reduced Zones (NRZs). The NRZs have now become a secondary source of U and are releasing U into the ground water due to seasonal water table fluctuations. Microorganisms that mediate the mobilization and retention of U are likely to reside in these zones enriched with organic matter that comprises their energy source of carbon (C) for respiration. In this study, we are measuring microbial respiration (basal and substrate induced) by the MicroRespTM system, which is a quick screening method for respiratory activity in natural samples. This can provide information about the microbial community composition at certain depths and insight into their metabolic pathways which may explain U behavior in the ground water. In addition, we are determining elemental composition in the sediments by X-ray fluorescence spectroscopy (XRF) and elemental analysis (EA). Water soluble cations, anions and organic C is determined by inductively coupled plasma (ICP), mass spectrometry, ion chromatography (IC) and non-purgeable organic carbon (NPOC) analyses, respectively. If the behavior of the microbial community in the NRZ environment (enriched in both U and C) differs from that in unsaturated sediments, this can provide crucial clues to understand what causes U to be retained or released from the NRZs. This information will be used to develop and improve models aimed at predicting U mobility in the floodplain groundwater systems.
Seasonal Hydrologic Controls on Uranium and Iron Biogeochemistry in a Riparian Aquifer
NASA Astrophysics Data System (ADS)
Wilkins, M.; Williams, K. H.; Danczak, R. E.; Yabusaki, S.; Fang, Y.; Hobson, C.
2015-12-01
The maintenance of geochemically reducing conditions is generally optimal for the formation and preservation of reduced metals and mineral phases that can limit contaminant fate and transport. At a riparian aquifer near Rifle, CO, we tracked over six months the biogeochemical response within the aquifer to an annual pulse of dissolved oxygen (DO) that results from snowmelt-driven changes in Colorado River stage. In reduced portions of the aquifer (naturally reduced zones; NRZs) the re-oxidation of abundant iron sulfide minerals was the dominant oxygen-consuming process, and resulted in little DO intrusion into the deeper aquifer. In less reduced areas, DO intruded through the entire vertical profile of the aquifer. Across both regions, these perturbations resulted in changes to the microbial community structure, and aqueous metal pools. Two potentially different mechanisms of uranium mobilization were observed; (1) re-oxidation of reduced U(IV) phases in response to DO intrusion, and (2) mobilization of U(VI) from the vadose zone during water table rise. This high-resolution, long-term monitoring of aquifer biogeochemistry at the Rifle site has revealed dynamic microbial and geochemical responses to predictable, annual hydrologic perturbations, and offers an opportunity to further refine modeling approaches for such regions.
Laser-Assisted Atom Probe Tomography of Deformed Minerals: A Zircon Case Study.
La Fontaine, Alexandre; Piazolo, Sandra; Trimby, Patrick; Yang, Limei; Cairney, Julie M
2017-04-01
The application of atom probe tomography to the study of minerals is a rapidly growing area. Picosecond-pulsed, ultraviolet laser (UV-355 nm) assisted atom probe tomography has been used to analyze trace element mobility within dislocations and low-angle boundaries in plastically deformed specimens of the nonconductive mineral zircon (ZrSiO4), a key material to date the earth's geological events. Here we discuss important experimental aspects inherent in the atom probe tomography investigation of this important mineral, providing insights into the challenges in atom probe tomography characterization of minerals as a whole. We studied the influence of atom probe tomography analysis parameters on features of the mass spectra, such as the thermal tail, as well as the overall data quality. Three zircon samples with different uranium and lead content were analyzed, and particular attention was paid to ion identification in the mass spectra and detection limits of the key trace elements, lead and uranium. We also discuss the correlative use of electron backscattered diffraction in a scanning electron microscope to map the deformation in the zircon grains, and the combined use of transmission Kikuchi diffraction and focused ion beam sample preparation to assist preparation of the final atom probe tip.
Jurgens, Bryant C.; Burow, Karen R.; Dalgish, Barbara A.; Shelton, Jennifer L.
2008-01-01
Ground-water chemistry in the zone of contribution of a public-supply well in Modesto, California, was studied by the U.S. Geological Survey National Water Quality Assessment (NAWQA) Program's topical team for Transport of Anthropogenic and Natural Contaminants (TANC) to supply wells. Twenty-three monitoring wells were installed in Modesto to record baseline hydraulic information and to collect water-quality samples. The monitoring wells were divided into four categories that represent the chemistry of different depths and volumes of the aquifer: (1) water-table wells were screened between 8.5 and 11.7 m (meter) (28 and 38.5 ft [foot]) below land surface (bls) and were within 5 m (16 ft) of the water table; (2) shallow wells were screened between 29 and 35 m (95 and 115 ft) bls; (3) intermediate wells were screened between 50.6 and 65.5 m (166 and 215 ft) bls; and (4) deep wells are screened between 100 to 106 m (328 and 348 ft) bls. Inorganic, organic, isotope, and age-dating tracers were used to characterize the geochemical conditions in the aquifer and understand the mechanisms of mobilization and movement of selected constituents from source areas to a public-supply well. The ground-water system within the study area has been significantly altered by human activities. Water levels in monitoring wells indicated that horizontal movement of ground water was generally from the agricultural areas in the northeast towards a regional water-level depression within the city in the southwest. However, intensive pumping and irrigation recharge in the study area has caused large quantities of ground water to move vertically downward within the regional and local flow systems. Analysis of age tracers indicated that ground-water age varied from recent recharge at the water table to more than 1,000 years in the deep part of the aquifer. The mean age of shallow ground water was determined to be between 30 and 40 years. Intermediate ground water was determined to be a mixture of modern (Post-1950) and old (Pre-1950) ground water. As a result, concentrations of age tracers were detectable but diluted by older ground water. Deep ground water generally represented water that was recharged under natural conditions and therefore had much older ages. Ground water reaching the public-supply well was a mixture of older intermediate and deep ground water and young shallow ground water that has been anthropogenically-influenced to a greater extent than intermediate ground water. Uranium and nitrate pose the most significant threat to the quality of water discharged from the public-supply well. Although pesticides and VOCs were present in ground water from the public-supply well and monitoring wells, currently concentrations of these contaminants are generally less than one-hundredth the concentration of drinking water standards. In contrast, both uranium and nitrate were above half the concentration of drinking water standards for public-supply well samples, and were above drinking water standards for several water-table and shallow monitoring wells. Shallow ground water contributes roughly 20 percent of the total flow to the public-supply well and was the entry point of most contaminants reaching the public-supply well. Naturally-occurring uranium, which is commonly adsorbed to aquifer sediments, was mobilized by oxygen-rich, high-alkalinity water, causing concentrations in some monitoring wells to be above the drinking-water standard of 30 ug/L (microgram per liter). Adsorption experiments, sediment extractions, and uranium isotopes indicated uranium in water-table and shallow ground water was leached from aquifer sediments. Uranium is strongly correlated to bicarbonate concentrations (as measured by alkalinity) in ground water. Bicarbonate can effectively limit uranium adsorption to sediments. As a result, continued downward movement of high-alkalinity, oxygen-rich ground water will likely lead to larger portions of the aquifer having
Uranium(IV) adsorption by natural organic matter in anoxic sediments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bone, Sharon E.; Dynes, James J.; Cliff, John
Uranium is an important carbon-free fuel source and environmental contaminant that accumulates in the tetravalent state, U(IV), in anoxic sediments, such as ore deposits, marine basins, and contaminated aquifers. However, little is known about the speciation of U(IV) in low-temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2+x) in anoxic sediments; however, studies now show that this is not often the case. Yet a model of U(IV) speciation in the absence of mineral formation under field-relevant conditions has not yetmore » been developed. Uranium(IV) speciation controls its reactivity, particularly its susceptibility to oxidative mobilization, impacting its distribution and toxicity. Here we show adsorption to organic carbon and organic carbon-coated clays dominate U(IV) speciation in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that U(IV) speciation is dictated by the mode of reduction (i.e., whether reduction is mediated by microbes or by inorganic reductants), our results demonstrate that mineral formation can be diminished in favor of adsorption, regardless of reduction pathway. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider U(IV) adsorption to organic matter within the sediment environment.« less
Uranium(IV) adsorption by natural organic matter in anoxic sediments
Bone, Sharon E.; Dynes, James J.; Cliff, John; ...
2017-01-09
Uranium is an important carbon-free fuel source and environmental contaminant that accumulates in the tetravalent state, U(IV), in anoxic sediments, such as ore deposits, marine basins, and contaminated aquifers. However, little is known about the speciation of U(IV) in low-temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2+x) in anoxic sediments; however, studies now show that this is not often the case. Yet a model of U(IV) speciation in the absence of mineral formation under field-relevant conditions has not yetmore » been developed. Uranium(IV) speciation controls its reactivity, particularly its susceptibility to oxidative mobilization, impacting its distribution and toxicity. Here we show adsorption to organic carbon and organic carbon-coated clays dominate U(IV) speciation in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that U(IV) speciation is dictated by the mode of reduction (i.e., whether reduction is mediated by microbes or by inorganic reductants), our results demonstrate that mineral formation can be diminished in favor of adsorption, regardless of reduction pathway. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider U(IV) adsorption to organic matter within the sediment environment.« less
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
Linking Chaotic Advection with Subsurface Biogeochemical Processes
NASA Astrophysics Data System (ADS)
Mays, D. C.; Freedman, V. L.; White, S. K.; Fang, Y.; Neupauer, R.
2017-12-01
This work investigates the extent to which groundwater flow kinematics drive subsurface biogeochemical processes. In terms of groundwater flow kinematics, we consider chaotic advection, whose essential ingredient is stretching and folding of plumes. Chaotic advection is appealing within the context of groundwater remediation because it has been shown to optimize plume spreading in the laminar flows characteristic of aquifers. In terms of subsurface biogeochemical processes, we consider an existing model for microbially-mediated reduction of relatively mobile uranium(VI) to relatively immobile uranium(IV) following injection of acetate into a floodplain aquifer beneath a former uranium mill in Rifle, Colorado. This model has been implemented in the reactive transport code eSTOMP, the massively parallel version of STOMP (Subsurface Transport Over Multiple Phases). This presentation will report preliminary numerical simulations in which the hydraulic boundary conditions in the eSTOMP model are manipulated to simulate chaotic advection resulting from engineered injection and extraction of water through a manifold of wells surrounding the plume of injected acetate. This approach provides an avenue to simulate the impact of chaotic advection within the existing framework of the eSTOMP code.
Refining the site conceptual model at a former uranium mill site in Riverton, Wyoming, USA
Dam, William; Campbell, Sam; Johnson, Ray; ...
2015-07-07
Milling activities at a former uranium mill site near Riverton, Wyoming, USA, contaminated the shallow groundwater beneath and downgradient of the site. Although the mill operated for <6 years (1958-1963), its impact remains an environmental liability. Groundwater modeling predicted that contaminant concentrations were declining steadily, which confirmed the conceptual site model (CSM). However, local flooding in 2010 mobilized contaminants that migrated downgradient from the Riverton site and resulted in a dramatic increase in groundwater contaminant concentrations. This observation indicated that the original CSM was inadequate to explain site conditions and needed to be refined. In response to the new observationsmore » after the flood, a collaborative investigation to better understand site conditions and processes commenced. This investigation included installing 103 boreholes to collect soil and groundwater samples, sampling and analysis of evaporite minerals along the bank of the Little Wind River, an analysis of evaportranspiration in the shallow aquifer, and sampling naturally organic-rich sediments near groundwater discharge areas. The enhanced characterization revealed that the existing CSM did not account for high uranium concentrations in groundwater remaining on the former mill site and groundwater plume stagnation near the Little Wind River. Observations from the flood and subsequent investigations indicate that additional characterization is still needed to continue refining the CSM and determine the viability of the natural flushing compliance strategy. Additional sampling, analysis, and testing of soil and groundwater are necessary to investigate secondary contaminant sources, mobilization of contaminants during floods, geochemical processes, contaminant plume stagnation, distribution of evaporite minerals and organic-rich sediments, and mechanisms and rates of contaminant transfer from soil to groundwater. Future data collection will be used to continually revise the CSM and evaluate the compliance strategy at the site.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Methe, Barbara; Lipton, Mary; Mahadevan, Krishna
Microbes exist in communities in the environment where they are fundamental drivers of global carbon, nutrient and metal cycles. In subsurface environments, they possess significant metabolic potential to affect these global cycles including the transformation of radionuclides. This study examined the influence of microbial communities in sediment zones undergoing biogeochemical cycling of carbon, nutrients and metals including natural attenuation of uranium. This study examined the relationship of both the microbiota (taxonomy) and their metabolic capacity (function) in driving carbon, nutrient and metal cycles including uranium reduction at the Department of Energy (DOE) Rifle Integrated Field Research Challenge (RIFRC). Objectives ofmore » this project were: 1) to apply systems-level biology through application of ‘metaomics’ approaches (collective analyses of whole microbial community DNA, RNA and protein) to the study of microbial environmental processes and their relationship to C, N and metals including the influence of microbial communities on uranium contaminant mobility in subsurface settings undergoing natural attenuation, 2) improve methodologies for data generation using metaomics (collectively metagenomics, metatranscriptomics and proteomics) technologies and analysis and interpretation of that data and 3) use the data generated from these studies towards microbial community-scale metabolic modeling. The strategy for examining these subsurface microbial communities was to generate sequence reads from microbial community DNA (metagenomics or whole genome shotgun sequencing (WGS)) and RNA (metatranscriptomcs or RNAseq) and protein information using proteomics. Results were analyzed independently and through computational modeling. Overall, the community model generated information on the microbial community structure that was observed using metaomic approaches at RIFRC sites and thus provides an important framework for continued community modeling development. The model as created is capable of predicting the response of the community structure in changing environments such as anoxic/oxic conditions or limitations by carbon or nutrients. The ability to more accurately model these responses is critical to understanding carbon and energy flows in an ecosystem is critical towards improving our ability to make predictions that can be used to design more efficient remediation and management strategies, and better understand the implications of environmental perturbations on these ecosystems.« less
NASA Astrophysics Data System (ADS)
Cardarelli, E.; Bargar, J.; Williams, K. H.; Dam, W. L.; Francis, C.
2015-12-01
Throughout the Colorado River Basin (CRB), uranium (U) persists as a relic contaminant of former ore processing activities. Elevated solid-phase U levels exist in fine-grained, naturally-reduced zone (NRZ) sediments intermittently found within the subsurface floodplain alluvium of the following Department of Energy-Legacy Management sites: Rifle, CO; Naturita, CO; and Grand Junction, CO. Coupled with groundwater fluctuations that alter the subsurface redox conditions, previous evidence from Rifle, CO suggests this resupply of U may be controlled by microbially-produced nitrite and nitrate. Nitrification, the two-step process of archaeal and bacterial ammonia-oxidation followed by bacterial nitrite oxidation, generates nitrate under oxic conditions. Our hypothesis is that when elevated groundwater levels recede and the subsurface system becomes anoxic, the nitrate diffuses into the reduced interiors of the NRZ and stimulates denitrification, the stepwise anaerobic reduction of nitrate/nitrite to dinitrogen gas. Denitrification may then be coupled to the oxidation of sediment-bound U(IV) forming mobile U(VI), allowing it to resupply U into local groundwater supplies. A key step in substantiating this hypothesis is to demonstrate the presence of nitrogen-cycling organisms in U-contaminated, NRZ sediments from the upper CRB. Here we investigate how the diversity and abundances of nitrifying and denitrifying microbial populations change throughout the NRZs of the subsurface by using functional gene markers for ammonia-oxidation (amoA, encoding the α-subunit of ammonia monooxygenase) and denitrification (nirK, nirS, encoding nitrite reductase). Microbial diversity has been assessed via clone libraries, while abundances have been determined through quantitative polymerase chain reaction (qPCR), elucidating how relative numbers of nitrifiers (amoA) and denitrifiers (nirK, nirS) vary with depth, vary with location, and relate to uranium release within NRZs in sediment cores spanning the upper CRB. Early findings from Rifle, CO indicate elevated abundances of ammonia-oxidizers seem to correlate with elevated uranium concentrations emphasizing the critical need to understand how nitrogen-cycling organisms influence subsurface U redox chemistry and mobility.
Bao, Chen; Wu, Hongfei; Li, Li; Newcomer, Darrell; Long, Philip E; Williams, Kenneth H
2014-09-02
We aim to understand the scale-dependent evolution of uranium bioreduction during a field experiment at a former uranium mill site near Rifle, Colorado. Acetate was injected to stimulate Fe-reducing bacteria (FeRB) and to immobilize aqueous U(VI) to insoluble U(IV). Bicarbonate was coinjected in half of the domain to mobilize sorbed U(VI). We used reactive transport modeling to integrate hydraulic and geochemical data and to quantify rates at the grid block (0.25 m) and experimental field scale (tens of meters). Although local rates varied by orders of magnitude in conjunction with biostimulation fronts propagating downstream, field-scale rates were dominated by those orders of magnitude higher rates at a few selected hot spots where Fe(III), U(VI), and FeRB were at their maxima in the vicinity of the injection wells. At particular locations, the hot moments with maximum rates negatively corresponded to their distance from the injection wells. Although bicarbonate injection enhanced local rates near the injection wells by a maximum of 39.4%, its effect at the field scale was limited to a maximum of 10.0%. We propose a rate-versus-measurement-length relationship (log R' = -0.63 log L - 2.20, with R' in μmol/mg cell protein/day and L in meters) for orders-of-magnitude estimation of uranium bioreduction rates across scales.
Thivya, C; Chidambaram, S; Keesari, Tirumalesh; Prasanna, M V; Thilagavathi, R; Adithya, V S; Singaraja, C
2016-04-01
Uranium is a radioactive element normally present in hexavalent form as U(VI) in solution and elevated levels in drinking water cause health hazards. Representative groundwater samples were collected from different litho-units in this region and were analyzed for total U and major and minor ions. Results indicate that the highest U concentration (113 µg l(-1)) was found in granitic terrains of this region and about 10 % of the samples exceed the permissible limit for drinking water. Among different species of U in aqueous media, carbonate complexes [UO2(CO3)(2)(2-)] are found to be dominant. Groundwater with higher U has higher pCO2 values, indicating weathering by bicarbonate ions resulting in preferential mobilization of U in groundwater. The major minerals uraninite and coffinite were found to be supersaturated and are likely to control the distribution of U in the study area. Nature of U in groundwater, the effects of lithology on hydrochemistry and factors controlling its distribution in hard rock aquifers of Madurai district are highlighted in this paper.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Arfsten, Darryl P.; Schaeffer, David J.; Johnson, Eric W.
Depleted uranium (DU) projectiles have been used in battle in Iraq and the Balkans and will continue to be a significant armor-penetrating munition for the US military. As demonstrated in the Persian Gulf War, battle injury from DU projectiles and shrapnel is a possibility, and removal of embedded DU fragments from the body is not always practical because of their location in the body or their small size. Previous studies in rodents have demonstrated that implanted DU mobilizes and translocates to the gonads, and natural uranium may be toxic to spermatazoa and the male reproductive tract. In this study, themore » effects of implanted DU pellets on sperm concentration, motility, and male reproductive success were evaluated in adult (P1) Sprague-Dawley rats implanted with 0, 12, or 20, DU pellets of 1x2 mm or 12 or 20 tantalum (Ta) steel pellets of 1x2 mm. Twenty DU pellets of 1x2 mm (760 mg) implanted in a 500-g rat are equal to approximately 0.2 pound of DU in a 154-lb (70-kg) person. Urinary analysis found that male rats implanted with DU were excreting uranium at postimplantation days 27 and 117 with the amount dependent on dose. No deaths or evidence of toxicity occurred in P1 males over the 150-day postimplantation study period. When assessed at postimplantation day 150, the concentration, motion, and velocity of sperm isolated from DU-implanted animals were not significantly different from those of sham surgery controls. Velocity and motion of sperm isolated from rats treated with the positive control compound {alpha}-chlorohydrin were significantly reduced compared with sham surgery controls. There was no evidence of a detrimental effect of DU implantation on mating success at 30-45 days and 120-145 days postimplantation. The results of this study suggest that implantation of up to 20 DU pellets of 1x2 mm in rats for approximately 21% of their adult lifespan does not have an adverse impact on male reproductive success, sperm concentration, or sperm velocity.« less
SLUDGE RETRIEVAL FROM HANFORD K WEST BASIN SETTLER TANKS
DOE Office of Scientific and Technical Information (OSTI.GOV)
ERPENBECK EG; LESHIKAR GA
In 2010, an innovative, remotely operated retrieval system was deployed to successfully retrieve over 99.7% of the radioactive sludge from ten submerged tanks in Hanford's K-West Basin. As part of K-West Basin cleanup, the accumulated sludge needed to be removed from the 0.5 meter diameter by 5 meter long settler tanks and transferred approximately 45 meters to an underwater container for sampling and waste treatment. The abrasive, dense, non-homogeneous sludge was the product of the washing process of corroded nuclear fuel. It consists of small (less than 600 micron) particles of uranium metal, uranium oxide, and various other constituents, potentiallymore » agglomerated or cohesive after 10 years of storage. The Settler Tank Retrieval System (STRS) was developed to access, mobilize and pump out the sludge from each tank using a standardized process of retrieval head insertion, periodic high pressure water spray, retraction, and continuous pumping of the sludge. Blind operations were guided by monitoring flow rate, radiation levels in the sludge stream, and solids concentration. The technology developed and employed in the STRS can potentially be adapted to similar problematic waste tanks or pipes that must be remotely accessed to achieve mobilization and retrieval of the sludge within.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhong, Lirong; Szecsody, James E.; Truex, Michael J.
Use of gas-phase amendments for in situ remediation of inorganic contaminants in unsaturated sediments of the vadose zone may be advantageous, but there has been limited development and testing of gas remediation technologies. Treatment with ammonia gas has been studied and has a potential for use in treating inorganic contaminants such as uranium because it induces a high pore-water pH causing mineral dissolution and subsequent formation of stable precipitates that decrease the mobility of some contaminants. For field application, knowledge of ammonia transport and the geochemical reactions induced by ammonia is needed. Laboratory studies were conducted to support calculations neededmore » for field treatment design, to quantify advective and diffusive ammonia transport in unsaturated sediments, to evaluate reactions among gas, sediment, and water, and to study reaction-induced pore-water chemistry changes as a function of ammonia delivery conditions. Ammonia gas quickly partitions into sediment pore water and increases pH up to 13.2. Injected ammonia gas front movement can be reasonably predicted by gas flow rate and equilibrium partitioning. The ammonia gas diffusion rate is a function of the water content in the sediment. Measured diffusion front movement was 0.05, 0.03, and 0.02 cm/hr. in sediments with 2.0%, 8.7%, and 13.0% water content, respectively. Sodium, aluminum, and silica pore-water concentrations increase on exposure to ammonia and then decline as aluminosilicates precipitate with declining pH. When uranium is present in the sediment and pore water, up to 85% of the water-leachable uranium was immobilized by ammonia treatment.« less
The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz
Fox, P.M.; Davis, J.A.; Zachara, J.M.
2006-01-01
Recent studies of uranium(VI) geochemistry have focused on the potentially important role of the aqueous species, CaUO2 (CO3)32- and Ca2 UO2(CO3)30(aq), on inhibition of microbial reduction and uranium(VI) aqueous speciation in contaminated groundwater. However, to our knowledge, there have been no direct studies of the effects of these species on U(VI) adsorption by mineral phases. The sorption of U(VI) on quartz and ferrihydrite was investigated in NaNO3 solutions equilibrated with either ambient air (430 ppm CO2) or 2% CO2 in the presence of 0, 1.8, or 8.9 mM Ca2+. Under conditions where the Ca2UO2(CO3)30 (aq) species predominates U(VI) aqueous speciation, the presence of Ca in solution lowered U(VI) adsorption on quartz from 77% in the absence of Ca to 42% and 10% at Ca concentrations of 1.8 and 8.9 mM, respectively. U(VI) adsorption to ferrihydrite decreased from 83% in the absence of Ca to 57% in the presence of 1.8 mM Ca. Surface complexation model predictions that included the formation constant for aqueous Ca2UO2(CO3)30(aq) accurately simulated the effect of Ca2+ on U(VI) sorption onto quartz and ferrihydrite within the thermodynamic uncertainty of the stability constant value. This study confirms that Ca2+ can have a significant impact on the aqueous speciation of U(VI), and consequently, on the sorption and mobility of U(VI) in aquifers. ?? 2005 Elsevier Inc. All rights reserved.
Radiation shielding composition
Quapp, William J.; Lessing, Paul A.
2000-12-26
A composition for use as a radiation shield. The shield is a concrete product containing a stable uranium aggregate for attenuating gamma rays and a neutron absorbing component, the uranium aggregate and neutron absorbing component being present in the concrete product in sufficient amounts to provide a concrete having a density between about 4 and about 15 grams/cm.sup.3 and which will at a predetermined thickness, attenuate gamma rays and absorb neutrons from a radioactive material of projected gamma ray and neutron emissions over a determined time period. The composition is preferably in the form of a container for storing radioactive materials that emit gamma rays and neutrons. The concrete container preferably comprises a metal liner and/or a metal outer shell. The resulting radiation shielding container has the potential of being structurally sound, stable over a long period of time, and, if desired, readily mobile.
Radiation shielding composition
Quapp, William J.; Lessing, Paul A.
1998-01-01
A composition for use as a radiation shield. The shield is a concrete product containing a stable uranium aggregate for attenuating gamma rays and a neutron absorbing component, the uranium aggregate and neutron absorbing component being present in the concrete product in sufficient amounts to provide a concrete having a density between about 4 and about 15 grams/cm.sup.3 and which will at a predetermined thickness, attenuate gamma rays and absorb neutrons from a radioactive material of projected gamma ray and neutron emissions over a determined time period. The composition is preferably in the form of a container for storing radioactive materials that emit gamma rays and neutrons. The concrete container preferably comprises a metal liner and/or a metal outer shell. The resulting radiation shielding container has the potential of being structurally sound, stable over a long period of time, and, if desired, readily mobile.
Molecular Simulations of the Diffusion of Uranyl Carbonate Species in Nanosized Mineral Fractures
NASA Astrophysics Data System (ADS)
Kerisit, S.; Liu, C.
2010-12-01
Uranium is a major groundwater contaminant at uranium processing and mining sites as a result of intentional and accidental discharges of uranium-containing waste products into subsurface environments. Recent characterization has shown that uranium preferentially associates with intragrain and intra-aggregate domains in some of the uranium-contaminated sediments collected from the US Department of Energy Hanford Site [1, 2]. In these sediments, uranium existed as precipitated and/or adsorbed phases in grain micropores with nano- to microscale sizes. Desorption and diffusion characterization studies and continuum-scale modeling indicated that ion diffusion in the microfractures is a major mechanism that led to preferential uranium concentration in the microfracture regions and will control the future mobility of uranium in the subsurface sediments [1, 3-4]. However, the diffusion properties of uranyl species in the intragrain regions, especially at the solid-liquid interface, are still poorly understood. Therefore, a general aim of this work is to provide atomic-level insights into the contribution of microscopic surface effects to the slow diffusion process of uranyl species in porous media with nano- to microsized fractures. In this presentation, we will first present molecular dynamics (MD) simulations of feldspar-water interfaces to investigate their interfacial structure and dynamics and establish a theoretical framework for subsequent simulations of water and ion diffusion at these interfaces [5]. We will then report on MD simulations carried out to probe the effects of confinement and of the presence of the mineral surface on the diffusion of water and electrolyte ions in nanosized feldspar fractures [6]. Several properties of the mineral-water interface were varied, such as the fracture width, the ionic strength of the contacting solution, and the surface charge. Our calculations reveal a 2.0-2.5 nm interfacial region within which the diffusion properties of water and that of the electrolyte ions differ significantly from those in bulk aqueous solutions. We will then present MD simulations of the diffusion of a series of alkaline-earth uranyl carbonate species in aqueous solutions [7]. The MD simulations show that the alkaline-earth uranyl carbonate complexes have distinct water exchange dynamics, which could lead to different reactivities. Finally, we will present recent results on the diffusion and adsorption of uranyl carbonate species in intragrain micropores, modeled with the feldspar-water interfaces mentioned in the above, to help interpret the diffusion behavior of uranium in contaminated sediments. [1] Liu C. et al. Geochim. Cosmochim. Acta 68 4519 (2004) [2] McKinley J. P. et al. Geochim. Cosmochim. Acta 70 1873 (2006) [3] Liu C. et al. Water Resour. Res. 42 W12420 (2006) [4] Ilton E. S. et al. Environ. Sci. Technol. 42 1565 (2009) [5] Kerisit S. et al. Geochim. Cosmochim. Acta 72 1481 (2008) [6] Kerisit S. and Liu C. Environ. Sci. Technol. 43 777 (2009) [7] Kerisit S. and Liu C. Geochim. Cosmochim. Acta 74 4937 (2010)
NASA Astrophysics Data System (ADS)
Domnick, Urs; Cook, Nigel J.; Bluck, Russel; Brown, Callan; Ciobanu, Cristiana L.
2018-02-01
The Blackbush uranium deposit (JORC Inferred Resource: 12,580 tonnes U), located on the north-eastern Eyre Peninsula, is currently the only sediment-hosted U deposit investigated in detail in the Gawler Craton. Uranium is hosted within Eocene sandstone of the Kanaka Beds, overlying Mesoproterozoic granites of the Samphire pluton, affiliated with the Hiltaba Intrusive Suite ( 1.6 Ga). These are considered the most probable source rocks for uranium mineralisation. By constraining the petrography and mineralogy of the granites, insights into the post-emplacement evolution can be gained, which may provide an exploration indicator for other sediment-hosted uranium systems. Three geochemically distinct granite types were identified in the Samphire Pluton and correspond to domains interpreted from geophysical data. All granites show complex alteration overprints and textures with increasing intensity closer to the deposit, as well as crosscutting veining. Alkali feldspar has been replaced by porous K-feldspar and albite, and plagioclase is overprinted by an assemblage of porous albite + sericite ± calc-silicates (prehnite, pumpellyite and epidote). This style of feldspar alteration is regionally widespread and known from Hiltaba-aged granites associated with iron-oxide copper-gold mineralisation at Olympic Dam and in the Moonta-Wallaroo region. In two granite types biotite is replaced by calcic garnet. Calc-silicates are indicative of Ca-metasomatism, sourced from the anorthite component of altered plagioclase. Minor clay alteration of feldspars is present in all samples. Mineral assemblages in veins include quartz + hematite, hematite + coffinite, fluorite + quartz, and clay minerals. Minor chlorite and sericite are found in all vein types. All granite types are anomalously rich in U (concentrations between 10 and 81 ppm). Highly variable Th/U ratios, as well as hydrothermal U minerals (mostly coffinite) in granites and veins, are clear evidence for U mobility. Uranium may have been preconcentrated in veins in the upper parts of the pluton, and was subsequently leached after deposition of the sediment.
Mukherjee, Arpan; Wheaton, Garrett H.; Blum, Paul H.; Kelly, Robert M.
2012-01-01
Thermoacidophilic archaea are found in heavy metal-rich environments, and, in some cases, these microorganisms are causative agents of metal mobilization through cellular processes related to their bioenergetics. Given the nature of their habitats, these microorganisms must deal with the potentially toxic effect of heavy metals. Here, we show that two thermoacidophilic Metallosphaera species with nearly identical (99.99%) genomes differed significantly in their sensitivity and reactivity to uranium (U). Metallosphaera prunae, isolated from a smoldering heap on a uranium mine in Thüringen, Germany, could be viewed as a “spontaneous mutant” of Metallosphaera sedula, an isolate from Pisciarelli Solfatara near Naples. Metallosphaera prunae tolerated triuranium octaoxide (U3O8) and soluble uranium [U(VI)] to a much greater extent than M. sedula. Within 15 min following exposure to “U(VI) shock,” M. sedula, and not M. prunae, exhibited transcriptomic features associated with severe stress response. Furthermore, within 15 min post-U(VI) shock, M. prunae, and not M. sedula, showed evidence of substantial degradation of cellular RNA, suggesting that transcriptional and translational processes were aborted as a dynamic mechanism for resisting U toxicity; by 60 min post-U(VI) shock, RNA integrity in M. prunae recovered, and known modes for heavy metal resistance were activated. In addition, M. sedula rapidly oxidized solid U3O8 to soluble U(VI) for bioenergetic purposes, a chemolithoautotrophic feature not previously reported. M. prunae, however, did not solubilize solid U3O8 to any significant extent, thereby not exacerbating U(VI) toxicity. These results point to uranium extremophily as an adaptive, rather than intrinsic, feature for Metallosphaera species, driven by environmental factors. PMID:23010932
[Uranium exposure and cancer risk: a review of epidemiological studies].
Tirmarche, M; Baysson, H; Telle-Lamberton, M
2004-02-01
At the end of 2000, certain diseases including leukemia were reported among soldiers who participated in the Balkan and in the Gulf wars. Depleted uranium used during these conflicts was considered as a possible cause. Its radiotoxicity is close to that of natural uranium. This paper reviews the epidemiological knowledge of uranium, the means of exposure and the associated risk of cancer. The only available epidemiological data concerns nuclear workers exposed to uranium. A review of the international literature is proposed by distinguishing between uranium miners and other workers of the nuclear industry. French studies are described in details. In ionizing radiation epidemiology, contamination by uranium is often cited as a risk factor, but the dose-effect relationship is rarely studied. Retrospective assessment of individual exposure is generally insufficient. Moreover, it is difficult to distinguish between uranium radiotoxicity, its chemical toxicity and the radiotoxicity of its progeny. A causal relation between lung cancer and radon exposure, a gas derived from the decay of uranium, has been demonstrated in epidemiological studies of miners. Among other nuclear workers exposed to uranium, there is a mortality deficit from all causes (healthy worker effect). No cancer site appears systematically in excess compared to the national population; very few studies describe a dose-response relationship. Only studies with a precise reconstruction of doses and sufficient numbers of workers will allow a better assessment of risks associated with uranium exposure at levels encountered in industry or during conflicts using depleted uranium weapons.
MICROSCALE METABOLIC, REDOX AND ABIOTIC REACTIONS IN HANFORD 300 AREA SUBSURFACE SEDIMENTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Beyenal, Haluk; McLEan, Jeff; Majors, Paul
2013-11-14
The Hanford 300 Area is a unique site due to periodic hydrologic influence of river water resulting in changes in groundwater elevation and flow direction. This area is also highly subject to uranium remobilization, the source of which is currently believed to be the region at the base of the vadose zone that is subject to period saturation due to the changes in the water levels in the Columbia River. We found that microbial processes and redox and abiotic reactions which operate at the microscale were critical to understanding factors controlling the macroscopic fate and transport of contaminants in themore » subsurface. The combined laboratory and field research showed how microscale conditions control uranium mobility and how biotic, abiotic and redox reactions relate to each other. Our findings extended the current knowledge to examine U(VI) reduction and immobilization using natural 300 Area communities as well as selected model organisms on redox-sensitive and redox-insensitive minerals. Using innovative techniques developed specifically to probe biogeochemical processes at the microscale, our research expanded our current understanding of the roles played by mineral surfaces, bacterial competition, and local biotic, abiotic and redox reaction rates on the reduction and immobilization of uranium.« less
U(VI) adsorption on aquifer sediments at the Hanford Site.
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.
NASA Astrophysics Data System (ADS)
Scheibe, T. D.; Fang, Y.; Roden, E. E.; Brooks, S. C.; Chien, Y.; Murray, C. J.
2004-05-01
Uranium is a significant groundwater contaminant at many former mining and processing sites. In its oxidized state, U(VI) is soluble and mobile, although strongly retarded by sorption to natural iron oxide surfaces. It has been demonstrated that commonly occurring subsurface microorganisms can reduce uranium and other metals when provided sufficient carbon as an electron donor. Reduced U(IV) precipitates as a solid phase; therefore biostimulation provides a potential strategy for in situ removal from contaminated groundwater. However, these biogeochemical reactions occur in the context of a complex heterogeneous environment in which flow and transport dynamics and abiotic reactions can have significant impacts. We have constructed a high-resolution numerical model of groundwater flow and multicomponent reactive transport that incorporates heterogeneity in hydraulic conductivity and initial Fe(III) distribution, microbial growth and transport dynamics, and effects of sorption or precipitation of biogenic Fe(II) on availability of Fe(III) as an electron acceptor. The biogeochemical reaction models and their parameters are based on laboratory experiments; the heterogeneous field-scale property distributions are based on interpretations of geophysical and other observations at a highly characterized field site. The model is being run in Monte Carlo mode to examine the controls that these factors exert on 1) the initial distribution of sorbed uranium in an oxic environment and 2) the reduction and immobilization of uranium upon introduction of a soluble electron donor.
Uranium induces oxidative stress in lung epithelial cells
Periyakaruppan, Adaikkappan; Kumar, Felix; Sarkar, Shubhashish; Sharma, Chidananda S.
2009-01-01
Uranium compounds are widely used in the nuclear fuel cycle, antitank weapons, tank armor, and also as a pigment to color ceramics and glass. Effective management of waste uranium compounds is necessary to prevent exposure to avoid adverse health effects on the population. Health risks associated with uranium exposure includes kidney disease and respiratory disorders. In addition, several published results have shown uranium or depleted uranium causes DNA damage, mutagenicity, cancer and neurological defects. In the current study, uranium toxicity was evaluated in rat lung epithelial cells. The study shows uranium induces significant oxidative stress in rat lung epithelial cells followed by concomitant decrease in the antioxidant potential of the cells. Treatment with uranium to rat lung epithelial cells also decreased cell proliferation after 72 h in culture. The decrease in cell proliferation was attributed to loss of total glutathione and superoxide dismutase in the presence of uranium. Thus the results indicate the ineffectiveness of antioxidant system’s response to the oxidative stress induced by uranium in the cells. PMID:17124605
Radiation shielding composition
Quapp, W.J.; Lessing, P.A.
1998-07-28
A composition is disclosed for use as a radiation shield. The shield is a concrete product containing a stable uranium aggregate for attenuating gamma rays and a neutron absorbing component, the uranium aggregate and neutron absorbing component being present in the concrete product in sufficient amounts to provide a concrete having a density between about 4 and about 15 grams/cm{sup 3} and which will at a predetermined thickness, attenuate gamma rays and absorb neutrons from a radioactive material of projected gamma ray and neutron emissions over a determined time period. The composition is preferably in the form of a container for storing radioactive materials that emit gamma rays and neutrons. The concrete container preferably comprises a metal liner and/or a metal outer shell. The resulting radiation shielding container has the potential of being structurally sound, stable over a long period of time, and, if desired, readily mobile. 5 figs.
NASA Astrophysics Data System (ADS)
Starikov, S. V.; Kolotova, L. N.; Kuksin, A. Yu.; Smirnova, D. E.; Tseplyaev, V. I.
2018-02-01
We studied structure and thermodynamic properties of cubic and tetragonal phases of pure uranium and U-Mo alloys using atomistic simulations: molecular dynamics and density functional theory. The main attention was paid to the metastable γ0 -phase that is formed in U-Mo alloys at low temperature. Structure of γ0 -phase is similar to body-centered tetragonal (bct) lattice with displacement of a central atom in the basic cell along [ 001 ] direction. Such displacements have opposite orientations for part of the neighbouring basic cells. In this case, such ordering of the displacements can be designated as antiferro-displacement. Formation of such complex structure may be interpreted through forming of short U-U bonds. At heating, the tetragonal structure transforms into cubic γs -phase, still showing ordering of central atom displacements. With rise in temperature, γs -phase transforms to γ-phase with a quasi body-centered cubic (q-bcc) lattice. The local positions of uranium atoms in γ-phase correspond to γs -phase, however, orientations of the central atom displacements become disordered. Transition from γ0 to γ can be considered as antiferro-to paraelastic transition of order-disorder type. This approach to the structure description of uranium alloy allows to explain a number of unusual features found in the experiments: anisotropy of lattice at low temperature; remarkably high self-diffusion mobility in γ-phase; decreasing of electrical resistivity at heating for some alloys. In addition, important part of this work is the development of new interatomic potential for U-Mo system made with taking into account details of studied structures.
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.
Carbon diffusion in molten uranium: an ab initio molecular dynamics study
NASA Astrophysics Data System (ADS)
Garrett, Kerry E.; Abrecht, David G.; Kessler, Sean H.; Henson, Neil J.; Devanathan, Ram; Schwantes, Jon M.; Reilly, Dallas D.
2018-04-01
In this work we used ab initio molecular dynamics within the framework of density functional theory and the projector-augmented wave method to study carbon diffusion in liquid uranium at temperatures above 1600 K. The electronic interactions of carbon and uranium were described using the local density approximation (LDA). The self-diffusion of uranium based on this approach is compared with literature computational and experimental results for liquid uranium. The temperature dependence of carbon and uranium diffusion in the melt was evaluated by fitting the resulting diffusion coefficients to an Arrhenius relationship. We found that the LDA calculated activation energy for carbon was nearly twice that of uranium: 0.55 ± 0.03 eV for carbon compared to 0.32 ± 0.04 eV for uranium. Structural analysis of the liquid uranium-carbon system is also discussed.
Numerical simulation of transient, incongruent vaporization induced by high power laser
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tsai, C.H.
1981-01-01
A mathematical model and numerical calculations were developed to solve the heat and mass transfer problems specifically for uranum oxide subject to laser irradiation. It can easily be modified for other heat sources or/and other materials. In the uranium-oxygen system, oxygen is the preferentially vaporizing component, and as a result of the finite mobility of oxygen in the solid, an oxygen deficiency is set up near the surface. Because of the bivariant behavior of uranium oxide, the heat transfer problem and the oxygen diffusion problem are coupled and a numerical method of simultaneously solving the two boundary value problems ismore » studied. The temperature dependence of the thermal properties and oxygen diffusivity, as well as the highly ablative effect on the surface, leads to considerable non-linearities in both the governing differential equations and the boundary conditions. Based on the earlier work done in this laboratory by Olstad and Olander on Iron and on Zirconium hydride, the generality of the problem is expanded and the efficiency of the numerical scheme is improved. The finite difference method, along with some advanced numerical techniques, is found to be an efficient way to solve this problem.« less
Differential lead retention in zircons: implications for nuclear waste containment.
Gentry, R V; Sworski, T J; McKown, H S; Smith, D H; Eby, R E; Christie, W H
1982-04-16
An innovative ultrasensitive technique was used for lead isotopic analysis of individual zircons extracted from granite core samples at depths of 960, 2170, 2900, 3930, and 4310 meters. The results show that lead, a relatively mobile element compared to the nuclear waste-related actinides uranium and thorium, has been highly retained at elevated temperatures (105 degrees to 313 degrees C) under conditions relevant to the burial of synthetic rock waste containers in deep granite holes.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sharp, Jonathan O.
Project Overview: The impact of the original seed award was substantially increased by leveraging a postdoctoral fellowship (Marie Curie Postdoctoral Fellowship) and parallel funds from (A) synergistic project supported by NSF and (B) with DOE collaborators (PI’s Ranville and Williams) as well as no-cost extension that greatly increased the impact and publications associated with the project. In aligning with SBR priorities, the project’s focus was extended more broadly to explore coupled biogeochemical analysis of metal (im)mobilization processes beyond uranium with a foundation in integrating microbial ecology with geochemical analyses. This included investigations of arsenic and zinc during sulfate reducing conditionsmore » in addition to direct microbial reduction of metals. Complimentary work with NSF funding and collaborative DOE interactions further increased the project scope to investigate metal (im)mobilization coupled to biogeochemical perturbations in forest ecosystems with an emphasis on coupled carbon and metal biogeochemistry. In total, the project was highly impactful and resulted in 9 publications and directly supported salary/tuition for 3 graduate students at various stages of their academic careers as well as my promotion to Associate Professor. In going forward, findings provided inspiration for a two subsequent proposals with collaborators at Lawrence Berkeley Laboratory and others that are currently in review (as of March 2016).« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yabusaki, Steven B.; Fang, Yilin; Williams, Kenneth H.
2011-11-01
Field experiments at a former uranium mill tailings site have identified the potential for stimulating indigenous bacteria to catalyze the conversion of aqueous uranium in the +6 oxidation state to immobile solid-associated uranium in the +4 oxidation state. This effectively removes uranium from solution resulting in groundwater concentrations below actionable standards. Three-dimensional, coupled variably-saturated flow and biogeochemical reactive transport modeling of a 2008 in situ uranium bioremediation field experiment is used to better understand the interplay of transport rates and biogeochemical reaction rates that determine the location and magnitude of key reaction products. A comprehensive reaction network, developed largely throughmore » previous 1-D modeling studies, was used to simulate the impacts on uranium behavior of pulsed acetate amendment, seasonal water table variation, spatially-variable physical (hydraulic conductivity, porosity) and geochemical (reactive surface area) material properties. A principal challenge is the mechanistic representation of biologically-mediated terminal electron acceptor process (TEAP) reactions whose products significantly alter geochemical controls on uranium mobility through increases in pH, alkalinity, exchangeable cations, and highly reactive reduction products. In general, these simulations of the 2008 Big Rusty acetate biostimulation field experiment in Rifle, Colorado confirmed previously identified behaviors including (1) initial dominance by iron reducing bacteria that concomitantly reduce aqueous U(VI), (2) sulfate reducing bacteria that become dominant after {approx}30 days and outcompete iron reducers for the acetate electron donor, (3) continuing iron-reducer activity and U(VI) bioreduction during dominantly sulfate reducing conditions, and (4) lower apparent U(VI) removal from groundwater during dominantly sulfate reducing conditions. New knowledge on simultaneously active metal and sulfate reducers has been incorporated into the modeling. In this case, an initially small population of slow growing sulfate reducers is active from the initiation of biostimulation. Three-dimensional, variably saturated flow modeling was used to address impacts of a falling water table during acetate injection. These impacts included a significant reduction in aquifer saturated thickness and isolation of residual reactants and products, as well as unmitigated uranium, in the newly unsaturated vadose zone. High permeability sandy gravel structures resulted in locally high flow rates in the vicinity of injection wells that increased acetate dilution. In downgradient locations, these structures created preferential flow paths for acetate delivery that enhanced local zones of TEAP reactivity and subsidiary reactions. Conversely, smaller transport rates associated with the lower permeability lithofacies (e.g., fine) and vadose zone were shown to limit acetate access and reaction. Once accessed by acetate, however, these same zones limited subsequent acetate dilution and provided longer residence times that resulted in higher concentrations of TEAP products when terminal electron donors and acceptors were not limiting. Finally, facies-based porosity and reactive surface area variations were shown to affect aqueous uranium concentration distributions; however, the ranges were sufficiently small to preserve general trends. Large computer memory and high computational performance were required to simulate the detailed coupled process models for multiple biogeochemical components in highly resolved heterogeneous materials for the 110-day field experiment and 50 days of post-biostimulation behavior. In this case, a highly-scalable subsurface simulator operating on 128 processor cores for 12 hours was used to simulate each realization. An equivalent simulation without parallel processing would have taken 60 days, assuming sufficient memory was available.« less
NASA Astrophysics Data System (ADS)
Fritschle, Tobias; Daly, J. Stephen; Whitehouse, Martin J.; Buhre, Stephan; McConnell, Brian; The Iretherm Team
2015-04-01
Ordovician to Devonian (Caledonian) granites are common in the Iapetus Suture Zone (ISZ) in Ireland and Britain. Some of these, e.g., the buried Kentstown and Glenamaddy granites, are situated beneath Upper Palaeozoic sedimentary basins, and hence are potential geothermal targets. Numerous granites of similar age and related origin (Fritschle et al., 2014) are exposed astride the ISZ. They are considered to be analogous to the buried ones, and their geochemical characteristics are used as a proxy for the buried granites as samples from deep drilling are naturally limited. The whole-rock geochemistry of nine granite intrusions (71 samples, including both hydrothermally altered and unaltered samples) varies significantly, but with no obvious geographical control. The granites are S- and I-Types with ASI (Aluminium Saturation Index) between 0.7 - 1.4. Average heat production rates range from 1.4 μW/m³ for the Leinster Granite to 4.9 μW/m³ for the Drogheda Granite (Fritschle et al., 2015). The heat-producing elements uranium (U), thorium (Th) and potassium (K) and calculated heat production rates generally correlate positively with niobium and rubidium concentrations. However, S-Type compared to I-Type granites show elevated abundances in rubidium (>130 ppm) and usually have a lower Th/U ratio. Altered samples tend to have a higher Th/U ratio compared to unaltered ones. Within individual plutons trends of decreasing heat production rates with increasing Th/U ratios were observed. This trend is attributed to the hydrothermal redistribution of the mobile heat-producing element uranium. This is also implied by uranium-enrichment in hydrothermally generated Ca and Si-veinlets. Metasomatic processes such as hydrothermal alteration appear capable of significantly redistributing mobile elements such as uranium. Hence, these processes may act as a major mechanism controlling the granite's heat production budget, often shaping a pluton's geothermal exploitation potential. Fritschle, T., Daly, J.S., Whitehouse, M.J., Buhre, S., McConnell, B., 2015. Geothermal potential of Caledonian granites astride the Iapetus Suture Zone in Ireland and the Isle of Man - Implications for EGS prospectivity. Proceedings World Geothermal Congress 2015, in press. Fritschle, T., Daly, J.S., Whitehouse, M.J., McConnell, B., Buhre, S., 2014. Zircon geochronology and Hf-O isotope geochemistry from granites in the Iapetus Suture Zone in Ireland and the Isle of Man. Geophysical Research Abstracts 16, EGU-2014-801.
Laurent, Olivier; Gomolka, Maria; Haylock, Richard; Blanchardon, Eric; Giussani, Augusto; Atkinson, Will; Baatout, Sarah; Bingham, Derek; Cardis, Elisabeth; Hall, Janet; Tomasek, Ladislav; Ancelet, Sophie; Badie, Christophe; Bethel, Gary; Bertho, Jean-Marc; Bouet, Ségolène; Bull, Richard; Challeton-de Vathaire, Cécile; Cockerill, Rupert; Davesne, Estelle; Ebrahimian, Teni; Engels, Hilde; Gillies, Michael; Grellier, James; Grison, Stephane; Gueguen, Yann; Hornhardt, Sabine; Ibanez, Chrystelle; Kabacik, Sylwia; Kotik, Lukas; Kreuzer, Michaela; Lebacq, Anne Laure; Marsh, James; Nosske, Dietmar; O'Hagan, Jackie; Pernot, Eileen; Puncher, Matthew; Rage, Estelle; Riddell, Tony; Roy, Laurence; Samson, Eric; Souidi, Maamar; Turner, Michelle C; Zhivin, Sergey; Laurier, Dominique
2016-06-01
The potential health impacts of chronic exposures to uranium, as they occur in occupational settings, are not well characterized. Most epidemiological studies have been limited by small sample sizes, and a lack of harmonization of methods used to quantify radiation doses resulting from uranium exposure. Experimental studies have shown that uranium has biological effects, but their implications for human health are not clear. New studies that would combine the strengths of large, well-designed epidemiological datasets with those of state-of-the-art biological methods would help improve the characterization of the biological and health effects of occupational uranium exposure. The aim of the European Commission concerted action CURE (Concerted Uranium Research in Europe) was to develop protocols for such a future collaborative research project, in which dosimetry, epidemiology and biology would be integrated to better characterize the effects of occupational uranium exposure. These protocols were developed from existing European cohorts of workers exposed to uranium together with expertise in epidemiology, biology and dosimetry of CURE partner institutions. The preparatory work of CURE should allow a large scale collaborative project to be launched, in order to better characterize the effects of uranium exposure and more generally of alpha particles and low doses of ionizing radiation.
Carbon diffusion in molten uranium: an ab initio molecular dynamics study
DOE Office of Scientific and Technical Information (OSTI.GOV)
Garrett, Kerry E.; Abrecht, David G.; Kessler, Sean H.
In this work we used ab initio molecular dynamics (AIMD) within the framework of density functional theory (DFT) and the projector-augmented wave (PAW) method to study carbon diffusion in liquid uranium at temperatures above 1600 K. The electronic interactions of carbon and uranium were described using the local density approximation (LDA). The self-diffusion of uranium based on this approach is compared with literature computational and experimental results for liquid uranium. The temperature dependence of carbon and uranium diffusion in the melt was evaluated by fitting the resulting diffusion coefficients to an Arrhenius relationship. We found that the LDA calculated activationmore » energy for carbon was nearly twice that of uranium: 0.55±0.03 eV for carbon compared to 0.32±0.04 eV for uranium. Structural analysis of the liquid uranium-carbon system is also discussed.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D.
In-situ recovery (ISR) of uranium (U) from sandstone-type roll-front deposits is a technology that involves the injection of solutions that consist of ground water fortified with oxygen and carbonate to promote the oxidative dissolution of U, which is pumped to recovery facilities located at the surface that capture the dissolved U and recycle the treated water. The ISR process alters the geochemical conditions in the subsurface creating conditions that are more favorable to the migration of uranium and other metals associated with the uranium deposit. There is a lack of clear understanding of the impact of ISR mining on themore » aquifer and host rocks of the post-mined site and the fate of residual U and other metals within the mined ore zone. We performed detailed petrographic, mineralogical, and geochemical analyses of several samples taken from about 7 m of core of the formerly the ISR-mined Smith Ranch–Highland uranium deposit in Wyoming. We show that previously mined cores contain significant residual uranium (U) present as coatings on pyrite and carbonaceous fragments. Coffinite was identified in three samples. Core samples with higher organic (> 1 wt.%) and clay (> 6–17 wt.%) contents yielded higher 234U/ 238U activity ratios (1.0–1.48) than those with lower organic and clay fractions. The ISR mining was inefficient in mobilizing U from the carbonaceous materials, which retained considerable U concentrations (374–11,534 ppm). This is in contrast with the deeper part of the ore zone, which was highly depleted in U and had very low 234U/ 238U activity ratios. This probably is due to greater contact with the lixiviant (leaching solution) during ISR mining. EXAFS analyses performed on grains with the highest U and Fe concentrations reveal that Fe is present in a reduced form as pyrite and U occurs mostly as U(IV) complexed by organic matter or as U(IV) phases of carbonate complexes. Moreover, U–O distances of ~ 2.05 Å were noted, indicating the potential formation of other poorly defined U(IV/VI) species. We also noted a small contribution from Udouble bond; length as m-dashO at 1.79 Å, which indicates that U is partially oxidized. There is no apparent U–S or U–Fe interaction in any of the U spectra analyzed. However, SEM analysis of thin sections prepared from the same core material reveals surficial U associated with pyrite which is probably a minor fraction of the total U present as thin coatings on the surface of pyrite. Our data show the presence of different structurally variable uranium forms associated with the mined cores. U associated with carbonaceous materials is probably from the original U mobilization that accumulated in the organic matter-rich areas under reducing conditions during shallow burial diagenesis. U associated with pyrite represents a small fraction of the total U and was likely deposited as a result of chemical reduction by pyrite. Our data suggest that areas rich in carbonaceous materials had limited exposure to the lixiviant solution, continue to be reducing, and still hold significant U resources. Because of their limited access to fluid flow, these areas might not contribute significantly to post-mining U release or attenuation. Areas with pyrite that are accessible to fluids seem to be more reactive and could act as reductants and facilitate U reduction and accumulation, limiting its migration.« less
WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D.; ...
2014-10-08
In-situ recovery (ISR) of uranium (U) from sandstone-type roll-front deposits is a technology that involves the injection of solutions that consist of ground water fortified with oxygen and carbonate to promote the oxidative dissolution of U, which is pumped to recovery facilities located at the surface that capture the dissolved U and recycle the treated water. The ISR process alters the geochemical conditions in the subsurface creating conditions that are more favorable to the migration of uranium and other metals associated with the uranium deposit. There is a lack of clear understanding of the impact of ISR mining on themore » aquifer and host rocks of the post-mined site and the fate of residual U and other metals within the mined ore zone. We performed detailed petrographic, mineralogical, and geochemical analyses of several samples taken from about 7 m of core of the formerly the ISR-mined Smith Ranch–Highland uranium deposit in Wyoming. We show that previously mined cores contain significant residual uranium (U) present as coatings on pyrite and carbonaceous fragments. Coffinite was identified in three samples. Core samples with higher organic (> 1 wt.%) and clay (> 6–17 wt.%) contents yielded higher 234U/ 238U activity ratios (1.0–1.48) than those with lower organic and clay fractions. The ISR mining was inefficient in mobilizing U from the carbonaceous materials, which retained considerable U concentrations (374–11,534 ppm). This is in contrast with the deeper part of the ore zone, which was highly depleted in U and had very low 234U/ 238U activity ratios. This probably is due to greater contact with the lixiviant (leaching solution) during ISR mining. EXAFS analyses performed on grains with the highest U and Fe concentrations reveal that Fe is present in a reduced form as pyrite and U occurs mostly as U(IV) complexed by organic matter or as U(IV) phases of carbonate complexes. Moreover, U–O distances of ~ 2.05 Å were noted, indicating the potential formation of other poorly defined U(IV/VI) species. We also noted a small contribution from Udouble bond; length as m-dashO at 1.79 Å, which indicates that U is partially oxidized. There is no apparent U–S or U–Fe interaction in any of the U spectra analyzed. However, SEM analysis of thin sections prepared from the same core material reveals surficial U associated with pyrite which is probably a minor fraction of the total U present as thin coatings on the surface of pyrite. Our data show the presence of different structurally variable uranium forms associated with the mined cores. U associated with carbonaceous materials is probably from the original U mobilization that accumulated in the organic matter-rich areas under reducing conditions during shallow burial diagenesis. U associated with pyrite represents a small fraction of the total U and was likely deposited as a result of chemical reduction by pyrite. Our data suggest that areas rich in carbonaceous materials had limited exposure to the lixiviant solution, continue to be reducing, and still hold significant U resources. Because of their limited access to fluid flow, these areas might not contribute significantly to post-mining U release or attenuation. Areas with pyrite that are accessible to fluids seem to be more reactive and could act as reductants and facilitate U reduction and accumulation, limiting its migration.« less
Plant-uptake of uranium: Hydroponic and soil system studies
Ramaswami, A.; Carr, P.; Burkhardt, M.
2001-01-01
Limited information is available on screening and selection of terrestrial plants for uptake and translocation of uranium from soil. This article evaluates the removal of uranium from water and soil by selected plants, comparing plant performance in hydroponic systems with that in two soil systems (a sandy-loam soil and an organic-rich soil). Plants selected for this study were Sunflower (Helianthus giganteus), Spring Vetch (Vicia sativa), Hairy Vetch (Vicia villosa), Juniper (Juniperus monosperma), Indian Mustard (Brassica juncea), and Bush Bean (Phaseolus nanus). Plant performance was evaluated both in terms of the percent uranium extracted from the three systems, as well as the biological absorption coefficient (BAC) that normalized uranium uptake to plant biomass. Study results indicate that uranium extraction efficiency decreased sharply across hydroponic, sandy and organic soil systems, indicating that soil organic matter sequestered uranium, rendering it largely unavailable for plant uptake. These results indicate that site-specific soils must be used to screen plants for uranium extraction capability; plant behavior in hydroponic systems does not correlate well with that in soil systems. One plant species, Juniper, exhibited consistent uranium extraction efficiencies and BACs in both sandy and organic soils, suggesting unique uranium extraction capabilities.
Cadigan, R.A.; Felmlee, J.K.
1982-01-01
Major radioactive mineral springs are probably related to deep zones of active metamorphism in areas of orogenic tectonism. The most common precipitate is travertine, a chemically precipitated rock composed chiefly of calcium carbonate, but also containing other minerals. The mineral springs are surface manifestations of hydrothermal conduit systems which extend downward many kilometers to hot source rocks. Conduits are kept open by fluid pressure exerted by carbon dioxide-charged waters rising to the surface propelled by heat and gas (CO2 and steam) pressure. On reaching the surface, the dissolved carbon dioxide is released from solution, and calcium carbonate is precipitated. Springs also contain sulfur species (for example, H2S and HS-), and radon, helium and methane as entrained or dissolved gases. The HS- ion can react to form hydrogen sulfide gas, sulfate salts, and native sulfur. Chemical salts and native sulfur precipitate at the surface. The sulfur may partly oxidize to produce detectable sulfur dioxide gas. Radioactivity is due to the presence of radium-226, radon-222, radium-228, and radon-220, and other daughter products of uranium-238 and thorium-232. Uranium and thorium are not present in economically significant amounts in most radioactive spring precipitates. Most radium is coprecipitated at the surface with barite. Barite (barium sulfate) forms in the barium-containing spring water as a product of the oxidation of sulfur species to sulfate ions. The relatively insoluble barium sulfate precipitates and removes much of the radium from solution. Radium coprecipitates to a lesser extent with manganese-barium- and iron-oxy hydroxides. R-mode factor analysis of abundances of elements suggests that 65 percent of the variance of the different elements is affected by seven factors interpreted as follows: (1) Silica and silicate contamination and precipitation; (2) Carbonate travertine precipitation; (3) Radium coprecipitation; (4) Evaporite precipitation; (5) Hydrous limonite precipitation and coprecipitated elements including uranium; (6) Rare earth elements deposited with detrital contamination (?); (7) Metal carbonate adsorption and precipitation. Economically recoverable minerals occurring at some localities in spring precipitates are ores of iron, manganese, sulfur, tungsten and barium and ornamental travertine. Continental radioactive mineral springs occur in areas of crustal thickening caused by overthrusting of crustal plates, and intrusion and metamorphism. Sedimentary rocks on the lower plate are trapped between the plates and form a zone of metamorphism. Connate waters, carbonate rocks and organic-carbon-bearing rocks react to extreme pressure and temperature to produce carbon dioxide, and steam. Fractures are forced open by gas and fluid pressures. Deep-circulating meteoric waters then come in contact with the reactive products, and a hydrothermal cell forms. When hot mineral-charged waters reach the surface they form the familiar hot mineral springs. Hot springs also occur in relation to igneous intrusive action or volcanism both of which may be products of the crustal plate overthrusting. Uranium and thorium in the sedimentary rocks undergoing metamorphism are sometimes mobilized, but mobilization is generally restricted to an acid hydrothermal environment; much is redeposited in favorable environments in the metamorphosed sediments. Radium and radon, which are highly mobile in both acid and alkaline aqueous media move upward into the hydrothermal cell and to the surface.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Katsenovich, Yelena; Cardona, Claudia; Szecsody, Jim
Remediation of uranium (U) contamination in the deep vadose zone (VZ) sediments abundant in calcite mineral is a challenging task considering the formation of highly stable and mobile uranyl complexes with carbonate and calcium in pore water composition. There is a concern that uranium contamination in the VZ can serve as a continued source for groundwater pollution, creating a risk to human health and the environment through the groundwater pathway. This requires in-situ remediation of the radionuclide-contaminated VZ to convert soluble U species to low solubility precipitates that are stable in the natural environment. Injection of reactive gasses (e.g., NHmore » 3) is a promising technology to decrease U mobility in the unsaturated zone without the addition of liquid amendments. The NH 3 injection creates alkaline conditions that can alter the sediment pore water composition due to a release of elements from minerals (via desorption and dissolution) that are present in the sediment. However, it is not known how VZ pore water constituents (Si, Al 3+, HCO 3 -, and Ca 2 +) would affect U(VI) removal/precipitation in alkaline conditions. This study quantified the role of major pore water constituents typically present in the arid and semi-arid environments of the western regions of the U.S and identified solid uranium-bearing phases that could potentially precipitate from solutions approximating pore water compositions after pH manipulations via ammonia gas injections. Triplicate samples were prepared using six Si (5, 50 100, 150, 200, and 250 mM), six HCO 3 - (0, 3, 25, 50, 75, and 100 mM), and two Ca 2+ (5 and 10 mM) concentrations. The concentration of aluminum and uranium was kept constant at 5 mM and 0.0084 mM, respectively, in all synthetic formulations tested. Results showed that the percentage of U(VI) removal was controlled by the Si/Al molar ratios and Ca 2+ concentrations. Regardless of the bicarbonate concentration tested, the percentage of U(VI) removed increased as the Si/Al ratios were increased. However, higher Ca concentrations correlated with higher U(VI) removal, ranging between 96% and 99%, at low Si/Al ratios. The SEM images of dried precipitates displayed dense amorphous regions high in silica content, where EDS elemental analysis unveiled higher U atomic percentages. The formation of uranyl silicate and carbonate minerals was also predicted by the speciation modeling. XRD analysis revealed the presence of uranyl carbonate mineral phases (andersonite, grimselite); however, uranyl silicates predicted (Na-boltwoodite) were not identified experimentally, possibly due to the amorphous nature of the silica solid phases observed in our experiments.« less
Katsenovich, Yelena; Cardona, Claudia; Szecsody, Jim; ...
2018-03-06
Remediation of uranium (U) contamination in the deep vadose zone (VZ) sediments abundant in calcite mineral is a challenging task considering the formation of highly stable and mobile uranyl complexes with carbonate and calcium in pore water composition. There is a concern that uranium contamination in the VZ can serve as a continued source for groundwater pollution, creating a risk to human health and the environment through the groundwater pathway. This requires in-situ remediation of the radionuclide-contaminated VZ to convert soluble U species to low solubility precipitates that are stable in the natural environment. Injection of reactive gasses (e.g., NHmore » 3) is a promising technology to decrease U mobility in the unsaturated zone without the addition of liquid amendments. The NH 3 injection creates alkaline conditions that can alter the sediment pore water composition due to a release of elements from minerals (via desorption and dissolution) that are present in the sediment. However, it is not known how VZ pore water constituents (Si, Al 3+, HCO 3 -, and Ca 2 +) would affect U(VI) removal/precipitation in alkaline conditions. This study quantified the role of major pore water constituents typically present in the arid and semi-arid environments of the western regions of the U.S and identified solid uranium-bearing phases that could potentially precipitate from solutions approximating pore water compositions after pH manipulations via ammonia gas injections. Triplicate samples were prepared using six Si (5, 50 100, 150, 200, and 250 mM), six HCO 3 - (0, 3, 25, 50, 75, and 100 mM), and two Ca 2+ (5 and 10 mM) concentrations. The concentration of aluminum and uranium was kept constant at 5 mM and 0.0084 mM, respectively, in all synthetic formulations tested. Results showed that the percentage of U(VI) removal was controlled by the Si/Al molar ratios and Ca 2+ concentrations. Regardless of the bicarbonate concentration tested, the percentage of U(VI) removed increased as the Si/Al ratios were increased. However, higher Ca concentrations correlated with higher U(VI) removal, ranging between 96% and 99%, at low Si/Al ratios. The SEM images of dried precipitates displayed dense amorphous regions high in silica content, where EDS elemental analysis unveiled higher U atomic percentages. The formation of uranyl silicate and carbonate minerals was also predicted by the speciation modeling. XRD analysis revealed the presence of uranyl carbonate mineral phases (andersonite, grimselite); however, uranyl silicates predicted (Na-boltwoodite) were not identified experimentally, possibly due to the amorphous nature of the silica solid phases observed in our experiments.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bao, Chen; Wu, Hongfei; Li, Li
2014-09-02
We aim to understand the scale-dependent evolution of uranium bioreduction during a field experiment at a former uranium mill site near Rifle, Colorado. Acetate was injected to stimulate Fe-reducing bacteria (FeRB) and to immobilize aqueous U(VI) to insoluble U(IV). Bicarbonate was coinjected in half of the domain to mobilize sorbed U(VI). We used reactive transport modeling to integrate hydraulic and geochemical data and to quantify rates at the grid block (0.25 m) and experimental field scale (tens of meters). Although local rates varied by orders of magnitude in conjunction with biostimulation fronts propagating downstream, field-scale rates were dominated by thosemore » orders of magnitude higher rates at a few selected hot spots where Fe(III), U(VI), and FeRB were at their maxima in the vicinity of the injection wells. At particular locations, the hot moments with maximum rates negatively corresponded to their distance from the injection wells. Although bicarbonate injection enhanced local rates near the injection wells by a maximum of 39.4%, its effect at the field scale was limited to a maximum of 10.0%. We propose a rate-versus-measurement-length relationship (log R' = -0.63« less
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.
Uranium in bone: metabolic and autoradiographic studies in the rat.
Priest, N D; Howells, G R; Green, D; Haines, J W
1982-03-01
The distribution and retention of intravenously injected hexavalent uranium-233 in the skeleton of the female rat has been investigated using a variety of autoradiographic and radiochemical techniques. These showed that approximately one third of the injected uranium is deposited in the skeleton where it is retained with an initial biological half-time of approximately 40 days. The studies also showed that: 1 Uranium is initially deposited onto all types of bone surface, but preferentially onto those that are accreting. 2 Uranium is deposited in the calcifying zones of skeletal cartilage. 3 Bone accretion results in the burial of surface deposits of uranium. 4 Bone resorption causes the removal of uranium from surfaces. 5 Resorbed uranium is not retained by osteoclasts and macrophages in the bone marrow. 6 Uranium removed from bone surfaces enters the bloodstream where most is either redeposited in bone or excreted via the kidneys. 7 The recycling of resorbed uranium within the skeleton tends to produce a uniform level of uranium contamination throughout mineralized bone. These results are taken to indicate that uranium deposition in bone shares characteristics in common with both the 'volume-seeking radionuclides' typified by the alkaline earth elements and with the 'bone surface-seeking radionuclides' typified by plutonium.
Challenges dealing with depleted uranium in Germany - Reuse or disposal
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moeller, Kai D.
2007-07-01
During enrichment large amounts of depleted Uranium are produced. In Germany every year 2.800 tons of depleted uranium are generated. In Germany depleted uranium is not classified as radioactive waste but a resource for further enrichment. Therefore since 1996 depleted Uranium is sent to ROSATOM in Russia. However it still has to be dealt with the second generation of depleted Uranium. To evaluate the alternative actions in case a solution has to be found in Germany, several studies have been initiated by the Federal Ministry of the Environment. The work that has been carried out evaluated various possibilities to dealmore » with depleted uranium. The international studies on this field and the situation in Germany have been analyzed. In case no further enrichment is planned the depleted uranium has to be stored. In the enrichment process UF{sub 6} is generated. It is an international consensus that for storage it should be converted to U{sub 3}O{sub 8}. The necessary technique is well established. If the depleted Uranium would have to be characterized as radioactive waste, a final disposal would become necessary. For the planned Konrad repository - a repository for non heat generating radioactive waste - the amount of Uranium is limited by the licensing authority. The existing license would not allow the final disposal of large amounts of depleted Uranium in the Konrad repository. The potential effect on the safety case has not been roughly analyzed. As a result it may be necessary to think about alternatives. Several possibilities for the use of depleted uranium in the industry have been identified. Studies indicate that the properties of Uranium would make it useful in some industrial fields. Nevertheless many practical and legal questions are open. One further option may be the use as shielding e.g. in casks for transport or disposal. Possible techniques for using depleted Uranium as shielding are the use of the metallic Uranium as well as the inclusion in concrete. Another possibility could be the use of depleted uranium for the blending of High enriched Uranium (HEU) or with Plutonium to MOX-elements. (authors)« less
An Evaluation of a Networked Radiation Detection System
2010-03-01
conducted at the site using RAT (Cooper, 2008a): “Beginning in the 1940’ s , widespread mining and milling of uranium ore for national defense and energy...contamination…” in order to determine future sampling points (Cooper, 2007). 2. 4 May 2005, conducted mobile air monitoring during the removal of 30...provide site-wide estimates of emissions…” at Warren (OH) Recycling Inc.®’ s 85 acre landfill emitting hydrogen sulfide (H2S) (Cooper, 2007). 4. 7 July
Preparation of carbon coated Fe3O4 nanoparticles for magnetic separation of uranium
NASA Astrophysics Data System (ADS)
Zhang, Xiaofei; Wang, Jun
2018-01-01
Uranium(VI) was removed from aqueous solutions using carbon coated Fe3O4 nanoparticles (Fe3O4@C). Batch experiments were conducted to study the effects of initial pH, shaking time and temperature on uranium sorption efficiency. It was found that the maximum adsorption capacity of the Fe3O4@C toward uranium(VI) was ∼120.20 mg g-1 when the initial uranium(VI) concentration was 100 mg L-1, displaying a high efficiency for the removal of uranium(VI) ions. Kinetics of the uranium(VI) removal is found to follow pseudo-second-order rate equation. In addition, the uranium(VI)-loaded Fe3O4@C nanoparticles can be recovered easily from aqueous solution by magnetic separation and regenerated by acid treatment. Present study suggested that magnetic Fe3O4@C composite particles can be used as an effective and recyclable adsorbent for the removal of uranium(VI) from aqueous solutions.
Decontamination of uranium-contaminated waste oil using supercritical fluid and nitric acid.
Sung, Jinhyun; Kim, Jungsoo; Lee, Youngbae; Seol, Jeunggun; Ryu, Jaebong; Park, Kwangheon
2011-07-01
The waste oil used in nuclear fuel processing is contaminated with uranium because of its contact with materials or environments containing uranium. Under current law, waste oil that has been contaminated with uranium is very difficult to dispose of at a radioactive waste disposal site. To dispose of the uranium-contaminated waste oil, the uranium was separated from the contaminated waste oil. Supercritical R-22 is an excellent solvent for extracting clean oil from uranium-contaminated waste oil. The critical temperature of R-22 is 96.15 °C and the critical pressure is 49.9 bar. In this study, a process to remove uranium from the uranium-contaminated waste oil using supercritical R-22 was developed. The waste oil has a small amount of additives containing N, S or P, such as amines, dithiocarbamates and dialkyldithiophosphates. It seems that these organic additives form uranium-combined compounds. For this reason, dissolution of uranium from the uranium-combined compounds using nitric acid was needed. The efficiency of the removal of uranium from the uranium-contaminated waste oil using supercritical R-22 extraction and nitric acid treatment was determined.
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 mobility and accumulation along the Rio Paguate, Jackpile Mine in Laguna Pueblo, NM.
Blake, Johanna M; De Vore, Cherie L; Avasarala, Sumant; Ali, Abdul-Mehdi; Roldan, Claudia; Bowers, Fenton; Spilde, Michael N; Artyushkova, Kateryna; Kirk, Matthew F; Peterson, Eric; Rodriguez-Freire, Lucia; Cerrato, José M
2017-04-19
The mobility and accumulation of uranium (U) along the Rio Paguate, adjacent to the Jackpile Mine, in Laguna Pueblo, New Mexico was investigated using aqueous chemistry, electron microprobe, X-ray diffraction and spectroscopy analyses. Given that it is not common to identify elevated concentrations of U in surface water sources, the Rio Paguate is a unique site that concerns the Laguna Pueblo community. This study aims to better understand the solid chemistry of abandoned mine waste sediments from the Jackpile Mine and identify key hydrogeological and geochemical processes that affect the fate of U along the Rio Paguate. Solid analyses using X-ray fluorescence determined that sediments located in the Jackpile Mine contain ranges of 320 to 9200 mg kg -1 U. The presence of coffinite, a U(iv)-bearing mineral, was identified by X-ray diffraction analyses in abandoned mine waste solids exposed to several decades of weathering and oxidation. The dissolution of these U-bearing minerals from abandoned mine wastes could contribute to U mobility during rain events. The U concentration in surface waters sampled closest to mine wastes are highest during the southwestern monsoon season. Samples collected from September 2014 to August 2016 showed higher U concentrations in surface water adjacent to the Jackpile Mine (35.3 to 772 μg L -1 ) compared with those at a wetland 4.5 kilometers downstream of the mine (5.77 to 110 μg L -1 ). Sediments co-located in the stream bed and bank along the reach between the mine and wetland had low U concentrations (range 1-5 mg kg -1 ) compared to concentrations in wetland sediments with higher organic matter (14-15%) and U concentrations (2-21 mg kg -1 ). Approximately 10% of the total U in wetland sediments was amenable to complexation with 1 mM sodium bicarbonate in batch experiments; a decrease of U concentration in solution was observed over time in these experiments likely due to re-association with sediments in the reactor. The findings from this study provide new insights about how hydrologic events may affect the reactivity of U present in mine waste solids exposed to surface oxidizing conditions, and the influence of organic-rich sediments on U accumulation in the Rio Paguate.
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.
Rare-earth element fractionation in uranium ore and its U(VI) alteration minerals
Balboni, Enrica; Spano, T; Cook, N; ...
2017-10-20
We developed a cation exchange chromatography method employing sulfonated polysterene cation resin (DOWEX AG50-X8) in order to separate rare-earth elements (REEs) from uranium-rich materials. The chemical separation scheme is designed to reduce matrix effects and consequently yield enhanced ionization efficiencies for concentration determinations of REEs without significant fractionation using solution mode-inductively coupled plasma mass spectrometry (ICP-MS) analysis. This method was then applied to determine REE abundances in four uraninite (ideally UO 2) samples and their associated U(VI) alteration minerals. In three of the samples analyzed, the concentration of REEs for primary uraninite are higher than those for their corresponding secondarymore » uranium alteration phases. The results for U(VI) alteration minerals of two samples indicate enrichment of the light REEs (LREEs) over the heavy REEs (HREEs). This differential mobilization is attributed to differences in the mineralogical composition of the U(VI) alteration. There is a lack of fractionation of the LREEs in the uraninite alteration rind that is composed of U(VI) minerals containing Ca 2+ as the interlayer cation (uranophane and bequerelite); contrarily, U(VI) alteration minerals containing K + and Pb 2+ as interlayer cations (fourmarierite, dumontite) indicate fractionation (enrichment) of the LREEs. Our results have implications for nuclear forensic analyses since a comparison is reported between the REE abundances for the CUP-2 (processed uranium ore) certified reference material and previously determined values for uranium ore concentrate (UOC) produced from the same U deposit (Blind River/Elliott Lake, Canada). UOCs represent the most common form of interdicted nuclear material and consequently is material frequently targeted for forensic analysis. The comparison reveals similar chondrite normalized REE signatures but variable absolute abundances. Based on the results reported here, the latter may be attributed to the differing REE abundances between primary ore and associated alteration phases, and/or is related to varying fabrication processes adopted during production of UOC.« less
Rare-earth element fractionation in uranium ore and its U(VI) alteration minerals
DOE Office of Scientific and Technical Information (OSTI.GOV)
Balboni, Enrica; Spano, T; Cook, N
We developed a cation exchange chromatography method employing sulfonated polysterene cation resin (DOWEX AG50-X8) in order to separate rare-earth elements (REEs) from uranium-rich materials. The chemical separation scheme is designed to reduce matrix effects and consequently yield enhanced ionization efficiencies for concentration determinations of REEs without significant fractionation using solution mode-inductively coupled plasma mass spectrometry (ICP-MS) analysis. This method was then applied to determine REE abundances in four uraninite (ideally UO 2) samples and their associated U(VI) alteration minerals. In three of the samples analyzed, the concentration of REEs for primary uraninite are higher than those for their corresponding secondarymore » uranium alteration phases. The results for U(VI) alteration minerals of two samples indicate enrichment of the light REEs (LREEs) over the heavy REEs (HREEs). This differential mobilization is attributed to differences in the mineralogical composition of the U(VI) alteration. There is a lack of fractionation of the LREEs in the uraninite alteration rind that is composed of U(VI) minerals containing Ca 2+ as the interlayer cation (uranophane and bequerelite); contrarily, U(VI) alteration minerals containing K + and Pb 2+ as interlayer cations (fourmarierite, dumontite) indicate fractionation (enrichment) of the LREEs. Our results have implications for nuclear forensic analyses since a comparison is reported between the REE abundances for the CUP-2 (processed uranium ore) certified reference material and previously determined values for uranium ore concentrate (UOC) produced from the same U deposit (Blind River/Elliott Lake, Canada). UOCs represent the most common form of interdicted nuclear material and consequently is material frequently targeted for forensic analysis. The comparison reveals similar chondrite normalized REE signatures but variable absolute abundances. Based on the results reported here, the latter may be attributed to the differing REE abundances between primary ore and associated alteration phases, and/or is related to varying fabrication processes adopted during production of UOC.« less
NASA Astrophysics Data System (ADS)
Višňák, Jakub; Steudtner, Robin; Kassahun, Andrea; Hoth, Nils
2017-09-01
Natural waters' uranium level monitoring is of great importance for health and environmental protection. One possible detection method is the Time-Resolved Laser-Induced Fluorescence Spectroscopy (TRLFS), which offers the possibility to distinguish different uranium species. The analytical identification of aqueous uranium species in natural water samples is of distinct importance since individual species differ significantly in sorption properties and mobility in the environment. Samples originate from former uranium mine sites and have been provided by Wismut GmbH, Germany. They have been characterized by total elemental concentrations and TRLFS spectra. Uranium in the samples is supposed to be in form of uranyl(VI) complexes mostly with carbonate (CO32- ) and bicarbonate (HCO3- ) and to lesser extend with sulphate (SO42- ), arsenate (AsO43- ), hydroxo (OH- ), nitrate (NO3- ) and other ligands. Presence of alkaline earth metal dications (M = Ca2+ , Mg2+ , Sr2+ ) will cause most of uranyl to prefer ternary complex species, e.g. Mn(UO2)(CO3)32n-4 (n ɛ {1; 2}). From species quenching the luminescence, Cl- and Fe2+ should be mentioned. Measurement has been done under cryogenic conditions to increase the luminescence signal. Data analysis has been based on Singular Value Decomposition and monoexponential fit of corresponding loadings (for separate TRLFS spectra, the "Factor analysis of Time Series" (FATS) method) and Parallel Factor Analysis (PARAFAC, all data analysed simultaneously). From individual component spectra, excitation energies T00, uranyl symmetric mode vibrational frequencies ωgs and excitation driven U-Oyl bond elongation ΔR have been determined and compared with quasirelativistic (TD)DFT/B3LYP theoretical predictions to cross -check experimental data interpretation. Note to the reader: Several errors have been produced in the initial version of this article. This new version published on 23 October 2017 contains all the corrections.
Translocation of uranium from water to foodstuff while cooking.
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.
NASA Astrophysics Data System (ADS)
Ingham, Edwina S.; Cook, Nigel J.; Cliff, John; Ciobanu, Cristiana L.; Huddleston, Adam
2014-01-01
The common sulfide mineral pyrite is abundant throughout sedimentary uranium systems at Pepegoona, Pepegoona West and Pannikan, Lake Eyre Basin, South Australia. Combined chemical, isotopic and microstructural analysis of pyrite indicates variation in fluid composition, sulfur source and precipitation conditions during a protracted mineralization event. The results show the significant role played by pyrite as a metal scavenger and monitor of fluid changes in low-temperature hydrothermal systems. In-situ micrometer-scale sulfur isotope analyses of pyrite demonstrated broad-scale isotopic heterogeneity (δ34S = -43.9 to +32.4‰VCDT), indicative of complex, multi-faceted pyrite evolution, and sulfur derived from more than a single source. Preserved textures support this assertion and indicate a genetic model involving more than one phase of pyrite formation. Authigenic pyrite underwent prolonged evolution and recrystallization, evidenced by a genetic relationship between archetypal framboidal aggregates and pyrite euhedra. Secondary hydrothermal pyrite commonly displays hyper-enrichment of several trace elements (Mn, Co, Ni, As, Se, Mo, Sb, W and Tl) in ore-bearing horizons. Hydrothermal fluids of magmatic and meteoric origins supplied metals to the system but the geochemical signature of pyrite suggests a dominantly granitic source and also the influence of mafic rock types. Irregular variation in δ34S, coupled with oscillatory trace element zonation in secondary pyrite, is interpreted in terms of continuous variations in fluid composition and cycles of diagenetic recrystallization. A late-stage oxidizing fluid may have mobilized selenium from pre-existing pyrite. Subsequent restoration of reduced conditions within the aquifer caused ongoing pyrite re-crystallization and precipitation of selenium as native selenium. These results provide the first qualitative constraints on the formation mechanisms of the uranium deposits at Beverley North. Insights into depositional conditions and sources of both sulfide and uranium mineralization and an improved understanding of pyrite geochemistry can also underpin an effective vector for uranium exploration at Beverley North and other sedimentary systems of the Lake Eyre Basin, as well as in comparable geological environments elsewhere. Average intensity of 32S signal in counts per second × 108.Drift corrected 34S/32S prior to IMF calibration.Two-sigma propagated uncertainty on individual measurements.
Jain, Rohan; Peräniemi, Sirpa; Jordan, Norbert; Vogel, Manja; Weiss, Stephan; Foerstendorf, Harald; Lakaniemi, Aino-Maija
2018-05-24
This study demonstrated the removal and recovery of uranium(VI) in a fed-batch stirred tank reactor (STR) using waste digested activated sludge (WDAS). The batch adsorption experiments showed that WDAS can adsorb 200 (±9.0) mg of uranium(VI) per g of WDAS. The maximum adsorption of uranium(VI) was achieved even at an acidic initial pH of 2.7 which increased to a pH of 4.0 in the equilibrium state. Desorption of uranium(VI) from WDAS was successfully demonstrated from the release of more than 95% of uranium(VI) using both acidic (0.5 M HCl) and alkaline (1.0 M Na 2 CO 3 ) eluents. Due to the fast kinetics of uranium(VI) adsorption onto WDAS, the fed-batch STR was successfully operated at a mixing time of 15 min. Twelve consecutive uranium(VI) adsorption steps with an average adsorption efficiency of 91.5% required only two desorption steps to elute more than 95% of uranium(VI) from WDAS. Uranium(VI) was shown to interact predominantly with the phosphoryl and carboxyl groups of the WDAS, as revealed by in situ infrared spectroscopy and time-resolved laser-induced fluorescence spectroscopy studies. This study provides a proof-of-concept of the use of fed-batch STR process based on WDAS for the removal and recovery of uranium(VI). Copyright © 2018 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sanchez, L.G.; Cellini, R.F.
1959-01-01
The thermal decomposition of some intermediate compounds in the metallurgy of uranium such as uranium peroxide, ammonium uranate, ammonium uranium pentafluoride, uranium tetrafluoride, and UO/sub 2/, were studied using Chevenard's thermobalance. Some data on the pyrolysis of synthetic mixtures of intermediate compounds which may appear during the industrial processing are given. Thermogravimetric methods of control are suggested for use in uranium metallurgy. (tr-auth)
NASA Astrophysics Data System (ADS)
Yang, G.; Maher, K.; Caers, J.
2015-12-01
Groundwater contamination associated with remediated uranium mill tailings is a challenging environmental problem, particularly within the Colorado River Basin. To examine the effectiveness of in-situ bioremediation of U(VI), acetate injection has been proposed and tested at the Rifle pilot site. There have been several geologic modeling and simulated contaminant transport investigations, to evaluate the potential outcomes of the process and identify crucial factors for successful uranium reduction. Ultimately, findings from these studies would contribute to accurate predictions of the efficacy of uranium reduction. However, all these previous studies have considered limited model complexities, either because of the concern that data is too sparse to resolve such complex systems or because some parameters are assumed to be less important. Such simplified initial modeling, however, limits the predictive power of the model. Moreover, previous studies have not yet focused on spatial heterogeneity of various modeling components and its impact on the spatial distribution of the immobilized uranium (U(IV)). In this study, we study the impact of uncertainty on 21 parameters on model responses by means of recently developed distance-based global sensitivity analysis (DGSA), to study the main effects and interactions of parameters of various types. The 21 parameters include, for example, spatial variability of initial uranium concentration, mean hydraulic conductivity, and variogram structures of hydraulic conductivity. DGSA allows for studying multi-variate model responses based on spatial and non-spatial model parameters. When calculating the distances between model responses, in addition to the overall uranium reduction efficacy, we also considered the spatial profiles of the immobilized uranium concentration as target response. Results show that the mean hydraulic conductivity and the mineral reaction rate are the two most sensitive parameters with regard to the overall uranium reduction. But in terms of spatial distribution of immobilized uranium, initial conditions of uranium concentration and spatial uncertainty in hydraulic conductivity also become important. These analyses serve as the first step of further prediction practices of the complex uranium transport and reaction systems.
Uranium in the Wyoming Landscape Conservation Initiative study area, southwestern Wyoming
Wilson, Anna B.
2015-10-20
In the WLCI study area, all uranium areas except Poison Basin and Ketchum Buttes contain roll-front deposits in Eocene (56–34 Ma) sedimentary rocks. Tabular sandstone-hosted uranium deposits are also recognized within the study area.
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
Uranium removal from aqueous solution by coir pith: equilibrium and kinetic studies.
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.
Sandstone type uranium deposits in the Ordos Basin, Northwest China: A case study and an overview
NASA Astrophysics Data System (ADS)
Akhtar, Shamim; Yang, Xiaoyong; Pirajno, Franco
2017-09-01
This paper provides a comprehensive review on studies of sandstone type uranium deposits in the Ordos Basin, Northwest China. As the second largest sedimentary basin, the Ordos Basin has great potential for targeting sandstone type U mineralization. The newly found and explored Dongsheng and Diantou sandstone type uranium deposits are hosted in the Middle Jurassic Zhilou Formation. A large number of investigations have been conducted to trace the source rock compositions and relationship between lithic subarkose sandstone host rock and uranium mineralization. An optical microscopy study reveals two types of alteration associated with the U mineralization: chloritization and sericitization. Some unusual mineral structures, with compositional similarity to coffinite, have been identified in a secondary pyrite by SEM These mineral phases are proposed to be of bacterial origin, following high resolution mapping of uranium minerals and trace element determinations in situ. Moreover, geochemical studies of REE and trace elements constrained the mechanism of uranium enrichment, displaying LREE enrichment relative to HREE. Trace elements such as Pb, Mo and Ba have a direct relationship with uranium enrichment and can be used as index for mineralization. The source of uranium ore forming fluids and related geological processes have been studied using H, O and C isotope systematics of fluid inclusions in quartz veins and the calcite cement of sandstone rocks hosting U mineralization. Both H and O isotopic compositions of fluid inclusions reveal that ore forming fluids are a mixture of meteoric water and magmatic water. The C and S isotopes of the cementing material of sandstone suggest organic origin and bacterial sulfate reduction (BSR), providing an important clue for U mineralization. Discussion of the ore genesis shows that the greenish gray sandstone plays a crucial role during processes leading to uranium mineralization. Consequently, an oxidation-reduction model for sandstone-type uranium deposit is proposed, which can elucidate the source of uranium in the deposits of the Ordos Basin, based on the role of organic materials and sulfate reducing bacteria. We discuss the mechanism of uranium deposition responsible for the genesis of these large sandstone type uranium deposits in this unique sedimentary basin.
Cancer risk in nuclear workers occupationally exposed to uranium-emphasis on internal exposure.
Canu, Irina Guseva; Ellis, Elizabeth Dupree; Tirmarche, Margot
2008-01-01
Workers involved in the nuclear fuel cycle have a potential for internal exposure to uranium. The present review of epidemiological studies of these workers aims to elucidate the relationship between occupational internal uranium exposure and cancer risk. Eighteen cohort and 5 nested case-control studies published since 1980 are reviewed. Workers occupationally exposed to uranium appear to be at increased risk of mortality from neoplasms of the lung, larynx, and lymphatic and haematopoietic tissue. Currently available evidence for a positive association between internal exposure to uranium and the risk of cancer is limited. The common weaknesses in reviewed studies include low statistical power and inaccurate assessment of internal exposure to uranium. Further investigations should focus on precise assessment of occupational exposure and address the issue of potential confounders.
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.
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.
Amidoxime Polymers for Uranium Adsorption: Influence of Comonomers and Temperature
Wiechert, Alexander I.; Das, Sadananda; Yiacoumi, Sotira
2017-01-01
Recovering uranium from seawater has been the subject of many studies for decades, and has recently seen significant progress in materials development since the U.S. Department of Energy (DOE) has become involved. With DOE direction, the uranium uptake for amidoxime-based polymer adsorbents has more than tripled in capacity. In an effort to better understand how these new adsorbent materials behave under different environmental stimuli, several experimental and modeling based studies have been employed to investigate impacts of competing ions, salinity, pH, and other factors on uranium uptake. For this study, the effect of temperature and type of comonomer on uranium adsorption by three different amidoxime adsorbents (AF1, 38H, AI8) was examined. Experimental measurements of uranium uptake were taken in 1−L batch reactors from 10 to 40 °C. A chemisorption model was developed and applied in order to estimate unknown system parameters through optimization. Experimental results demonstrated that the overall uranium chemisorption process for all three materials is endothermic, which was also mirrored in the model results. Model simulations show very good agreement with the data and were able to predict the temperature effect on uranium adsorption as experimental conditions changed. This model may be used for predicting uranium uptake by other amidoxime materials. PMID:29113060
Spectral Induced Polarization Response of Biofilm Formation in Hanford Vadose Zone Sediment
NASA Astrophysics Data System (ADS)
Garcia, A.; Katsenovich, Y.; Lee, B.; Whitman, D.
2017-12-01
As a result of the U.S. Nuclear weapons program during the second world war and the cold war, there now exists a significant amount of uranium contamination at the U.S. Department of Energy Hanford site located in Washington state. In-situ immobilization of mobile uranium via injections of a soluble sodium tripolyphosphate amendment may prove effective in the formation of insoluble uranyl phosphate mineral, autunite. However, the injected polyphosphate undergoes hydrolysis in aqueous solutions to form orthophosphate, which serves as a readily available nutrient for the various microorganisms in the sediment. Sediment-filled column experiments conducted under saturated oxygen restricted conditions using geophysical Spectral Induced Polarization technique have shown the impact of microbes on the dissolution of autunite, a calcium uranyl phosphate mineral. Spectral Induced Polarization may be an effective way to track changes indicative of bacterial activities on the surrounding environment. This method can be a cost-effective alternative to the drilling of boreholes at a field scale.
NASA Astrophysics Data System (ADS)
Sharma, S. P.; Biswas, A.
2012-12-01
South Purulia Shear Zone (SPSZ) is an important region for prospecting of uranium mineralization. Geological studies and hydro-uranium anomaly suggest the presence of Uranium deposit around Raghunathpur village which lies about 8 km north of SPSZ. However, detailed geophysical investigations have not been carried out in this region for investigation of uranium mineralization. Since surface signature of uranium mineralization is not depicted near the location, a deeper subsurface source is expected for hydro uranium anomaly. To delineate the subsurface structure and to investigate the origin of hydro-uranium anomaly present in the area, Vertical Electrical Sounding (VES) using Schlumberger array and Gradient Resistivity Profiling (GRP) were performed at different locations along a profile perpendicular to the South Purulia Shear Zone. Apparent resistivity computed from the measured sounding data at various locations shows a continuously increasing trend. As a result, conventional apparent resistivity data is not able to detect the possible source of hydro uranium anomaly. An innovative approach is applied which depicts the apparent conductivity in the subsurface revealed a possible connection from SPSZ to Raghunathpur. On the other hand resistivity profiling data suggests a low resistive zone which is also characterized by low Self-Potential (SP) anomaly zone. Since SPSZ is characterized by the source of uranium mineralization; hydro-uranium anomaly at Raghunathpur is connected with the SPSZ. The conducting zone has been delineated from SPSZ to Raghunathpur at deeper depths which could be uranium bearing. Since the location is also characterized by a low gravity and high magnetic anomaly zone, this conducting zone is likely to be mineralized zone. Keywords: Apparent resistivity; apparent conductivity; Self Potential; Uranium mineralization; shear zone; hydro-uranium anomaly.
Preparation and biosorption evaluation of Bacillus subtilis/alginate–chitosan microcapsule
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
Bicarbonate Impact on U(VI) Bioreduction in a Shallow Alluvial Aquifer
DOE Office of Scientific and Technical Information (OSTI.GOV)
Long, Philip E.; Williams, Kenneth H.; Davis, James A.
Field-scale biostimulation and desorption tracer experiments conducted in a uranium (U) contaminated, shallow alluvial aquifer have provided insight into the coupling of microbiology, biogeochemistry, and hydrogeology that control U mobility in the subsurface. Initial experiments successfully tested the concept that Fe-reducing bacteria such as Geobacter sp. could enzymatically reduce soluble U(VI) to insoluble U(IV) during in situ electron donor amendment (Anderson et al. 2003, Williams et al. 2011). In parallel, in situ desorption tracer tests using bicarbonate amendment demonstrated rate-limited U(VI) desorption (Fox et al. 2012). These results and prior laboratory studies underscored the importance of enzymatic U(VI)-reduction and suggestedmore » the ability to combine desorption and bioreduction of U(VI). Here we report the results of a new field experiment in which bicarbonate-promoted uranium desorption and acetate amendment were combined and compared to an acetate amendment-only experiment in the same experimental plot. Results confirm that bicarbonate amendment to alluvial aquifer desorbs U(VI) and increases the abundance of Ca-uranyl-carbonato complexes. At the same time, that the rate of acetate-promoted enzymatic U(VI) reduction was greater in the presence of added bicarbonate in spite of the increased dominance of Ca-uranyl-carbonato aqueous complexes. A model-simulated peak rate of U(VI) reduction was ~3.8 times higher during acetate-bicarbonate treatment than under acetate-only conditions. Lack of consistent differences in microbial community structure between acetate-bicarbonate and acetate-only treatments suggest that a significantly higher rate of U(VI) reduction the bicarbonate-impacted sediment may be due to a higher intrinsic rate of microbial reduction induced by elevated concentrations of the bicarbonate oxyanion. The findings indicate that bicarbonate amendment may be useful in improving the engineered bioremediation of uranium in aquifers.« less
Bicarbonate impact on U(VI) bioreduction in a shallow alluvial aquifer
NASA Astrophysics Data System (ADS)
Long, Philip E.; Williams, Kenneth H.; Davis, James A.; Fox, Patricia M.; Wilkins, Michael J.; Yabusaki, Steven B.; Fang, Yilin; Waichler, Scott R.; Berman, Elena S. F.; Gupta, Manish; Chandler, Darrell P.; Murray, Chris; Peacock, Aaron D.; Giloteaux, Ludovic; Handley, Kim M.; Lovley, Derek R.; Banfield, Jillian F.
2015-02-01
Field-scale biostimulation and desorption tracer experiments conducted in a uranium (U) contaminated, shallow alluvial aquifer have provided insight into the coupling of microbiology, biogeochemistry, and hydrogeology that control U mobility in the subsurface. Initial experiments successfully tested the concept that Fe-reducing bacteria such as Geobacter sp. could enzymatically reduce soluble U(VI) to insoluble U(IV) during in situ electron donor amendment (Anderson et al., 2003; Williams et al., 2011). In parallel, in situ desorption tracer tests using bicarbonate amendment demonstrated rate-limited U(VI) desorption (Fox et al., 2012). These results and prior laboratory studies underscored the importance of enzymatic U(VI)-reduction and suggested the ability to combine desorption and bioreduction of U(VI). Here we report the results of a new field experiment in which bicarbonate-promoted uranium desorption and acetate amendment were combined and compared to an acetate amendment-only experiment in the same experimental plot. Results confirm that bicarbonate amendment to alluvial aquifer sediments desorbs U(VI) and increases the abundance of Ca-uranyl-carbonato complexes. At the same time, the rate of acetate-promoted enzymatic U(VI) reduction was greater in the presence of added bicarbonate in spite of the increased dominance of Ca-uranyl-carbonato aqueous complexes. A model-simulated peak rate of U(VI) reduction was ∼3.8 times higher during acetate-bicarbonate treatment than under acetate-only conditions. Lack of consistent differences in microbial community structure between acetate-bicarbonate and acetate-only treatments suggest that a significantly higher rate of U(VI) reduction in the bicarbonate-impacted sediment may be due to a higher intrinsic rate of microbial reduction induced by elevated concentrations of the bicarbonate oxyanion. The findings indicate that bicarbonate amendment may be useful in improving the engineered bioremediation of uranium in aquifers.
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
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
Role of U(VI) Reduction by Geobacter species
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lovely, Derrick
2008-12-23
Previous work had suggested that Acholeplasma palmae has a higher capacity for uranium sorption than other bacteria studied. Sorption studies were performed with cells in suspension in various solutions containing uranium, and results were used to generate uranium-biosorption isotherms. Results from this study showed that the U(VI) sorption capacity of G. uraniireducens was relatively similar in simple solutions, such as sodium chloride or bicarbonate. However, this ability to sorb uranium significantly decreased in groundwater. This suggested that certain chemicals present in the groundwater were inhibiting the ability of cell components of Geobacter to adsorb uranium. It was hypothesized that uraniummore » removal would also be diminished in the bicarbonate solution. However, this did not seem to be the case, as uranium was as easily removed in the bicarbonate solution as in the sodium chloride solution.« less
URANIUM IN ROCK MINERALS OF THE INTRUSION OF KYZL-OMPUL MOUNTAINS (NORTH KIRGISIA) (in Russian)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Leonova, L.L.; Pogiblova, L.S.
1961-01-01
The uranium distribution in rock minerals (syenites, granosyenites, and alaskite granites) of the Kyzyl-Ompul raassif is studied. Alaskite granites are characterized by the granite type of uranium distribution in minerals, about 50 percent of this element being connected with rockforming and about 50 percent with accessory uranium minerals. ln syenites uranium (about 70 percent) is bound to rockforming minerals. The same minerals from syenites and granites strongly differ by their uranium content and are constant in the ranges of each of those rock types. Granosyenites have aa intermediate (between syenites and granites) type of uranium distribution in minerals. (auth)
Dangelmayr, Martin A.; Reimus, Paul W.; Wasserman, Naomi L.; ...
2017-05-01
The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47more » relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dangelmayr, Martin A.; Reimus, Paul W.; Wasserman, Naomi L.
The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47more » relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.« less
Effect of nephrotoxic treatment with gentamicin on rats chronically exposed to uranium.
Rouas, Caroline; Stefani, Johanna; Grison, Stéphane; Grandcolas, Line; Baudelin, Cédric; Dublineau, Isabelle; Pallardy, Marc; Gueguen, Yann
2011-01-11
Uranium is a radioactive heavy metal with a predominantly chemical toxicity, affecting especially the kidneys and more particularly the proximal tubular structure. Until now, few experimental studies have examined the effect of chronic low-dose exposure to uranium on kidney integrity: these mainly analyse standard markers such as creatinine and urea, and none has studied the effect of additional co-exposure to a nephrotoxic agent on rats chronically exposed to uranium. The aim of the present study is to examine the potential cumulative effect of treating uranium-exposed rats with a nephrotoxic drug. Neither physiological indicators (diuresis and creatinine clearance) nor standard plasma and urine markers (creatinine, urea and total protein) levels were deteriorated when uranium exposure was combined with gentamicin-induced nephrotoxicity. A histological study confirmed the preferential impact of gentamicin on the tubular structure and showed that uranium did not aggravate the histopathological renal lesions. Finally, the use of novel markers of kidney toxicity, such as KIM-1, osteopontin and kallikrein, provides new knowledge about the nephrotoxicity threshold of gentamicin, and allows us to conclude that under our experimental conditions, low dose uranium exposure did not induce signs of nephrotoxicity or enhance renal sensitivity to another nephrotoxicant. Copyright © 2010 Elsevier Ireland Ltd. All rights reserved.
Gao, Lidi; Kano, Naoki; Sato, Yuichi; Li, Chong; Zhang, Shuang; Imaizumi, Hiroshi
2012-01-01
In order to investigate the behavior, distribution, and characteristics of heavy metals including rare earth elements (REEs), thorium (Th), and uranium (U) in sludge, the total and fractional concentrations of these elements in sludge collected from an industry water treatment plant were determined and compared with those in natural soil. In addition, the removal/recovery process of heavy metals (Pb, Cr, and Ni) from the polluted sludge was studied with biosurfactant (saponin and sophorolipid) elution by batch and column experiments to evaluate the efficiency of biosurfactant for the removal of heavy metals. Consequently, the following matters have been largely clarified. (1) Heavy metallic elements in sludge have generally larger concentrations and exist as more unstable fraction than those in natural soil. (2) Nonionic saponin including carboxyl group is more efficient than sophorolipid for the removal of heavy metals in polluted sludge. Saponin has selectivity for the mobilization of heavy metals and mainly reacts with heavy metals in F3 (the fraction bound to carbonates) and F5 (the fraction bound to Fe-Mn oxides). (3) The recovery efficiency of heavy metals (Pb, Ni, and Cr) reached about 90–100% using a precipitation method with alkaline solution. PMID:22693485
INTERACTIONS AMONG PHOSPHATE AMENDMENTS, MICROBES AND URANIUM MOBILITY IN CONTAMINATED SEDIMENTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Knox, A
2007-08-30
The use of sequestering agents for the transformation of radionuclides in low concentrations in contaminated soils/sediments offers considerable potential for long-term environmental cleanup. This study evaluated the influence of four phosphate amendments and two microbial amendments on U availability. The synchrotron X-ray fluorescence mapping of the untreated U-contaminated sediment showed that U was closely associated with Mn. All tested phosphate amendments reduced aqueous U concentration more than 90%, likely due to formation of insoluble phosphate precipitates. The addition of A. piechaudii and P. putida alone were found to reduce U concentrations 63% and 31% respectively. Uranium sorption in phosphate treatmentsmore » was significantly reduced in the presence of microbes. However, increased microbial activity in the treated sediment led to reduction of phosphate effectiveness. The average U concentration in 1 M MgCl{sub 2} extract from U amended sediment was 437 {micro}g/kg, but in the same sediment without microbes (autoclaved sediment), the extractable U concentration was only 103 {micro}g/kg. When the autoclaved amended sediment was treated with autoclaved biological apatite, U concentration in the 1 M MgCl{sub 2} extract was {approx}0 {micro}g/kg. Together these tests suggest that microbes may enhance U leaching and reduce phosphate amendment remedial effectiveness.« less
Otton, J.K.; Zielinski, R.A.; Been, J.M.
1989-01-01
Uraniferous Holocene sediments occur in the Carson Range of Nevada and California, U.S.A., between Lake Tahoe and Carson Valley. The hosts for the uranium include peat and interbedded organic-rich sand, silt, and mud that underly valley floors, fens, and marshes along stream valleys between the crest of the range and the edge of Lake Tahoe. The known uranium accumulations extend along the Carson Range from the area just southeast of South Lake Tahoe northward to the area just east of Carson City; however, they almost certainly continue beyond the study area to the north, west, and south. Due to the young age of the accumulations, uranium in them is in gross disequilibrium with its highly radioactive daughter products. These accumulations have thus escaped discovery with radiation detection equipment in the past. The uranium content of these sediments approaches 0.6 percent; however, the average is in the range of 300-500 ppm. Waters associated with these sediments locally contain as much as 177 ppb uranium. Modest levels of helium and radon also occur in these waters. Uraniferous waters are clearly entering the private and public water supply systems in some parts of the study area; however, it is not known how much uranium is reaching users of these water supplies. Many of the waters sampled in the study area exceed the published health effects guidance level of the Environmental Protection Agency. Regulatory standards for uranium in waters have not been published, however. Much uranium is stored in the sediments along these stream valleys. Estimates for a marsh and a fen along one drainage are 24,000 and 15,000 kg, respectively. The potential effects of man-induced environmental changes on the uranium are uncertain. Laboratory studies of uraniferous sediment rich in organic matter may allow us to evaluate the potential of liberating uranium from such sediments and creating transient increases in the level of uranium moving in water in the natural environment. ?? 1989 Springer-Verlag New York Inc.
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
Uranium in groundwater--Fertilizers versus geogenic sources.
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.
Enriched but not depleted uranium affects central nervous system in long-term exposed rat.
Houpert, Pascale; Lestaevel, Philippe; Bussy, Cyrill; Paquet, François; Gourmelon, Patrick
2005-12-01
Uranium is well known to induce chemical toxicity in kidneys, but several other target organs, such as central nervous system, could be also affected. Thus in the present study, the effects on sleep-wake cycle and behavior were studied after chronic oral exposure to enriched or depleted uranium. Rats exposed to 4% enriched uranium for 1.5 months through drinking water, accumulated twice as much uranium in some key areas such as the hippocampus, hypothalamus and adrenals than did control rats. This accumulation was correlated with an increase of about 38% of the amount of paradoxical sleep, a reduction of their spatial working memory capacities and an increase in their anxiety. Exposure to depleted uranium for 1.5 months did not induce these effects, suggesting that the radiological activity induces the primary events of these effects of uranium.
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.
Raoultella sp. SM1, a novel iron-reducing and uranium-precipitating strain.
Sklodowska, Aleksandra; Mielnicki, Sebastian; Drewniak, Lukasz
2018-03-01
The main aim of this study was the characterisation of novel Raoutella isolate, an iron-reducing and uranium-precipitating strain, originating from microbial mats occurring in the sediments of a closed down uranium mine in Kowary (SW Poland). Characterisation was done in the context of its potential role in the functioning of these mats and the possibility to use them in uranium removal/recovery processes. In our experiment, we observed the biological precipitation of iron and uranium's secondary minerals containing oxygen, potassium, sodium and phosphor, which were identified as ningyoite-like minerals. The isolated strain, Raoultella sp. SM1, was also able to dissimilatory reduce iron (III) and uranium (VI) in the presence of citrate as an electron donor. Our studies allowed us to characterise a new strain which may be used as a model microorganism in the study of Fe and U respiratory processes and which may be useful in the bioremediation of uranium-contaminated waters and sediments. During this process, uranium may be immobilised in ningyoite-like minerals and can then be recovered in nano/micro-particle form, which may be easily transformed to uraninite. Copyright © 2017 Elsevier Ltd. All rights reserved.
Uranium in drinking water: renal effects of long-term ingestion by an aboriginal community.
Zamora, Maria L Limson; Zielinski, Jan M; Moodie, Gerry B; Falcomer, Renato A F; Hunt, Wendy C; Capello, Kevin
2009-01-01
The authors conducted a study of an aboriginal community to determine if kidney func-tion had been affected by the chronic ingestion of uranium in drinking water from the community's drilled wells. Uranium concentrations in drinking water varied from < 1 to 845 ppb. This nonin-vasive study relied on the measurement of a combination of urinary indicators of kidney function and markers for cell toxicity. In all, 54 individuals (12-73 years old) participated in the study. Correlation of uranium excreted in urine with bio-indicators at p
Williamson, Adam J; Morris, Katherine; Law, Gareth T W; Rizoulis, Athanasios; Charnock, John M; Lloyd, Jonathan R
2014-11-18
Although there is consensus that microorganisms significantly influence uranium speciation and mobility in the subsurface under circumneutral conditions, microbiologically mediated U(VI) redox cycling under alkaline conditions relevant to the geological disposal of cementitious intermediate level radioactive waste, remains unexplored. Here, we describe microcosm experiments that investigate the biogeochemical fate of U(VI) at pH 10-10.5, using sediments from a legacy lime working site, stimulated with an added electron donor, and incubated in the presence and absence of added Fe(III) as ferrihydrite. In systems without added Fe(III), partial U(VI) reduction occurred, forming a U(IV)-bearing non-uraninite phase which underwent reoxidation in the presence of air (O2) and to some extent nitrate. By contrast, in the presence of added Fe(III), U(VI) was first removed from solution by sorption to the Fe(III) mineral, followed by bioreduction and (bio)magnetite formation coupled to formation of a complex U(IV)-bearing phase with uraninite present, which also underwent air (O2) and partial nitrate reoxidation. 16S rRNA gene pyrosequencing showed that Gram-positive bacteria affiliated with the Firmicutes and Bacteroidetes dominated in the post-reduction sediments. These data provide the first insights into uranium biogeochemistry at high pH and have significant implications for the long-term fate of uranium in geological disposal in both engineered barrier systems and the alkaline, chemically disturbed geosphere.
NASA Astrophysics Data System (ADS)
Bajabaa, S. A.; Abd El-Naby, H.; Dawood, Y.
2009-12-01
The fate and transport of heavy metals and radioelements in groundwater aquifers in five wadis located in the Al Qunfudhah and Wadi Haliy quadrangles were investigated. These wadis are an important source of water to the Red Sea coastal plain. Copper, zinc and other base-metals mineralization occur at eastern parts of these quadrangles that dominates the water catchments area of these wadis. Water, rock and soil samples were collected from all wadis and they were analyzed for major, trace elements, heavy metals and stable isotopes. The chemical and isotopic results showed active water/rock interaction. The preliminary investigation of the data analyses showed some samples with high heavy metals and uranium contents. Generally, the uranium and heavy metal contents are higher in samples collected from the upstream area of each wadi where the crystalline rocks are exposed and direct contact with the runoff. The uranium contents were as high as 120 ppb in some water samples. These elevated values are mainly due to two factors water rock interaction and concentration through evaporation. It was also observed to have elevated heavy metal contents near mining activates, which suggests that these mining activates are playing an important role in mobilizing the heavy elements and in turn affecting the water quality in these wadis.
NASA Astrophysics Data System (ADS)
Dillard, J. G.; Moers, H.; Klewe-Nebenius, H.; Kirch, G.; Pfennig, G.; Ache, H. J.
1984-09-01
The adsorption of methyl iodide on uranium and on uranium dioxide has been studied at 25 °C. Surfaces of the substrates were characterized before and after adsorption by X-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy (AES). The XPS binding energy results indicate that CH 3I adsorption on uranium yields a carbide-type carbon, UC, and uranium iodide, UI 3. On uranium dioxide the carbon electron binding energy measurements are consistent with the formation of a hydrocarbon, —CH 3-type moiety. The interpretation of XPS and AES spectral features for CH 3I adsorption on uranium suggest that a complex dissociative adsorption reaction takes place. Adsorption of CH 3I on UO 2 occurs via a dissociative process. Saturation coverage occurs on uranium at approximately two langmuir (1 L = 10 -6 Torr s) exposure whereas saturation coverage on uranium dioxide is found at about five langmuir.
Absorption of Thermal Neutrons in Uranium
DOE R&D Accomplishments Database
Creutz, E. C.; Wilson, R. R.; Wigner, E. P.
1941-09-26
A knowledge of the absorption processes for neutrons in uranium is important for planning a chain reaction experiment. The absorption of thermal neutrons in uranium and uranium oxide has been studied. Neutrons from the cyclotron were slowed down by passage through a graphite block. A uranium or uranium oxide sphere was placed at various positions in the block. The neutron intensity at different points in the sphere and in the graphite was measured by observing the activity induced in detectors or uranium oxide or manganese. It was found that both the fission activity in the uranium oxide and the activity induced in manganese was affected by non-thermal neutrons. An experimental correction for such effects was made by making measurements with the detectors surrounded by cadmium. After such corrections the results from three methods of procedure with the uranium oxide detectors and from the manganese detectors were consistent to within a few per cent.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gartman, Brandy N.; Qafoku, Nikolla
2016-03-09
Uranium (U) contaminated subsurface systems are common on a global scale mainly because of its essential role in the production of plutonium for nuclear weapons and other nuclear energy and research activities. Studying the behavior and fate of U in these systems is challenging because of heterogeneities of different types (i.e., physical, chemical and mineralogical) and a complex network of often time-dependent hydrological, biological and chemical reactions and processes that occur sequentially or simultaneously, affecting and/or controlling U mobility. A U contaminated site, i.e., the Integrated Field Research Challenge site in Rifle, CO, USA (a former U mill site) ismore » the focus of this discussion. The overall objectives of this chapter are to 1) provide an overview of the contamination levels (U and other co-contaminants) at this field site; 2) review and discuss different aspects of mineral-U contaminant interactions in reduced and oxidized environments, and in the presence of co-contaminants; 3) present results from a systematic macroscopic, microscopic, and spectroscopic study as an example of the current research efforts and the state-of-knowledge in this important research area; and 4) offer insightful conclusive remarks and future research needs about reactions and processes that control U and other contaminants’ fate and behavior under hydraulically saturated conditions. The implications and applications presented in this chapter are valid for U contaminated sites across the world.« less
NASA Astrophysics Data System (ADS)
Ye, Fa-wang; Liu, De-chang
2008-12-01
Practices of sandstone-type uranium exploration in recent years in China indicate that the uranium mineralization alteration information is of great importance for selecting a new uranium target or prospecting in outer area of the known uranium ore district. Taking a case study of BASHIBULAKE uranium ore district, this paper mainly presents the technical minds and methods of extracting the reduced alteration information by oil and gas in BASHIBULAKE ore district using ASTER data. First, the regional geological setting and study status in BASHIBULAKE uranium ore district are introduced in brief. Then, the spectral characteristics of altered sandstone and un-altered sandstone in BASHIBULAKE ore district are analyzed deeply. Based on the spectral analysis, two technical minds to extract the remote sensing reduced alteration information are proposed, and the un-mixing method is introduced to process ASTER data to extract the reduced alteration information in BASHIBULAKE ore district. From the enhanced images, three remote sensing anomaly zones are discovered, and their geological and prospecting significances are further made sure by taking the advantages of multi-bands in SWIR of ASTER data. Finally, the distribution and intensity of the reduced alteration information in Cretaceous system and its relationship with the genesis of uranium deposit are discussed, the specific suggestions for uranium prospecting orientation in outer of BASHIBULAKE ore district are also proposed.
Exposure assessment of natural uranium from drinking water.
Jakhu, Rajan; Mehra, Rohit; Mittal, H M
2016-12-08
The uranium concentration in the drinking water of the residents of the Jaipur and Ajmer districts of Rajasthan has been measured for exposure assessment. The daily intake of uranium from the drinking water for the residents of the study area is found to vary from 0.4 to 123.9 μg per day. For the average uranium ingestion rate of 35.2 μg per day for a long term exposure period of 60 years, estimations have been made for the retention of uranium in different body organs and its excretion with time using ICRP's biokinetic model of uranium. Radioactive and chemical toxicity of uranium has been reported and discussed in detail in the present manuscript.
Biosorption characteristics of Uranium (VI) from aqueous solution by pollen pini.
Wang, Feihong; Tan, Lichao; Liu, Qi; Li, Rumin; Li, Zhanshuang; Zhang, Hongsen; Hu, Songxia; Liu, Lianhe; Wang, Jun
2015-12-01
Uranium biosorption from aqueous solutions by pollen pini (Pinus massoniana pollen) was studied in a bath system. The biosorbent was characterized by Fourier-transform infrared spectroscopy and scanning electron microscope. The influences of pH, contact time and initial uranium concentration at room temperature were investigated and the experimental curves were obtained. The pollen pini exhibited the highest uranium sorption capacity at pH 5.0 after 2 h contact. At pH 2.5 pollen pini also exhibited a good uranium loading capacity (>15%). Therefore biosorption characteristics of uranium from aqueous solution onto pollen pini were examined at pH 2.5 as well. The kinetics followed a pseudo-second-order rate equation and adsorption process was well fitted with the Freundlich isotherm at both pH. The adsorption of uranium by the biosorbent was confirmed by energy dispersive spectroscopy. The present study suggested that pollen pini could be a suitable biosorbent for biosorption uranium (VI) from aqueous solution in a fast, low cost and convenient approach. Copyright © 2015 Elsevier Ltd. All rights reserved.
Role of U(VI) Adsorption in U(VI) Reduction by Geobacter Species.
DOE Office of Scientific and Technical Information (OSTI.GOV)
None, None
2009-03-09
Previous work had suggested that Acholeplasma palmae has a higher capacity for uranium sorption than other bacteria studied. Sorption studies were performed with cells in suspension in various solutions containing uranium and results were used to generate uranium-biosorption isotherms.
Identification of Uranyl Minerals Using Oxygen K-Edge X Ray Absorption Spectroscopy
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ward, Jesse D.; Bowden, Mark E.; Resch, Charles T.
2016-03-01
Uranium analysis is consistently needed throughout the fuel cycle, from mining to fuel fabrication to environmental monitoring. Although most of the world’s uranium is immobilized as pitchblende or uraninite, there exists a plethora of secondary uranium minerals, nearly all of which contain the uranyl cation. Analysis of uranyl compounds can provide clues as to a sample’s facility of origin and chemical history. X-ray absorption spectroscopy is one technique that could enhance our ability to identify uranium minerals. Although there is limited chemical information to be gained from the uranium X-ray absorption edges, recent studies have successfully used ligand NEXAFS tomore » study the physical chemistry of various uranium compounds. This study extends the use of ligand NEXAFS to analyze a suite of uranium minerals. We find that major classes of uranyl compounds (carbonate, oxyhydroxide, silicate, and phosphate) exhibit characteristic lineshapes in the oxygen K-edge absorption spectra. As a result, this work establishes a library of reference spectra that can be used to classify unknown uranyl minerals.« less
Amidoxime Polymers for Uranium Adsorption: Influence of Comonomers and Temperature
Ladshaw, Austin P.; Wiechert, Alexander I.; Das, Sadananda; ...
2017-11-04
Recovering uranium from seawater has been the subject of many studies for decades, and has recently seen significant progress in materials development since the U.S. Department of Energy (DOE) has become involved. With DOE direction, the uranium uptake for amidoxime-based polymer adsorbents has more than tripled in capacity. In an effort to better understand how these new adsorbent materials behave under different environmental stimuli, several experimental and modeling based studies have been employed to investigate impacts of competing ions, salinity, pH, and other factors on uranium uptake. For this study, the effect of temperature and type of comonomer on uraniummore » adsorption by three different amidoxime adsorbents (AF1, 38H, AI8) was examined. Experimental measurements of uranium uptake were taken in 1–L batch reactors from 10 to 40 °C. A chemisorption model was developed and applied in order to estimate unknown system parameters through optimization. Experimental results demonstrated that the overall uranium chemisorption process for all three materials is endothermic, which was also mirrored in the model results. Model simulations show very good agreement with the data and were able to predict the temperature effect on uranium adsorption as experimental conditions changed. Here, this model may be used for predicting uranium uptake by other amidoxime materials.« less
Amidoxime Polymers for Uranium Adsorption: Influence of Comonomers and Temperature
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ladshaw, Austin P.; Wiechert, Alexander I.; Das, Sadananda
Recovering uranium from seawater has been the subject of many studies for decades, and has recently seen significant progress in materials development since the U.S. Department of Energy (DOE) has become involved. With DOE direction, the uranium uptake for amidoxime-based polymer adsorbents has more than tripled in capacity. In an effort to better understand how these new adsorbent materials behave under different environmental stimuli, several experimental and modeling based studies have been employed to investigate impacts of competing ions, salinity, pH, and other factors on uranium uptake. For this study, the effect of temperature and type of comonomer on uraniummore » adsorption by three different amidoxime adsorbents (AF1, 38H, AI8) was examined. Experimental measurements of uranium uptake were taken in 1–L batch reactors from 10 to 40 °C. A chemisorption model was developed and applied in order to estimate unknown system parameters through optimization. Experimental results demonstrated that the overall uranium chemisorption process for all three materials is endothermic, which was also mirrored in the model results. Model simulations show very good agreement with the data and were able to predict the temperature effect on uranium adsorption as experimental conditions changed. Here, this model may be used for predicting uranium uptake by other amidoxime materials.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Penley, H.M.; Schot, E.H.; Sewell, J.M.
1978-11-01
Three sheared areas in the crystalline Piedmont and Blue Ridge provinces, from which uranium occurrences or anomalous radioactivity have been reported, were studied to determine their favorability for uranium mineralization. The study, which involved a literature review, geologic reconnaissance, ground radiometric surveys, and sampling of rock outcrops for petrographic and chemical analyses, indicates that more-detailed investigations of these and similar areas are warranted. In each area, surface leaching and deep residual cover make it difficult to assess the potential for uranium mineralization on the basis of results from chemical analyses for U/sub 3/O/sub 8/ and the radiometric surveys. Although anomalousmore » radioactivity and anomalous chemical uranium values were noted in only a few rock exposures and samples from the shear zones, the potential for uranium mineralization at depth could be much greater than indicated by these surface data. The study indicates that shear zones within Precambiran granitic basement complexes (such as the Wilson Creek Gneiss of western North Carolina, the Cranberry Gneiss of eastern Tennessee, and the Toxaway Gneiss of western South Carolina) are favorable as hosts for uranium and may contain subsurface deposits. Mylonitized graphitic schists immediately north of the Towaliga fault in Alabama and Georgia may be favorable host rocks for uranium.« less
Equilibrium, kinetic and thermodynamic studies of uranium biosorption by calcium alginate beads.
Bai, Jing; Fan, Fangli; Wu, Xiaolei; Tian, Wei; Zhao, Liang; Yin, Xiaojie; Fan, Fuyou; Li, Zhan; Tian, Longlong; Wang, Yang; Qin, Zhi; Guo, Junsheng
2013-12-01
Calcium alginate beads are potential biosorbent for radionuclides removal as they contain carboxyl groups. However, until now limited information is available concerning the uptake behavior of uranium by this polymer gel, especially when sorption equilibrium, kinetics and thermodynamics are concerned. In present work, batch experiments were carried out to study the equilibrium, kinetics and thermodynamics of uranium sorption by calcium alginate beads. The effects of initial solution pH, sorbent amount, initial uranium concentration and temperature on uranium sorption were also investigated. The determined optimal conditions were: initial solution pH of 3.0, added sorbent amount of 40 mg, and uranium sorption capacity increased with increasing initial uranium concentration and temperature. Equilibrium data obtained under different temperatures were fitted better with Langmuir model than Freundlich model, uranium sorption was dominated by a monolayer way. The kinetic data can be well depicted by the pseudo-second-order kinetic model. The activation energy derived from Arrhenius equation was 30.0 kJ/mol and the sorption process had a chemical nature. Thermodynamic constants such as ΔH(0), ΔS(0) and ΔG(0) were also evaluated, results of thermodynamic study showed that the sorption process was endothermic and spontaneous. Copyright © 2013 Elsevier Ltd. All rights reserved.
Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements
DOE Office of Scientific and Technical Information (OSTI.GOV)
Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn
2009-03-01
Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that themore » equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.« less
National Uranium Resource Evaluation, Tularosa Quadrangle, New Mexico
DOE Office of Scientific and Technical Information (OSTI.GOV)
Berry, V.P.; Nagy, P.A.; Spreng, W.C.
1981-12-01
Uranium favorability of the Tularosa Quadrangle, New Mexico, was evaluated to a depth of 1500 m using National Uranium Resource Evaluation criteria. Uranium occurrences reported in the literature were located, sampled, and described in detail. Areas of anomalous radioactivity, interpreted from an aerial radiometric survey, and geochemical anomalies, interpreted from hydrogeochemical and stream-sediment reconnaissance, were also investigated. Additionally, several hundred rock samples were studied in thin section, and supplemental geochemical analyses of rock and water samples were completed. Fluorometric analyses were completed for samples from the Black Range Primitive Area to augment previously available geochemical data. Subsurface favorability was evaluatedmore » using gamma-ray logs and descriptive logs of sample cuttings. One area of uranium favorability was delineated, based on the data made available from this study. This area is the Nogal Canyon cauldron margin zone. Within the zone, characterized by concentric and radial fractures, resurgent doming, ring-dike volcanism, and intracauldron sedimentation, uranium conentration is confined to magmatic-hydrothermal and volcanogenic uranium deposits.« less
The role of extracellular DNA in uranium precipitation and biomineralisation.
Hufton, Joseph; Harding, John H; Romero-González, Maria E
2016-10-26
Bacterial extra polymeric substances (EPS) have been associated with the extracellular precipitation of uranium. Here we report findings on the biomineralisation of uranium, with extracellular DNA (eDNA) used as a model biomolecule representative of EPS. The complexation and precipitation of eDNA with uranium were investigated as a function of pH, ionic strength and varying concentrations of reactants. The role of phosphate moieties in the biomineralisation mechanism was studied by enzymatically releasing phosphate (ePO 4 ) from eDNA compared to abiotic phosphate (aPO 4 ). The eDNA-uranium precipitates and uranium minerals obtained were characterised by Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FT-IR) spectroscopy, Scanning Electron Microscopy-Energy Dispersive X-Ray analysis (SEM-EDX), X-Ray Powder Diffraction (XRD) and X-Ray Photoelectron Spectroscopy (XPS). ATR-FT-IR showed that at pH 5, the eDNA-uranium precipitation mechanism was predominantly mediated by interactions with phosphate moieties from eDNA. At pH 2, the uranium interactions with eDNA occur mainly through phosphate. The solubility equilibrium was dependent on pH with the formation of precipitate reduced as the pH increased. The XRD data confirmed the formation of a uranium phosphate precipitate when synthesised using ePO 4 . XPS and SEM-EDX studies showed the incorporation of carbon and nitrogen groups from the enzymatic orthophosphate hydrolysis on the obtained precipitated. These results suggested that the removal of uranium from solution occurs via two mechanisms: complexation by eDNA molecules and precipitation of a uranium phosphate mineral of the type (UO 2 HPO 4 )·xH 2 O by enzymatic orthophosphate hydrolysis. This demonstrated that eDNA from bacterial EPS is a key contributor to uranium biomineralisation.
Meta-analysis of depleted uranium levels in the Balkan region.
Besic, Larisa; Muhovic, Imer; Asic, Adna; Kurtovic-Kozaric, Amina
2017-06-01
In recent years, contradicting data has been published on the connection between the presence of depleted uranium and an increased cancer incidence among military personnel deployed in the Balkans during the 1992-1999 wars. This has led to numerous research articles investigating possible depleted uranium contamination of the afflicted regions of the Balkan Peninsula, namely Bosnia & Herzegovina, Serbia, Kosovo and Montenegro. The aim of this study was to collect data from previously published reports investigating the levels of depleted uranium in the Balkans and to present the data in the form of a meta-analysis. This would provide a clear image of the extent of depleted uranium contamination after the Balkan conflict. In addition, we tested the hypothesis that there is a correlation between the levels of depleted uranium and the assumed depleted uranium-related health effects. Our results suggest that the majority of the examined sites contain natural uranium, while the area of Kosovo appears to be most heavily afflicted by depleted uranium pollution, followed by Bosnia & Herzegovina. Furthermore, the results indicate that it is not possible to make a valid correlation between the health effects and depleted uranium-contaminated areas. We therefore suggest a structured collaborative plan of action where long-term monitoring of the residents of depleted uranium-afflicted areas would be performed. In conclusion, while the possibility of depleted uranium toxicity in post-conflict regions appears to exist, there currently exists no definitive proof of such effects, due to insufficient studies of potentially afflicted populations, in addition to the lack of a common epidemiological approach in the reviewed literature. Copyright © 2017 Elsevier Ltd. All rights reserved.
Uranium Bioreduction and Biomineralization.
Wufuer, Rehemanjiang; Wei, Yongyang; Lin, Qinghua; Wang, Huawei; Song, Wenjuan; Liu, Wen; Zhang, Daoyong; Pan, Xiangliang; Gadd, Geoffrey Michael
2017-01-01
Following the development of nuclear science and technology, uranium contamination has been an ever increasing concern worldwide because of its potential for migration from the waste repositories and long-term contaminated environments. Physical and chemical techniques for uranium pollution are expensive and challenging. An alternative to these technologies is microbially mediated uranium bioremediation in contaminated water and soil environments due to its reduced cost and environmental friendliness. To date, four basic mechanisms of uranium bioremediation-uranium bioreduction, biosorption, biomineralization, and bioaccumulation-have been established, of which uranium bioreduction and biomineralization have been studied extensively. The objective of this review is to provide an understanding of recent developments in these two fields in relation to relevant microorganisms, mechanisms, influential factors, and obstacles. Copyright © 2017 Elsevier Inc. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Guillet, H.
1959-02-01
A description is given of direct fluorination of preconcentrated uranium ores in order to obtain the hexafluoride. After normal sulfuric acid treatment of the ore to eliminate silica, the uranium is precipitated by lime to obtain either impure calcium uranate of medium grade, or containing around 10% of uranium. This concentrate is dried in an inert atmosphere and then treated with a current of elementary fluorine. The uranium hexafluoride formed is condensed at the outlet of the reaction vessel and may be used either for reduction to tetrafluoride and the subsequent manufacture of uranium metal or as the initial productmore » in a diffusion plant. (auth)« less
Chronic Exposure to Uranium from Gestation: Effects on Behavior and Neurogenesis in Adulthood
Dinocourt, Céline; Culeux, Cécile; Legrand, Marie; Elie, Christelle; Lestaevel, Philippe
2017-01-01
Uranium exposure leads to cerebral dysfunction involving for instance biochemical, neurochemical and neurobehavioral effects. Most studies have focused on mechanisms in uranium-exposed adult animals. However, recent data on developing animals have shown that the developing brain is also sensitive to uranium. Models of uranium exposure during brain development highlight the need to improve our understanding of the effects of uranium. In a model in which uranium exposure began from the first day of gestation, we studied the neurobehavioral consequences as well as the progression of hippocampal neurogenesis in animals from dams exposed to uranium. Our results show that 2-month-old rats exposed to uranium from gestational day 1 displayed deficits in special memory and a prominent depressive-like phenotype. Cell proliferation was not disturbed in these animals, as shown by 5-bromo-2′deoxyuridine (BrdU)/neuronal specific nuclear protein (NeuN) immunostaining in the dentate gyrus. However, in some animals, the pyramidal cell layer was dispersed in the CA3 region. From our previous results with the same model, the hypothesis of alterations of neurogenesis at prior stages of development is worth considering, but is probably not the only one. Therefore, further investigations are needed to correlate cerebral dysfunction and its underlying mechanistic pathways. PMID:28513543
Chronic Exposure to Uranium from Gestation: Effects on Behavior and Neurogenesis in Adulthood.
Dinocourt, Céline; Culeux, Cécile; Legrand, Marie; Elie, Christelle; Lestaevel, Philippe
2017-05-17
Uranium exposure leads to cerebral dysfunction involving for instance biochemical, neurochemical and neurobehavioral effects. Most studies have focused on mechanisms in uranium-exposed adult animals. However, recent data on developing animals have shown that the developing brain is also sensitive to uranium. Models of uranium exposure during brain development highlight the need to improve our understanding of the effects of uranium. In a model in which uranium exposure began from the first day of gestation, we studied the neurobehavioral consequences as well as the progression of hippocampal neurogenesis in animals from dams exposed to uranium. Our results show that 2-month-old rats exposed to uranium from gestational day 1 displayed deficits in special memory and a prominent depressive-like phenotype. Cell proliferation was not disturbed in these animals, as shown by 5-bromo-2'deoxyuridine (BrdU)/neuronal specific nuclear protein (NeuN) immunostaining in the dentate gyrus. However, in some animals, the pyramidal cell layer was dispersed in the CA3 region. From our previous results with the same model, the hypothesis of alterations of neurogenesis at prior stages of development is worth considering, but is probably not the only one. Therefore, further investigations are needed to correlate cerebral dysfunction and its underlying mechanistic pathways.
Fermentation and Hydrogen Metabolism Affect Uranium Reduction by Clostridia
Gao, Weimin; Francis, Arokiasamy J.
2013-01-01
Previously, it has been shown that not only is uranium reduction under fermentation condition common among clostridia species, but also the strains differed in the extent of their capability and the pH of the culture significantly affected uranium(VI) reduction. In this study, using HPLC and GC techniques, metabolic properties of those clostridial strains active in uranium reduction under fermentation conditions have been characterized and their effects on capability variance of uranium reduction discussed. Then, the relationship between hydrogen metabolism and uranium reduction has been further explored and the important role played by hydrogenase in uranium(VI) and iron(III) reduction by clostridiamore » demonstrated. When hydrogen was provided as the headspace gas, uranium(VI) reduction occurred in the presence of whole cells of clostridia. This is in contrast to that of nitrogen as the headspace gas. Without clostridia cells, hydrogen alone could not result in uranium(VI) reduction. In alignment with this observation, it was also found that either copper(II) addition or iron depletion in the medium could compromise uranium reduction by clostridia. In the end, a comprehensive model was proposed to explain uranium reduction by clostridia and its relationship to the overall metabolism especially hydrogen (H 2 ) production.« less
Incorporation of Uranium: II. Distribution of Uranium Absorbed through the Lungs and the Skin
Walinder, G.; Fries, B.; Billaudelle, U.
1967-01-01
In experiments on mice, rabbits, and piglets the distribution of uranium was studied at different times after exposure. Uranium was administered by inhalation (mice) and through the skin (rabbits and piglets). These investigations show that the uptakes of uranium in different organs of the three species are highly dependent on the amounts administered. There seems to be a saturation effect in the spleen and bone tissue whenever the uranium concentration in the blood exceeds a certain level. The effect in the kidney is completely different. If, in a series of animals, the quantity of uranium is continuously increased, the uptakes by the kidneys increase more rapidly than the quantities administered. This observation seems to be consistent with the toxic effects of uranium on the capillary system in the renal cortex. Polyphloretin phosphate, a compound which reduces permeability, was investigated with respect to its effect on the uptake of uranium deposited in skin wounds in rabbits and piglets. It significantly reduced the absorption of uranium, even from depots in deep wounds. The findings are discussed with reference to the routine screening of persons exposed to uranium at AB Atomenergi. Images PMID:6073090
Health effects of uranium: new research findings.
Brugge, Doug; Buchner, Virginia
2011-01-01
Recent plans for a nuclear renaissance in both established and emerging economies have prompted increased interest in uranium mining. With the potential for more uranium mining worldwide and a growth in the literature on the toxicology and epidemiology of uranium and uranium mining, we found it timely to review the current state of knowledge. Here, we present a review of the health effects of uranium mining, with an emphasis on newer findings (2005-2011). Uranium mining can contaminate air, water, and soil. The chemical toxicity of the metal constitutes the primary environmental health hazard, with the radioactivity of uranium a secondary concern. The update of the toxicologic evidence on uranium adds to the established findings regarding nephrotoxicity, genotoxicity, and developmental defects. Additional novel toxicologic findings, including some at the molecular level, are now emerging that raise the biological plausibility of adverse effects on the brain, on reproduction, including estrogenic effects, on gene expression, and on uranium metabolism. Historically, most epidemiology on uranium mining has focused on mine workers and radon exposure. Although that situation is still overwhelmingly true, a smaller emerging literature has begun to form around environmental exposure in residential areas near uranium mining and processing facilities. We present and critique such studies. Clearly, more epidemiologic research is needed to contribute to causal inference. As much damage is irreversible, and possibly cumulative, present efforts must be vigorous to limit environmental uranium contamination and exposure.
The role of uranium-arene bonding in H2O reduction catalysis
NASA Astrophysics Data System (ADS)
Halter, Dominik P.; Heinemann, Frank W.; Maron, Laurent; Meyer, Karsten
2018-03-01
The reactivity of uranium compounds towards small molecules typically occurs through stoichiometric rather than catalytic processes. Examples of uranium catalysts reacting with water are particularly scarce, because stable uranyl groups form that preclude the recovery of the uranium compound. Recently, however, an arene-anchored, electron-rich uranium complex has been shown to facilitate the electrocatalytic formation of H2 from H2O. Here, we present the precise role of uranium-arene δ bonding in intermediates of the catalytic cycle, as well as details of the atypical two-electron oxidative addition of H2O to the trivalent uranium catalyst. Both aspects were explored by synthesizing mid- and high-valent uranium-oxo intermediates and by performing comparative studies with a structurally related complex that cannot engage in δ bonding. The redox activity of the arene anchor and a covalent δ-bonding interaction with the uranium ion during H2 formation were supported by density functional theory analysis. Detailed insight into this catalytic system may inspire the design of ligands for new uranium catalysts.
Evaluation of Non-Oxide Fuel for Fission-based Nuclear Reactors on Spacecraft
smaller and potentially lighter core, whichis a significant advantage. The results of this study indicate that use of both UC and UN may result in significant weight savings due tohigher uranium loading density....The goal of this project was to study the performance of atypical uranium-based fuels in a nuclear reactor capable of producing 1 megawattof thermal...UN), or uranium carbide (UC) and compared their performance to uranium oxide (UO2) which is thefuel form used in the vast majority of commercial
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.
Novel Sensor for the In Situ Measurement of Uranium Fluxes
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hatfield, Kirk
2015-02-10
The goal of this project was to develop a sensor that incorporates the field-tested concepts of the passive flux meter to provide direct in situ measures of flux for uranium and groundwater in porous media. Measurable contaminant fluxes [J] are essentially the product of concentration [C] and groundwater flux or specific discharge [q ]. The sensor measures [J] and [q] by changes in contaminant and tracer amounts respectively on a sorbent. By using measurement rather than inference from static parameters, the sensor can directly advance conceptual and computational models for field scale simulations. The sensor was deployed in conjunction withmore » DOE in obtaining field-scale quantification of subsurface processes affecting uranium transport (e.g., advection) and transformation (e.g., uranium attenuation) at the Rifle IFRC Site in Rifle, Colorado. Project results have expanded our current understanding of how field-scale spatial variations in fluxes of uranium, groundwater and salient electron donor/acceptors are coupled to spatial variations in measured microbial biomass/community composition, effective field-scale uranium mass balances, attenuation, and stability. The coupling between uranium, various nutrients and micro flora can be used to estimate field-scale rates of uranium attenuation and field-scale transitions in microbial communities. This research focuses on uranium (VI), but the sensor principles and design are applicable to field-scale fate and transport of other radionuclides. Laboratory studies focused on sorbent selection and calibration, along with sensor development and validation under controlled conditions. Field studies were conducted at the Rifle IFRC Site in Rifle, Colorado. These studies were closely coordinated with existing SBR (formerly ERSP) projects to complement data collection. Small field tests were conducted during the first two years that focused on evaluating field-scale deployment procedures and validating sensor performance under controlled field conditions. In the third and fourth year a suite of larger field studies were conducted. For these studies, the uranium flux sensor was used with uranium speciation measurements and molecular-biological tools to characterize microbial community and active biomass at synonymous wells distributed in a large grid. These field efforts quantified spatial changes in uranium flux and field-scale rates of uranium attenuation (ambient and stimulated), uranium stability, and quantitatively assessed how fluxes and effective reaction rates were coupled to spatial variations in microbial community and active biomass. Analyses of data from these field experiments were used to generate estimates of Monod kinetic parameters that are ‘effective’ in nature and optimal for modeling uranium fate and transport at the field-scale. This project provided the opportunity to develop the first sensor that provides direct measures of both uranium (VI) and groundwater flux. A multidisciplinary team was assembled to include two geochemists, a microbiologist, and two quantitative contaminant hydrologists. Now that the project is complete, the sensor can be deployed at DOE sites to evaluate field-scale uranium attenuation, source behavior, the efficacy of remediation, and off-site risk. Because the sensor requires no power, it can be deployed at remote sites for periods of days to months. The fundamental science derived from this project can be used to advance the development of predictive models for various transport and attenuation processes in aquifers. Proper development of these models is critical for long-term stewardship of contaminated sites in the context of predicting uranium source behavior, remediation performance, and off-site risk.« less
Detection of uranium using laser-induced breakdown spectroscopy.
Chinni, Rosemarie C; Cremers, David A; Radziemski, Leon J; Bostian, Melissa; Navarro-Northrup, Claudia
2009-11-01
The goal of this work is a detailed study of uranium detection by laser-induced breakdown spectroscopy (LIBS) for application to activities associated with environmental surveillance and detecting weapons of mass destruction (WMD). The study was used to assist development of LIBS instruments for standoff detection of bulk radiological and nuclear materials and these materials distributed as contaminants on surfaces. Uranium spectra were analyzed under a variety of different conditions at room pressure, reduced pressures, and in an argon atmosphere. All spectra displayed a high apparent background due to the high density of uranium lines. Time decay curves of selected uranium lines were monitored and compared to other elements in an attempt to maximize detection capabilities for each species in the complicated uranium spectrum. A survey of the LIBS uranium spectra was conducted and relative emission line strengths were determined over the range of 260 to 800 nm. These spectra provide a guide for selection of the strongest LIBS analytical lines for uranium detection in different spectral regions. A detection limit for uranium in soil of 0.26% w/w was obtained at close range and 0.5% w/w was achieved at a distance of 30 m. Surface detection limits were substrate dependent and ranged from 13 to 150 microg/cm2. Double-pulse experiments (both collinear and orthogonal arrangements) were shown to enhance the uranium signal in some cases. Based on the results of this work, a short critique is given of the applicability of LIBS for the detection of uranium residues on surfaces for environmental monitoring and WMD surveillance.
Volcanogenic Uranium Deposits: Geology, Geochemical Processes, and Criteria for Resource Assessment
Nash, J. Thomas
2010-01-01
Felsic volcanic rocks have long been considered a primary source of uranium for many kinds of uranium deposits, but volcanogenic uranium deposits themselves have generally not been important resources. Until the past few years, resource summaries for the United States or the world generally include volcanogenic in the broad category of 'other deposits' because they comprised less than 0.5 percent of past production or estimated resources. Exploration in the United States from the 1940s through 1982 discovered hundreds of prospects in volcanic rocks, of which fewer than 20 had some recorded production. Intensive exploration in the late 1970s found some large deposits, but low grades (less than about 0.10 percent U3O8) discouraged economic development. A few deposits in the world, drilled in the 1980s and 1990s, are now known to contain large resources (>20,000 tonnes U3O8). However, research on ore-forming processes and exploration for volcanogenic deposits has lagged behind other kinds of uranium deposits and has not utilized advances in understanding of geology, geochemistry, and paleohydrology of ore deposits in general and epithermal deposits in particular. This review outlines new ways to explore and assess for volcanogenic deposits, using new concepts of convection, fluid mixing, and high heat flow to mobilize uranium from volcanic source rocks and form deposits that are postulated to be large. Much can also be learned from studies of epithermal metal deposits, such as the important roles of extensional tectonics, bimodal volcanism, and fracture-flow systems related to resurgent calderas. Regional resource assessment is helped by genetic concepts, but hampered by limited information on frontier areas and undiscovered districts. Diagnostic data used to define ore deposit genesis, such as stable isotopic data, are rarely available for frontier areas. A volcanic environment classification, with three classes (proximal, distal, and pre-volcanic structures), permits use of geologic features on 1:500,000 to 1:100,000 scale maps. Geochemical databases for volcanic rocks are postulated to be more effective than databases for stream sediments or surface radioactivity, both of which tend to be inconsistent because of variable leaching of uranium from soils. Based on empirical associations, spatial associations with areas of wet paleoclimate, adjacent oil and gas fields, or evaporite beds are deemed positive. Most difficult to estimate is the location of depositional traps and reduction zones, in part because they are mere points at regional scale. Grade and tonnage data are reviewed and discussed for 32 deposits in the world. Experience of mining engineers and geologists in Asia suggests that tonnages could be higher than presently known in the Western Hemisphere. Geological analysis, and new data from Asia, suggest a typical or median deposit tonnage of about 5,000 tonnes U3O8, and an optimistic forecast of discoveries in the range of 5,000 to 20,000 tonnes U3O8. The likely grade of undiscovered deposits could be about 0.15 percent U3O8 , based on both western and eastern examples. Volcanic terrane is under-explored, relative to other kinds of uranium deposits, and is considered a favorable frontier area for new discoveries.
Phase discrimination of uranium oxides using laser-induced breakdown spectroscopy
NASA Astrophysics Data System (ADS)
Campbell, Keri R.; Wozniak, Nicholas R.; Colgan, James P.; Judge, Elizabeth J.; Barefield, James E.; Kilcrease, David P.; Wilkerson, Marianne P.; Czerwinski, Ken R.; Clegg, Samuel M.
2017-08-01
Nuclear forensics goals for characterizing samples of interest include qualitative and quantitative analysis of major and trace elements, isotopic analysis, phase identification, and physical analysis. These samples may include uranium oxides UO2, U3O8, and UO3, which play an important role in the front end of the nuclear fuel cycle, from mining to fuel fabrication. The focus of this study is to compare the ratios of the intensities of uranium and oxygen emission lines which can be used to distinguish between different uranium oxide materials using Laser-Induced Breakdown Spectroscopy (LIBS). Measurements at varying laser powers were made under an argon atmosphere at 585 Torr to ensure the oxygen emission intensity was originating from the sample, and not from the atmosphere. Fifteen uranium emission lines were used to compare experimental results with theoretical calculations in order to determine the plasma conditions. Using a laser energy of 26 mJ, the uranium lines 591.539 and 682.692 nm provide the highest degree of discrimination between the uranium oxides. The study presented here suggests that LIBS is useful for discriminating uranium oxide phases, UO2, U3O8, and UO3.
Mironov, Vladislav P; Matusevich, Janna L; Kudrjashov, Vladimir P; Boulyga, Sergei F; Becker, J Sabine
2002-12-01
This work presents experimental results on the distribution of irradiated reactor uranium from fallout after the accident at Chernobyl Nuclear Power Plant (NPP) in comparison to natural uranium distribution in different soil types. Oxidation processes and vertical migration of irradiated uranium in soils typical of the 30 km relocation area around Chernobyl NPP were studied using 236U as the tracer for irradiated reactor uranium and inductively coupled plasma mass spectrometry as the analytical method for uranium isotope ratio measurements. Measurements of natural uranium yielded significant variations of its concentration in upper soil layers from 2 x 10(-7) g g(-1) to 3.4 x 10(-6) g g(-1). Concentrations of irradiated uranium in the upper 0-10 cm soil layers at the investigated sampling sites varied from 5 x 10(-12) g g(-1) to 2 x 10(-6) g g(-1) depending on the distance from Chernobyl NPP. In the majority of investigated soil profiles 78% to 97% of irradiated "Chernobyl" uranium is still contained in the upper 0-10 cm soil layers. The physical and chemical characteristics of the soil do not have any significant influence on processes of fuel particle destruction. Results obtained using carbonate leaching of 236U confirmed that more than 60% of irradiated "Chernobyl" uranium is still in a tetravalent form, ie. it is included in the fuel matrix (non-oxidized fuel UO2). The average value of the destruction rate of fuel particles determined for the Western radioactive trace (k = 0.030 +/- 0.005 yr(-1)) and for the Northern radioactive trace (k = 0.035 + 0.009 yr(-1)) coincide within experimental errors. Use of leaching of fission products in comparison to leaching of uranium for study of the destruction rate of fuel particles yielded poor coincidence due to the fact that use of fission products does not take into account differences in the chemical properties of fission products and fuel matrix (uranium).
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reimus, Paul William
A two-part field study was conducted in Smith Ranch-Highland in-situ recovery (ISR) near Douglas, Wyoming, to evaluate the restorative capacity of the aquifer downgradient (i.e., hydrologically downstream) of a Uranium ISR mining site with respect to the transport of uranium and other potential contaminants in groundwater after mining has ceased. The study was partially conducted by checking the Uranium content and the alkalinity of separate wells, some wells had been restored and others had not. A map and in-depth procedures of the study are included.
INTERNAL EXPOSURE TO URANIUM IN A POOLED COHORT OF GASEOUS DIFFUSION PLANT WORKERS
Anderson, Jeri L.; Apostoaei, A. Iulian; Yiin, James H.; Fleming, Donald A.; Tseng, Chih-Yu; Chen, Pi-Hsueh
2015-01-01
Intakes and absorbed organ doses were estimated for 29 303 workers employed at three former US gaseous diffusion plants as part of a study of cause-specific mortality and cancer incidence in uranium enrichment workers. Uranium urinalysis data (>600 000 urine samples) were available for 58 % of the pooled cohort. Facility records provided uranium gravimetric and radioactivity concentration data and allowed estimation of enrichment levels of uranium to which workers may have been exposed. Urine data were generally recorded with facility department numbers, which were also available in study subjects’ work histories. Bioassay data were imputed for study subjects with no recorded sample results (33 % of pooled cohort) by assigning department average urine uranium concentration. Gravimetric data were converted to 24-h uranium activity excretion using department average specific activities. Intakes and organ doses were calculated assuming chronic exposure by inhalation to a 5-µm activity median aerodynamic diameter aerosol of soluble uranium. Median intakes varied between 0.31 and 0.74 Bq d−1 for the three facilities. Median organ doses for the three facilities varied between 0.019 and 0.051, 0.68 and 1.8, 0.078 and 0.22, 0.28 and 0.74, and 0.094 and 0.25 mGy for lung, bone surface, red bone marrow, kidneys, and liver, respectively. Estimated intakes and organ doses for study subjects with imputed bioassay data were similar in magnitude. PMID:26113578
Stitt, C A; Harker, N J; Hallam, K R; Paraskevoulakos, C; Banos, A; Rennie, S; Jowsey, J; Scott, T B
2015-01-01
Synchrotron X-rays have been used to study the oxidation of uranium and uranium hydride when encapsulated in grout and stored in de-ionised water for 10 months. Periodic synchrotron X-ray tomography and X-ray powder diffraction have allowed measurement and identification of the arising corrosion products and the rates of corrosion. The oxidation rates of the uranium metal and uranium hydride were slower than empirically derived rates previously reported for each reactant in an anoxic water system, but without encapsulation in grout. This was attributed to the grout acting as a physical barrier limiting the access of oxidising species to the uranium surface. Uranium hydride was observed to persist throughout the 10 month storage period and industrial consequences of this observed persistence are discussed.
Harker, N. J.; Hallam, K. R.; Paraskevoulakos, C.; Banos, A.; Rennie, S.; Jowsey, J.
2015-01-01
Synchrotron X-rays have been used to study the oxidation of uranium and uranium hydride when encapsulated in grout and stored in de-ionised water for 10 months. Periodic synchrotron X-ray tomography and X-ray powder diffraction have allowed measurement and identification of the arising corrosion products and the rates of corrosion. The oxidation rates of the uranium metal and uranium hydride were slower than empirically derived rates previously reported for each reactant in an anoxic water system, but without encapsulation in grout. This was attributed to the grout acting as a physical barrier limiting the access of oxidising species to the uranium surface. Uranium hydride was observed to persist throughout the 10 month storage period and industrial consequences of this observed persistence are discussed. PMID:26176551
Miller, W. Roger; Houston, R.S.; Karlstrom, K.E.; Hopkins, D.M.; Ficklin, W.H.
1977-01-01
Metasedimentary rocks of Precambrian X age in and near the Snowy Range wilderness study area of southeastern Wyoming are lithologically and chronologically similar to those on the north shore of Lake Huron in Canada. The rocks in Canada contain major deposits of uranium in quartz-pebble conglomerates near the base of the metasedimentary sequence. Similar conglomerates in the Deep Lake Formation in the Medicine Bow Mountains of southeastern Wyoming are slightly radioactive and may contain deposits of uranium and other valuable heavy metals. During the summer of 1976, a geological and geochemical pilot study was conducted in the vicinity of Arrastre Lake in the Medicine Bow Mountains to determine the most effective exploration methods for evaluating the uranium potential of the Snowy Range wilderness study area. The area around Arrastre Lake was selected because of the presence of a radioactive lens within a quartz-pebble conglomerate of the Deep Lake Formation. The results of the survey indicate possible uranium mineralization in the subsurface rocks of this formation. The radon content of the dilute waters of the area is much higher than can be accounted for by the uranium content of the surface rocks. Two sources for the high content of the radon are possible. In either case, the high values of radon obtained in this study are a positive indication of uranium mineralization in the subsurface rocks. The determination of the radon content of water samples is the recommended geochemical technique for uranium exploration in the area. The determination of uranium in water and in organic-rich bog material is also recommended.
From dust to dose: Effects of forest disturbance on increased inhalation exposure.
Whicker, Jeffrey J; Pinder, John E; Breshears, David D; Eberhart, Craig F
2006-09-15
Ecosystem disturbances that remove vegetation and disturb surface soils are major causes of excessive soil erosion and can result in accelerated transport of soils contaminated with hazardous materials. Accelerated wind erosion in disturbed lands that are contaminated is of particular concern because of potential increased inhalation exposure, yet measurements regarding these relationships are lacking. The importance of this was highlighted when, in May of 2000, the Cerro Grande fire burned over roughly 30% of Los Alamos National Laboratory (LANL), mostly in ponderosa pine (Pinus ponderosa) forest, and through areas with soils containing contaminants, particularly excess depleted and natural uranium. Additionally, post-fire thinning was performed in burned and unburned forests on about 25% of LANL land. The first goal of this study was to assess the potential for increased inhalation dose from uranium contaminated soils via wind-driven resuspension of soil following the Cerro Grande Fire and subsequent forest thinning. This was done through analysis of post-disturbance measurements of uranium air concentrations and their relationships with wind velocity and seasonal vegetation cover. We found a 14% average increase in uranium air concentrations at LANL perimeter locations after the fire, and the greatest air concentrations occurred during the months of April-June when wind velocities are highest, no snow cover, and low vegetation cover. The second goal was to develop a methodology to assess the relative contribution of each disturbance type towards increasing public and worker exposure to these resuspended soils. Measurements of wind-driven dust flux in severely burned, moderately burned, thinned, and unburned/unthinned forest areas were used to assess horizontal dust flux (HDF) in these areas. Using empirically derived relationships between measurements of HDF and respirible dust, coupled with onsite uranium soil concentrations, we estimate relative increases in inhalation doses for workers ranging from 15% to 38%. Despite the potential for increased doses resulting from these forest disturbances, the estimated annual dose rate for the public was <1 microSv yr(-1), which is far below the dose limits for public exposures, and the upper-bound dose rate for a LANL worker was estimated to be 140 microSv yr(-1), far below the 5 x 10(4) microSv yr(-1) occupational dose limit. These results show the importance of ecosystem disturbance in increasing mobility of soil-bound contaminants, which can ultimately increase exposure. However, it is important to investigate the magnitude of the increases when deciding appropriate strategies for management and long-term stewardship of contaminated lands.
Lazareva, Svetlana; Ismagilov, Zinfer; Kuznetsov, Vadim; Shikina, Nadezhda; Kerzhentsev, Mikhail
2018-02-05
Huge amounts of nuclear waste, including depleted uranium, significantly contribute to the adverse environmental situation throughout the world. An approach to the effective use of uranium oxides in catalysts for the deep oxidation of chlorine-containing hydrocarbons is suggested. Investigation of the catalytic activity of the synthesized supported uranium oxide catalysts doped with Cr, Mn and Co transition metals in the chlorobenzene oxidation showed that these catalysts are comparable with conventional commercial ones. Physicochemical properties of the catalysts were studied by X-ray diffraction, temperature-programmed reduction with hydrogen (H 2 -TPR), and Fourier transform infrared spectroscopy. The higher activity of Mn- and Co-containing uranium oxide catalysts in the H 2 -TPR and oxidation of chlorobenzene in comparison with non-uranium catalysts may be related to the formation of a new disperse phase represented by uranates. The study of chlorobenzene adsorption revealed that the surface oxygen is involved in the catalytic process.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ariani, Menik; Su'ud, Zaki; Waris, Abdul
2012-06-06
A conceptual design study of Gas Cooled Fast Reactors with Modified CANDLE burn-up scheme has been performed. In this study, design GCFR with Helium coolant which can be continuously operated by supplying mixed Natural Uranium/Thorium without fuel enrichment plant or fuel reprocessing plant. The active reactor cores are divided into two region, Thorium fuel region and Uranium fuel region. Each fuel core regions are subdivided into ten parts (region-1 until region-10) with the same volume in the axial direction. The fresh Natural Uranium and Thorium is initially put in region-1, after one cycle of 10 years of burn-up it ismore » shifted to region-2 and the each region-1 is filled by fresh natural Uranium/Thorium fuel. This concept is basically applied to all regions in both cores area, i.e. shifted the core of i{sup th} region into i+1 region after the end of 10 years burn-up cycle. For the next cycles, we will add only Natural Uranium and Thorium on each region-1. The calculation results show the reactivity reached by mixed Natural Uranium/Thorium with volume ratio is 4.7:1. This reactor can results power thermal 550 MWth. After reactor start-up the operation, furthermore reactor only needs Natural Uranium/Thorium supply for continue operation along 100 years.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kim, Haeyeon; G. Eggert, Roderick; W. Carlsen, Brett
Phosphate rock contains significant amounts of uranium, although in low concentrations. Recovery of uranium as a by-product from phosphoric acid, an intermediate product produced during the recovery of phosphorus from phosphate rock, is not unprecedented. Phosphoric acid plants ceased to produce uranium as a by-product in the early 1990s with the fall of uranium prices. In the last decade, this topic has regained attention due to higher uranium prices and expected increase in demand for uranium. Our study revisits the topic and estimates how much uranium might be recoverable from current phosphoric acid production in the United States and whatmore » the associated costs might be considering two different recovery processes: solvent extraction and ion exchange. Based on U.S. phosphoric acid production in 2014, 5.5 million pounds of U 3O 8 could have been recovered, more than domestic U.S. mine production of uranium in the same year. Annualized costs for a hypothetical uranium recovery plant are US$48-66 per pound U 3O 8 for solvent extraction, the process used historically in the United States to recover uranium from phosphoric acid. For ion exchange, not yet proven at a commercial scale for uranium recovery, the estimated costs are US$33-54 per pound U 3O 8. Our results suggest that it is technically possible for the United States to recover significant quantities of uranium from current phosphoric acid production. And for this type of uranium production to be economically attractive on a large scale, either recovery costs must fall or uranium prices rise.« less
Kim, Haeyeon; G. Eggert, Roderick; W. Carlsen, Brett; ...
2016-06-16
Phosphate rock contains significant amounts of uranium, although in low concentrations. Recovery of uranium as a by-product from phosphoric acid, an intermediate product produced during the recovery of phosphorus from phosphate rock, is not unprecedented. Phosphoric acid plants ceased to produce uranium as a by-product in the early 1990s with the fall of uranium prices. In the last decade, this topic has regained attention due to higher uranium prices and expected increase in demand for uranium. Our study revisits the topic and estimates how much uranium might be recoverable from current phosphoric acid production in the United States and whatmore » the associated costs might be considering two different recovery processes: solvent extraction and ion exchange. Based on U.S. phosphoric acid production in 2014, 5.5 million pounds of U 3O 8 could have been recovered, more than domestic U.S. mine production of uranium in the same year. Annualized costs for a hypothetical uranium recovery plant are US$48-66 per pound U 3O 8 for solvent extraction, the process used historically in the United States to recover uranium from phosphoric acid. For ion exchange, not yet proven at a commercial scale for uranium recovery, the estimated costs are US$33-54 per pound U 3O 8. Our results suggest that it is technically possible for the United States to recover significant quantities of uranium from current phosphoric acid production. And for this type of uranium production to be economically attractive on a large scale, either recovery costs must fall or uranium prices rise.« less
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
Urinary excretion of uranium in adult inhabitants of the Czech Republic.
Malátová, Irena; Bečková, Věra; Kotík, Lukáš
2016-02-01
The main aim of this study was to determine and evaluate urinary excretion of uranium in the general public of the Czech Republic. This value should serve as a baseline for distinguishing possible increase in uranium content in population living near legacy sites of mining and processing uranium ores and also to help to distinguish the proportion of the uranium content in urine among uranium miners resulting from inhaled dust. The geometric mean of the uranium concentration in urine of 74 inhabitants of the Czech Republic was 0.091 mBq/L (7.4 ng/L) with the 95% confidence interval 0.071-0.12 mBq/L (5.7-9.6 ng/L) respectively. The geometric mean of the daily excretion was 0.15 mBq/d (12.4 ng/d) with the 95% confidence interval 0.12-0.20 mBq/d (9.5-16.1 ng/d) respectively. Despite the legacy of uranium mines and plants processing uranium ore in the Czech Republic, the levels of uranium in urine and therefore, also human body content of uranium, is similar to other countries, esp. Germany, Slovenia and USA. Significant difference in the daily urinary excretion of uranium was found between individuals using public supply and private water wells as a source of drinking water. Age dependence of daily urinary excretion of uranium was not found. Mean values and their range are comparable to other countries, esp. Germany, Slovenia and USA. Copyright © 2015 Elsevier Ltd. All rights reserved.
Uranium(VI) interactions with mackinawite in the presence and absence of bicarbonate and oxygen.
Gallegos, Tanya J; Fuller, Christopher C; Webb, Samuel M; Betterton, William
2013-07-02
Mackinawite, Fe(II)S, samples loaded with uranium (10(-5), 10(-4), and 10(-3) mol U/g FeS) at pH 5, 7, and 9, were characterized using X-ray absorption spectroscopy and X-ray diffraction to determine the effects of pH, bicarbonate, and oxidation on uptake. Under anoxic conditions, a 5 g/L suspension of mackinawite lowered 5 × 10(-5) M uranium(VI) to below 30 ppb (1.26 × 10(-7) M) U. Between 82 and 88% of the uranium removed from solution by mackinawite was U(IV) and was nearly completely reduced to U(IV) when 0.012 M bicarbonate was added. Near-neighbor coordination consisting of uranium-oxygen and uranium-uranium distances indicates the formation of uraninite in the presence and absence of bicarbonate, suggesting reductive precipitation as the dominant removal mechanism. Following equilibration in air, mackinawite was oxidized to mainly goethite and sulfur and about 76% of U(IV) was reoxidized to U(VI) with coordination of uranium to axial and equatorial oxygen, similar to uranyl. Additionally, uranium-iron distances, typical of coprecipitation of uranium with iron oxides, and uranium-sulfur distances indicating bidentate coordination of U(VI) to sulfate were evident. The affinity of mackinawite and its oxidation products for U(VI) provides impetus for further study of mackinawite as a potential reactive medium for remediation of uranium-contaminated water.
Organic geochemical analysis of sedimentary organic matter associated with uranium
Leventhal, J.S.; Daws, T.A.; Frye, J.S.
1986-01-01
Samples of sedimentary organic matter from several geologic environments and ages which are enriched in uranium (56 ppm to 12%) have been characterized. The three analytical techniqyes used to study the samples were Rock-Eval pyrolysis, pyrolysis-gas chromatography-mass spectrometry, and solid-state C-13 nuclear magnetic resonance (NMR) spectroscopy. In samples with low uranium content, the pyrolysis-gas chromatography products contain oxygenated functional groups (as hydroxyl) and molecules with both aliphatic and aromatic carbon atoms. These samples with low uranium content give measurable Rock-Eval hydrocarbon and organic-CO2 yields, and C-13 NMR values of > 30% aliphatic carbon. In contrast, uranium-rich samples have few hydrocarbon pyrolysis products, increased Rock-Eval organic-CO2 contents and > 70% aromatic carbon contents from C-13 NMR. The increase in aromaticity and decrease in hydrocarbon pyrolysis yield are related to the amount of uranium and the age of the uranium minerals, which correspond to the degree of radiation damage. The three analytical techniques give complementary results. Increase in Rock-Eval organic-CO2 yield correlates with uranium content for samples from the Grants uranium region. Calculations show that the amount of organic-CO2 corresponds to the quantity of uranium chemically reduced by the organic matter for the Grants uranium region samples. ?? 1986.
Kinetics of triscarbonato uranyl reduction by aqueous ferrous iron: a theoretical study.
Wander, Matthew C F; Kerisit, Sebastien; Rosso, Kevin M; Schoonen, Martin A A
2006-08-10
Uranium is a pollutant whose mobility is strongly dependent on its oxidation state. While U(VI) in the form of the uranyl cation is readily reduced by a range of natural reductants, by contrast complexation of uranyl by carbonate greatly reduces its reduction potential and imposes increased electron transfer (ET) distances. Very little is known about the elementary processes involved in uranium reduction from U(VI) to U(V) to U(IV) in general. In this study, we examine the theoretical kinetics of ET from ferrous iron to triscarbonato uranyl in aqueous solution. A combination of molecular dynamics (MD) simulations and density functional theory (DFT) electronic structure calculations is employed to compute the parameters that enter into Marcus' ET model, including the thermodynamic driving forces, reorganization energies, and electronic coupling matrix elements. MD simulations predict that two ferrous iron atoms will bind in an inner-sphere fashion to the three-membered carbonate ring of triscarbonato uranyl, forming the charge-neutral ternary Fe(2)UO(2)(CO(3))(3)(H(2)O)(8) complex. Through a sequential proton-coupled electron-transfer mechanism (PCET), the first ET step converting U(VI) to U(V) is predicted by DFT to occur with an electronic barrier that corresponds to a rate on the order of approximately 1 s(-1). The second ET step converting U(V) to U(IV) is predicted to be significantly endergonic. Therefore, U(V) is a stabilized end product in this ET system, in agreement with experiment.
Lu-Fritts, Pai-Yue; Kottyan, Leah C.; James, Judith A.; Xie, Changchung; Buckholz, Jeanette M.; Pinney, Susan M.; Harley, John B.
2014-01-01
Objective Explore the hypothesis that cases of SLE will be found more frequently in community members with high prior uranium exposure in the Fernald Community Cohort (FCC). Methods A nested case control study was performed. The FCC is a volunteer population that lived near a uranium ore processing plant in Fernald, Ohio, USA during plant operation and members were monitored for 18 years. Uranium plant workers were excluded. SLE cases were identified using American College of Rheumatology classification criteria, laboratory testing, and medical record review. Each case was matched to four age-, race-, and sex-matched controls. Sera from potential cases and controls were screened for autoantibodies. Cumulative uranium particulate exposure was calculated using a dosimetry model. Logistic regression with covariates was used to calculate odds ratios (OR) with 95% confidence intervals (CI). Results The FCC includes 4,187 individuals with background uranium exposure, 1,273 with moderate exposure, and 2,756 with higher exposure. SLE was confirmed in 23 of 31 individuals with a lupus ICD9 code, and in 2 of 43 other individuals prescribed hydroxychloroquine. The female:male ratio was 5.25:1. Of the 25 SLE cases, 12 were in the higher exposure group. SLE was associated with higher uranium exposure (OR 3.92, 95% CI 1.131-13.588, p = 0.031). Conclusion High uranium exposure is associated with SLE relative to matched controls in this sample of uranium exposed individuals. Potential explanations for this relationship include possible autoimmune or estrogen effects of uranium, somatic mutation, epigenetic effects, or effects of some other unidentified accompanying exposure. PMID:25103365
Brugge, Doug; de Lemos, Jamie L; Oldmixon, Beth
2005-01-01
Natural uranium exposure derives from the mining, milling, and processing of uranium ore, as well as from ingestion of groundwater that is naturally contaminated with uranium. Ingestion and inhalation are the primary routes of entry into the body. Absorption of uranium from the lungs or digestive track is typically low but can vary depending on compound specific solubility. From the blood, two-thirds of the uranium is excreted in urine over the first 24 hours and up to 80% to 90% of uranium deposited in the bone leaves the body within 1.5 years. The primary health outcomes of concern documented with respect to uranium are renal, developmental, reproductive, diminished bone growth, and DNA damage. The reported health effects derive from experimental animal studies and human epidemiology. The Lowest Observed Adverse Effect Level (LOAEL) derived from animal studies is 50 microg/m3 for inhalation and 60 ug/kg body weight/day for ingestion. The current respiratory standard of the Occupational Safety and Health Administration (OSHA), 50 microg/m3, affords no margin of safety. Considering the safety factors for species and individual variation, the ingestion LOAEL corresponds to the daily consumption set by the World Health Organization Drinking Water Standard at 2 microg/L. Based on economic considerations, the United States Environmental Protection Agency maximum contaminant level is 30 microg/L. Further research is needed, with particular attention on the impact of uranium on indigenous populations, on routes of exposure in communities near uranium sites, on the combined exposures present at many uranium sites, on human developmental defects, and on health effects at or below established exposure standards.
Polovov, Ilya B; Volkovich, Vladimir A; Charnock, John M; Kralj, Brett; Lewin, Robert G; Kinoshita, Hajime; May, Iain; Sharrad, Clint A
2008-09-01
Soluble uranium chloride species, in the oxidation states of III+, IV+, V+, and VI+, have been chemically generated in high-temperature alkali chloride melts. These reactions were monitored by in situ electronic absorption spectroscopy. In situ X-ray absorption spectroscopy of uranium(VI) in a molten LiCl-KCl eutectic was used to determine the immediate coordination environment about the uranium. The dominant species in the melt was [UO 2Cl 4] (2-). Further analysis of the extended X-ray absorption fine structure data and Raman spectroscopy of the melts quenched back to room temperature indicated the possibility of ordering beyond the first coordination sphere of [UO 2Cl 4] (2-). The electrolytic generation of uranium(III) in a molten LiCl-KCl eutectic was also investigated. Anodic dissolution of uranium metal was found to be more efficient at producing uranium(III) in high-temperature melts than the cathodic reduction of uranium(IV). These high-temperature electrolytic processes were studied by in situ electronic absorption spectroelectrochemistry, and we have also developed in situ X-ray absorption spectroelectrochemistry techniques to probe both the uranium oxidation state and the uranium coordination environment in these melts.
Use of Polyphosphate to Decrease Uranium Leaching in Hanford 300 Area Smear Zone Sediments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Szecsody, James E.; Zhong, Lirong; Oostrom, Martinus
2012-09-30
The primary objective of this study is to summarize the laboratory investigations performed to evaluate short- and long-term effects of phosphate treatment on uranium leaching from 300 area smear zone sediments. Column studies were used to compare uranium leaching in phosphate-treated to untreated sediments over a year with multiple stop flow events to evaluate longevity of the uranium leaching rate and mass. A secondary objective was to compare polyphosphate injection, polyphosphate/xanthan injection, and polyphosphate infiltration technologies that deliver phosphate to sediment.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhang, Fan; Parker, Jack C.; Watson, David B
This study investigates uranium and technetium sorption onto aluminum and iron hydroxides during titration of acidic groundwater. The contaminated groundwater exhibits oxic conditions with high concentrations of NO{sub 3}{sup -}, SO{sub 4}{sup 2-}, U, Tc, and various metal cations. More than 90% of U and Tc was removed from the aqueous phase as Al and Fe precipitated above pH 5.5, but was partially resolublized at higher pH values. An equilibrium hydrolysis and precipitation reaction model adequately described variations in aqueous concentrations of metal cations. An anion exchange reaction model was incorporated to simulate sulfate, U and Tc sorption onto variablymore » charged (pH-dependent) Al and Fe hydroxides. Modeling results indicate that competitive sorption/desorption on mixed mineral phases needs to be considered to adequately predict U and Tc mobility. The model could be useful for future studies of the speciation of U, Tc and co-existing ions during pre- and post-groundwater treatment practices.« less
Pyrophoric behaviour of uranium hydride and uranium powders
NASA Astrophysics Data System (ADS)
Le Guyadec, F.; Génin, X.; Bayle, J. P.; Dugne, O.; Duhart-Barone, A.; Ablitzer, C.
2010-01-01
Thermal stability and spontaneous ignition conditions of uranium hydride and uranium metal fine powders have been studied and observed in an original and dedicated experimental device placed inside a glove box under flowing pure argon. Pure uranium hydride powder with low amount of oxide (<0.5 wt.%) was obtained by heat treatment at low temperature in flowing Ar/5%H2. Pure uranium powder was obtained by dehydration in flowing pure argon. Those fine powders showed spontaneous ignition at room temperature in air. An in situ CCD-camera displayed ignition associated with powder temperature measurement. Characterization of powders before and after ignition was performed by XRD measurements and SEM observations. Oxidation mechanisms are proposed.
Estimated Marine Residence Times for Drowned Barbadian Paleoreefs
NASA Astrophysics Data System (ADS)
Mey, J. L.
2008-12-01
Fossil corals are used to estimate past sea level and also to calibrate 14C ages with the aid of U-Th and U-Pa dating methods. These coral fossils have often been subaerially exposed and thus are affected by diagenesis during their initial interaction with fresh water. In an effort to understand when such disequilibria in fossil coral reefs occurred, we have quantified our 'dissolution-cum-adsorption' model (Mey, 2008) for the uranium series disequilibria using a geometrical construction, based on the evolution of the activities in a 230Th/238U versus 234U/238U diagram for closed versus open systems. The traditional age equations for the uranium-series with excess daughters have been used to construct a relationship between (i) the angles of the equal age lines in the 230Th/238U versus 234U/238U activity diagrams, and (ii) the quantified angles of the regressed lines of several uranium series disequilibria trends from Barbados. Our results indicate that the severity of the Barbados uranium series disequilibria is not only explained by 234U and 230Th addition, but may also reflect a loss of 238U through dissolution of coral skeletal structure. The net effect is 238U removal, whereas 234U and 230Th remain; thus, the disequilibria for the extant coral increase the excess daughters' ratio. Our results further indicate that the activity of 234U is reduced (compared to 230Th), as would be expected in regard to the lower mobility of trapped 230Th. It is proposed that the major dissolution that caused the uranium series disequilibria occurred during one relatively short-lived event when the paleoreefs experienced the very first freshwater exposure. During this event, the diagenetic potential was at its maximum for redistribution of the uranium series; this then caused the 234U and the 230Th to behave in a systematic way, resulting in linear trends. The linear trends in the open system uranium series were set early, as shown in the 230Th/238U versus 234U/238U activity diagrams. The timing of the first exposure of the freshwater in the reefs is calculated based on the results of our new model. From the relationship between, (i) dissolution, (ii) in-grown 230Th, and (iii) excess 234U, we derived that the 60,000 old Marine Isotope stage 3 (MIS 3) reef was exposed to freshwater 36-38,000 years after growth in the marine environment. We have calculated these 'marine residence times' for the MIS 3 5a, 5c, 5e, 6.0, 7a and 7c reefs; our results correspond with the duration of the sea level high stand in each of the stages. References: Mey, J. L., (2008) The Uranium Series Diagenesis and the Morphology of Drowned Barbadian Paleoreefs, PhD dissertation, 325pp: Graduate Center, City University of New York, New York.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Saccomanno, G.
This work supported by the United States of Energy, continues to add data on the health affects of cigarette smoking and radon exposure on uranium miners. Since the last Technical Progress Report in July or 1991, 537 sputum cytology samples have been collected on the 300 uranium workers in the surveillance study. To date there are 436 lung cancer cases in the Uranium Miner Tumor Registry with diagnostic slides from surgery and/or autopsy; an additional 40 cases have been diagnosed with sputum cytology only. In March of 1991 the Geno Saccomanno Uranium Workers Archive was established at St. Mary`s Hospitalmore » and Medical Center as a depository for biological specimens and epidemiological data from the 17,700 uranium miners who have been a part or the study.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Saccomanno, G.
This work supported by the United States of Energy, continues to add data on the health affects of cigarette smoking and radon exposure on uranium miners. Since the last Technical Progress Report in July or 1991, 537 sputum cytology samples have been collected on the 300 uranium workers in the surveillance study. To date there are 436 lung cancer cases in the Uranium Miner Tumor Registry with diagnostic slides from surgery and/or autopsy; an additional 40 cases have been diagnosed with sputum cytology only. In March of 1991 the Geno Saccomanno Uranium Workers Archive was established at St. Mary's Hospitalmore » and Medical Center as a depository for biological specimens and epidemiological data from the 17,700 uranium miners who have been a part or the study.« less
NASA Astrophysics Data System (ADS)
Tran, E. L.; Teutsch, N.; Klein-BenDavid, O.; Weisbrod, N.
2017-12-01
When radionuclides are leaked into the subsurface due to engineered waste disposal container failure, the ultimate barrier to migration of radionuclides into local aquifers is sorption to the surrounding rock matrix and sediments, which often includes a bentonite backfill. The extent of this sorption is dependent on pH, ionic strength, surface area availability, radionuclide concentration, surface mineral composition, and solution chemistry. Colloidal-sized bentonite particles eroded from the backfill have been shown to facilitate the transport of radionuclides sorbed to them away from their source. Thus, sorption of radionuclides such as uranium and cesium to bentonite surfaces can be both a mobilization or retardation factor. Though numerous studies have been conducted to-date on sorption of radionuclides under low ionic strength and carbonate-poor conditions, there has been little research conducted on the behavior of radionuclides in high salinities and carbonate rich conditions typical of aquifers in the vicinity of some potential nuclear repositories. This study attempts to characterize the sorption properties of U(VI) and Cs to bentonite colloids under these conditions using controlled batch experiments. Results indicated that U(VI) undergoes little to no sorption to bentonite colloids in a high-salinity (TDS= 9000 mg/L) artificial groundwater. This lack of sorption was attributed to the formation of CaUO2(CO3)22- and Ca2UO2(CO3)3 aqueous ions which stabilize the UO22+ ions in solution. In contrast, Cs exhibited greater sorption, the extent to which was influenced greatly by the matrix water's ionic strength and the colloid concentration used. Surprisingly, when both U and Cs were together, the presence of U(VI) in solution decreased Cs sorption, possibly due to the formation of stabilizing CaUO2(CO3)22- anions. The implications of this research are that rather than undergoing colloid-facilitated transport, U(VI) is expected to migrate similarly to a conservative dissolved species under these conditions, and little retardation through sorption onto the surrounding rock matrix is predicted. Cs is expected to undergo more sorption, though U(VI) presence may have a mobilizing effect.
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
Zielinski, Robert A.
1979-01-01
Well-characterized samples of rhyolitic obsidian, perlite and felsite from a single lava flow are leached of U by alkaline oxidizing solutions under open-system conditions. Pressure, temperature, flow rate and solution composition are held constant in order to evaluate the relative importance of differences in surface area and crystallinity. Under the experimental conditions U removal from crushed glassy samples proceeds by a mechanism of glass dissolution in which U and silica are dissolved in approximately equal weight fractions. The rate of U removal from crushed glassy samples increases with decreasing average grain size (surface area). Initial rapid loss of a small component (≈ 2.5%) of the total U from crushed felsite. followed by much slower U loss, reflects variable rates of attack of numerous uranium sites. The fractions of U removed during the experiment ranged from 3.2% (felsite) to 27% (perlite). An empirical method for evaluating the relative rate of U loss from contemporaneous volcanic rocks is presented which incorporates leaching results and rock permeability data.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Andersson, Anders David Ragnar; Pastore, Giovanni; Liu, Xiang-Yang
2014-11-07
This report summarizes the development of new fission gas diffusion models from lower length scale simulations and assessment of these models in terms of annealing experiments and fission gas release simulations using the BISON fuel performance code. Based on the mechanisms established from density functional theory (DFT) and empirical potential calculations, continuum models for diffusion of xenon (Xe) in UO 2 were derived for both intrinsic conditions and under irradiation. The importance of the large X eU3O cluster (a Xe atom in a uranium + oxygen vacancy trap site with two bound uranium vacancies) is emphasized, which is a consequencemore » of its high mobility and stability. These models were implemented in the MARMOT phase field code, which is used to calculate effective Xe diffusivities for various irradiation conditions. The effective diffusivities were used in BISON to calculate fission gas release for a number of test cases. The results are assessed against experimental data and future directions for research are outlined based on the conclusions.« less
Märten, Arno; Berger, Dietrich; Köhler, Mirko; Merten, Dirk
2015-12-01
We reconstructed the contamination history of an area influenced by 40 years of uranium mining and subsequent remediation actions using dendroanalysis (i.e., the determination of the elemental content of tree rings). The uranium content in the tree rings of four individual oak trees (Quercus sp.) was determined by laser ablation with inductively coupled plasma mass spectrometry (LA-ICP-MS). This technique allows the investigation of trace metals in solid samples with a spatial resolution of 250 μm and a detection limit below 0.01 μg/g for uranium. The investigations show that in three of the four oaks sampled, there were temporally similar uranium concentrations. These were approximately 2 orders of magnitude higher (0.15 to 0.4 μg/g) than those from before the period of active mining (concentrations below 0.01 μg/g). After the mining was terminated and the area was restored, the uranium contents in the wood decreased by approximately 1 order of magnitude. The similar radial uranium distribution patterns of the three trees were confirmed by correlation analysis. In combination with the results of soil analyses, it was determined that there was a heterogeneous contamination in the forest investigated. This could be confirmed by pre-remediation soil uranium contents from literature. The uranium contents in the tree rings of the oaks investigated reflect the contamination history of the study area. This study demonstrates that the dendrochemical analysis of oak tree rings is a suitable technique for investigating past and recent uranium contamination in mining areas.
Study on immobilization and migration of nuclide u in superficial soil of uranium tailings pond
NASA Astrophysics Data System (ADS)
Chang, Zhe; Zhou, Shukui
2017-05-01
The uranium tailings in southern China was used as the object of study to study the fixation and migration characteristics of nuclide U in shallow tailings. The results showed that the precipitation of tailings in the tailings soil was not linearly related to the depth during the acid rain leaching process. Tailings soil in the role of fixatives, when the lime as a fixative, the tailings of different soil uranium in 20 days after the re-precipitation. However, when lime and ammonium phosphate were used as fixing agents, the cumulative precipitation of U had a significant effect, and the migration of uranium was inhibited.
Absorption, accumulation and biological effects of depleted uranium in Peyer's patches of rats.
Dublineau, I; Grison, S; Grandcolas, L; Baudelin, C; Tessier, C; Suhard, D; Frelon, S; Cossonnet, C; Claraz, M; Ritt, J; Paquet, P; Voisin, P; Gourmelon, P
2006-10-29
The digestive tract is the entry route for radionuclides following the ingestion of contaminated food and/or water wells. It was recently characterized that the small intestine was the main area of uranium absorption throughout the gastrointestinal tract. This study was designed to determine the role played by the Peyer's patches in the intestinal absorption of uranium, as well as the possible accumulation of this radionuclide in lymphoid follicles and the toxicological or pathological consequences on the Peyer's patch function subsequent to the passage and/or accumulation of uranium. Results of experiments performed in Ussing chambers indicate that the apparent permeability to uranium in the intestine was higher (10-fold) in the mucosa than in Peyer's patches ((6.21+/-1.21 to 0.55+/-0.35)x10(-6)cm/s, respectively), demonstrating that the small intestinal epithelium was the preferential pathway for the transmucosal passage of uranium. A quantitative analysis of uranium by ICP-MS following chronic contamination with depleted uranium during 3 or 9 months showed a preferential accumulation of uranium in Peyer's patches (1355% and 1266%, respectively, at 3 and 9 months) as compared with epithelium (890% and 747%, respectively, at 3 and 9 months). Uranium was also detected in the mesenteric lymph nodes ( approximately 5-fold after contamination with DU). The biological effects of this accumulation of depleted uranium after chronic contamination were investigated in Peyer's patches. There was no induction of the apoptosis pathway after chronic DU contamination in Peyer's patches. The results indicate no change in the cytokine expression (Il-10, TGF-beta, IFN-gamma, TNF-alpha, MCP-1) in Peyer's patches and in mesenteric lymph nodes, and no modification in the uptake of yeast cells by Peyer's patches. In conclusion, this study shows that the Peyer's patches were a site of retention for uranium following the chronic ingestion of this radionuclide, without any biological consequences of such accumulation on Peyer's patch functions.
Bone as a Possible Target of Chemical Toxicity of Natural Uranium in Drinking Water
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
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Shusterman, Jennifer A.
We are measuring freshly separated uranium samples using modern list mode (event-by-event) electronics with high resolution HPGe detectors to study the in-growth behaviors of uranium daughters’ gamma-rays. These data will show how we can use gamma-ray spectroscopy to determine the separation date for processed uranium. With this knowledge, one can obtain proper uranium isotope ratios using standard safeguards accountability software such as U-235 or MGAU.
Application of remote sensor data to geologic analysis of the Bonanza test site Colorado
NASA Technical Reports Server (NTRS)
Lee, K. (Compiler)
1975-01-01
Selected samples of anomalous surface features commonly associated with the various types of uranium deposits are presented and recommendations for sensor applications are given. The features studied include: epigenetic uranium ore roll type; precambrian basal conglomerate type; vein-type uranium deposits; pipe-structure or diatreme deposits; evaporitic uranium deposits. The hydrogeology of the Mosquito Range and the San Luis Valley is also examined.
2006-10-01
Embedded Depleted Uranium and Heavy-Metal Tungsten Alloy in Rodents PRINCIPAL INVESTIGATOR: John F. Kalinich, Ph.D...Carcinogenicity and Immunotoxicity of Embedded Depleted Uranium and Heavy- Metal Tungsten Alloy in Rodents 5b. GRANT NUMBER DAMD17-01-1-0821 5c...ABSTRACT This study investigated the carcinogenic and immunotoxic potential of embedded fragments of depleted uranium (DU) and a heavy-metal tungsten
Vanhoudt, Nathalie; Vandenhove, Hildegarde; Horemans, Nele; Wannijn, Jean; Van Hees, May; Vangronsveld, Jaco; Cuypers, Ann
2010-11-01
Uranium never occurs as a single pollutant in the environment, but always in combination with other stressors such as ionizing radiation. As effects induced by multiple contaminants can differ markedly from the effects induced by the individual stressors, this multiple pollution context should not be neglected. In this study, effects on growth, nutrient uptake and oxidative stress induced by the single stressors uranium and gamma radiation are compared with the effects induced by the combination of both stressors. By doing this, we aim to better understand the effects induced by the combined stressors but also to get more insight in stressor-specific response mechanisms. Eighteen-day-old Arabidopsis thaliana seedlings were exposed for 3 days to 10 muM uranium and 3.5 Gy gamma radiation. Gamma radiation interfered with uranium uptake, resulting in decreased uranium concentrations in the roots, but with higher transport to the leaves. This resulted in a better root growth but increased leaf lipid peroxidation. For the other endpoints studied, effects under combined exposure were mostly determined by uranium presence and only limited influenced by gamma presence. Furthermore, an important role is suggested for CAT1/2/3 gene expression under uranium and mixed stressor conditions in the leaves.
Conceptual Core Analysis of Long Life PWR Utilizing Thorium-Uranium Fuel Cycle
NASA Astrophysics Data System (ADS)
Rouf; Su'ud, Zaki
2016-08-01
Conceptual core analysis of long life PWR utilizing thorium-uranium based fuel has conducted. The purpose of this study is to evaluate neutronic behavior of reactor core using combined thorium and enriched uranium fuel. Based on this fuel composition, reactor core have higher conversion ratio rather than conventional fuel which could give longer operation length. This simulation performed using SRAC Code System based on library SRACLIB-JDL32. The calculation carried out for (Th-U)O2 and (Th-U)C fuel with uranium composition 30 - 40% and gadolinium (Gd2O3) as burnable poison 0,0125%. The fuel composition adjusted to obtain burn up length 10 - 15 years under thermal power 600 - 1000 MWt. The key properties such as uranium enrichment, fuel volume fraction, percentage of uranium are evaluated. Core calculation on this study adopted R-Z geometry divided by 3 region, each region have different uranium enrichment. The result show multiplication factor every burn up step for 15 years operation length, power distribution behavior, power peaking factor, and conversion ratio. The optimum core design achieved when thermal power 600 MWt, percentage of uranium 35%, U-235 enrichment 11 - 13%, with 14 years operation length, axial and radial power peaking factor about 1.5 and 1.2 respectively.
Guéguen, Yann; Roy, Laurence; Hornhardt, Sabine; Badie, Christophe; Hall, Janet; Baatout, Sarah; Pernot, Eileen; Tomasek, Ladislav; Laurent, Olivier; Ebrahimian, Teni; Ibanez, Chrystelle; Grison, Stephane; Kabacik, Sylwia; Laurier, Dominique; Gomolka, Maria
2017-01-01
Despite substantial experimental and epidemiological research, there is limited knowledge of the uranium-induce health effects after chronic low-dose exposures in humans. Biological markers can objectively characterize pathological processes or environmental responses to uranium and confounding agents. The integration of such biological markers into a molecular epidemiological study would be a useful approach to improve and refine estimations of uranium-induced health risks. To initiate such a study, Concerted Uranium Research in Europe (CURE) was established, and involves biologists, epidemiologists and dosimetrists. The aims of the biological work package of CURE were: 1. To identify biomarkers and biological specimens relevant to uranium exposure; 2. To define standard operating procedures (SOPs); and 3. To set up a common protocol (logistic, questionnaire, ethical aspects) to perform a large-scale molecular epidemiologic study in uranium-exposed cohorts. An intensive literature review was performed and led to the identification of biomarkers related to: 1. retention organs (lungs, kidneys and bone); 2. other systems/organs with suspected effects (cardiovascular system, central nervous system and lympho-hematopoietic system); 3. target molecules (DNA damage, genomic instability); and 4. high-throughput methods for the identification of new biomarkers. To obtain high-quality biological materials, SOPs were established for the sampling and storage of different biospecimens. A questionnaire was developed to assess potential confounding factors. The proposed strategy can be adapted to other internal exposures and should improve the characterization of the biological and health effects that are relevant for risk assessment.
NASA Astrophysics Data System (ADS)
Johnson, T.; Hammond, G. E.; Versteeg, R. J.; Zachara, J. M.
2013-12-01
The Hanford 300 Area, located adjacent to the Columbia River in south-central Washington, USA, is the site of former research and uranium fuel rod fabrication facilities. Waste disposal practices at site included discharging between 33 and 59 metric tons of uranium over a 40 year period into shallow infiltration galleries, resulting in persistent uranium contamination within the vadose and saturated zones. Uranium transport from the vadose zone to the saturated zone is intimately linked with water table fluctuations and river water intrusion driven by upstream dam operations. As river stage increases, the water table rises into the vadose zone and mobilizes contaminated pore water. At the same time, river water moves inland into the aquifer, and river water chemistry facilitates further mobilization by enabling uranium desorption from contaminated sediments. As river stage decreases, flow moves toward the river, ultimately discharging contaminated water at the river bed. River water specific conductance at the 300 Area varies around 0.018 S/m whereas groundwater specific conductance varies around 0.043 S/m. This contrast provides the opportunity to monitor groundwater/river water interaction by imaging changes in bulk conductivity within the saturated zone using time-lapse electrical resistivity tomography. Previous efforts have demonstrated this capability, but have also shown that disconnecting regularization constraints at the water table is critical for obtaining meaningful time-lapse images. Because the water table moves with time, the regularization constraints must also be transient to accommodate the water table boundary. This was previously accomplished with 2D time-lapse ERT imaging by using a finely discretized computational mesh within the water table interval, enabling a relatively smooth water table to be defined without modifying the mesh. However, in 3D this approach requires a computational mesh with an untenable number of elements. In order to accommodate the water table boundary in 3D, we propose a time-lapse warping mesh inversion, whereby mesh elements that traverse the water table are modified to generate a smooth boundary at the known water table position, enabling regularization constraints to be accurately disconnected across the water table boundary at a given time. We demonstrate the approach using a surface ERT array installed adjacent to the Columbia River at the 300 Area, consisting of 352 electrodes and covering an area of approximately 350 m x 350 m. Using autonomous data collection, transmission, and filtering tools coupled with high performance computing resources, the 4D imaging process is automated and executed in real time. Each time lapse survey consists of approximately 40,000 measurements and 4 surveys are collected and processed per day from April 1st , 2013 to September 30th, 2013. The data are inverted on an unstructured tetrahedral mesh that honors LiDAR-based surface topography and is comprised of approximately 905,000 elements. Imaging results show the dynamic 4D extent of river water intrusion, and are validated with well-based fluid conductivity measurements at each monitoring well within the imaging domain.
Uranium Associations with Kidney Outcomes Vary by Urine Concentration Adjustment Method
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
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(VI) interactions with mackinawite in the presence and absence of bicarbonate and oxygen
Gallegos, Tanya J.; Fuller, Christopher C.; Webb, Samuel M.; Betterton, William J.
2013-01-01
Mackinawite, Fe(II)S, samples loaded with uranium (10-5, 10-4, and 10-3 mol U/g FeS) at pH 5, 7, and 9, were characterized using X-ray absorption spectroscopy and X-ray diffraction to determine the effects of pH, bicarbonate, and oxidation on uptake. Under anoxic conditions, a 5 g/L suspension of mackinawite lowered 5 × 10-5 M uranium(VI) to below 30 ppb (1.26 × 10-7 M) U. Between 82 and 88% of the uranium removed from solution by mackinawite was U(IV) and was nearly completely reduced to U(IV) when 0.012 M bicarbonate was added. Near-neighbor coordination consisting of uranium–oxygen and uranium-uranium distances indicates the formation of uraninite in the presence and absence of bicarbonate, suggesting reductive precipitation as the dominant removal mechanism. Following equilibration in air, mackinawite was oxidized to mainly goethite and sulfur and about 76% of U(IV) was reoxidized to U(VI) with coordination of uranium to axial and equatorial oxygen, similar to uranyl. Additionally, uranium-iron distances, typical of coprecipitation of uranium with iron oxides, and uranium-sulfur distances indicating bidentate coordination of U(VI) to sulfate were evident. The affinity of mackinawite and its oxidation products for U(VI) provides impetus for further study of mackinawite as a potential reactive medium for remediation of uranium-contaminated water.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Buck, E.C.; Cunnane, J.C.; Brown, N.R.
A combination of optical microscopy, scanning electron microscopy with backscattered electron detection (SEM/BSE), and analytical electron microscopy (AEM) is being used to determine the nature of uranium in soils from the Fernald Environmental Management Project. The information gained from these studies is being used to develop and test remediation technologies. Investigations using SEM have shown that uranium is contained within particles that are typically 1 to 100 {mu}m in diameter. Further analysis with AEM has shown that these uranium-rich regions are made up of discrete uranium-bearing phases. The distribution of these uranium phases was found to be inhomogeneous at themore » microscopic level.« less
The Main Factors of Uranium Accumulation in the Ishim Plain Saline Lakes (Western Siberia)
NASA Astrophysics Data System (ADS)
Vladimirov, A. G.; Krivonogov, S. K.; Karpov, A. V.; Nikolaeva, I. V.; Razvorotneva, L. I.; Kolpakova, M. N.; Moroz, E. N.
2018-04-01
Hydrochemical analysis of the high-salinity lakes in the Ishim Plain (>250-300 g/L) located at the border with the Northern Kazakhstan uranium ore province is performed. The studies have shown that the main factor of concentration and redistribution of uranium in the lake basins of the Ishim Plain are the processes of intense salt deflation causing sanding of lakes and uranium depletion in the near-surface layer of the bottom deposits. The correlation between the hydroxide forms of uranium binding in the bottom lacustrine deposits of the Ishim Plain and the coffinite composition of the Semizbai deposit makes it possible to consider this province to be promising for the discovery of hydromineral uranium deposits.
Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation
Mayer, Klaus; Wallenius, Maria; Lützenkirchen, Klaus; Horta, Joan; Nicholl, Adrian; Rasmussen, Gert; van Belle, Pieter; Varga, Zsolt; Buda, Razvan; Erdmann, Nicole; Kratz, Jens-Volker; Trautmann, Norbert; Fifield, L Keith; Tims, Stephen G; Fröhlich, Michaela B; Steier, Peter
2015-01-01
Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel.3b,d, 4 Through measurement of the 230Th/234U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the 87Sr/86Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of 236U and 239Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence. PMID:26501922
Uranium and the Central Nervous System: What Should We Learn from Recent New Tools and Findings?
Dinocourt, Céline
2017-01-01
Increasing industrial and military use of uranium has led to environmental pollution, which may result in uranium reaching the brain and causing cerebral dysfunction. A recent literature review has discussed data published over the last 10 years on uranium and its effects on brain function (Dinocourt C, Legrand M, Dublineau I, et al., Toxicology 337:58-71, 2015). New models of uranium exposure during neonatal brain development and the emergence of new technologies (omics and epigenetics) are of value in identifying new specific targets of uranium. Here we review the latest studies of neurogenesis, epigenetics, and metabolic dysfunctions and the identification of new biomarkers used to establish potential pathophysiological states of neurodevelopmental and neurodegenerative diseases.
Leukemia and exposure to ionizing radiation among German uranium miners.
Möhner, Matthias; Lindtner, Manfred; Otten, Heinz; Gille, Hans-G
2006-04-01
It is well known that uranium miners are at an increased risk of lung cancer. Whether they also have an increased risk for other cancer sites remains under discussion. The aim of this study was to examine the leukemia risk among miners. An individually matched case-control study of former uranium miners in East Germany was conducted with 377 cases and 980 controls. Using conditional logistic regression models, a dose-response relationship between leukemia risk and radon progeny could not be confirmed. Yet, a significantly elevated risk is seen in the category > or = 400 mSv when combining gamma-radiation and long-lived radionuclides. The results suggest that an elevated risk for leukemia is restricted to employees with a very long occupational career in underground uranium mining or uranium processing. Moreover, the study does not support the hypothesis of an association between exposure to short-lived radon progeny and leukemia risk. Copyright 2006 Wiley-Liss, Inc.
Uranium quantification in semen by inductively coupled plasma mass spectrometry
Todorov, Todor I.; Ejnik, John W.; Guandalini, Gustavo S.; Xu, Hanna; Hoover, Dennis; Anderson, Larry W.; Squibb, Katherine; McDiarmid, Melissa A.; Centeno, Jose A.
2013-01-01
In this study we report uranium analysis for human semen samples. Uranium quantification was performed by inductively coupled plasma mass spectrometry. No additives, such as chymotrypsin or bovine serum albumin, were used for semen liquefaction, as they showed significant uranium content. For method validation we spiked 2 g aliquots of pooled control semen at three different levels of uranium: low at 5 pg/g, medium at 50 pg/g, and high at 1000 pg/g. The detection limit was determined to be 0.8 pg/g uranium in human semen. The data reproduced within 1.4–7% RSD and spike recoveries were 97–100%. The uranium level of the unspiked, pooled control semen was 2.9 pg/g of semen (n = 10). In addition six semen samples from a cohort of Veterans exposed to depleted uranium (DU) in the 1991 Gulf War were analyzed with no knowledge of their exposure history. Uranium levels in the Veterans’ semen samples ranged from undetectable (<0.8 pg/g) to 3350 pg/g. This wide concentration range for uranium in semen is consistent with known differences in current DU body burdens in these individuals, some of whom have retained embedded DU fragments.
Depleted uranium analysis in blood by inductively coupled plasma mass spectrometry
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.
Alternative alkaline conditioning of amidoxime based adsorbent for uranium extraction from seawater
Das, Sadananda; Liao, Wei -Po; Byers, Maggie Flicker; ...
2015-10-18
Alkaline conditioning of the amidoxime based adsorbents is a significant step in the preparation of the adsorbent for uranium uptake from seawater. The effects of various alkaline conditioning parameters such as the type of alkaline reagent, reaction temperature, and reaction time were investigated with respect to uranium adsorption capacity from simulated seawater (spiked with 8 ppm uranium) and natural seawater (from Sequim Bay, WA). An adsorbent (AF1) was prepared at the Oak Ridge National Laboratory by radiation-induced graft polymerization (RIGP) with acrylonitrile and itaconic acid onto high-surface-area polyethylene fibers. For the AF1 adsorbent, sodium hydroxide emerged as a better reagentmore » for alkaline conditioning over potassium hydroxide, which has typically been used in previous studies, because of higher uranium uptake capacity and lower cost over the other candidate alkaline reagents investigated in this study. Furthermore, the use of sodium hydroxide in place of potassium hydroxide is shown to result in a 21–30% decrease in the cost of uranium recovery.« less
Assessment of age-dependent uranium intake due to drinking water in Hyderabad, India.
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).
Alternative Alkaline Conditioning of Amidoxime Based Adsorbent for Uranium Extraction from Seawater
DOE Office of Scientific and Technical Information (OSTI.GOV)
Das, S.; Liao, W. -P.; Flicker Byers, M.
2016-04-20
Alkaline conditioning of the amidoxime based adsorbents is a significant step in the preparation of the adsorbent for uranium uptake from seawater. The effects of various alkaline conditioning parameters such as the type of alkaline reagent, reaction temperature, and reaction time were investigated with respect to uranium adsorption capacity from simulated seawater (spiked with 8 ppm uranium) and natural seawater (from Sequim Bay, WA). An adsorbent (AF1) was prepared at the Oak Ridge National Laboratory by radiation-induced graft polymerization (RIGP) with acrylonitrile and itaconic acid onto high-surface-area polyethylene fibers. For the AF1 adsorbent, sodium hydroxide emerged as a better reagentmore » for alkaline conditioning over potassium hydroxide, which has typically been used in previous studies, because of higher uranium uptake capacity and lower cost over the other candidate alkaline reagents investigated in this study. Use of sodium hydroxide in place of potassium hydroxide is shown to result in a 21-30% decrease in the cost of uranium recovery.« less
Alternative alkaline conditioning of amidoxime based adsorbent for uranium extraction from seawater
DOE Office of Scientific and Technical Information (OSTI.GOV)
Das, Sadananda; Liao, Wei -Po; Byers, Maggie Flicker
Alkaline conditioning of the amidoxime based adsorbents is a significant step in the preparation of the adsorbent for uranium uptake from seawater. The effects of various alkaline conditioning parameters such as the type of alkaline reagent, reaction temperature, and reaction time were investigated with respect to uranium adsorption capacity from simulated seawater (spiked with 8 ppm uranium) and natural seawater (from Sequim Bay, WA). An adsorbent (AF1) was prepared at the Oak Ridge National Laboratory by radiation-induced graft polymerization (RIGP) with acrylonitrile and itaconic acid onto high-surface-area polyethylene fibers. For the AF1 adsorbent, sodium hydroxide emerged as a better reagentmore » for alkaline conditioning over potassium hydroxide, which has typically been used in previous studies, because of higher uranium uptake capacity and lower cost over the other candidate alkaline reagents investigated in this study. Furthermore, the use of sodium hydroxide in place of potassium hydroxide is shown to result in a 21–30% decrease in the cost of uranium recovery.« less
Ladshaw, Austin P.; Ivanov, Alexander S.; Das, Sadananda; ...
2018-03-27
Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material’s relatively poor selectivity of uranium over its main competitormore » vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that coupling ab initio calculations with process level adsorption modeling provides accurate predictions of the adsorption capacity and selectivity of the sorbent materials. Furthermore, this work demonstrates that this multiscale modeling paradigm could be utilized to aid in the selection of superior ligands or ligand compositions for the selective capture of metal ions. Furthermore, this first-principles integrated modeling approach opens the door to the in silico design of next-generation adsorbents with potentially superior efficiency and selectivity for uranium over vanadium in seawater.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ladshaw, Austin P.; Ivanov, Alexander S.; Das, Sadananda
Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material’s relatively poor selectivity of uranium over its main competitormore » vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that coupling ab initio calculations with process level adsorption modeling provides accurate predictions of the adsorption capacity and selectivity of the sorbent materials. Furthermore, this work demonstrates that this multiscale modeling paradigm could be utilized to aid in the selection of superior ligands or ligand compositions for the selective capture of metal ions. Furthermore, this first-principles integrated modeling approach opens the door to the in silico design of next-generation adsorbents with potentially superior efficiency and selectivity for uranium over vanadium in seawater.« less
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.
Ladshaw, Austin P; Ivanov, Alexander S; Das, Sadananda; Bryantsev, Vyacheslav S; Tsouris, Costas; Yiacoumi, Sotira
2018-04-18
Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material's relatively poor selectivity of uranium over its main competitor vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that coupling ab initio calculations with process level adsorption modeling provides accurate predictions of the adsorption capacity and selectivity of the sorbent materials. Furthermore, this work demonstrates that this multiscale modeling paradigm could be utilized to aid in the selection of superior ligands or ligand compositions for the selective capture of metal ions. Therefore, this first-principles integrated modeling approach opens the door to the in silico design of next-generation adsorbents with potentially superior efficiency and selectivity for uranium over vanadium in seawater.
Mondani, Laure; Benzerara, Karim; Carrière, Marie; Christen, Richard; Mamindy-Pajany, Yannick; Février, Laureline; Marmier, Nicolas; Achouak, Wafa; Nardoux, Pascal; Berthomieu, Catherine; Chapon, Virginie
2011-01-01
This study investigated the influence of uranium on the indigenous bacterial community structure in natural soils with high uranium content. Radioactive soil samples exhibiting 0.26% - 25.5% U in mass were analyzed and compared with nearby control soils containing trace uranium. EXAFS and XRD analyses of soils revealed the presence of U(VI) and uranium-phosphate mineral phases, identified as sabugalite and meta-autunite. A comparative analysis of bacterial community fingerprints using denaturing gradient gel electrophoresis (DGGE) revealed the presence of a complex population in both control and uranium-rich samples. However, bacterial communities inhabiting uraniferous soils exhibited specific fingerprints that were remarkably stable over time, in contrast to populations from nearby control samples. Representatives of Acidobacteria, Proteobacteria, and seven others phyla were detected in DGGE bands specific to uraniferous samples. In particular, sequences related to iron-reducing bacteria such as Geobacter and Geothrix were identified concomitantly with iron-oxidizing species such as Gallionella and Sideroxydans. All together, our results demonstrate that uranium exerts a permanent high pressure on soil bacterial communities and suggest the existence of a uranium redox cycle mediated by bacteria in the soil.
Exogenous contamination of uranium in human scalp hair.
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.
Mondani, Laure; Benzerara, Karim; Carrière, Marie; Christen, Richard; Mamindy-Pajany, Yannick; Février, Laureline; Marmier, Nicolas; Achouak, Wafa; Nardoux, Pascal; Berthomieu, Catherine; Chapon, Virginie
2011-01-01
This study investigated the influence of uranium on the indigenous bacterial community structure in natural soils with high uranium content. Radioactive soil samples exhibiting 0.26% - 25.5% U in mass were analyzed and compared with nearby control soils containing trace uranium. EXAFS and XRD analyses of soils revealed the presence of U(VI) and uranium-phosphate mineral phases, identified as sabugalite and meta-autunite. A comparative analysis of bacterial community fingerprints using denaturing gradient gel electrophoresis (DGGE) revealed the presence of a complex population in both control and uranium-rich samples. However, bacterial communities inhabiting uraniferous soils exhibited specific fingerprints that were remarkably stable over time, in contrast to populations from nearby control samples. Representatives of Acidobacteria, Proteobacteria, and seven others phyla were detected in DGGE bands specific to uraniferous samples. In particular, sequences related to iron-reducing bacteria such as Geobacter and Geothrix were identified concomitantly with iron-oxidizing species such as Gallionella and Sideroxydans. All together, our results demonstrate that uranium exerts a permanent high pressure on soil bacterial communities and suggest the existence of a uranium redox cycle mediated by bacteria in the soil. PMID:21998695
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wang, Taiping; Khangaonkar, Tarang; Long, Wen
2014-02-07
In recent years, with the rapid growth of global energy demand, the interest in extracting uranium from seawater for nuclear energy has been renewed. While extracting seawater uranium is not yet commercially viable, it serves as a “backstop” to the conventional uranium resources and provides an essentially unlimited supply of uranium resource. With recent advances in seawater uranium extraction technology, extracting uranium from seawater could be economically feasible when the extraction devices are deployed at a large scale (e.g., several hundred km2). There is concern however that the large scale deployment of adsorbent farms could result in potential impacts tomore » the hydrodynamic flow field in an oceanic setting. In this study, a kelp-type structure module was incorporated into a coastal ocean model to simulate the blockage effect of uranium extraction devices on the flow field. The module was quantitatively validated against laboratory flume experiments for both velocity and turbulence profiles. The model-data comparison showed an overall good agreement and validated the approach of applying the model to assess the potential hydrodynamic impact of uranium extraction devices or other underwater structures in coastal oceans.« less
The brain is a target organ after acute exposure to depleted uranium.
Lestaevel, P; Houpert, P; Bussy, C; Dhieux, B; Gourmelon, P; Paquet, F
2005-09-01
The health effects of depleted uranium (DU) are mainly caused by its chemical toxicity. Although the kidneys are the main target organs for uranium toxicity, uranium can also reach the brain. In this paper, the central effects of acute exposure to DU were studied in relation to health parameters and the sleep-wake cycle of adult rats. Animals were injected intraperitoneally with 144+/-10 microg DU kg-1 as nitrate. Three days after injection, the amounts of uranium in the kidneys represented 2.6 microg of DU g-1 of tissue, considered as a sub-nephrotoxic dosage. The central effect of uranium could be seen through a decrease in food intake as early as the first day after exposure and shorter paradoxical sleep 3 days after acute DU exposure (-18% of controls). With a lower dosage of DU (70+/-8 microg DU kg-1), no significant effect was observed on the sleep-wake cycle. The present study intends to illustrate the fact that the brain is a target organ, as are the kidneys, after acute exposure to a moderate dosage of DU. The mechanisms by which uranium causes these early neurophysiological perturbations shall be discussed.
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
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
Determining Changes in Groundwater Quality during Managed Aquifer Recharge
NASA Astrophysics Data System (ADS)
Gambhir, T.; Houlihan, M.; Fakhreddine, S.; Dadakis, J.; Fendorf, S. E.
2016-12-01
Managed aquifer recharge (MAR) is becoming an increasingly prevalent technology for improving the sustainability of freshwater supply. However, recharge water can alter the geochemical conditions of the aquifer, mobilizing contaminants native to the aquifer sediments. Geochemical alterations on deep (>300 m) injection of highly treated recycled wastewater for MAR has received limited attention. We aim to determine how residual disinfectants used in water treatment processes, specifically the strong oxidants chloramine and hydrogen peroxide, affect metal mobilization within deep injection wells of the Orange County Water District. Furthermore, as the treated recharge water has very low ionic strength (44.6 mg L-1 total dissolved solids), we tested how differing concentrations of magnesium chloride and calcium chloride affected metal mobilization within deep aquifers. Continuous flow experiments were conducted on columns dry packed with sediments from a deep injection MAR site in Orange County, CA. The effluent was analyzed for shifts in water quality, including aqueous concentrations of arsenic, uranium, and chromium. Interaction between the sediment and oxic recharge solution causes naturally-occurring arsenopyrite to repartition onto iron oxides. The stability of arsenic on the newly precipitated iron oxides is dependent on pH changes during recharge.
Zablotska, Lydia B; Lane, Rachel S D; Frost, Stanley E
2013-01-01
Objectives Uranium processing workers are exposed to uranium and radium compounds from the ore dust and to γ-ray radiation, but less to radon decay products (RDP), typical of the uranium miners. We examined the risks of these exposures in a cohort of workers from Port Hope radium and uranium refinery and processing plant. Design A retrospective cohort study with carefully documented exposures, which allowed separation of those with primary exposures to radium and uranium. Settings Port Hope, Ontario, Canada, uranium processors with no mining experience. Participants 3000 male and female workers first employed (1932–1980) and followed for mortality (1950–1999) and cancer incidence (1969–1999). Outcome measures Cohort mortality and incidence were compared with the general Canadian population. Poisson regression was used to evaluate the association between cumulative RDP exposures and γ-ray doses and causes of death and cancers potentially related to radium and uranium processing. Results Overall, workers had lower mortality and cancer incidence compared with the general Canadian population. In analyses restricted to men (n=2645), the person-year weighted mean cumulative RDP exposure was 15.9 working level months (WLM) and the mean cumulative whole-body γ-ray dose was 134.4 millisieverts. We observed small, non-statistically significant increases in radiation risks of mortality and incidence of lung cancer due to RDP exposures (excess relative risks/100 WLM=0.21, 95% CI <−0.45 to 1.59 and 0.77, 95% CI <−0.19 to 3.39, respectively), with similar risks for those exposed to radium and uranium. All other causes of death and cancer incidence were not significantly associated with RDP exposures or γ-ray doses or a combination of both. Conclusions In one of the largest cohort studies of workers exposed to radium, uranium and γ-ray doses, no significant radiation-associated risks were observed for any cancer site or cause of death. Continued follow-up and pooling with other cohorts of workers exposed to by-products of radium and uranium processing could provide valuable insight into occupational risks and suspected differences in risk with uranium miners. PMID:23449746
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.
Raymond-Whish, Stefanie; Mayer, Loretta P.; O’Neal, Tamara; Martinez, Alisyn; Sellers, Marilee A.; Christian, Patricia J.; Marion, Samuel L.; Begay, Carlyle; Propper, Catherine R.; Hoyer, Patricia B.; Dyer, Cheryl A.
2007-01-01
Background The deleterious impact of uranium on human health has been linked to its radioactive and heavy metal–chemical properties. Decades of research has defined the causal relationship between uranium mining/milling and onset of kidney and respiratory diseases 25 years later. Objective We investigated the hypothesis that uranium, similar to other heavy metals such as cadmium, acts like estrogen. Methods In several experiments, we exposed intact, ovariectomized, or pregnant mice to depleted uranium in drinking water [ranging from 0.5 μg/L (0.001 μM) to 28 mg/L (120 μM). Results Mice that drank uranium-containing water exhibited estrogenic responses including selective reduction of primary follicles, increased uterine weight, greater uterine luminal epithelial cell height, accelerated vaginal opening, and persistent presence of cornified vaginal cells. Coincident treatment with the antiestrogen ICI 182,780 blocked these responses to uranium or the synthetic estrogen diethylstilbestrol. In addition, mouse dams that drank uranium-containing water delivered grossly normal pups, but they had significantly fewer primordial follicles than pups whose dams drank control tap water. Conclusions Because of the decades of uranium mining/milling in the Colorado plateau in the Four Corners region of the American Southwest, the uranium concentration and the route of exposure used in these studies are environmentally relevant. Our data support the conclusion that uranium is an endocrine-disrupting chemical and populations exposed to environmental uranium should be followed for increased risk of fertility problems and reproductive cancers. PMID:18087588
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.
Occurrences of uranium at Clinton, Hunterdon County, New Jersey
McKeown, F.A.; Klemic, H.; Choquette, P.W.
1954-01-01
An occurrence of uranium at Clinton, Hunterdon County, N. J. was first brought to the attention of the U.S. Geological Survey when Mr. Thomas L. Eak of Avenel, N. J. submitted to the Survey a sample containing 0.068 percent uranium. Subsequent examinations of the area around Clinton indicated that detailed mapping and study were warranted. The uranium occurrences at Clinton are in or associated with fault zones in the Kittatinny limestone of Cambro-Ordovician age. The limestone generally light gray, thick bedded, and dolomitic; chert is common but not abundant. Regionally and locally, faults are the most significant structural features. The local faults at Clinton are the loci for most of the uranium. The largest fault can be traced for about 700 feet and is radioactive everywhere it crops out. Samples from this fault contain as much as 0.038 percent uranium; the average content is about 0.010 percent uranium. Uranium also occurs disseminated in two 4-inch layers of black feldspathic dolomite and in several zones of residual soil derived from the Kittatinny limestone. The black layers contain as much as 0.046 percent uranium and can be traced only about 20 feet along strike. They are cut by a small fault that is also radioactive. The radioactive soil zones are roughly elongated parallel to bedding. Soil from them contains up to 0.008 percent uranium. The uranium occurrences are best explained by a supergene origin. The sampling, mapping, and radioactivity testing of uranium occurrences at Clinton indicate they are too low grade to be of current economic interest.
Subsurface Conditions Controlling Uranium Incorporation in Iron Oxides: A Redox Stable Sink
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fendorf, Scott
2016-04-05
Toxic metals and radionuclides throughout the U.S. Department of Energy Complex pose a serious threat to ecosystems and to human health. Of particular concern is the redox-sensitive radionuclide uranium, which is classified as a priority pollutant in soils and groundwaters at most DOE sites owing to its large inventory, its health risks, and its mobility with respect to primary waste sources. The goal of this research was to contribute to the long-term mission of the Subsurface Biogeochemistry Program by determining reactions of uranium with iron (hydr)oxides that lead to long-term stabilization of this pervasive contaminant. The research objectives of thismore » project were thus to (1) identify the (bio)geochemical conditions, including those of the solid-phase, promoting uranium incorporation in Fe (hydr)oxides, (2) determine the magnitude of uranium incorporation under a variety of relevant subsurface conditions in order to quantify the importance of this pathway when in competition with reduction or adsorption; (3) identify the mechanism(s) of U(VI/V) incorporation in Fe (hydr)oxides; and (4) determine the stability of these phases under different biogeochemical (inclusive of redox) conditions. Our research demonstrates that redox transformations are capable of achieving U incorporation into goethite at ambient temperatures, and that this transformation occurs within days at U and Fe(II) concentrations that are common in subsurface geochemical environments with natural ferrihydrites—inclusive of those with natural impurities. Increasing Fe(II) or U concentration, or initial pH, made U(VI) reduction to U(IV) a more competitive sequestration pathway in this system, presumably by increasing the relative rate of U reduction. Uranium concentrations commonly found in contaminated subsurface environments are often on the order of 1-10 μM, and groundwater Fe(II) concentrations can reach exceed 1 mM in reduced zones of the subsurface. The redox-driven U(V) incorporation mechanism may help to explain U retention in some geologic materials, improving our understanding of U-based geochronology and the redox status of ancient geochemical environments. Additionally, U(VI) may be incorporated within silicate minerals though encapsulation of U-bearing iron oxides, leading to a redox stable solid. Our research detailing previously unrecognized mechanism of U incorporation within sediment minerals may even lead to new approaches for in situ contamination remediation techniques, and will help refine models of U fate and transport in reduced subsurface zones.« less
Immobilization of uranium in contaminated soil by natural apatite addition
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mrdakovic Popic, Jelena; Stojanovic, Mirjana; Milosevic, Sinisa
2007-07-01
Available in abstract form only. Full text of publication follows: The goal of this study was to evaluate the effectiveness of Serbian natural mineral apatite as soil additive for reducing the migration of uranium from contaminated sediments. In laboratory study we investigated the sorption properties of domestic apatite upon different experimental conditions, such as pH, adsorbent mass, reaction period, concentration of P{sub 2}O{sub 5} in apatite, solid/liquid ratio. In second part of study, we did the quantification of uranium in soil samples, taken from uranium mine site 'Kalna', by sequential extraction method. The same procedure was, also, used for uraniummore » determination in contaminated soil samples after apatite addition, in order to determine the changes in U distribution in soil fraction. The obtained results showed the significant level of immobilization (96.7%) upon certain conditions. Increase of %P{sub 2}O{sub 5} in apatite and process of mechano-chemical activation led to increase of immobilization capacity from 17.50% till 91.64%. The best results for uranium binding were obtained at pH 5.5 and reaction period 60 days (98.04%) The sequential extraction showed the presence of uranium (48.2%) in potentially available soil fractions, but with the apatite addition uranium content in these fractions decreased (30.64%), what is considering environmental aspect significant fact. In situ immobilization of radionuclide using inexpensive sequestering agents, such as apatite, is very adequate for big contaminated areas of soil with low level of contamination. This investigation study on natural apatite from deposit 'Lisina' Serbia was the first one of this type in our country. Key words: apatite, uranium, immobilization, soil, contamination. (authors)« less
Uranium from German Nuclear Power Projects of the 1940s--A Nuclear Forensic Investigation.
Mayer, Klaus; Wallenius, Maria; Lützenkirchen, Klaus; Horta, Joan; Nicholl, Adrian; Rasmussen, Gert; van Belle, Pieter; Varga, Zsolt; Buda, Razvan; Erdmann, Nicole; Kratz, Jens-Volker; Trautmann, Norbert; Fifield, L Keith; Tims, Stephen G; Fröhlich, Michaela B; Steier, Peter
2015-11-02
Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Brown, L. D.; Abdulaziz, R.; Jervis, R.; Bharath, V. J.; Atwood, R. C.; Reinhard, C.; Connor, L. D.; Simons, S. J. R.; Inman, D.; Brett, D. J. L.; Shearing, P. R.
2015-09-01
The electrochemical reduction of uranium dioxide to metallic uranium has been investigated in lithium chloride-potassium chloride eutectic molten salt. Laboratory based electrochemical studies have been coupled with in situ energy dispersive X-ray diffraction, for the first time, to deduce the reduction pathway. No intermediate phases were identified using the X-ray diffraction before, during or after electroreduction to form α-uranium. This suggests that the electrochemical reduction occurs via a single, 4-electron-step, process. The rate of formation of α-uranium is seen to decrease during electrolysis and could be a result of a build-up of oxygen anions in the molten salt. Slow transport of O2- ions away from the UO2 working electrode could impede the electrochemical reduction.
Hinck, Jo E.; Linder, Greg L.; Finger, Susan E.; Little, Edward E.; Tillitt, Donald E.; Kuhne, Wendy
2010-01-01
This chapter compiles available chemical and radiation toxicity information for plants and animals from the scientific literature on naturally occurring uranium and associated radionuclides. Specifically, chemical and radiation hazards associated with radionuclides in the uranium decay series including uranium, thallium, thorium, bismuth, radium, radon, protactinium, polonium, actinium, and francium were the focus of the literature compilation. In addition, exposure pathways and a food web specific to the segregation areas were developed. Major biological exposure pathways considered were ingestion, inhalation, absorption, and bioaccumulation, and biota categories included microbes, invertebrates, plants, fishes, amphibians, reptiles, birds, and mammals. These data were developed for incorporation into a risk assessment to be conducted as part of an environmental impact statement for the Bureau of Land Management, which would identify representative plants and animals and their relative sensitivities to exposure of uranium and associated radionuclides. This chapter provides pertinent information to aid in the development of such an ecological risk assessment but does not estimate or derive guidance thresholds for radionuclides associated with uranium. Previous studies have not attempted to quantify the risks to biota caused directly by the chemical or radiation releases at uranium mining sites, although some information is available for uranium mill tailings and uranium mine closure activities. Research into the biological impacts of uranium exposure is strongly biased towards human health and exposure related to enriched or depleted uranium associated with the nuclear energy industry rather than naturally occurring uranium associated with uranium mining. Nevertheless, studies have reported that uranium and other radionuclides can affect the survival, growth, and reproduction of plants and animals. Exposure to chemical and radiation hazards is influenced by a plant’s or an animal’s life history and surrounding environment. Various species of plants, invertebrates, fishes, amphibians, reptiles, birds, and mammals found in the segregation areas that are considered species of concern by State and Federal agencies were included in the development of the site-specific food web. The utilization of subterranean habitats (burrows in uranium-rich areas, burrows in waste rock piles or reclaimed mining areas, mine tunnels) in the seasonally variable but consistently hot, arid environment is of particular concern in the segregation areas. Certain species of reptiles, amphibians, birds, and mammals in the segregation areas spend significant amounts of time in burrows where they can inhale or ingest uranium and other radionuclides through digging, eating, preening, and hibernating. Herbivores may also be exposed though the ingestion of radionuclides that have been aerially deposited on vegetation. Measured tissues concentrations of uranium and other radionuclides are not available for any species of concern in the segregation areas. The sensitivity of these animals to uranium exposure is unknown based on the existing scientific literature, and species-specific uranium presumptive effects levels were only available for two endangered fish species known to inhabit the segregation areas. Overall, the chemical toxicity data available for biological receptors of concern were limited, although chemical and radiation toxicity guidance values are available from several sources. However, caution should be used when directly applying these values to northern Arizona given the unique habitat and life history strategies of biological receptors in the segregation areas and the fact that some guidance values are based on models rather than empirical (laboratory or field) data. No chemical toxicity information based on empirical data is available for reptiles, birds, or wild mammals; therefore, the risks associated with uranium and other radionuclides are unknown for these biota.
Cola soft drinks for evaluating the bioaccessibility of uranium in contaminated mine soils.
Lottermoser, Bernd G; Schnug, Ewald; Haneklaus, Silvia
2011-08-15
There is a rising need for scientifically sound and quantitative as well as simple, rapid, cheap and readily available soil testing procedures. The purpose of this study was to explore selected soft drinks (Coca-Cola Classic®, Diet Coke®, Coke Zero®) as indicators of bioaccessible uranium and other trace elements (As, Ce, Cu, La, Mn, Ni, Pb, Th, Y, Zn) in contaminated soils of the Mary Kathleen uranium mine site, Australia. Data of single extraction tests using Coca-Cola Classic®, Diet Coke® and Coke Zero® demonstrate that extractable arsenic, copper, lanthanum, manganese, nickel, yttrium and zinc concentrations correlate significantly with DTPA- and CaCl₂-extractable metals. Moreover, the correlation between DTPA-extractable uranium and that extracted using Coca-Cola Classic® is close to unity (+0.98), with reduced correlations for Diet Coke® (+0.66) and Coke Zero® (+0.55). Also, Coca-Cola Classic® extracts uranium concentrations near identical to DTPA, whereas distinctly higher uranium fractions were extracted using Diet Coke® and Coke Zero®. Results of this study demonstrate that the use of Coca-Cola Classic® in single extraction tests provided an excellent indication of bioaccessible uranium in the analysed soils and of uranium uptake into leaves and stems of the Sodom apple (Calotropis procera). Moreover, the unconventional reagent is superior in terms of availability, costs, preparation and disposal compared to traditional chemicals. Contaminated site assessments and rehabilitation of uranium mine sites require a solid understanding of the chemical speciation of environmentally significant elements for estimating their translocation in soils and plant uptake. Therefore, Cola soft drinks have potential applications in single extraction tests of uranium contaminated soils and may be used for environmental impact assessments of uranium mine sites, nuclear fuel processing plants and waste storage and disposal facilities. Copyright © 2011 Elsevier B.V. All rights reserved.
Uranium content and leachable fraction of fluorspars
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.
Effect of pH and Pressure on Uranium Removal from Drinking Water Using NF/RO Membranes.
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.
NASA Astrophysics Data System (ADS)
Israelsson, A.; Eriksson, M.; Pettersson, H. B. L.
2015-06-01
In the present study the distribution of uranium in single human hair shafts has been evaluated using two synchrotron radiation (SR) based micro X-ray fluorescence techniques; SR μ-XRF and confocal SR μ-XRF. The hair shafts originated from persons that have been exposed to elevated uranium concentrations. Two different groups have been studied, i) workers at a nuclear fuel fabrication factory, exposed mainly by inhalation and ii) owners of drilled bedrock wells exposed by ingestion of water. The measurements were carried out on the FLUO beamline at the synchrotron radiation facility ANKA, Karlsruhe. The experiment was optimized to detect U with a beam size of 6.8 μm × 3 μm beam focus allowing detection down to ppb levels of U in 10 s (SR μ-XRF setup) and 70 s (SR confocal μ-XRF setup) measurements. It was found that the uranium was present in a 10-15 μm peripheral layer of the hair shafts for both groups studied. Furthermore, potential external hair contamination was studied by scanning of unwashed hair shafts from the workers. Sites of very high uranium signal were identified as particles containing uranium. Such particles, were also seen in complementary analyses using variable pressure electron microscope coupled with energy dispersive X-ray analyzer (ESEM-EDX). However, the particles were not visible in washed hair shafts. These findings can further increase the understanding of uranium excretion in hair and its potential use as a biomonitor.
Kukreti, B M; Kumar, Pramod; Sharma, G K
2015-10-01
Exploratory drilling was undertaken in the Lostoin block, West Khasi Hills district of Meghalaya based on the geological extension to the major uranium deposit in the basin. Gamma ray logging of drilled boreholes shows considerable subsurface mineralization in the block. However, environmental and exploration related challenges such as climatic, logistic, limited core drilling and poor core recovery etc. in the block severely restricted the study of uranium exploration related index parameters for the block with a high degree confidence. The present study examines these exploration related challenges and develops an integrated approach using representative sampling of reconnoitory boreholes in the block. Experimental findings validate a similar geochemically coherent nature of radio elements (K, Ra and Th) in the Lostoin block uranium hosting environment with respect to the known block of Mahadek basin and uranium enrichment is confirmed by the lower U to Th correlation index (0.268) of hosting environment. A mineralized zone investigation in the block shows parent (refers to the actual parent uranium concentration at a location and not a secondary concentration such as the daughter elements which produce the signal from a total gamma ray measurement) favoring uranium mineralization. The confidence parameters generated under the present study have implications for the assessment of the inferred category of uranium ore in the block and setting up a road map for the systematic exploration of large uranium potential occurring over extended areas in the basin amid prevailing environmental and exploratory impediments. Copyright © 2015 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.
Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, particle size, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population andmore » composition, which mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfatereducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. The results of this study suggest that reductive immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.
Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less
Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.; ...
2016-12-29
Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less
NASA Astrophysics Data System (ADS)
Grijalva-Rodríguez, T.; Valencia-Moreno, M.; Calmus, T.; Del Rio-Salas, R.; Balcázar-García, M.
2017-12-01
This work reviews the characteristics of the El Horror uranium prospect in northeastern Sonora, Mexico. It was formerly detected by a radiometric anomaly after airborne gamma ray exploration carried out in the 70's by the Mexican government. As a promising site to contain important uranium resources, the El Horror was re-evaluated by CFE (Federal Electricity Commission) by in situ gamma ray surveys. The study also incorporates rock and stream sediment ICP-MS geochemistry, X-ray diffraction, X-ray fluorescence, Raman spectrometry and Scanning Electron Microscopy (SEM) to provide a better understanding of the radiometric anomaly. The results show that, instead of a single anomaly, it comprises at least five individual anomalies hosted in hydrothermally altered Laramide (80-40 Ma) andesitic volcanic rocks of the Tarahumara Formation. Concentrations for elemental uranium and uranium calculated from gamma ray surveys (i.e., equivalent uranium) are not spatially coincident within the anomaly, but, at least at some degree, they do so in specific sites. X-ray diffraction and Raman spectrometry revealed the presence of rutile/anatase, uvite, bukouvskyte and allanite as the more likely mineral phases to contain uranium. SEM studies revealed a process of iron-rich concretion formation, suggesting that uranium was initially incorporated to the system by adsorption, but was largely removed later during incorporation of Fe+3 ions. Stream sediment geochemistry reveals that the highest uranium concentrations are derived from the southern part of the Sierra La Madera batholith (∼63 Ma), and decrease toward the El Horror anomaly.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dam, William; Campbell, Sam; Johnson, Ray
Milling activities at a former uranium mill site near Riverton, Wyoming, USA, contaminated the shallow groundwater beneath and downgradient of the site. Although the mill operated for <6 years (1958-1963), its impact remains an environmental liability. Groundwater modeling predicted that contaminant concentrations were declining steadily, which confirmed the conceptual site model (CSM). However, local flooding in 2010 mobilized contaminants that migrated downgradient from the Riverton site and resulted in a dramatic increase in groundwater contaminant concentrations. This observation indicated that the original CSM was inadequate to explain site conditions and needed to be refined. In response to the new observationsmore » after the flood, a collaborative investigation to better understand site conditions and processes commenced. This investigation included installing 103 boreholes to collect soil and groundwater samples, sampling and analysis of evaporite minerals along the bank of the Little Wind River, an analysis of evaportranspiration in the shallow aquifer, and sampling naturally organic-rich sediments near groundwater discharge areas. The enhanced characterization revealed that the existing CSM did not account for high uranium concentrations in groundwater remaining on the former mill site and groundwater plume stagnation near the Little Wind River. Observations from the flood and subsequent investigations indicate that additional characterization is still needed to continue refining the CSM and determine the viability of the natural flushing compliance strategy. Additional sampling, analysis, and testing of soil and groundwater are necessary to investigate secondary contaminant sources, mobilization of contaminants during floods, geochemical processes, contaminant plume stagnation, distribution of evaporite minerals and organic-rich sediments, and mechanisms and rates of contaminant transfer from soil to groundwater. Future data collection will be used to continually revise the CSM and evaluate the compliance strategy at the site.« less
NASA Astrophysics Data System (ADS)
Naftz, D. L.; Walton-Day, K. E.; Fuller, C.; Dam, W. L.; Briggs, M. A.; Snyder, T.
2015-12-01
Legacy uranium (U) mining and processing activities have resulted in soil and water contamination on Federal, state, and tribal lands in the western United States. Sites include legacy mill sites associated with U extraction now managed by the Department of Energy and thousands of waste dumps associated with U exploration, mining, and processing. Recently (2012), over 400,000 hectares of federally managed land in northern Arizona was withdrawn from consideration of mining for a 20-year period to protect the Grand Canyon watershed from potentially adverse effects of U mineral exploration and development. Ore from active and recently active U mines in the Colorado Plateau, the Henry Mountains Complex, and the Arizona Strip is transported to the only currently (2015) active conventional mill site in the western United States, located in Utah. Previous and ongoing U.S. Geological Survey assessments to examine U mobility at a variety of legacy and active sites associated with ore exploration, extraction, and processing will be presented as field-scale examples. Topics associated with site investigations will include: (1) offsite migration of radionuclides associated with the operation of the White Mesa U mill; (2) long-term contaminant transport from legacy U waste dumps on Bureau of Land Management regulated land in Utah; (3) application of incremental soil sampling techniques to determine pre- and post-mining radionuclide levels associated with planned and operating U mines in northern Arizona; (4) application of fiber optic digital temperature sensing equipment to identify areas where shallow groundwater containing elevated U levels may be discharging to a river adjacent to a reclaimed mill site in central Wyoming; and (5) field-scale manipulation of groundwater chemistry to limit U migration from a legacy upgrader site in southeastern Utah.
Ramie (Boehmeria nivea)'s uranium bioconcentration and tolerance attributes.
Wang, Wei-Hong; Luo, Xue-Gang; Liu, Lai; Zhang, Yan; Zhao, Hao-Zhou
2018-04-01
The authors sampled and analyzed 15 species of dominant wild plants in Huanan uranium tailings pond in China, whose tailings' uranium contents were 3.21-120.52 μg/g. Among the 15 species of wild plants, ramie (Boehmeria nivea) had the strongest uranium bioconcentration and transfer capacities. In order to study the uranium bioconcentration and tolerance attributes of ramie in detail, and provide a reference for the screening remediation plants to phytoremedy on a large scale in uranium tailings pond, a ramie cultivar Xiangzhu No. 7 pot experiment was carried out. We found that both wild ramie and Xiangzhu No. 7 could bioconcentrate uranium, but there were two differences. One was wild ramie's shoots bioconcentrated uranium up to 20 μg/g (which can be regarded as the critical content value of the shoot of uranium hyperaccumulator) even the soil uranium content was as low as 5.874 μg/g while Xiangzhu No. 7's shoots could reach 20 μg/g only when the uranium treatment concentrations were 275 μg/g or more; the other was that all the transfer factors of 3 wild samples were >1, and the transfer factors of 27 out of 28 pot experiment samples were <1. Probably wild ramie was a uranium hyperaccumulator. Xiangzhu No. 7 satisfied the needs of uranium hyperaccumulator on accumulation capability, tolerance capability, bioconcentration factor, but not transfer capability, so Xiangzhu No. 7 was not a uranium hyperaccumulator. We analyzed the possible reasons why there were differences in the uranium bioconcentration and transfer attributes between wild ramie and Xiangzhu No. 7., and proposed the direction for further research. In our opinion, both the plants which bioconcentrate contaminants in the shoots and roots can act as phytoextractors. Although Xiangzhu No. 7's biomass and accumulation of uranium were concentrated on the roots, the roots were small in volume and easy to harvest. And Xiangzhu No. 7's cultivating skills and protection measures had been developed very well. Xiangzhu No. 7's whole bioconcentration factors and the roots' bioconcentration factors, which were 1.200-1.834 and 1.460-2.341, respectively, increased with the increases of uranium contents of pot soil when the soil's uranium contents are 25-175 μg/g, so it can act as a potential phytoextractor when Huanan uranium tailings pond is phytoremediated. Copyright © 2018. Published by Elsevier Ltd.
Lead and uranium group abundances in cosmic rays
NASA Technical Reports Server (NTRS)
Yadav, J. S.; Perelygin, V. P.
1985-01-01
The importance of Lead and Uranium group abundances in cosmic rays is discussed in understanding their evolution and propagation. The electronic detectors can provide good charge resolution but poor data statistics. The plastic detectors can provide somewhat better statistics but charge resolution deteriorates. The extraterrestrial crystals can provide good statistics but with poor charge resolution. Recent studies of extraterrestrial crystals regarding their calibration to accelerated uranium ion beam and track etch kinetics are discussed. It is hoped that a charge resolution of two charge units can be achieved provided an additional parameter is taken into account. The prospects to study abundances of Lead group, Uranium group and superheavy element in extraterrestrial crystals are discussed, and usefulness of these studies in the light of studies with electronic and plastic detectors is assessed.
Bao, Yi-zhong; Wang, Dan; Hu, Yu-xing; Xu, Ai-hong; Sun, Mei-zhen; Chen, Hong-hong
2011-11-01
This study is to assess the efficacy of BPCBG on the decorporation of uranium (VI) and protecting human renal proximal tubular epithelial cells (HK-2) against uranium-induced damage. BPCBG at different doses was injected intramuscularly to male SD rats immediately after a single intraperitoneal injection of UO2(CH3COO)2. Twenty-four hours later uranium contents in urine, kidneys and femurs were measured by ICP-MS. After HK-2 cells were exposed to UO2(CH3COO)2 immediately or for 24 h followed by BPCBG treatment at different doses for another 24 or 48 h, the uranium contents in HK-2 cells were measured by ICP-MS, the cell survival was assayed by cell counting kit-8 assay, formation of micronuclei was determined by the cytokinesis-block (CB) micronucleus assay and the production of intracellular reactive oxygen species (ROS) was detected by 2',7'-dichlorofluorescin diacetate (DCFH-DA) oxidation. DTPA-CaNa3 was used as control. It was found that BPCBG at dosages of 60, 120, and 600 micromol kg(-1) resulted in 37%-61% increase in 24 h-urinary uranium excretion, and significantly decreased the amount of uranium retention in kidney and bone to 41%-31% and 86%-42% of uranium-treated group, respectively. After HK-2 cells that had been pre-treated with UO2(CH3COO)2 for 24 h were treated with the chelators for another 24 h, 55%-60% of the intracellular uranium was removed by 10-250 micromol L(-1) of BPCBG. Treatment of uranium-treated HK-2 cells with BPCBG significantly enhanced the cell survival, decreased the formation of micronuclei and inhibited the production of intracellular ROS. Although DTPA-CaNa3 markedly reduced the uranium retention in kidney of rats and HK-2 cells, its efficacy of uranium removal from body was significantly lower than that of BPCBG and it could not protect uranium-induced cell damage. It can be concluded that BPCBG effectively decorporated the uranium from UO2(CH3COO)2-treated rats and HK-2 cells, which was better than DTPA-CaNa3. It could also scavenge the uranium-induced intracellular ROS and protect against the uranium-induced cell damage. BPCBG is worth further investigation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Saccomanno, G.
''Early Lung Cancer Detection in Uranium Miners with Abnormal Sputum Cytology'' was funded by the Department of Energy to monitor the health effects of radon exposure and/or cigarette smoke on uranium workers from the Colorado Plateau. The resulting Saccomanno Uranium Workers Archive and data base has been used as a source of information to prove eligibility for compensation under the Radiation Exposure Compensation Act and as the source of primary data tissue for a subcontract and other collaborations with outside investigators. The latter includes a study of radon exposure and lung cancer risk in a non-smoking cohort of uranium minersmore » (subcontract); a study of genetic markers for lung cancer susceptibility; and a study of {sup 210}Pb accumulation in the skull as a biomarker of radon exposure.« less
Health Effects and Environmental Justice Concerns of Exposure to Uranium in Drinking Water.
Corlin, Laura; Rock, Tommy; Cordova, Jamie; Woodin, Mark; Durant, John L; Gute, David M; Ingram, Jani; Brugge, Doug
2016-12-01
We discuss the recent epidemiologic literature regarding health effects of uranium exposure in drinking water focusing on the chemical characteristics of uranium. While there is strong toxicologic evidence for renal and reproductive effects as well as DNA damage, the epidemiologic evidence for these effects in people exposed to uranium in drinking water is limited. Further, epidemiologic evidence is lacking for cardiovascular and oncogenic effects. One challenge in characterizing health effects of uranium in drinking water is the paucity of long-term cohort studies with individual level exposure assessment. Nevertheless, there are environmental justice concerns due to the substantial exposures for certain populations. For example, we present original data suggesting that individuals living in the Navajo Nation are exposed to high levels of uranium in unregulated well water used for drinking. In 10 out of 185 samples (5.4 %), concentrations of uranium exceeded standards under the Safe Drinking Water Act. Therefore, efforts to mitigate exposure to toxic elements in drinking water are warranted and should be prioritized.
Rodríguez, P Blanco; Tomé, F Vera; Fernández, M Pérez; Lozano, J C
2006-05-15
The linearity assumption of the validation of soil-to-plant transfer factors of natural uranium and (226)Ra was tested using Helianthus annuus L. (sunflower) grown in a hydroponic medium. Transfer of natural uranium and (226)Ra was tested in both the aerial fraction of plants and in the overall seedlings (roots and shoots). The results show that the linearity assumption can be considered valid in the hydroponic growth of sunflowers for the radionuclides studied. The ability of sunflowers to translocate uranium and (226)Ra was also investigated, as well as the feasibility of using sunflower plants to remove uranium and radium from contaminated water, and by extension, their potential for phytoextraction. In this sense, the removal percentages obtained for natural uranium and (226)Ra were 24% and 42%, respectively. Practically all the uranium is accumulated in the roots. However, 86% of the (226)Ra activity concentration in roots was translocated to the aerial part.
Isolation and characterization of a uranium(VI)-nitride triple bond
NASA Astrophysics Data System (ADS)
King, David M.; Tuna, Floriana; McInnes, Eric J. L.; McMaster, Jonathan; Lewis, William; Blake, Alexander J.; Liddle, Stephen T.
2013-06-01
The nature and extent of covalency in uranium bonding is still unclear compared with that of transition metals, and there is great interest in studying uranium-ligand multiple bonds. Although U=O and U=NR double bonds (where R is an alkyl group) are well-known analogues to transition-metal oxo and imido complexes, the uranium(VI)-nitride triple bond has long remained a synthetic target in actinide chemistry. Here, we report the preparation of a uranium(VI)-nitride triple bond. We highlight the importance of (1) ancillary ligand design, (2) employing mild redox reactions instead of harsh photochemical methods that decompose transiently formed uranium(VI) nitrides, (3) an electrostatically stabilizing sodium ion during nitride installation, (4) selecting the right sodium sequestering reagent, (5) inner versus outer sphere oxidation and (6) stability with respect to the uranium oxidation state. Computational analyses suggest covalent contributions to U≡N triple bonds that are surprisingly comparable to those of their group 6 transition-metal nitride counterparts.
Uranium mining and lung cancer among Navajo men in New Mexico and Arizona, 1969 to 1993.
Gilliland, F D; Hunt, W C; Pardilla, M; Key, C R
2000-03-01
Navajo men who were underground miners have excess risk of lung cancer. To further characterize the long-term consequences of uranium mining in this high-risk population, we examined lung cancer incidence among Navajo men residing in New Mexico and Arizona from 1969 to 1993 and conducted a population-based case-control study to estimate the risk of lung cancer for Navajo uranium miners. Uranium mining contributed substantially to lung cancer among Navajo men over the 25-year period following the end of mining for the Navajo Nation. Sixty-three (67%) of the 94-incident lung cancers among Navajo men occurred in former uranium miners. The relative risk for a history of mining was 28.6 (95% confidence interval, 13.2-61.7). Smoking did not account for the strong relationship between lung cancer and uranium mining. The Navajo experience with uranium mining is a unique example of exposure in a single occupation accounting for the majority of lung cancers in an entire population.
Yiin, James H; Anderson, Jeri L; Bertke, Stephen J; Tollerud, David J
2018-05-09
To examine dose-response relationships between internal uranium exposures and select outcomes among a cohort of uranium enrichment workers. Cox regression was conducted to examine associations between selected health outcomes and cumulative internal uranium with consideration for external ionizing radiation, work-related medical X-rays and contaminant radionuclides technetium ( 99 Tc) and plutonium ( 239 Pu) as potential confounders. Elevated and monotonically increasing mortality risks were observed for kidney cancer, chronic renal diseases, and multiple myeloma, and the association with internal uranium absorbed organ dose was statistically significant for multiple myeloma. Adjustment for potential confounders had minimal impact on the risk estimates. Kidney cancer, chronic renal disease, and multiple myeloma mortality risks were elevated with increasing internal uranium absorbed organ dose. The findings add to evidence of an association between internal exposure to uranium and cancer. Future investigation includes a study of cancer incidence in this cohort. © 2018 Wiley Periodicals, Inc.
Zhivin, Sergey; Guseva Canu, Irina; Samson, Eric; Laurent, Olivier; Grellier, James; Collomb, Philippe; Zablotska, Lydia B; Laurier, Dominique
2016-03-01
Until recently, enrichment of uranium for civil and military purposes in France was carried out by gaseous diffusion using rapidly soluble uranium compounds. We analysed the relationship between exposure to soluble uranium compounds and exposure to external γ-radiation and mortality in a cohort of 4688 French uranium enrichment workers who were employed between 1964 and 2006. Data on individual annual exposure to radiological and non-radiological hazards were collected for workers of the AREVA NC, CEA and Eurodif uranium enrichment plants from job-exposure matrixes and external dosimetry records, differentiating between natural, enriched and depleted uranium. Cause-specific mortality was compared with the French general population via standardised mortality ratios (SMR), and was analysed via Poisson regression using log-linear and linear excess relative risk models. Over the period of follow-up, 131 161 person-years at risk were accrued and 21% of the subjects had died. A strong healthy worker effect was observed: all causes SMR=0.69, 95% CI 0.65 to 0.74. SMR for pleural cancer was significantly increased (2.3, 95% CI 1.06 to 4.4), but was only based on nine cases. Internal uranium and external γ-radiation exposures were not significantly associated with any cause of mortality. This is the first study of French uranium enrichment workers. Although limited in statistical power, further follow-up of this cohort, estimation of internal uranium doses and pooling with similar cohorts should elucidate potential risks associated with exposure to soluble uranium compounds. Published by the BMJ Publishing Group Limited. For permission to use (where not already granted under a licence) please go to http://www.bmj.com/company/products-services/rights-and-licensing/
Development of practical decontamination process for the removal of uranium from gravel.
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.
Uranium and its decay products in samples contaminated with uranium mine and mill waste
NASA Astrophysics Data System (ADS)
Benedik, L.; Klemencic, H.; Repinc, U.; Vrecek, P.
2003-05-01
The routine determination of the activity concentrations of uranium isotopes (^{238}U, ^{235}U and ^{234}U), thorium isotopes (^{212}Th, ^{230}TI, and ^{228}Th), ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in the environment is one of the most important tasks in uranium mining areas. Natural radionuclides contribute negligibly to the extemal radiation dose, but in the case of ingestion or inhalation can represent a very serious hazard. The objective of this study was to determine the activities of uranium and its decay products ^{230}Th, ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in sediments and water below sources of contamination (uranium mine, disposal sites and individual inflows) using gamma and alpha spectrometry, beta counting, the liquid scintillation technique and radiochemical neutron activation analysis.
Uranium levels in the diet of São Paulo City residents.
Garcia, F; Barioni, A; Arruda-Neto, J D T; Deppman, A; Milian, F; Mesa, J; Rodriguez, O
2006-07-01
Natural levels of uranium in the diet of São Paulo City residents were studied, and radionuclide concentrations were measured by the fission track method on samples of typical adult food items. This information was used to evaluate the daily intake of uranium in individuals living in São Paulo City which is, according to our findings, around 0.97 microg U/day. Using the ICRP Uranium-model, we estimated the uranium accumulation and committed doses in some tissues and organs, as function of time. We compared the output of the ICRP uranium biokinetic model, tailored for the conditions prevailing in São Paulo, with experimental data from other localities. Such comparison was possible by means of a simple method we developed, which allows normalization among experimental results from different regions where distinct values of chronic daily intake are observed.
Beroni, E.P.; McKeown, F.A.
1952-01-01
Previous discoveries and studies of radioactive lignites of Tertiary age in North Dakota, South Dakota, Montana, and Wyoming led the Geological Survey in 1950 to do reconnaissance in the Green River and Uinta Basin of Wyoming and Utah, where similar lignites were believed to be present. Because of the common association of uranium with copper deposits and the presence of such deposits in the Uinta Basin, several areas containing copper-uranium minerals were also examined. No deposits commercially exploitable under present conditions were found. Samples of coal from the Bear River formation at Sage, Wyo., assayed 0.004 to 0.013 percent uranium in the ash; in the old Uteland copper mine in Uinta County, Utah, 0.007 to 0.017 percent uranium; in a freshwater limestone, Duchesne County, Utah, as much as 0.019 percent uranium; and in the Mesaverde formation at the Snow and Bonniebell claims near Jensen, Uintah County, Utah, 0.003 to 0.090 percent uranium. Maps were made and samples were taken at the Skull Creek carnotite deposits in Moffat County, Colo. (0.006 to 0.16 percent uranium); at the Fair-U claims in Routt County, Colo. (0.002 to 0.040 percent uranium); and at the Lucky Strike claims near Kremmling in Grand County, Colo. (0.006 to 0.018 percent uranium).
Study on kinetics of adsorption of humic acid modified by ferric chloride on U(VI)
NASA Astrophysics Data System (ADS)
Zhang, Y. Y.; Lv, J. W.; Song, Y.; Dong, X. J.; Fang, Q.
2017-11-01
In order to reveal the adsorption mechanism of the ferric chloride modified humic acid on uranium, the influence of pH value and contact time of adsorption on uranium was studied through a series of batch experiments. Meanwhile, the adsorption kinetics was analyzed with pseudo-first order kinetic model and pseudo-second order kinetic model. The results show that adsorption is affected by the pH value of the solution and by contract time, and the best condition for adsorption on uranium is at pH=5 and the adsorption equilibrium time is about 80 min. Kinetics of HA-Fe adsorption on uranium accords with pseudo-second order kinetic model. The adsorption is mainly chemical adsorption, and complexes were produced by the reaction between uranium ions and the functional groups on the surface of HA-Fe, which can provide reference for further study of humic acid effecting on the migration of U(VI) in soil.
NASA Astrophysics Data System (ADS)
Markwitz, Vanessa; Porwal, Alok; Campbell McCuaig, T.; Kreuzer, Oliver P.
2010-05-01
Uranium deposits are usually classified based on the characteristics of their host rocks and geological environments (Dahlkamp, 1993; OECD/NEA Red Book and IAEA, 2000; Cuney, 2009). The traditional unconformity-related deposit types are the most economical deposits in the world, with the highest grades amongst all uranium deposit types. In order to predict undiscovered uranium deposits, there is a need to understand the spatial association of uranium mineralization with structures and unconformities. Hydrothermal uranium deposits develop by uranium enriched fluids from source rocks, transported along permeable pathways to their depositional environment. Unconformities are not only separating competent from incompetent sequences, but provide the physico-chemical gradient in the depositional environment. They acted as important fluid flow pathways for uranium to migrate not only for surface-derived oxygenated fluids, but also for high oxidized metamorphic and magmatic fluids, dominated by their geological environment in which the unconformities occur. We have carried out comprehensive empirical spatial analyses of various types of uranium deposits in Australia, and first results indicate that there is a strong spatial correlation between unconformities and uranium deposits, not only for traditional unconformity-related deposits but also for other styles. As a start we analysed uranium deposits in Queensland and in particular Proterozoic metasomatic-related deposits in the Mount Isa Inlier and Late Carboniferous to Early Permian volcanic-hosted uranium occurrences in Georgetown and Charters Towers Regions show strong spatial associations with contemporary and older unconformities. The Georgetown Inlier in northern Queensland consists of a diverse range of rocks, including Proterozoic and early Palaeozoic metamorphic rocks and granites and late Palaeozoic volcanic rocks and related granites. Uranium-molybdenum (+/- fluorine) mineralization in the Georgetown inlier varies from strata- to structure-bound and occurs above regional unconformities. The Proterozoic basins in the Mount Isa Inlier rest unconformably on Palaeoproterozoic basement accompanied by volcanic and igneous rocks, which were deformed and metamorphosed in the Mesoproterozoic. Uranium occurrences in the Western Succession of Mount Isa are either hosted in clastic metasediments or mafic volcanics that belong to the Palaeoproterozoic Eastern Creek Volcanics. Uranium and vanadium mineralization occur in metasomatised and hematite-magnetite-carbonate alteration zones, bounded by major faults and regional unconformities. The results of this study highlight the importance of unconformities in uranium minerals systems as possible fluid pathways and/or surfaces of physico-chemical contrast that could have facilitated the precipitation of uranium, not only in classical unconformity style uranium deposits but in several other styles of uranium mineralization as well. References Cuney, M., 2009. The extreme diversity of uranium deposits. Mineralium Deposita, 44, 3-9. Dahlkamp, F. J., 1993. Uranium ore deposits. Springer, Berlin, p 460. OECD / NEA Red Book & IAEA, 2000. Uranium 1999: Resources, Production and Demand. OECD Nuclear Energy Agency and International Atomic Energy Agency, Paris.
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
28 CFR 79.53 - Proof of employment as a miller.
Code of Federal Regulations, 2010 CFR
2010-07-01
... EXPOSURE COMPENSATION ACT Eligibility Criteria for Claims by Uranium Millers § 79.53 Proof of employment as... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942-1990; (2) Records of a uranium worker census performed by the PHS at various times during the period...
Measurement of the Auger parameter and Wagner plot for uranium compounds
DOE Office of Scientific and Technical Information (OSTI.GOV)
Holliday, Kiel S.; Siekhaus, Wigbert; Nelson, Art J.
2013-05-15
In this study, the photoemission from the U 4f{sub 7/2} and 4d{sub 5/2} states and the U N{sub 6}O{sub 45}O{sub 45} and N{sub 67}O{sub 45}V x-ray excited Auger transitions were measured for a range of uranium compounds. The data are presented in Wagner plots and the Auger parameter is calculated to determine the utility of this technique in the analysis of uranium materials. It was demonstrated that the equal core-level shift assumption holds for uranium. It was therefore possible to quantify the relative relaxation energies, and uranium was found to have localized core-hole shielding. The position of compounds within themore » Wagner plot made it possible to infer information on bonding character and local electron density. The relative ionicity of the uranium compounds studied follows the trend UF{sub 4} > UO{sub 3} > U{sub 3}O{sub 8} > U{sub 4}O{sub 9}/U{sub 3}O{sub 7} Almost-Equal-To UO{sub 2} > URu{sub 2}Si{sub 2}.« less
31 CFR 540.317 - Uranium feed; natural uranium feed.
Code of Federal Regulations, 2011 CFR
2011-07-01
... 31 Money and Finance:Treasury 3 2011-07-01 2011-07-01 false Uranium feed; natural uranium feed...) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The term uranium feed or natural uranium feed means natural uranium in the form of UF6 suitable for uranium...
31 CFR 540.317 - Uranium feed; natural uranium feed.
Code of Federal Regulations, 2010 CFR
2010-07-01
... 31 Money and Finance: Treasury 3 2010-07-01 2010-07-01 false Uranium feed; natural uranium feed...) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The term uranium feed or natural uranium feed means natural uranium in the form of UF6 suitable for uranium...
Process for continuous production of metallic uranium and uranium alloys
Hayden, H.W. Jr.; Horton, J.A.; Elliott, G.R.B.
1995-06-06
A method is described for forming metallic uranium, or a uranium alloy, from uranium oxide in a manner which substantially eliminates the formation of uranium-containing wastes. A source of uranium dioxide is first provided, for example, by reducing uranium trioxide (UO{sub 3}), or any other substantially stable uranium oxide, to form the uranium dioxide (UO{sub 2}). This uranium dioxide is then chlorinated to form uranium tetrachloride (UCl{sub 4}), and the uranium tetrachloride is then reduced to metallic uranium by reacting the uranium chloride with a metal which will form the chloride of the metal. This last step may be carried out in the presence of another metal capable of forming one or more alloys with metallic uranium to thereby lower the melting point of the reduced uranium product. The metal chloride formed during the uranium tetrachloride reduction step may then be reduced in an electrolysis cell to recover and recycle the metal back to the uranium tetrachloride reduction operation and the chlorine gas back to the uranium dioxide chlorination operation. 4 figs.
Process for continuous production of metallic uranium and uranium alloys
Hayden, Jr., Howard W.; Horton, James A.; Elliott, Guy R. B.
1995-01-01
A method is described for forming metallic uranium, or a uranium alloy, from uranium oxide in a manner which substantially eliminates the formation of uranium-containing wastes. A source of uranium dioxide is first provided, for example, by reducing uranium trioxide (UO.sub.3), or any other substantially stable uranium oxide, to form the uranium dioxide (UO.sub.2). This uranium dioxide is then chlorinated to form uranium tetrachloride (UCl.sub.4), and the uranium tetrachloride is then reduced to metallic uranium by reacting the uranium chloride with a metal which will form the chloride of the metal. This last step may be carried out in the presence of another metal capable of forming one or more alloys with metallic uranium to thereby lower the melting point of the reduced uranium product. The metal chloride formed during the uranium tetrachloride reduction step may then be reduced in an electrolysis cell to recover and recycle the metal back to the uranium tetrachloride reduction operation and the chlorine gas back to the uranium dioxide chlorination operation.
NASA Astrophysics Data System (ADS)
Truche, Laurent; Joubert, Gilles; Dargent, Maxime; Martz, Pierre; Cathelineau, Michel; Rigaudier, Thomas; Quirt, David
2018-07-01
Hydrogen (H2)-rich fluids are observed in a wide variety of geologic settings including gas seeps in serpentinized ultramafic rocks, sub-seafloor hydrothermal vents, fracture networks in crystalline rocks from continental and oceanic crust, and volcanic gases. Natural hydrogen sources can sustain deep microbial ecosystems, induce abiotic hydrocarbons synthesis and trigger the formation of prebiotic organic compounds. However, due to its extreme mobility and small size, hydrogen is not easily trapped in the crust. If not rapidly consumed by redox reactions mediated by bacteria or suitable mineral catalysts it diffuses through the rocks and migrates toward the surface. Therefore, H2 is not supposed to accumulate in the crust. We challenge this view by demonstrating that significant amount of H2 may be adsorbed by clay minerals and remain trapped beneath the surface. Here, we report for the first time H2 content in clay-rich rocks, mainly composed of illite, chlorite, and kaolinite from the Cigar Lake uranium ore deposit (northern Saskatchewan, Canada). Thermal desorption measurements reveal that H2 is enriched up to 500 ppm (i.e. 0.25 mol kg-1 of rock) in these water-saturated rocks having a very low total organic content (<0.5 wt%). Such hydrogen uptake is comparable and even exceeds adsorbed methane capacities reported elsewhere for pure clay minerals or shales. Sudoite (Al-Mg di-trioctahedral chlorite) is probably the main mineral responsible for H2 adsorption in the present case. The presence of multiple binding sites in interlinked nanopores between crystal layers of illite-chlorite particles offers the ideal conditions for hydrogen sorption. We demonstrate that 4 to 17% of H2 produced by water radiolysis over the 1.4-Ga-lifetime of the Cigar Lake uranium ore deposit has been trapped in the surrounding clay alteration haloes. As a result, sorption processes on layered silicates must not be overlooked as they may exert an important control on the fate and mobility of H2 in the crust. Furthermore, the high capacity of clay minerals to sorb molecular hydrogen may also open up new opportunities for exploration of unexpected energy resources and for H2 storage based on geo-inspired materials.
Uranium Biominerals Precipitated by an Environmental Isolate of Serratia under Anaerobic Conditions.
Newsome, Laura; Morris, Katherine; Lloyd, Jonathan R
2015-01-01
Stimulating the microbially-mediated precipitation of uranium biominerals may be used to treat groundwater contamination at nuclear sites. The majority of studies to date have focussed on the reductive precipitation of uranium as U(IV) by U(VI)- and Fe(III)-reducing bacteria such as Geobacter and Shewanella species, although other mechanisms of uranium removal from solution can occur, including the precipitation of uranyl phosphates via bacterial phosphatase activity. Here we present the results of uranium biomineralisation experiments using an isolate of Serratia obtained from a sediment sample representative of the Sellafield nuclear site, UK. When supplied with glycerol phosphate, this Serratia strain was able to precipitate 1 mM of soluble U(VI) as uranyl phosphate minerals from the autunite group, under anaerobic and fermentative conditions. Under phosphate-limited anaerobic conditions and with glycerol as the electron donor, non-growing Serratia cells could precipitate 0.5 mM of uranium supplied as soluble U(VI), via reduction to nano-crystalline U(IV) uraninite. Some evidence for the reduction of solid phase uranyl(VI) phosphate was also observed. This study highlights the potential for Serratia and related species to play a role in the bioremediation of uranium contamination, via a range of different metabolic pathways, dependent on culturing or in situ conditions.
Uranium Biominerals Precipitated by an Environmental Isolate of Serratia under Anaerobic Conditions
Newsome, Laura; Morris, Katherine; Lloyd, Jonathan. R.
2015-01-01
Stimulating the microbially-mediated precipitation of uranium biominerals may be used to treat groundwater contamination at nuclear sites. The majority of studies to date have focussed on the reductive precipitation of uranium as U(IV) by U(VI)- and Fe(III)-reducing bacteria such as Geobacter and Shewanella species, although other mechanisms of uranium removal from solution can occur, including the precipitation of uranyl phosphates via bacterial phosphatase activity. Here we present the results of uranium biomineralisation experiments using an isolate of Serratia obtained from a sediment sample representative of the Sellafield nuclear site, UK. When supplied with glycerol phosphate, this Serratia strain was able to precipitate 1 mM of soluble U(VI) as uranyl phosphate minerals from the autunite group, under anaerobic and fermentative conditions. Under phosphate-limited anaerobic conditions and with glycerol as the electron donor, non-growing Serratia cells could precipitate 0.5 mM of uranium supplied as soluble U(VI), via reduction to nano-crystalline U(IV) uraninite. Some evidence for the reduction of solid phase uranyl(VI) phosphate was also observed. This study highlights the potential for Serratia and related species to play a role in the bioremediation of uranium contamination, via a range of different metabolic pathways, dependent on culturing or in situ conditions. PMID:26132209
NASA Astrophysics Data System (ADS)
Yang, Hee-Chul; Kim, Hyung-Ju; Lee, Si-Young; Yang, In-Hwan; Chung, Dong-Yong
2017-06-01
The thermochemical properties of uranium compounds have attracted much interest in relation to thermochemical treatments and the safe disposal of radioactive waste bearing uranium compounds. The characteristics of the thermal decomposition of uranium metaphosphate, U(PO3)4, into uranium pyrophosphate, UP2O7, have been studied from the view point of reaction kinetics and acting mechanisms. A mixture of U(PO3)4 and UP2O7 was prepared from the pyrolysis residue of uranium-bearing spent TBP. A kinetic analysis of the reaction of U(PO3)4 into UP2O7 was conducted using an isoconversional method and a master plot method on the basis of data from a non-isothermal thermogravimetric analysis. The thermal decomposition of U(PO3)4 into UP2O7 followed a single-step reaction with an activation energy of 175.29 ± 1.58 kJ mol-1. The most probable kinetic model was determined as a type of nucleation and nuclei-growth models, the Avrami-Erofeev model (A3), which describes that there are certain restrictions on nuclei growth of UP2O7 during the solid-state decomposition of U(PO3)4.
Radioactive equilibrium in ancient marine sediments
Breger, I.A.
1955-01-01
Radioactive equilibrium in eight marine sedimentary formations has been studied by means of direct determinations of uranium, radium and thorium. Alpha-particle counting has also been carried out in order to cross-calibrate thick-source counting techniques. The maximum deviation from radioactive equilibrium that has been noted is 11 per cent-indicating that there is probably equilibrium in all the formations analyzed. Thick-source alpha-particle counting by means of a proportional counter or an ionization chamber leads to high results when the samples contain less than about 10 p.p.m. of uranium. For samples having a higher content of uranium the results are in excellent agreement with each other and with those obtained by direct analytical techniques. The thorium contents that have been obtained correspond well to the average values reported in the literature. The uranium content of marine sediments may be appreciably higher than the average values that have been reported for sedimentary rocks. Data show that there is up to fourteen times the percentage of uranium as of thorium in the formations studied and that the percentage of thorium never exceeds that of uranium. While the proximity of a depositional environment to a land mass may influence the concentration of uranium in a marine sediment, this is not true with thorium. ?? 1955.
NASA Astrophysics Data System (ADS)
Figueiredo, M. O.; Silva, T. P.; Batista, M. J.; Leote, J.; Ferreira, M. L.; Limpo, V.
2009-04-01
Portugal has been a uranium-producer since the beginning of the last century. The uranium-rich area of Alto Alentejo, East-central Portugal, was identified more than fifty years ago [1]. Almost all the uranium-bearing mineralization occurs in schistose rocks of the contact metamorphic aureole produced by intrusion of the Hercynian monzonitic granite of Alto Alentejo into the pre-Ordovitian schist-greywacke complex forming deposits of vein and dissemination type. The Nisa uranium-reservoir, situated at the sharp border of a large and arch shaped granite pluton, was identified in 1957 [2] but its exploitation was considered economically impracticable until recently. However, its existence and the accumulated detritus of these prospect efforts are a concern for local populations [3]. A study of the near-surface soils close to the Nisa reservoir was therefore undertaken to assess the uranium retention by adsorption on clay components under the form of uranyl ions, [UO2]2+ [4-6] and its eventual release into the aquifer groundwater. As an attempt to very quickly appraise the presence of uranium in as-collected near-surface sediment samples a combination of laboratory X-ray techniques was designed: X-ray diffraction (XRD) to identify the mineral phases and roughly estimate its relative proportion plus X-ray fluorescence spectrometry in wavelength dispersive mode (XRF-WDS) to ascertain the presence of uranium and tentatively evaluate its content by comparison with selected chemical components of the soil. A description of the experimental methodology adopted for the implemented easy-and-quick uranium assay is presented. Obtained results compare quite well to the data of certified time-consuming analytical tests of uranium in those soil samples. [1] L. Pilar (1966) Conditions of formation of Nisa uranium deposit (in Portuguese). Comunic. Serv. Geol. Portugal, tomo L, 50-85. [2] C. Gonçalves & J.V. Teixeira Lopes (1971) Uranium deposit of Nisa: geological aspects of its discovery and valorisation (in Portuguese). Internal Rept., JEN, 20 pp. [3] http://www.naturtejo.com [4] J.A. Davis et al. (2006) Processes affecting transport of uranium in a suboxic aquifer. Phys. Chem. of the Earth 31, 548-555. [5] Y. Arai et al. (2007) Spectroscopic evidence for uranium bearing precipitates in Vadose zone sediments at the Hanford 300-Area site. Environ. Sci. Technol. 41, 4633-4639. [6] A. Kremleva, S. Krüger & N. Rösch (2008) Density functional model studies of uranyl adsorption on (001) surfaces of kaolinite. Langmuir 24, 9515-9524.
URANIUM RECOVERY FROM COMPOSITE UF$sub 4$ REDUCTION BOMB WASTES
DOE Office of Scientific and Technical Information (OSTI.GOV)
Johnson, E R; Doyle, R L; Coleman, J R
1954-01-28
A number of techniques have been investigated on a laboratory-scale for separating uranium from fluorides during the recovery of uranium from UF4 reduction bomb wastes (C-oxide) by an HCl leach - NH4OH precipitation process. Among these are included adsorption of fluorides from filtered leach liquors, fractional precipitation of fluorides and uranium, complexing of fluorides into forms soluble in slightly acid solutions, and fluoride volatilization from the uranium concentrate. Solubility studies of CaF2 and MgF2 in aqueous hydrochloric acid at various acidities and temperatures were also conducted. A description of the production-scale processing of C-oxide in the FMPC scrap plant hasmore » been included.« less
PROGRESS WITH K BASINS SLUDGE RETRIEVAL STABILIZATION & PACKAGING AT THE HANFORD NUCLEAR SITE
DOE Office of Scientific and Technical Information (OSTI.GOV)
KNOLLMEYER, P.M.; PHILLIPS, C; TOWNSON, P.S.
This paper shows how Fluor Hanford and BNG America have combined nuclear plant skills from the U.S. and the U.K. to devise methods to retrieve and treat the sludge that has accumulated in K Basins at the Hanford Site over many years. Retrieving the sludge is the final stage in removing fuel and sludge from the basins to allow them to be decontaminated and decommissioned, so as to remove the threat of contamination of the Columbia River. A description is given of sludge retrieval using vacuum lances and specially developed nozzles and pumps into Consolidation Containers within the basins. Themore » special attention that had to be paid to the heat generation and potential criticality issues with the irradiated uranium-containing sludge is described. The processes developed to re-mobilize the sludge from the Consolidation Containers and pump it through flexible and transportable hose-in-hose piping to the treatment facility are explained with particular note made of dealing with the abrasive nature of the sludge. The treatment facility, housed in an existing Hanford building, is described, and the uranium-corrosion and grout packaging processes explained. The uranium corrosion process is a robust, tempered process very suitable for dealing with a range of differing sludge compositions. Optimization and simplification of the original sludge corrosion process design is described and the use of transportable and reusable equipment is indicated. The processes and techniques described in the paper are shown to have wide applicability to nuclear cleanup.« less
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ladd-Lively, Jennifer L
2014-01-01
The objective of this work was to determine the feasibility of using on-line multivariate statistical process control (MSPC) for safeguards applications in natural uranium conversion plants. Multivariate statistical process control is commonly used throughout industry for the detection of faults. For safeguards applications in uranium conversion plants, faults could include the diversion of intermediate products such as uranium dioxide, uranium tetrafluoride, and uranium hexafluoride. This study was limited to a 100 metric ton of uranium (MTU) per year natural uranium conversion plant (NUCP) using the wet solvent extraction method for the purification of uranium ore concentrate. A key component inmore » the multivariate statistical methodology is the Principal Component Analysis (PCA) approach for the analysis of data, development of the base case model, and evaluation of future operations. The PCA approach was implemented through the use of singular value decomposition of the data matrix where the data matrix represents normal operation of the plant. Component mole balances were used to model each of the process units in the NUCP. However, this approach could be applied to any data set. The monitoring framework developed in this research could be used to determine whether or not a diversion of material has occurred at an NUCP as part of an International Atomic Energy Agency (IAEA) safeguards system. This approach can be used to identify the key monitoring locations, as well as locations where monitoring is unimportant. Detection limits at the key monitoring locations can also be established using this technique. Several faulty scenarios were developed to test the monitoring framework after the base case or normal operating conditions of the PCA model were established. In all of the scenarios, the monitoring framework was able to detect the fault. Overall this study was successful at meeting the stated objective.« less
NASA Astrophysics Data System (ADS)
Lefebvre, Pierre; Noël, Vincent; Jemison, Noah; Weaver, Karrie; Bargar, John; Maher, Kate
2016-04-01
Uranium (U) groundwater contamination following oxidized U(VI) releases from weathering of mine tailings is a major concern at numerous sites across the Upper Colorado River Basin (CRB), USA. Uranium(IV)-bearing solids accumulated within naturally reduced zones (NRZs) characterized by elevated organic carbon and iron sulfide compounds. Subsequent re-oxidation of U(IV)solid to U(VI)aqueous then controls the release to groundwater and surface water, resulting in plume persistence and raising public health concerns. Thus, understanding the extent of uranium oxidation and reduction within NRZs is critical for assessing the persistence of the groundwater contamination. In this study, we measured solid-phase uranium isotope fractionation (δ238/235U) of sedimentary core samples from four study sites (Shiprock, NM, Grand Junction, Rifle and Naturita, CO) using a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS). We observe a strong correlation between U accumulation and the extent of isotopic fractionation, with Δ238U up to +1.8 ‰ between uranium-enriched and low concentration zones. The enrichment in the heavy isotopes within the NRZs appears to be especially important in the vadose zone, which is subject to variations in water table depth. According to previous studies, this isotopic signature is consistent with biotic reduction processes associated with metal-reducing bacteria. Positive correlations between the amount of iron sulfides and the accumulation of reduced uranium underline the importance of sulfate-reducing conditions for U(IV) retention. Furthermore, the positive fractionation associated with U reduction observed across all sites despite some variations in magnitude due to site characteristics, shows a regional trend across the Colorado River Basin. The maximum extent of 238U enrichment observed in the NRZ proximal to the water table further suggests that the redox cycling of uranium, with net release of U(VI) to the groundwater by non-fractionating oxidation, is occurring within this zone. Thus, release of uranium from the NRZs may play a critical role in the persistence of groundwater contamination at these sites.
Rapid removal of uranium from aqueous solutions using magnetic Fe3O4@SiO2 composite particles.
Fan, Fang-Li; Qin, Zhi; Bai, Jing; Rong, Wei-Dong; Fan, Fu-You; Tian, Wei; Wu, Xiao-Lei; Wang, Yang; Zhao, Liang
2012-04-01
Rapid removal of U(VI) from aqueous solutions was investigated using magnetic Fe(3)O(4)@SiO(2) composite particles as the novel adsorbent. Batch experiments were conducted to study the effects of initial pH, amount of adsorbent, shaking time and initial U(VI) concentrations on uranium sorption efficiency as well as the desorbing of U(VI). The sorption of uranium on Fe(3)O(4)@SiO(2) composite particles was pH-dependent, and the optimal pH was 6.0. In kinetics studies, the sorption equilibrium can be reached within 180 min, and the experimental data were well fitted by the pseudo-second-order model, and the equilibrium sorption capacities calculated by the model were almost the same as those determined by experiments. The Langmuir sorption isotherm model correlates well with the uranium sorption equilibrium data for the concentration range of 20-200 mg/L. The maximum uranium sorption capacity onto magnetic Fe(3)O(4)@SiO(2) composite particles was estimated to be about 52 mg/g at 25 °C. The highest values of uranium desorption (98%) was achieved using 0.01 M HCl as the desorbing agent. Fe(3)O(4)@SiO(2) composite particles showed a good selectivity for uranium from aqueous solution with other interfering cation ions. Present study suggested that magnetic Fe(3)O(4)@SiO(2) composite particles can be used as a potential adsorbent for sorption uranium and also provided a simple, fast separation method for removal of heavy metal ion from aqueous solution. Copyright © 2011 Elsevier Ltd. All rights reserved.
Redox-Active vs Redox-Innocent: A Comparison of Uranium Complexes Containing Diamine Ligands.
Pattenaude, Scott A; Mullane, Kimberly C; Schelter, Eric J; Ferrier, Maryline G; Stein, Benjamin W; Bone, Sharon E; Lezama Pacheco, Juan S; Kozimor, Stosh A; Fanwick, Phillip E; Zeller, Matthias; Bart, Suzanne C
2018-05-11
Uranium complexes ( Mes DAE) 2 U(THF) (1-DAE) and Cp 2 U( Mes DAE) (2-DAE) ( Mes DAE = [ArN-CH 2 CH 2 -NAr]; Ar = 2,4,6-trimethylphenyl (Mes)), bearing redox-innocent diamide ligands, have been synthesized and characterized for a full comparison with previously published, redox-active diimine complexes, ( Mes DAB Me ) 2 U(THF) (1-DAB) and Cp 2 U( Mes DAB Me ) (2-DAB) ( Mes DAB Me = [ArN═C(Me)C(Me)═NAr]; Ar = Mes). These redox-innocent analogues maintain an analogous steric environment to their redox-active ligand counterparts to facilitate a study aimed at determining the differing electronic behavior around the uranium center. Structural analysis by X-ray crystallography showed 1-DAE and 2-DAE have a structural environment very similar to 1-DAB and 2-DAB, respectively. The main difference occurs with coordination of the ene-backbone to the uranium center in the latter species. Electronic absorption spectroscopy reveals these new DAE complexes are nearly identical to each other. X-ray absorption spectroscopy suggests all four species contain +4 uranium ions. The data also indicates that there is an electronic difference between the bis(diamide)-THF uranium complexes as opposed to those that only contain one diamide and two cyclopentadienyl rings. Finally, magnetic measurements reveal that all complexes display temperature-dependent behavior consistent with uranium(IV) ions that do not include ligand radicals. Overall, this study determines that there is no significant bonding difference between the redox-innocent and redox-active ligand frameworks on uranium. Furthermore, there are no data to suggest covalent bonding character using the latter ligand framework on uranium, despite what is known for transition metals.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.
Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy’s Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments’ mineralogy, particle size, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population andmore » composition, which mainly determines the system’s performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments’ propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments’ ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. The results of this study suggest that reductive immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less
NASA Astrophysics Data System (ADS)
Kraiem, M.; Mayer, K.; Gouder, T.; Seibert, A.; Wiss, T.; Thiele, H.; Hiernaut, J.-P.
2010-01-01
Thermal ionization mass spectrometry (TIMS) is a well established instrumental technique for providing accurate and precise isotope ratio measurements of elements with reasonably low first ionization potential. In nuclear safeguards and in environmental research, it is often required to measure the isotope ratios in small samples of uranium. Empirical studies had shown that the ionization yield of uranium and plutonium in a TIMS ion source can be significantly increased in the presence of a carbon source. But, even though carbon appeared crucial in providing high ionization yields, processes taking place on the ionization surface were still not well understood. This paper describes the experimental results obtained from an extended study on the evaporation and ionization mechanisms of uranium occurring on a rhenium mass spectrometry filament in the presence of carbon. Solid state reactions were investigated using X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). Additionally, vaporization measurements were performed with a modified-Knudsen cell mass spectrometer for providing information on the neutral uranium species in the vapor phase. Upon heating, under vacuum, the uranyl nitrate sample was found to turn into a uranium carbide compound, independent of the type of carbon used as ionization enhancer. With further heating, uranium carbide leads to formation of single charged uranium metal ions and a small amount of uranium carbide ions. The results are relevant for a thorough understanding of the ion source chemistry of a uranyl nitrate sample under reducing conditions. The significant increase in ionization yield described by many authors on the basis of empirical results can be now fully explained and understood.
Gott, Garland B.; Erickson, Ralph L.
1952-01-01
Because of the common association of uranium and copper in several of the commercial uranium deposits in the Colorado Plateau Province, a reconnaissance was made of several known deposits of copper disseminated through sandstone to determine whether they might be a source of uranium. In order to obtain more information regarding the relationship between copper, uranium and carbonaceous materials, some of the uraniferious asphaltrite deposits in the Shinarump conglomerate along the west flank of the San Rafael Swell were also investigated briefly. During this reconnaissance 18 deposits were examined in New Mexico, eight in Utah, two in Idaho, and one each in Wyoming and Colorado. No uranium deposits of commercial grade are associated with the copper deposits that were examined. The uraniferous asphaltites in the Shinarump conglomerate of Triassic age on the west flank of the San Rafael Swell, however, are promising from the standpoint of commercial uranium production. Spectrographic analyses of crude oil, asphalt, and bituminous shales show a rather consistent suite of trace metals including vanadium, nickel, copper, cobalt, chromium, lead zinc, and molybdenum. The similarity of the metal assemblage, including uranium of the San Rafael Swell asphaltites, to the metal assemblage in crude oil and other bituminous materials suggests that these metals were concentrated in the asphaltites from petroleum. However, the hypothesis that uranium minerals were already present before the hydrocarbons were introduced and that some sort of replacement or uranium minerals by carbon compounds was effected after the petroleum migrated into the uranium deposit should not be disregarded. The widespread association of uranium with asphaltic material suggests that it also may have been concentrated by some agency connected with the formation of petroleum. The problem of the association of uranium and other trace metals with hydrocarbons should be studied further both in the field and in the laboratory.
NASA Astrophysics Data System (ADS)
Harris, R.; Reimus, P. W.; Ware, D.; Williams, K.; Chu, D.; Perkins, G.; Migdissov, A. A.; Bonwell, C.
2017-12-01
Uranium is primarily mined for nuclear power production using an aqueous extraction technique called in-situ recovery (ISR). ISR can pollute groundwater with residual uranium and other heavy metals. Reverse osmosis and groundwater sweep are currently used to restore groundwater after ISR mining, but are not permanent solutions. Sodium dithionite is being tested as part of a method to more permanently restore groundwater after ISR mining at the Smith-Ranch Highland site in Wyoming. Sodium dithionite is a chemical reductant that can reduce sediments that were oxidized during ISR. The reduced sediments can reduce soluble uranium (VI) in the groundwater to insoluble uranium (IV). Laboratory studies that use sodium dithionite to treat sediments and waters from the site may help predict how it will behave during a field deployment. An aqueous batch experiment showed that sodium dithionite reduced uranium in post-mined untreated groundwater from 38 ppm to less than 1 ppm after 1 day. A sediment reduction batch experiment showed that sodium dithionite-treated sediments were capable of reducing uranium in post-mined untreated groundwater from 38 ppm to 2 ppm after 7 days. One column experiment is showing post-mined sodium dithionite-treated sediments are capable of reducing uranium in post-mined groundwater for over 30 pore volumes past the initial injection. While these results are promising for field deployments of sodium dithionite, another column experiment with sodium dithionite-treated sediments containing uranium rich organic matter is showing net production of uranium instead of uranium uptake. Sodium dithionite appears to liberate uranium from the organic matter. Another sediment reduction experiment is being conducted to further investigate this hypothesis. These experiments are helping guide plans for field deployments of sodium dithionite at uranium ISR mining sites.
Miller, Andrew W; Rodriguez, Derrick R; Honeyman, Bruce D
2013-05-01
Intermediate scale tank studies were conducted to examine the effects of physical heterogeneity of aquifer material on uranium desorption and subsequent transport in order to bridge the scaling gap between bench and field scale systems. Uranium contaminated sediment from a former uranium mill field site was packed into two 2-D tanks with internal dimensions of 2.44×1.22×0.076 m (tank 1) and 2.44×0.61×0.076 m (tank 2). Tank 1 was packed in a physically homogenous manner, and tank 2 was packed with long lenses of high and low conductivities resulting in different flow fields within the tanks. Chemical gradients within the flow domain were altered by temporal changes in influent water chemistry. The uranium source was desorption from the sediment. Despite the physical differences in the flow fields, there were minimal differences in global uranium leaching behavior between the two tanks. The dominant uranium species in both tanks over time and space was Ca2UO2(CO3)3(0). However, the uranium/alkalinity relationships varied as a function of time in tank 1 and were independent of time in tank 2. After planned stop-flow events, small, short-lived rebounds were observed in tank 1 while no rebound of uranium concentrations was observed in tank 2. Despite appearing to be in local equilibrium with respect to uranium desorption, a previously derived surface complexation model was insufficient to describe uranium partitioning within the flow domain. This is the first in a pair of papers; the companion paper presents an intermediate scale 3-D tank experiment and inter-tank comparisons. For these systems, physical heterogeneity at or above the decimeter scale does not affect global scale uranium desorption and transport. Instead, uranium fluxes are controlled by chemistry dependent desorption patterns induced by changing the influent ionic composition. Published by Elsevier B.V.
NASA Astrophysics Data System (ADS)
Miller, Andrew W.; Rodriguez, Derrick R.; Honeyman, Bruce D.
2013-05-01
Intermediate scale tank studies were conducted to examine the effects of physical heterogeneity of aquifer material on uranium desorption and subsequent transport in order to bridge the scaling gap between bench and field scale systems. Uranium contaminated sediment from a former uranium mill field site was packed into two 2-D tanks with internal dimensions of 2.44 × 1.22 × 0.076 m (tank 1) and 2.44 × 0.61 × 0.076 m (tank 2). Tank 1 was packed in a physically homogenous manner, and tank 2 was packed with long lenses of high and low conductivities resulting in different flow fields within the tanks. Chemical gradients within the flow domain were altered by temporal changes in influent water chemistry. The uranium source was desorption from the sediment. Despite the physical differences in the flow fields, there were minimal differences in global uranium leaching behavior between the two tanks. The dominant uranium species in both tanks over time and space was Ca2UO2(CO3)30. However, the uranium/alkalinity relationships varied as a function of time in tank 1 and were independent of time in tank 2. After planned stop-flow events, small, short-lived rebounds were observed in tank 1 while no rebound of uranium concentrations was observed in tank 2. Despite appearing to be in local equilibrium with respect to uranium desorption, a previously derived surface complexation model was insufficient to describe uranium partitioning within the flow domain. This is the first in a pair of papers; the companion paper presents an intermediate scale 3-D tank experiment and inter-tank comparisons. For these systems, physical heterogeneity at or above the decimeter scale does not affect global scale uranium desorption and transport. Instead, uranium fluxes are controlled by chemistry dependent desorption patterns induced by changing the influent ionic composition.
The roles of organic matter in the formation of uranium deposits in sedimentary rocks
Spirakis, C.S.
1996-01-01
Because reduced uranium species have a much smaller solubility than oxidized uranium species and because of the strong association of organic matter (a powerful reductant) with many uranium ores, reduction has long been considered to be the precipitation mechanism for many types of uranium deposits. Organic matter may also be involved in the alterations in and around tabular uranium deposits, including dolomite precipitation, formation of silicified layers, iron-titanium oxide destruction, dissolution of quartz grains, and precipitation of clay minerals. The diagenetic processes that produced these alterations also consumed organic matter. Consequently, those tabular deposits that underwent the more advanced stages of diagenesis, including methanogenesis and organic acid generation, display the greatest range of alterations and contain the smallest amount of organic matter. Because of certain similarities between tabular uranium deposits and Precambrian unconformity-related deposits, some of the same processes might have been involved in the genesis of Precambrian unconformity-related deposits. Hydrologic studies place important constraints on genetic models of various types of uranium deposits. In roll-front deposits, oxidized waters carried uranium to reductants (organic matter and pyrite derived from sulfate reduction by organic matter). After these reductants were oxidized at any point in the host sandstone, uranium minerals were reoxidized and transported further down the flow path to react with additional reductants. In this manner, the uranium ore migrated through the sandstone at a rate slower than the mineralizing ground water. In the case of tabular uranium deposits, the recharge of surface water into the ground water during flooding of lakes carried soluble humic material to the water table or to an interface where humate precipitated in tabular layers. These humate layers then established the chemical conditions for mineralization and related alterations. In the case of Precambrian unconformity-related deposits, free thermal convection in the thick sandstones overlying the basement rocks carried uranium to concentrations of organic matter in the basement rocks.
Uptake of uranium from seawater by amidoxime-based polymeric adsorbent marine testing
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tsouris, C.; Kim, J.; Oyola, Y.
2013-07-01
Amidoxime-based polymer adsorbents in the form of functionalized fibers were prepared at the Oak Ridge National Laboratory (ORNL) and screened in laboratory experiments, in terms of uranium uptake capacity, using spiked uranium solution and seawater samples. Batch laboratory experiments conducted with 5-gallon seawater tanks provided equilibrium information. Based on results from 5-gallon experiments, the best adsorbent was selected for field-testing of uranium adsorption from seawater. Flow-through column tests have been performed at different marine sites to investigate the uranium uptake rate and equilibrium capacity under diverse biogeochemistry. The maximum amount of uranium uptake from seawater tests at Sequim, WA, wasmore » 3.3 mg U/g adsorbent after eight weeks of contact of the adsorbent with seawater. This amount was three times higher than the maximum adsorption capacity achieved in this study by a leading adsorbent developed by the Japan Atomic Energy Agency (JAEA), which was 1.1 mg U/g adsorbent at equilibrium. The initial uranium uptake rate of the ORNL adsorbent was 2.6 times higher than that of the JAEA adsorbent under similar conditions. A mathematical model derived from the mass balance of uranium was employed to describe the data. (authors)« less
Sustainability of uranium mining and milling: toward quantifying resources and eco-efficiency.
Mudd, Gavin M; Diesendorf, Mark
2008-04-01
The mining of uranium has long been a controversial public issue, and a renewed debate has emerged on the potential for nuclear power to help mitigate against climate change. The central thesis of pro-nuclear advocates is the lower carbon intensity of nuclear energy compared to fossil fuels, although there remains very little detailed analysis of the true carbon costs of nuclear energy. In this paper, we compile and analyze a range of data on uranium mining and milling, including uranium resources as well as sustainability metrics such as energy and water consumption and carbon emissions with respect to uranium production-arguably the first time for modern projects. The extent of economically recoverable uranium resources is clearly linked to exploration, technology, and economics but also inextricably to environmental costs such as energy/water/chemicals consumption, greenhouse gas emissions, and social issues. Overall, the data clearly show the sensitivity of sustainability assessments to the ore grade of the uranium deposit being mined and that significant gaps remain in complete sustainability reporting and accounting. This paper is a case study of the energy, water, and carbon costs of uranium mining and milling within the context of the nuclear energy chain.
Le Guernic, Antoine; Sanchez, Wilfried; Bado-Nilles, Anne; Palluel, Olivier; Turies, Cyril; Chadili, Edith; Cavalié, Isabelle; Delahaut, Laurence; Adam-Guillermin, Christelle; Porcher, Jean-Marc; Geffard, Alain; Betoulle, Stéphane; Gagnaire, Béatrice
2016-08-01
Human activities have led to increased levels of various pollutants including metals in aquatic ecosystems. Increase of metallic concentrations in aquatic environments represents a potential risk to exposed organisms, including fish. The aim of this study was to characterize the environmental risk to fish health linked to a polymetallic contamination from former uranium mines in France. This contamination is characterized by metals naturally present in the areas (manganese and iron), uranium, and metals (aluminum and barium) added to precipitate uranium and its decay products. Effects from mine releases in two contaminated ponds (Pontabrier for Haute-Vienne Department and Saint-Pierre for Cantal Department) were compared to those assessed at four other ponds outside the influence of mine tailings (two reference ponds/department). In this way, 360 adult three-spined sticklebacks (Gasterosteus aculeatus) were caged for 28 days in these six ponds before biomarker analyses (immune system, antioxidant system, biometry, histology, DNA integrity, etc.). Ponds receiving uranium mine tailings presented higher concentrations of uranium, manganese and aluminum, especially for the Haute-Vienne Department. This uranium contamination could explain the higher bioaccumulation of this metal in fish caged in Pontabrier and Saint-Pierre Ponds. In the same way, many fish biomarkers (antioxidant and immune systems, acetylcholinesterase activity and biometric parameters) were impacted by this environmental exposure to mine tailings. This study shows the interest of caging and the use of a multi-biomarker approach in the study of a complex metallic contamination.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wang, Guohui; Um, Wooyong; Wang, Zheming
The reaction of acidic radioactive waste with sediments can induce mineral transformation reactions that, in turn, control contaminant fate. Here, sediment weathering by synthetic uranium-containing acid solutions was investigated using bench-scale experiments to simulate waste disposal conditions at Hanford’s cribs, USA. During acid weathering, the presence of phosphate exerted a strong influence over uranium mineralogy and a rapidly precipitated, crystalline uranium phosphate phase (meta-ankoleite [K(UO2)(PO4)·3H2O]) was identified using spectroscopic and diffraction-based techniques. In phosphate-free system, uranium oxyhydroxide minerals such as K-compreignacite [K2(UO2)6O4(OH)6·7H2O] were formed. Single-pass flow-through (SPFT) and column leaching experiments using synthetic Hanford pore water showed that uranium precipitatedmore » as meta-ankoleite during acid weathering was strongly retained in the sediments, with an average release rate of 2.67E-12 mol g-1 s-1. In the absence of phosphate, uranium release was controlled by dissolution of uranium oxyhydroxide (compreignacite-type) mineral with a release rate of 1.05-2.42E-10 mol g-1 s-1. The uranium mineralogy and release rates determined for both systems in this study support the development of accurate U-release models for prediction of contaminant transport. These results suggest that phosphate minerals may be a good candidate for uranium remediation approaches at contaminated sites.« less
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
Wang, Guohui; Um, Wooyong; Wang, Zheming; Reinoso-Maset, Estela; Washton, Nancy M; Mueller, Karl T; Perdrial, Nicolas; O'Day, Peggy A; Chorover, Jon
2017-10-03
The reaction of acidic radioactive waste with sediments can induce mineral transformation reactions that, in turn, control contaminant fate. Here, sediment weathering by synthetic uranium-containing acid solutions was investigated using bench-scale experiments to simulate waste disposal conditions at Hanford's cribs (Hanford, WA). During acid weathering, the presence of phosphate exerted a strong influence over uranium mineralogy and a rapidly precipitated, crystalline uranium phosphate phase (meta-ankoleite [K(UO 2 )(PO 4 )·3H 2 O]) was identified using spectroscopic and diffraction-based techniques. In phosphate-free system, uranium oxyhydroxide minerals such as K-compreignacite [K 2 (UO 2 ) 6 O 4 (OH) 6 ·7H 2 O] were formed. Single-pass flow-through (SPFT) and column leaching experiments using synthetic Hanford pore water showed that uranium precipitated as meta-ankoleite during acid weathering was strongly retained in the sediments, with an average release rate of 2.67 × 10 -12 mol g -1 s -1 . In the absence of phosphate, uranium release was controlled by dissolution of uranium oxyhydroxide (compreignacite-type) mineral with a release rate of 1.05-2.42 × 10 -10 mol g -1 s -1 . The uranium mineralogy and release rates determined for both systems in this study support the development of accurate U-release models for the prediction of contaminant transport. These results suggest that phosphate minerals may be a good candidate for uranium remediation approaches at contaminated sites.
Method for converting uranium oxides to uranium metal
Duerksen, Walter K.
1988-01-01
A process is described for converting scrap and waste uranium oxide to uranium metal. The uranium oxide is sequentially reduced with a suitable reducing agent to a mixture of uranium metal and oxide products. The uranium metal is then converted to uranium hydride and the uranium hydride-containing mixture is then cooled to a temperature less than -100.degree. C. in an inert liquid which renders the uranium hydride ferromagnetic. The uranium hydride is then magnetically separated from the cooled mixture. The separated uranium hydride is readily converted to uranium metal by heating in an inert atmosphere. This process is environmentally acceptable and eliminates the use of hydrogen fluoride as well as the explosive conditions encountered in the previously employed bomb-reduction processes utilized for converting uranium oxides to uranium metal.
Kato, Masashi; Azimi, Mohammad Daud; Fayaz, Said Hafizullah; Shah, Muhammad Dawood; Hoque, Md Zahirul; Hamajima, Nobuyuki; Ohnuma, Shoko; Ohtsuka, Tomomi; Maeda, Masao; Yoshinaga, Masafumi
2016-12-01
Toxic elements in drinking water have great effects on human health. However, there is very limited information about toxic elements in drinking water in Afghanistan. In this study, levels of 10 elements (chromium, nickel, copper, arsenic, cadmium, antimony, barium, mercury, lead and uranium) in 227 well drinking water samples in Kabul, Afghanistan were examined for the first time. Chromium (in 0.9% of the 227 samples), arsenic (7.0%) and uranium (19.4%) exceeded the values in WHO health-based guidelines for drinking-water quality. Maximum chromium, arsenic and uranium levels in the water samples were 1.3-, 10.4- and 17.2-fold higher than the values in the guidelines, respectively. We next focused on uranium, which is the most seriously polluted element among the 10 elements. Mean ± SD (138.0 ± 1.4) of the 238 U/ 235 U isotopic ratio in the water samples was in the range of previously reported ratios for natural source uranium. We then examined the effect of our originally developed magnesium (Mg)-iron (Fe)-based hydrotalcite-like compounds (MF-HT) on adsorption for uranium. All of the uranium-polluted well water samples from Kabul (mean ± SD = 190.4 ± 113.9 μg/L; n = 11) could be remediated up to 1.2 ± 1.7 μg/L by 1% weight of our MF-HT within 60 s at very low cost (<0.001 cents/day/family) in theory. Thus, we demonstrated not only elevated levels of some toxic elements including natural source uranium but also an effective depurative for uranium in well drinking water from Kabul. Since our depurative is effective for remediation of arsenic as shown in our previous studies, its practical use in Kabul may be encouraged. Copyright © 2016 Elsevier Ltd. All rights reserved.
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.
NASA Astrophysics Data System (ADS)
Xu, J.; Veeramani, H.; Qafoku, N. P.; Singh, G.; Pruden, A.; Kukkadapu, R. K.; Hochella, M. F., Jr.
2015-12-01
A systematic flow-through column study was conducted using sediments and groundwater from the subsurface at the U.S. Department of Energy's Integrated Field Research Challenge (IFRC) site in Rifle, Colorado, to better understand the efficacy of uranium removal from the groundwater with and without biostimulation in the form of acetate amendments. The interactive effects of acetate amendment, groundwater/sediment geochemistry, and intrinsic bacterial community composition were evaluated using four types of sediments, collected from different uranium-contaminated (D08, LQ107, CD) or non-contaminated (RABS) aquifers. Subtle variations in the sediments' geochemistry in terms of mineral compositions, particle sizes, redox conditions, and metal(loid) co-contaminants had a marked effect on the uranium removal efficiency, following a descending trend of D08 (~ 90 to 95%) >> RABS (~ 20 to 25) ≥ LQ107 (~ 15 to 20%) > CD (~ -10 to 0%). Overall, biostimulation of the sediments with acetate drove deeper anoxic conditions and observable shifts in bacterial population structures. The abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, were highest in the sediments that performed best in terms of uranium removal. By comparison, no obvious associations were found between the uranium removal efficiency and the abundance of typical iron-reducing microorganisms, e.g., Geobacter spp. In the sediments where bacterial biomass was relatively low and sulfate-reduction was not detected (i.e., CD), abiotic adsorption onto fine mineral surfaces such as phyllosilates likely played a dominant role in the attenuation of aqueous uranium. In these scenarios, however, acetate amendment induced significant remobilization of the sequestered uranium and other heavy metals (e.g., strontium), leading to zero or negative uranium removal efficiencies (i.e., CD). The results of this study suggest that reductive immobilization of uranium can be effectively achieved under predominantly sulfate-reducing conditions in sediment microenvironments when bioavailable iron (III) (oxyhydr)oxides are mostly depleted, and provide insight into the integrated roles of sediment geochemistry, mineralogy, and bacterial population dynamics.
Comprehensive Evaluation of Soil Near Uranium Tailings, Beishan City, China.
Xun, Yan; Zhang, Xinjia; Chaoliang, Chen; Luo, Xuegang; Zhang, Yu
2018-06-01
To evaluate the impact of uranium tailings on soil composition and soil microbial, six soil samples at different distance from the uranium tailings (Beishan City, China) were collected for further analysis. Concentrations of radionuclides ( 238 U and 232 Th), heavy metals (Mn, Cd, Cr, Ni, Zn, and Pb) and organochlorine pesticide were determined by ICP-MS and GC, they were significantly higher than those of the control. And the Average Well Color Development as well as the Shannon, the Evenness, and the Simpson index were calculated to evaluate the soil microbial diversity. The carbon utilization model of soil microbial community was also analyzed by Biolog-eco. All results indicated that uranium tailings leaded to excessive radionuclides and heavy metals, and decreased the diversity of the soil microbial community. Our study will provide a valuable basis for soil quality evaluation around uranium tailing repositories and lay a foundation for the management and recovery of uranium tailings.
Uranium in the Surrounding of San Marcos-Sacramento River Environment (Chihuahua, Mexico)
Rentería-Villalobos, Marusia; Cortés, Manuel Reyes; Mantero, Juan; Manjón, Guillermo; García-Tenorio, Rafael; Herrera, Eduardo; Montero-Cabrera, Maria Elena
2012-01-01
The main interest of this study is to assess whether uranium deposits located in the San Marcos outcrops (NW of Chihuahua City, Mexico) could be considered as a source of U-isotopes in its surrounding environment. Uranium activity concentrations were determined in biota, ground, and surface water by either alpha or liquid scintillation spectrometries. Major ions were analyzed by ICP-OES in surface water and its suspended matter. For determining uranium activity in biota, samples were divided in parts. The results have shown a possible lixiviation and infiltration of uranium from geological substrate into the ground and surface water, and consequently, a transfer to biota. Calculated annual effective doses by ingestion suggest that U-isotopes in biota could not negligibly contribute to the neighboring population dose. By all these considerations, it is concluded that in this zone there is natural enhancement of uranium in all environmental samples analyzed in the present work. PMID:22536148
Identifying anthropogenic uranium compounds using soft X-ray near-edge absorption spectroscopy
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ward, Jesse D.; Bowden, Mark; Tom Resch, C.
2017-01-01
Uranium ores mined for industrial use are typically acid-leached to produce yellowcake and then converted into uranium halides for enrichment and purification. These anthropogenic chemical forms of uranium are distinct from their mineral counterparts. The purpose of this study is to use soft X-ray absorption spectroscopy to characterize several common anthropogenic uranium compounds important to the nuclear fuel cycle. Non-destructive chemical analyses of these compounds is important for process and environmental monitoring and X-ray absorption techniques have several advantages in this regard, including element-specificity, chemical sensitivity, and high spectral resolution. Oxygen K-edge spectra were collected for uranyl nitrate, uranyl fluoride,more » and uranyl chloride, and fluorine K-edge spectra were collected for uranyl fluoride and uranium tetrafluoride. Interpretation of the data is aided by comparisons to calculated spectra. These compounds have unique spectral signatures that can be used to identify unknown samples.« less
Finch, W.I.; Feng, S.; Zuyi, C.; McCammon, R.B.
1993-01-01
Four major types of uranium deposits occur in China: granite, volcanic, sandstone, and carbonaceous-siliceous-pelitic rock. These types are major sources of uranium in many parts of the world and account for about 95 percent of Chinese production. Descriptive models for each of these types record the diagnostic regional and local geologic features of the deposits that are important to genetic studies, exploration, and resource assessment. A fifth type of uranium deposit, metasomatite, is also modeled because of its high potential for production. These five types of uranium deposits occur irregularly in five tectonic provinces distributed from the northwest through central to southern China. ?? 1993 Oxford University Press.
Preliminary study on weapon grade uranium utilization in molten salt reactor miniFUJI
NASA Astrophysics Data System (ADS)
Aji, Indarta Kuncoro; Waris, A.
2014-09-01
Preliminary study on weapon grade uranium utilization in 25MWth and 50MWth of miniFUJI MSR (molten salt reactor) has been carried out. In this study, a very high enriched uranium that we called weapon grade uranium has been employed in UF4 composition. The 235U enrichment is 90 - 95 %. The results show that the 25MWth miniFUJI MSR can get its criticality condition for 1.56 %, 1.76%, and 1.96% of UF4 with 235U enrichment of at least 93%, 90%, and 90%, respectively. In contrast, the 50 MWth miniFUJI reactor can be critical for 1.96% of UF4 with 235U enrichment of at smallest amount 95%. The neutron spectra are almost similar for each power output.
A physical model for evaluating uranium nitride specific heat
NASA Astrophysics Data System (ADS)
Baranov, V. G.; Devyatko, Yu. N.; Tenishev, A. V.; Khlunov, A. V.; Khomyakov, O. V.
2013-03-01
Nitride fuel is one of perspective materials for the nuclear industry. But unlike the oxide and carbide uranium and mixed uranium-plutonium fuel, the nitride fuel is less studied. The present article is devoted to the development of a model for calculating UN specific heat on the basis of phonon spectrum data within the solid state theory.
A Review of Depleted Uranium Biological Effects: In vivo Studies
2010-11-01
organs - Uranium retention is long-term - DU causes some neurotoxicity - DU induces genotoxicity - DU urine is mutagenic - DU causes adverse oncogene...Behavior; Locomotor Brain Accumulation Sperm Effects Immune Effects Offspring Effects Behavior Yes Yes Yes No effects Decreased Inflammatory...in Unexposed Offspring Finding: DU Internalized Exposure Induces Germ Cell DNA Damage Uranium Distribution Behavior Neurobio Histopathology Sperm
Steven, Thomas A.
1984-01-01
PART A: Igneous activity in the Marysvale volcanic field of western Utah can be separated into many episodes of extrusion, intrusion, and hydrothermal activity. The rocks of the western Tushar Mountains, near the western part of the volcanic field, include intermediate-composition, calc-alkalic volcanic rocks erupted from scattered volcanoes in Oligocene through earliest Miocene time and related monzonitic intrusions emplaced 24-23 m.y. ago. Beginning 22-21 m.y. ago and extending through much of the later Cenozoic, a bimodal basalt-rhyolite assemblage was erupted widely throughout the volcanic field. Only volcanic and intrusive rocks belonging to the rhyolitic end member of this bimodal assemblage are present in the western Tushar Mountains; most of these rocks either fill the Mount Belknap caldera (19 m.y. old) or are part of the rhyolite of Gillies Hill (9---8 m.y. old). Episodic hydrothermal activity altered and mineralized rocks at many places in the western Tushar Mountains during Miocene time. The earliest activity took place in and adjacent to monzonitic calcalkalic intrusions emplaced in the vicinity of Indian Creek and Cork Ridge. These rocks were widely propylitized, and gold-bearing quartz-pyrite-carbonate veins formed in local fractures. Hydrothermal activity associated with the Mount Belknap caldera mobilized and redeposited uranium contained in the caldera-fill rocks and formed primary concentrations of lithophile elements (including molybdenum and uranium) in the vicinity of intrusive bodies. Hydrothermal activity associated with the rhyolite of Gillies Hill altered and mineralized rocks at several places along the fault zone that marks the western margin of the Tushar Mountains; the zoned alunite and gold deposits at Sheep Rock, the gold deposit at the Sunday Mine, and an alunite deposit near Indian Creek were thus produced. Resetting of isotopic ages suggests that another center of hydrothermally altered rocks associated with a buried pluton about 16 m.y. old may exist near Indian Creek just west of the Mount Belknap caldera. Geophysical evidence confirms the probability of a buried pluton near Indian Creek, and also indicates that another buried pluton probably exists beneath the 9-m.y.-old mineralized area at Sheep Rock. The mineral potential of the different hydrothermal systems, and the types of minerals deposited probably vary considerably from one period of mineralization to another and from one depth environment to another within a given system. PART B: The Big John caldera, on the western flank of the Tushar Mountains in the Marysvale volcanic field in west-central Utah, formed 23-22 m.y. ago in response to ash-flow eruptions of the Delano Peak Tuff Member of the Bullion Canyon Volcanics. These eruptions were near the end of the period of Oligocene-early Miocene calc-alkalic igneous activity that built a broad volcanic plateau in this part of Utah. About 22 m.y. ago, the composition of rocks erupted changed to a bimodal assemblage of mafic and silicic volcanics that was erupted episodically through the remainder of Cenozoic time. The alkali rhyolites are uranium rich in part, and are associated with all the known uranium deposits in the Marysvale volcanic field. The Big John caldera was a broad drained basin whose floor was covered by a layer of stream gravels when ash flows from the western source area of the Mount Belknap Volcanics filled the caldera with the Joe Lott Tuff Member about 19 m.y. ago. Devitrified and zeolitized rocks in the caldera fill have lost one-quarter to one-half of the uranium contained in the original magma. This mobilized uranium probably moved into the hydrologic regime, and some may have been redeposited in stream gravels underlying the Joe Lott within the caldera, or in gravels filling the original drainage channel that extended south from the caldera.
Distribution of naturally occurring radionuclides (U, Th) in Timahdit black shale (Morocco).
Galindo, C; Mougin, L; Fakhi, S; Nourreddine, A; Lamghari, A; Hannache, H
2007-01-01
Attention has been focused recently on the use of Moroccan black oil shale as the raw material for production of a new type of adsorbent and its application to U and Th removal from contaminated wastewaters. The purpose of the present work is to provide a better understanding of the composition and structure of this shale and to determine its natural content in uranium and thorium. A black shale collected from Timahdit (Morocco) was analyzed by powder X-ray diffraction and SEM techniques. It was found that calcite, dolomite, quartz and clays constitute the main composition of the inorganic matrix. Pyrite crystals are also present. A selective leaching procedure, followed by radiochemical purification and alpha-counting, was performed to assess the distribution of naturally occurring radionuclides. Leaching results indicate that 238U, 235U, 234U, 232Th, 230Th and 228Th have multiple modes of occurrence in the shale. U is interpreted to have been concentrated under anaerobic conditions. An integrated isotopic approach showed the preferential mobilization of uranium carried by humic acids to carbonate and apatite phases. Th is partitioned between silicate minerals and pyrite.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Shannon, S.S. Jr.
1980-05-01
Uranium and other elemental data resulting from the Hydrogeochemical and Stream Sediment Reconnaissance (HSSR) of the Durango National Topographic Map Series (NTMS) quadrangle, Colorado, by the Los Alamos Scientific Laboratory (LASL) are reported herein. The LASL is responsible for conducting the HSSR primarily in the states of New Mexico, Colorado, Wyoming, Montana, and Alaska. This study was conducted as part of the United States Department of Energy's National Uranium Resource Evaluation (NURE), which is designed to provide improved estimates of the availability and economics of nuclear fuel resources and to make available to industry information for use in exploration andmore » development of uranium resources. The HSSR data will ultimately be integrated with other NURE data (e.g., airborne radiometric surveys and geological investigations) to complete the entire NURE program. This report is a supplement to the HSSR uranium evaluation report for the Durango quadrangle which presented the field and uranium data for the 1518 water and 1604 sediment samples collected from 1804 locations in the quadrangle. The earlier report contains an evaluation of the uranium concentrations of the samples as well as descriptions of the geology, hydrology, climate, and uranium occurrences of the quadrangle. This supplement presents the sediment field and uranium data again and the analyses of 42 other elements in the sediments.« less
Petitot, Fabrice; Lestaevel, Philippe; Tourlonias, Elie; Mazzucco, Charline; Jacquinot, Sébastien; Dhieux, Bernadette; Delissen, Olivia; Tournier, Benjamin B; Gensdarmes, François; Beaunier, Patricia; Dublineau, Isabelle
2013-03-13
Uranium nanoparticles (<100 nm) can be released into the atmosphere during industrial stages of the nuclear fuel cycle and during remediation and decommissioning of nuclear facilities. Explosions and fires in nuclear reactors and the use of ammunition containing depleted uranium can also produce such aerosols. The risk of accidental inhalation of uranium nanoparticles by nuclear workers, military personnel or civilian populations must therefore be taken into account. In order to address this issue, the absorption rate of inhaled uranium nanoparticles needs to be characterised experimentally. For this purpose, rats were exposed to an aerosol containing 10⁷ particles of uranium per cm³ (CMD=38 nm) for 1h in a nose-only inhalation exposure system. Uranium concentrations deposited in the respiratory tract, blood, brain, skeleton and kidneys were determined by ICP-MS. Twenty-seven percent of the inhaled mass of uranium nanoparticles was deposited in the respiratory tract. One-fifth of UO₂ nanoparticles were rapidly cleared from lung (T(½)=2.4 h) and translocated to extrathoracic organs. However, the majority of the particles were cleared slowly (T(½)=141.5 d). Future long-term experimental studies concerning uranium nanoparticles should focus on the potential lung toxicity of the large fraction of particles cleared slowly from the respiratory tract after inhalation exposure. Copyright © 2013 Elsevier Ireland Ltd. All rights reserved.
Inhibition of poly(ADP-ribose)polymerase-1 and DNA repair by uranium
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.
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.
Products of in Situ Corrosion of Depleted Uranium Ammunition in Bosnia and Herzegovina Soils.
Wang, Yuheng; von Gunten, Konstantin; Bartova, Barbora; Meisser, Nicolas; Astner, Markus; Burger, Mario; Bernier-Latmani, Rizlan
2016-11-15
Hundreds of tons of depleted uranium (DU) ammunition were used in previous armed conflicts in Iraq, Bosnia and Herzegovina, and Serbia/Kosovo. The majority (>90%) of DU penetrators miss their target and, if left in the environment, corrode in these postconflict zones. Thus, the best way to understand the fate of bulk DU material in the environment is to characterize the corrosion products of intact DU penetrators under field conditions for extended periods of time. However, such studies are scarce. To fill this knowledge gap, we characterized corrosion products formed from two intact DU penetrators that remained in soils in Bosnia and Herzegovina for over seven years. We used a combination of X-ray powder diffraction, electron microscopy, and X-ray absorption spectroscopy. The results show that metaschoepite (UO 3 (H 2 O) 2 ) was a main component of the two DU corrosion products. Moreover, studtite ((UO 2 )O 2 (H 2 O) 2 ·2(H 2 O)) and becquerelite (Ca(UO 2 ) 6 O 4 (OH) 6 ·8(H 2 O)) were also identified in the corrosion products. Their formation through transformation of metaschoepite was a result of the geochemical conditions under which the penetrators corroded. Moreover, we propose that the transformation of metaschoepite to becquerelite or studtite in the DU corrosion products would decrease the potential for mobilization of U from corroded DU penetrators exposed to similar environments in postconflict areas.
Detection and characterization of uranium-humic complexes during 1D transport studies
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lesher, Emily K.; Honeyman, Bruce D.; Ranville, James F.
2013-05-01
The speciation and transport of uranium (VI) through porous media is highly dependent on solution conditions, the presence of complexing ligands, and the nature of the porous media. The dependency on many variables makes prediction of U transport in bench-scale experiments and in the field difficult. In particular, the identification of colloidal U phases poses a technical challenge. Transport of U in the presence and absence of natural organic matter (Suwannee River humic acid, SRHA) through silica sand and hematite coated silica sand was tested at pH 4 and 5 using static columns, where flow is controlled by gravity andmore » residence time between advective pore volume exchanges can be strictly controlled. The column effluents were characterized by traditional techniques including ICPMS quantification of total [U] and [Fe], TOC analysis of [DOC], and pH analysis, and also by non-traditional techniques: flow field flow fractionation with online ICPMS detection (FlFFF-ICPMS) and specific UV absorbance (SUVA) characterization of effluent fractions. Key results include that the transport of U through the columns was enhanced by pre-equilibration with SRHA, and previously deposited U was remobilized by the addition of SRHA. The advanced techniques yielded important insights on the mechanisms of transport: FlFFF-ICPMS identified a U-SRHA complex as the mobile U species and directly quantified relative amounts of the complex, while specific UV absorbance (SUVA) measurements indicated a composition-based fractionation onto the porous media.« less
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.
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.
NASA Astrophysics Data System (ADS)
Lexa, Dusan; Leibowitz, Leonard; Kropf, Jeremy
2000-03-01
The interaction between the (uranium trichloride + lithium chloride + potassium chloride) eutectic salt and zeolite 4A has been studied by temperature-resolved synchrotron powder X-ray diffraction, evolved gas analysis and differential scanning calorimetry, between 300 and 900 K. The onset of salt occlusion by the zeolite has been detected at 450 K. Evidence of a reaction between zeolitic water and uranium trichloride, leading to the formation of uranium dioxide, has appeared at 600 K. The uranium dioxide particle size increases from 2 nm at 600 K to 25 nm at 900 K - an indication of their extra-zeolitic location. No appreciable degradation of the zeolite structure has been observed.
Depleted uranium: an overview of its properties and health effects.
Shawky, S
2002-01-01
There has been much debate about the use of depleted uranium in the Gulf War and its health effects on United States and European war veterans. However, studies on the impact of this radioactive substance on the residents of the surrounding Gulf region are far from adequate. Depleted uranium introduces large quantities of radioactive material that is hazardous to biological organisms, continues to decay for millennia and is able to travel tens of kilometres in air. If depleted uranium were used in the Gulf War, its impact on the health of people in the area would have been considerable. This review of depleted uranium--its origin, properties, uses and effects on the human environment and health--aims to trigger further research on this subject.
Wooles, Ashley J; Mills, David P; Tuna, Floriana; McInnes, Eric J L; Law, Gareth T W; Fuller, Adam J; Kremer, Felipe; Ridgway, Mark; Lewis, William; Gagliardi, Laura; Vlaisavljevich, Bess; Liddle, Stephen T
2018-05-29
Despite the fact that non-aqueous uranium chemistry is over 60 years old, most polarised-covalent uranium-element multiple bonds involve formal uranium oxidation states IV, V, and VI. The paucity of uranium(III) congeners is because, in common with metal-ligand multiple bonding generally, such linkages involve strongly donating, charge-loaded ligands that bind best to electron-poor metals and inherently promote disproportionation of uranium(III). Here, we report the synthesis of hexauranium-methanediide nanometre-scale rings. Combined experimental and computational studies suggest overall the presence of formal uranium(III) and (IV) ions, though electron delocalisation in this Kramers system cannot be definitively ruled out, and the resulting polarised-covalent U = C bonds are supported by iodide and δ-bonded arene bridges. The arenes provide reservoirs that accommodate charge, thus avoiding inter-electronic repulsion that would destabilise these low oxidation state metal-ligand multiple bonds. Using arenes as electronic buffers could constitute a general synthetic strategy by which to stabilise otherwise inherently unstable metal-ligand linkages.
National Uranium Resource Evaluation: Durango Quadrangle, Colorado
DOE Office of Scientific and Technical Information (OSTI.GOV)
Theis, N.J.; Madson, M.E.; Rosenlund, G.C.
1981-06-01
The Durango Quadrangle (2/sup 0/), Colorado, was evaluated using National Uranium Resource Evaluation criteria to determine environments favorable for uranium deposits. General reconnaissance, geologic and radiometric investigations, was augmented by detailed surface examination and radiometric and geochemical studies in selected areas. Eight areas favorable for uranium deposits were delineated. Favorable geologic environments include roscoelite-type vanadium-uranium deposits in the Placerville and Barlow Creek-Hermosa Creek districts, sandstone uranium deposits along Hermosa Creek, and vein uranium deposits in the Precambrian rocks of the Needle Mountains area and in the Paleozoic rocks of the Tuckerville and Piedra River Canyon areas. The major portions ofmore » the San Juan volcanic field, the San Juan Basin, and the San Luis Basin within the quadrangle were judged unfavorable. Due to lack of information, the roscoelite belt below 1000 ft (300 m), the Eolus Granite below 0.5 mi (0.8 km), and the Lake City caldera are unevaluated. The Precambrian Y melasyenite of Ute Creek and the Animas Formation within the Southern Ute Indian Reservation are unevaluated due to lack of access.« less
McGuinness, Lora R.; Wilkins, Michael J.; Williams, Kenneth H.; Long, Philip E.; Kerkhof, Lee J.
2015-01-01
Understanding which organisms are capable of reducing uranium at historically contaminated sites provides crucial information needed to evaluate treatment options and outcomes. One approach is determination of the bacteria which directly respond to uranium addition. In this study, uranium amendments were made to groundwater samples from a site of ongoing biostimulation with acetate. The active microbes in the planktonic phase were deduced by monitoring ribosomes production via RT-PCR. The results indicated several microorganisms were synthesizing ribosomes in proportion with uranium amendment up to 2 μM. Concentrations of U (VI) >2 μM were generally found to inhibit ribosome synthesis. Two active bacteria responding to uranium addition in the field were close relatives of Desulfobacter postgateii and Geobacter bemidjiensis. Since RNA content often increases with growth rate, our findings suggest it is possible to rapidly elucidate active bacteria responding to the addition of uranium in field samples and provides a more targeted approach to stimulate specific populations to enhance radionuclide reduction in contaminated sites. PMID:26382047
Preliminary study of favorability for uranium resources in Juab County, Utah
DOE Office of Scientific and Technical Information (OSTI.GOV)
Leedom, S.H.; Mitchell, T.P.
1978-02-01
The best potential for large, low-grade uranium deposits in Juab County is in the hydrothermally altered vitric tuffs of Pliocene age. The lateral extent of the altered tuffs may be determined by subsurface studies around the perimeter of the volcanic centers in the Thomas Range and the Honeycomb Hills. Because the ring-fracture zone associated with collapse of the Thomas caldera was a major control for hydrothermal uranium deposits, delineation of the northern and eastern positions of the ring-fracture zone is critical in defining favorable areas for uranium deposits. A small, medium-grade ore deposit in tuffaceous sand of Pliocene age atmore » the Yellow Chief mine in Dugway Dell is unique in origin, and the probability of discovering another deposit of this type is low. A deposit of this type may be present under alluvial cover in the northwestern Drum Mountains along the southern extension of the ring-fracture zone of the Thomas caldera. Festoonlike iron oxide structures and uranium deposition within permeable sandstone horizons indicate that the Yellow Chief deposit was formed by recent ground-water circulation. Granitic intrusive rocks in the Deep Creek Range and in Desert Mountain contain isolated epigenetic vein-type deposits. These rocks could be a source of arkosic sediments buried in adjacent valleys. The Pleistocene lacustrine sediments and playa lake brines may contain concentrations of uranium leached from uranium-rich rocks.« less
Estimation and mapping of uranium content of geological units in France.
Ielsch, G; Cuney, M; Buscail, F; Rossi, F; Leon, A; Cushing, M E
2017-01-01
In France, natural radiation accounts for most of the population exposure to ionizing radiation. The Institute for Radiological Protection and Nuclear Safety (IRSN) carries out studies to evaluate the variability of natural radioactivity over the French territory. In this framework, the present study consisted in the evaluation of uranium concentrations in bedrocks. The objective was to provide estimate of uranium content of each geological unit defined in the geological map of France (1:1,000,000). The methodology was based on the interpretation of existing geochemical data (results of whole rock sample analysis) and the knowledge of petrology and lithology of the geological units, which allowed obtaining a first estimate of the uranium content of rocks. Then, this first estimate was improved thanks to some additional information. For example, some particular or regional sedimentary rocks which could present uranium contents higher than those generally observed for these lithologies, were identified. Moreover, databases on mining provided information on the location of uranium and coal/lignite mines and thus indicated the location of particular uranium-rich rocks. The geological units, defined from their boundaries extracted from the geological map of France (1:1,000,000), were finally classified into 5 categories based on their mean uranium content. The map obtained provided useful data for establishing the geogenic radon map of France, but also for mapping countrywide exposure to terrestrial radiation and for the evaluation of background levels of natural radioactivity used for impact assessment of anthropogenic activities. Copyright © 2016 Elsevier Ltd. All rights reserved.
Environmental and taxonomic bacterial diversity of anaerobic uranium(IV) bio-oxidation.
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.
Moure-Eraso, R
1999-01-01
This article evaluates how an observational epidemiologic study of federal agencies in uranium miners became an experiment of opportunity for radiation effects. Navajo miners and communities suffered environmental exposures caused by the practices of uranium mining and milling in the Navajo reservation during the 1947 to 1966 period. A historical review of the state-of-the-art knowledge of the health effects of uranium mining and milling during the years prior to 1947 was conducted. Contemporary prevention and remediation practices also were assessed. An appraisal of the summary of findings of a comprehensive evaluation of radiation human experimentation conducted by the U.S. federal government in 1995-96 (ACHRE) demonstrates that uranium miners, including Navajo miners, were the single group that was put more seriously at risk of harm from radiation exposures, with inadequate disclosure and often with fatal consequences. Uranium miners were unwilling and unaware victims of human experimentation to evaluate the health effects of radiation. The failure of the State and U.S. Governments to issue regulations or demand installation of known mine-dust exposure control measures caused widespread environmental damage in the Navajo Nation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Castor, S.B.; Berry, M.R.; Robins, J.W.
1977-11-01
This study delineates favorable areas for uranium resources in northeastern Washington and northern Idaho by identifying granitic rocks with relatively large amounts of uranium and (or) thorium. Results are based on analysis of 344 rock samples. Uranium analyses obtained by gamma-ray spectrometric data correlate closely with fluorometric determinations. On the basis of cumulative frequency distribution curves, more than 8 ppM equivalent uranium and more than 20 ppM equivalent thorium are considered anomalous for granitic rocks in northeastern Washington and northern Idaho. Granitic rocks anomalously high in uranium and (or) thorium are concentrated in two northeast-trending belts. The most prominent, themore » Midnite-Hall Mountain belt, includes the Midnite and Sherwood uranium mines, and two lesser but productive areas farther north. This belt follows the contact between Precambrian and Paleozoic rocks, which is also the locus of the Kootenai arc fold belt. The second belt of anomalously radioactive granitic rocks is along the Republic graben, a prominent linear structure in an area with no recorded uranium production. Anomalously radioactive granitic rocks are generally massive quartz monzonite, alaskite, or pegmatite, which contain abundant quartz and potash feldspar. They are also characterized by pink potash feldspar, commonly as large phenocrysts, and by the presence of muscovite. Several uranium and thorium minerals have been identified in these rocks. The two belts of anomalously radioactive plutons are considered favorable for uranium resources. Deposits could occur in the intrusive rocks themselves or in favorable environments in adjacent rocks. 13 figs., 2 tables.« less
SUMMARY REPORT ON THE STUDY OF BETA TREATMENT OF URANIUM
DOE Office of Scientific and Technical Information (OSTI.GOV)
Russell, R.B.; Wolff, A.K.
A study was made on the effects of beta treatment variables on the texture, grain size, and distortion in unalloyed dingot and ingot uranium. The effects of delta heat treatment, various cooling regimes, recrystallization, etc., were studied. (D.L.C.)
Li, W B; Karpas, Z; Salonen, L; Kurttio, P; Muikku, M; Wahl, W; Höllriegl, V; Hoeschen, C; Oeh, U
2009-06-01
To predict uranium in human hair due to chronic exposure through drinking water, a compartment representing human hair was added into the uranium biokinetic model developed by the International Commission on Radiological Protection (ICRP). The hair compartmental model was used to predict uranium excretion in human hair as a bioassay indicator due to elevated uranium intakes. Two excretion pathways, one starting from the compartment of plasma and the other from the compartment of intermediate turnover soft tissue, are assumed to transfer uranium to the compartment of hair. The transfer rate was determined from reported uranium contents in urine and in hair, taking into account the hair growth rate of 0.1 g d(-1). The fractional absorption in the gastrointestinal tract of 0.6% was found to fit best to describe the measured uranium levels among the users of drilled wells in Finland. The ingestion dose coefficient for (238)U, which includes its progeny of (234)Th, (234m)Pa, and (234)Pa, was calculated equal to 1.3 x 10(-8) Sv Bq(-1) according to the hair compartmental model. This estimate is smaller than the value of 4.5 x 10(-8) Sv Bq(-1) published by ICRP for the members of the public. In this new model, excretion of uranium through urine is better represented when excretion to the hair compartment is accounted for and hair analysis can provide a means for assessing the internal body burden of uranium. The model is applicable for chronic exposure as well as for an acute exposure incident. In the latter case, the hair sample can be collected and analyzed even several days after the incident, whereas urinalysis requires sample collection shortly after the exposure. The model developed in this study applies to ingestion intakes of uranium.
40 CFR 421.320 - Applicability: Description of the secondary uranium subcategory.
Code of Federal Regulations, 2012 CFR
2012-07-01
... secondary uranium subcategory. 421.320 Section 421.320 Protection of Environment ENVIRONMENTAL PROTECTION... CATEGORY Secondary Uranium Subcategory § 421.320 Applicability: Description of the secondary uranium... uranium (including depleted uranium) by secondary uranium facilities. ...
40 CFR 421.320 - Applicability: Description of the secondary uranium subcategory.
Code of Federal Regulations, 2011 CFR
2011-07-01
... secondary uranium subcategory. 421.320 Section 421.320 Protection of Environment ENVIRONMENTAL PROTECTION... CATEGORY Secondary Uranium Subcategory § 421.320 Applicability: Description of the secondary uranium... uranium (including depleted uranium) by secondary uranium facilities. ...
40 CFR 421.320 - Applicability: Description of the secondary uranium subcategory.
Code of Federal Regulations, 2013 CFR
2013-07-01
... secondary uranium subcategory. 421.320 Section 421.320 Protection of Environment ENVIRONMENTAL PROTECTION... CATEGORY Secondary Uranium Subcategory § 421.320 Applicability: Description of the secondary uranium... uranium (including depleted uranium) by secondary uranium facilities. ...
40 CFR 421.320 - Applicability: Description of the secondary uranium subcategory.
Code of Federal Regulations, 2014 CFR
2014-07-01
... secondary uranium subcategory. 421.320 Section 421.320 Protection of Environment ENVIRONMENTAL PROTECTION... CATEGORY Secondary Uranium Subcategory § 421.320 Applicability: Description of the secondary uranium... uranium (including depleted uranium) by secondary uranium facilities. ...
40 CFR 421.320 - Applicability: Description of the secondary uranium subcategory.
Code of Federal Regulations, 2010 CFR
2010-07-01
... secondary uranium subcategory. 421.320 Section 421.320 Protection of Environment ENVIRONMENTAL PROTECTION... CATEGORY Secondary Uranium Subcategory § 421.320 Applicability: Description of the secondary uranium... uranium (including depleted uranium) by secondary uranium facilities. ...
Bioremediation of uranium contamination with enzymatic uranium reduction
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.
Spagnul, Aurélie; Bouvier-Capely, Céline; Phan, Guillaume; Rebière, François; Fattal, Elias
2010-09-01
Cutaneous contamination represents the second highest contamination pathway in the nuclear industry. Despite that the entry of actinides such as uranium into the body through intact or wounded skin can induce a high internal exposure, no specific emergency treatment for cutaneous contamination exists. In the present work, an innovative formulation dedicated to uranium skin decontamination was developed. The galenic form consists in an oil-in-water nanoemulsion, which contains a tricarboxylic calixarene known for its high uranium affinity and selectivity. The physicochemical characterization of this topical form revealed that calixarene molecules are located at the surface of the dispersed oil droplets of the nanoemulsion, being thus potentially available for uranium chelation. It was demonstrated in preliminary in vitro experiments by using an adapted ultrafiltration method that the calixarene nanoemulsion was able to extract and retain more than 80% of uranium from an aqueous uranyl nitrate contamination solution. First ex vivo experiments carried out in Franz diffusion cells on pig ear skin explants during 24 h showed that the immediate application of the calixarene nanoemulsion on a skin contaminated by a uranyl nitrate solution allowed a uranium transcutaneous diffusion decrease of about 98% through intact and excoriated skins. The calixarene nanoemulsion developed in this study thus seems to be an efficient emergency system for uranium skin decontamination.
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.
Preliminary study on weapon grade uranium utilization in molten salt reactor miniFUJI
DOE Office of Scientific and Technical Information (OSTI.GOV)
Aji, Indarta Kuncoro; Waris, A., E-mail: awaris@fi.itb.ac.id
Preliminary study on weapon grade uranium utilization in 25MWth and 50MWth of miniFUJI MSR (molten salt reactor) has been carried out. In this study, a very high enriched uranium that we called weapon grade uranium has been employed in UF{sub 4} composition. The {sup 235}U enrichment is 90 - 95 %. The results show that the 25MWth miniFUJI MSR can get its criticality condition for 1.56 %, 1.76%, and 1.96% of UF{sub 4} with {sup 235}U enrichment of at least 93%, 90%, and 90%, respectively. In contrast, the 50 MWth miniFUJI reactor can be critical for 1.96% of UF{sub 4}more » with {sup 235}U enrichment of at smallest amount 95%. The neutron spectra are almost similar for each power output.« less
Module-oriented modeling of reactive transport with HYTEC
NASA Astrophysics Data System (ADS)
van der Lee, Jan; De Windt, Laurent; Lagneau, Vincent; Goblet, Patrick
2003-04-01
The paper introduces HYTEC, a coupled reactive transport code currently used for groundwater pollution studies, safety assessment of nuclear waste disposals, geochemical studies and interpretation of laboratory column experiments. Based on a known permeability field, HYTEC evaluates the groundwater flow paths, and simulates the migration of mobile matter (ions, organics, colloids) subject to geochemical reactions. The code forms part of a module-oriented structure which facilitates maintenance and improves coding flexibility. In particular, using the geochemical module CHESS as a common denominator for several reactive transport models significantly facilitates the development of new geochemical features which become automatically available to all models. A first example shows how the model can be used to assess migration of uranium from a sub-surface source under the effect of an oxidation front. The model also accounts for alteration of hydrodynamic parameters (local porosity, permeability) due to precipitation and dissolution of mineral phases, which potentially modifies the migration properties in general. The second example illustrates this feature.
Release behavior of uranium in uranium mill tailings under environmental conditions.
Liu, Bo; Peng, Tongjiang; Sun, Hongjuan; Yue, Huanjuan
2017-05-01
Uranium contamination is observed in sedimentary geochemical environments, but the geochemical and mineralogical processes that control uranium release from sediment are not fully appreciated. Identification of how sediments and water influence the release and migration of uranium is critical to improve the prevention of uranium contamination in soil and groundwater. To understand the process of uranium release and migration from uranium mill tailings under water chemistry conditions, uranium mill tailing samples from northwest China were investigated with batch leaching experiments. Results showed that water played an important role in uranium release from the tailing minerals. The uranium release was clearly influenced by contact time, liquid-solid ratio, particle size, and pH under water chemistry conditions. Longer contact time, higher liquid content, and extreme pH were all not conducive to the stabilization of uranium and accelerated the uranium release from the tailing mineral to the solution. The values of pH were found to significantly influence the extent and mechanisms of uranium release from minerals to water. Uranium release was monitored by a number of interactive processes, including dissolution of uranium-bearing minerals, uranium desorption from mineral surfaces, and formation of aqueous uranium complexes. Considering the impact of contact time, liquid-solid ratio, particle size, and pH on uranium release from uranium mill tailings, reducing the water content, decreasing the porosity of tailing dumps and controlling the pH of tailings were the key factors for prevention and management of environmental pollution in areas near uranium mines. Copyright © 2017 Elsevier Ltd. All rights reserved.
Bills, Donald J.; Brown, Kristin M.; Alpine, Andrea E.; Otton, James K.; Van Gosen, Bradley S.; Hinck, Jo Ellen; Tillman, Fred D.
2011-01-01
About 1 million acres of Federal land in the Grand Canyon region of Arizona were temporarily withdrawn from new mining claims in July 2009 by the Secretary of the Interior because of concern that increased uranium mining could have negative impacts on the land, water, people, and wildlife. During a 2-year interval, a Federal team led by the Bureau of Land Management is evaluating the effects of withdrawing these lands for extended periods. As part of this team, the U.S. Geological Survey (USGS) conducted a series of short-term studies to examine the historical effects of breccia-pipe uranium mining in the region. The USGS studies provide estimates of uranium resources affected by the possible land withdrawal, examine the effects of previous breccia-pipe mining, summarize water-chemistry data for streams and springs, and investigate potential biological pathways of exposure to uranium and associated contaminants. This fact sheet summarizes results through December 2009 and outlines further research needs.
NASA Astrophysics Data System (ADS)
Thomson, Robert K.; Cantat, Thibault; Scott, Brian L.; Morris, David E.; Batista, Enrique R.; Kiplinger, Jaqueline L.
2010-09-01
Uranium nitride [U≡N]x is an alternative nuclear fuel that has great potential in the expanding future of nuclear power; however, very little is known about the U≡N functionality. We show, for the first time, that a terminal uranium nitride complex can be generated by photolysis of an azide (U-N=N=N) precursor. The transient U≡N fragment is reactive and undergoes insertion into a ligand C-H bond to generate new N-H and N-C bonds. The mechanism of this unprecedented reaction has been evaluated through computational and spectroscopic studies, which reveal that the photochemical azide activation pathway can be shut down through coordination of the terminal azide ligand to the Lewis acid B(C6F5)3. These studies demonstrate that photochemistry can be a powerful tool for inducing redox transformations for organometallic actinide complexes, and that the terminal uranium nitride fragment is reactive, cleaving strong C-H bonds.
Development of Novel Sorbents for Uranium Extraction from Seawater
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lin, Wenbin; Taylor-Pashow, Kathryn
2014-01-08
As the uranium resource in terrestrial ores is limited, it is difficult to ensure a long-term sustainable nuclear energy technology. The oceans contain approximately 4.5 billion tons of uranium, which is one thousand times the amount of uranium in terrestrial ores. Development of technologies to recover the uranium from seawater would greatly improve the uranium resource availability, sustaining the fuel supply for nuclear energy. Several methods have been previously evaluated including solvent extraction, ion exchange, flotation, biomass collection, and adsorption; however, none have been found to be suitable for reasons such as cost effectiveness, long term stability, and selectivity. Recentmore » research has focused on the amidoxime functional group as a promising candidate for uranium sorption. Polymer beads and fibers have been functionalized with amidoxime functional groups, and uranium adsorption capacities as high as 1.5 g U/kg adsorbent have recently been reported with these types of materials. As uranium concentration in seawater is only ~3 ppb, great improvements to uranium collection systems must be made in order to make uranium extraction from seawater economically feasible. This proposed research intends to develop transformative technologies for economic uranium extraction from seawater. The Lin group will design advanced porous supports by taking advantage of recent breakthroughs in nanoscience and nanotechnology and incorporate high densities of well-designed chelators into such nanoporous supports to allow selective and efficient binding of uranyl ions from seawater. Several classes of nanoporous materials, including mesoporous silica nanoparticles (MSNs), mesoporous carbon nanoparticles (MCNs), meta-organic frameworks (MOFs), and covalent-organic frameworks (COFs), will be synthesized. Selective uranium-binding liagnds such as amidoxime will be incorporated into the nanoporous materials to afford a new generation of sorbent materials that will be evaluated for their uranium extraction efficiency. The initial testing of these materials for uranium binding will be carried out in the Lin group, but more detailed sorption studies will be carried out by Dr. Taylor-Pashow of Savannah River National Laboratory in order to obtain quantitative uranyl sorption selectivity and kinetics data for the proposed materials. The proposed nanostructured sorbent materials are expected to have higher binding capacities, enhanced extraction kinetics, optimal stripping efficiency for uranyl ions, and enhanced mechanical and chemical stabilities. This transformative research will significantly impact uranium extraction from seawater as well as benefit DOE’s efforts on environmental remediation by developing new materials and providing knowledge for enriching and sequestering ultralow concentrations of other metals.« less
Capstone Depleted Uranium Aerosols: Generation and Characterization
DOE Office of Scientific and Technical Information (OSTI.GOV)
Parkhurst, MaryAnn; Szrom, Fran; Guilmette, Ray
2004-10-19
In a study designed to provide an improved scientific basis for assessing possible health effects from inhaling depleted uranium (DU) aerosols, a series of DU penetrators was fired at an Abrams tank and a Bradley fighting vehicle. A robust sampling system was designed to collect aerosols in this difficult environment and continuously monitor the sampler flow rates. Aerosols collected were analyzed for uranium concentration and particle size distribution as a function of time. They were also analyzed for uranium oxide phases, particle morphology, and dissolution in vitro. The resulting data provide input useful in human health risk assessments.
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.
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
The mechanism of uranium biosorption by Rhizopus arrhizus
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tsezos, M.; Volesky, B.
1982-02-01
Biosorption of elements is a little understood phenomenon exhibited by some types of even nonliving microbial biomass. A common fungus Rhizopus arrhizus has been reportd to take up uranium from adqueous solutions to the extent of 180 mg U/sup 6 +//g. The mechanism of uranium sequestering by this type of biomass was studied by using experimental techniques such as electron microscopy, x-ray energy dispersion analysis, IR spectroscopy, and supporting evidence was obtained for a biosorption mechanism consisting of at least three processes. Uranium coordination and adsorption in the cell-wall chitin structure occur simultaneously and rapidly whereas precipitation of uranylhdroxide withinmore » the chitin microcrystalline cell-wall structure takes place at a lower rate. Interference of Fe/sup 2/ and Zn/sup 2 +/ coions with uranium biosorption is indicated.« less
28 CFR 79.43 - Proof of employment as a miner.
Code of Federal Regulations, 2011 CFR
2011-07-01
... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942...) Records of federally supported, health-related studies of uranium workers, including: (i) Studies conducted by Geno Saccamanno, M.D., St. Mary's Hospital, Grand Junction, Colorado; and (ii) Studies...
28 CFR 79.43 - Proof of employment as a miner.
Code of Federal Regulations, 2014 CFR
2014-07-01
... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942...) Records of federally supported, health-related studies of uranium workers, including: (i) Studies conducted by Geno Saccamanno, M.D., St. Mary's Hospital, Grand Junction, Colorado; and (ii) Studies...
28 CFR 79.43 - Proof of employment as a miner.
Code of Federal Regulations, 2012 CFR
2012-07-01
... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942...) Records of federally supported, health-related studies of uranium workers, including: (i) Studies conducted by Geno Saccamanno, M.D., St. Mary's Hospital, Grand Junction, Colorado; and (ii) Studies...
28 CFR 79.43 - Proof of employment as a miner.
Code of Federal Regulations, 2013 CFR
2013-07-01
... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942...) Records of federally supported, health-related studies of uranium workers, including: (i) Studies conducted by Geno Saccamanno, M.D., St. Mary's Hospital, Grand Junction, Colorado; and (ii) Studies...
28 CFR 79.43 - Proof of employment as a miner.
Code of Federal Regulations, 2010 CFR
2010-07-01
... Service (PHS) in the course of any health studies of uranium workers during or including the period 1942...) Records of federally supported, health-related studies of uranium workers, including: (i) Studies conducted by Geno Saccamanno, M.D., St. Mary's Hospital, Grand Junction, Colorado; and (ii) Studies...
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
Metallogenic evolution of uranium deposits in the Middle East and North Africa deposits
NASA Astrophysics Data System (ADS)
Howari, Fares; Goodell, Philip; Salman, Abdulaty
2016-02-01
This paper is briefly involved in classification and distributions of the Middle East and North Africa (MENA) uranium deposits. The study of these mineral systems can significantly contribute to our further understanding of the metallogeny of known and poorly explored deposits. This provides contribution to, and further enhancement of, current classifications and metallogenic models of uranium systems, allowing researchers to emphasize on unknown or poorly studied mineral systems found in MENA. The present study identified eight metallogenic types of uranium associated with: 1) the Archean rocks and intra-cratonic basins, 2) the Pan-African granites and rhyolites which are characterized by igneous activity, 3) Phanerozoic (Paleozoic) clastics, these deposits are the sedimentological response to Pan African magmatism, 4) Mesozoic (basal) clastics type e.g. Nubia sandstones which are characterized by uranium minerals, 5) regional sedimentary phosphate deposits which are categorized as geosynclinal, or continental margin deposits, on the shelf of the Tethys Ocean, 6) Cenozoic Intracratonic Felsic Magmatism of the Tibesti and Hoggar, and the sandstone U deposits of adjoining Niger. These are similar to the Pan-African magmatism metallogenic, 7) Calcretes, and 8) Resistate minerals which are often enriched in rare earth elements, sometimes including uranium. They are thus sometimes considered as U resources but poorly explored in the MENA region. These metallogenic types are described and discussed in the current paper.
NASA Astrophysics Data System (ADS)
Krawczyk-Bärsch, Evelyn; Lünsdorf, Heinrich; Pedersen, Karsten; Arnold, Thuro; Bok, Frank; Steudtner, Robin; Lehtinen, Anne; Brendler, Vinzenz
2012-11-01
In an underground rock characterization facility, the ONKALO tunnel in Finland, massive 5-10-mm thick biofilms were observed attached to tunnel walls where groundwater was seeping from bedrock fractures at a depth of 70 m. In laboratory experiments performed in a flow cell with detached biofilms to study the effect of uranium on the biofilm, uranium was added to the circulating groundwater (CGW) obtained from the fracture feeding the biofilm. The final uranium concentration in the CGW was adjusted to 4.25 × 10-5 M, in the range expected from a leaking spent nuclear fuel (SNF) canister in a future underground repository. The effects were investigated using microelectrodes to measure pH and Eh, time-resolved laser fluorescence spectroscopy (TRLFS), energy-filtered transmission electron microscopy (EF-TEM), and electron energy-loss spectroscopy (EELS) studies and thermodynamic calculations were utilized as well. The results indicated that the studied biofilms constituted their own microenvironments, which differed significantly from that of the CGW. A pH of 5.37 was recorded inside the biofilm, approximately 3.5 units lower than the pH observed in the CGW, due to sulfide oxidation to sulfuric acid in the biofilm. Similarly, the Eh of +73 mV inside the biofilm was approximately 420 mV lower than the Eh measured in the CGW. Adding uranium increased the pH in the biofilm to 7.27 and reduced the Eh to -164 mV. The changes of Eh and pH influenced the bioavailability of uranium, since microbial metabolic processes are sensitive to metals and their speciation. EF-TEM investigations indicated that uranium in the biofilm was immobilized intracellularly in microorganisms by the formation of metabolically mediated uranyl phosphate, similar to needle-shaped autunite (Ca[UO2]2[PO4]2·2-6H2O) or meta-autunite (Ca[UO2]2[PO4]2·10-12H2O). In contrast, TRLFS studies of the contaminated CGW identified aqueous uranium carbonate species, likely (Ca2UO2[CO3]3), formed due to the high concentration of carbonate in the CGW. The results agreed with thermodynamic calculations of the theoretically predominant field of uranium species, formed in the uranium-contaminated CGW at the measured geochemical parameters. This investigation clearly demonstrated that biological systems must be considered as a part of natural systems that can significantly influence radionuclide behavior. The results improve our understanding of the mechanisms of biofilm response to radionuclides in relation to safety assessments of SNF repositories.
,
1948-01-01
The accompanying map and sections show examples of the present state of information about the occurrence of the "Leached" uranium-bearing bed in the Florida pebble phosphate district. The dashed lines on the map define, as closely as present data permit, the limit of the area in which this bed contains significant amounts of uranium. The figures next to localities on the map indicate first, the thickness of the bed in feet; and second the uranium content in thousandths of percent. For example, the figures 16-10 next to the TVA localities in Secs. 9 and 10, T. 32 S., R. 26 E. indicate 16 feet at 0.010 percent uranium. A "0" by a locality indicates either that the uranium content is less than 0.001 percent or less than the concentration in the underlying phosphate beds (matrix of the miners) or that the leached bed is not present.
Atomic-scale Studies of Uranium Oxidation and Corrosion by Water Vapour.
Martin, T L; Coe, C; Bagot, P A J; Morrall, P; Smith, G D W; Scott, T; Moody, M P
2016-07-12
Understanding the corrosion of uranium is important for its safe, long-term storage. Uranium metal corrodes rapidly in air, but the exact mechanism remains subject to debate. Atom Probe Tomography was used to investigate the surface microstructure of metallic depleted uranium specimens following polishing and exposure to moist air. A complex, corrugated metal-oxide interface was observed, with approximately 60 at.% oxygen content within the oxide. Interestingly, a very thin (~5 nm) interfacial layer of uranium hydride was observed at the oxide-metal interface. Exposure to deuterated water vapour produced an equivalent deuteride signal at the metal-oxide interface, confirming the hydride as originating via the water vapour oxidation mechanism. Hydroxide ions were detected uniformly throughout the oxide, yet showed reduced prominence at the metal interface. These results support a proposed mechanism for the oxidation of uranium in water vapour environments where the transport of hydroxyl species and the formation of hydride are key to understanding the observed behaviour.
Atomic-scale Studies of Uranium Oxidation and Corrosion by Water Vapour
NASA Astrophysics Data System (ADS)
Martin, T. L.; Coe, C.; Bagot, P. A. J.; Morrall, P.; Smith, G. D. W.; Scott, T.; Moody, M. P.
2016-07-01
Understanding the corrosion of uranium is important for its safe, long-term storage. Uranium metal corrodes rapidly in air, but the exact mechanism remains subject to debate. Atom Probe Tomography was used to investigate the surface microstructure of metallic depleted uranium specimens following polishing and exposure to moist air. A complex, corrugated metal-oxide interface was observed, with approximately 60 at.% oxygen content within the oxide. Interestingly, a very thin (~5 nm) interfacial layer of uranium hydride was observed at the oxide-metal interface. Exposure to deuterated water vapour produced an equivalent deuteride signal at the metal-oxide interface, confirming the hydride as originating via the water vapour oxidation mechanism. Hydroxide ions were detected uniformly throughout the oxide, yet showed reduced prominence at the metal interface. These results support a proposed mechanism for the oxidation of uranium in water vapour environments where the transport of hydroxyl species and the formation of hydride are key to understanding the observed behaviour.
Identifying anthropogenic uranium compounds using soft X-ray near-edge absorption spectroscopy
NASA Astrophysics Data System (ADS)
Ward, Jesse D.; Bowden, Mark; Tom Resch, C.; Eiden, Gregory C.; Pemmaraju, C. D.; Prendergast, David; Duffin, Andrew M.
2017-01-01
Uranium ores mined for industrial use are typically acid-leached to produce yellowcake and then converted into uranium halides for enrichment and purification. These anthropogenic chemical forms of uranium are distinct from their mineral counterparts. The purpose of this study is to use soft X-ray absorption spectroscopy to characterize several common anthropogenic uranium compounds important to the nuclear fuel cycle. Chemical analyses of these compounds are important for process and environmental monitoring. X-ray absorption techniques have several advantages in this regard, including element-specificity, chemical sensitivity, and high spectral resolution. Oxygen K-edge spectra were collected for uranyl nitrate, uranyl fluoride, and uranyl chloride, and fluorine K-edge spectra were collected for uranyl fluoride and uranium tetrafluoride. Interpretation of the data is aided by comparisons to calculated spectra. The effect of hydration state on the sample, a potential complication in interpreting oxygen K-edge spectra, is discussed. These compounds have unique spectral signatures that can be used to identify unknown samples.
Kocher, Elizabeth; Rendon, Kristi J; Kesler, Denece; Boyce, Tawny Wilson; Myers, Orrin; Evans, Kandace; Cook, Linda S; Sood, Akshay
2016-01-01
There is a paucity of literature on the chest radiographic findings in uranium workers. To characterize the chest radiographic findings of pneumoconiosis in a New Mexican cohort of uranium workers. The most recent results from chest radiographs were abstracted in this cross-sectional study. Radiographs showed small pneumoconiotic opacities of profusion score of ≥ 1/0 in 155/429 (36.1%) uranium workers. The most common shape/size of the primary and secondary opacities was s (90.3%) and t (83.7%) types, respectively. Lower lung zones were the most affected. American Indians were the population group at greatest odds for having profusion score ≥ 1/0 (O.R. 2.65, 95% C.I. 1.61, 4.36). Uranium workers' pneumoconiosis is associated with predominantly lower lobe, irregular, and small opacities. Clinical providers and policymakers must consider uranium workers' pneumoconiosis in the differential diagnosis for lower lobe-predominant interstitial lung disease, in the appropriate exposure setting.
Atomic-scale Studies of Uranium Oxidation and Corrosion by Water Vapour
Martin, T. L.; Coe, C.; Bagot, P. A. J.; Morrall, P.; Smith, G. D. W; Scott, T.; Moody, M. P.
2016-01-01
Understanding the corrosion of uranium is important for its safe, long-term storage. Uranium metal corrodes rapidly in air, but the exact mechanism remains subject to debate. Atom Probe Tomography was used to investigate the surface microstructure of metallic depleted uranium specimens following polishing and exposure to moist air. A complex, corrugated metal-oxide interface was observed, with approximately 60 at.% oxygen content within the oxide. Interestingly, a very thin (~5 nm) interfacial layer of uranium hydride was observed at the oxide-metal interface. Exposure to deuterated water vapour produced an equivalent deuteride signal at the metal-oxide interface, confirming the hydride as originating via the water vapour oxidation mechanism. Hydroxide ions were detected uniformly throughout the oxide, yet showed reduced prominence at the metal interface. These results support a proposed mechanism for the oxidation of uranium in water vapour environments where the transport of hydroxyl species and the formation of hydride are key to understanding the observed behaviour. PMID:27403638
Heat-induced redistribution of surface oxide in uranium
NASA Astrophysics Data System (ADS)
Swissa, Eli; Shamir, Noah; Mintz, Moshe H.; Bloch, Joseph
1990-09-01
The redistribution of oxygen and uranium metal at the vicinity of the metal-oxide interface of native and grown oxides due to vacuum thermal annealing was studied for uranium and uranium-chromium alloy using Auger depth profiling and metallographic techniques. It was found that uranium metal is segregating out through the uranium oxide layer for annealing temperatures above 450°C. At the same time the oxide is redistributed in the metal below the oxide-metal interface in a diffusion like process. By applying a diffusion equation of a finite source, the diffusion coefficients for the process were obtained from the oxygen depth profiles measured for different annealing times. An Arrhenius like behavior was found for the diffusion coefficient between 400 and 800°C. The activation energy obtained was Ea = 15.4 ± 1.9 kcal/mole and the pre-exponential factor, D0 = 1.1 × 10 -8cm2/ s. An internal oxidation mechanism is proposed to explain the results.
PRODUCTION OF URANIUM METAL BY CARBON REDUCTION
Holden, R.B.; Powers, R.M.; Blaber, O.J.
1959-09-22
The preparation of uranium metal by the carbon reduction of an oxide of uranium is described. In a preferred embodiment of the invention a charge composed of carbon and uranium oxide is heated to a solid mass after which it is further heated under vacuum to a temperature of about 2000 deg C to produce a fused uranium metal. Slowly ccoling the fused mass produces a dendritic structure of uranium carbide in uranium metal. Reacting the solidified charge with deionized water hydrolyzes the uranium carbide to finely divide uranium dioxide which can be separated from the coarser uranium metal by ordinary filtration methods.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gill, Gary A.; Kuo, Li-Jung; Strivens, Jonathan E.
2015-12-01
The Fuel Resources Program at the U.S. Department of Energy’s (DOE), Office of Nuclear Energy (DOE-NE) is developing adsorbent technology to extract uranium from seawater. This technology is being developed to provide a sustainable and economically viable supply of uranium fuel for nuclear reactors (DOE, 2010). Among the key environmental variables to understand for adsorbent deployment in the coastal ocean is what effect flow-rates or linear velocity has on uranium adsorption capacity. The goal is to find a flow conditions that optimize uranium adsorption capacity in the shortest exposure time. Understanding these criteria will be critical in choosing a locationmore » for deployment of a marine adsorbent farm. The objective of this study was to identify at what linear velocity the adsorption kinetics for uranium extraction starts to drop off due to limitations in mass transport of uranium to the surface of the adsorbent fibers. Two independent laboratory-based experimental approaches using flow-through columns and recirculating flumes for adsorbent exposure were used to assess the effect of flow-rate (linear velocity) on the kinetic uptake of uranium on amidoxime-based polymeric adsorbent material. Time series observations over a 56 day period were conducted with flow-through columns over a 35-fold range in linear velocity from 0.29 to 10.2 cm/s, while the flume study was conducted over a narrower 11-fold range, from 0.48 to 5.52 cm/s. These ranges were specifically chosen to focus on the lower end of oceanic currents and expand above and below the linear velocity of ~ 2.5 cm/s adopted for marine testing of adsorbent material at PNNL.« less
Preliminary study of uranium favorability of the Boulder batholith, Montana
DOE Office of Scientific and Technical Information (OSTI.GOV)
Castor, S.B.; Robins, J.W.
1978-01-01
The Boulder batholith of southwestern Montana is a composite Late Cretaceous intrusive mass, mostly composed of quartz monzonite and granodiorite. This study was not restricted to the plutonic rocks; it also includes younger rocks that overlie the batholith, and older rocks that it intrudes. The Boulder batholith area has good overall potential for economic uranium deposits, because its geology is similar to that of areas that contain economic deposits elsewhere in the world, and because at least 35 uranium occurrences of several different types are present. Potential is greatest for the occurrence of small uranium deposits in chalcedony veins andmore » base-metal sulfide veins. Three areas may be favorable for large, low-grade deposits consisting of a number of closely spaced chalcedony veins and enriched wall rock; the Mooney claims, the Boulder area, and the Clancy area. In addition, there is a good possibility of by-product uranium production from phosphatic black shales in the project area. The potential for uranium deposits in breccia masses that cut prebatholith rocks, in manganese-quartz veins near Butte, and in a shear zone that cuts Tertiary rhyolite near Helena cannot be determined on the basis of available information. Low-grade, disseminated, primary uranium concentrations similar to porphyry deposits proposed by Armstrong (1974) may exist in the Boulder batholith, but the primary uranium content of most batholith rocks is low. The geologic environment adjacent to the Boulder batholith is similar in places to that at the Midnite mine in Washington. Some igneous rocks in the project area contain more than 10 ppM U/sub 3/O/sub 8/, and some metasedimentary rocks near the batholith contain reductants such as sulfides and carbonaceous material.« less
Study of Chemical Changes in Uranium Oxyfluoride Particles Progress Report March - October 2009
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kips, R; Kristo, M; Hutcheon, I
2009-11-22
Nuclear forensics relies on the analysis of certain sample characteristics to determine the origin and history of a nuclear material. In the specific case of uranium enrichment facilities, it is the release of trace amounts of uranium hexafluoride (UF{sub 6}) gas - used for the enrichment of uranium - that leaves a process-characteristic fingerprint. When UF{sub 6} gas interacts with atmospheric moisture, uranium oxyfluoride particles or particle agglomerates are formed with sizes ranging from several microns down to a few tens of nanometers. These particles are routinely collected by safeguards organizations, such as the International Atomic Energy Agency (IAEA), allowingmore » them to verify whether a facility is compliant with its declarations. Spectrometric analysis of uranium particles from UF{sub 6} hydrolysis has revealed the presence of both particles that contain fluorine, and particles that do not. It is therefore assumed that uranium oxyfluoride is unstable, and decomposes to form uranium oxide. Understanding the rate of fluorine loss in uranium oxyfluoride particles, and the parameters that control it, may therefore contribute to placing boundaries on the particle's exposure time in the environment. Expressly for the purpose of this study, we prepared a set of uranium oxyfluoride particles at the Institute for Reference Materials and Measurements (EU-JRC-IRMM) from a static release of UF{sub 6} in a humid atmosphere. The majority of the samples was stored in controlled temperature, humidity and lighting conditions. Single particles were characterized by a suite of micro-analytical techniques, including NanoSIMS, micro-Raman spectrometry (MRS), scanning (SEM) and transmission (TEM) electron microscopy, energy-dispersive X-ray spectrometry (EDX) and focused ion beam (FIB). The small particle size was found to be the main analytical challenge. The relative amount of fluorine, as well as the particle chemical composition and morphology were determined at different stages in the ageing process, and immediately after preparation. This report summarizes our most recent findings for each of the analytical techniques listed above, and provides an outlook on what remains to be resolved. Additional spectroscopic and mass spectrometric measurements were carried out at Pacific Northwest National Laboratory, but are not included in this summary.« less
Bland, D; Rona, R; Coggon, D; Anderson, J; Greenberg, N; Hull, L; Wessely, S
2007-01-01
Objectives To assess the distribution and risk factors of depleted uranium uptake in military personnel who had taken part in the invasion of Iraq in 2003. Methods Sector field inductively coupled plasma-mass spectrometry (SF-ICP-MS) was used to determine the uranium concentration and 238U/235U isotopic ratio in spot urine samples. The authors collected urine samples from four groups identified a priori as having different potential for exposure to depleted uranium. These groups were: combat personnel (n = 199); non-combat personnel (n = 96); medical personnel (n = 22); and “clean-up” personnel (n = 24) who had been involved in the maintenance, repair or clearance of potentially contaminated vehicles in Iraq. A short questionnaire was used to ascertain individual experience of circumstances in which depleted uranium exposure might have occurred. Results There was no statistically significant difference in the 238U/235U ratio between groups. Mean ratios by group varied from 138.0 (95% CI 137.3 to 138.7) for clean-up personnel to 138.2 (95% CI 138.0 to 138.5) for combat personnel, and were close to the ratio of 137.9 for natural uranium. The two highest individual ratios (146.9 and 147.7) were retested using more accurate, multiple collector inductively coupled plasma-mass spectrometry (MC-ICP-MS) and found to be within measurement of error of that for natural uranium. There were no significant differences in isotope ratio between participants according to self-reported circumstances of potential depleted uranium exposure. Conclusions Based on measurements using a SF-ICP-MS apparatus, this study provides reassurance following concern for potential widespread depleted uranium uptake in the UK military. The rare occurrence of elevated ratios may reflect the limits of accuracy of the SF-ICP-MS apparatus and not a real increase from the natural proportions of the isotopes. Any uptake of depleted uranium among participants in this study sample would be very unlikely to have any implications for health. PMID:17609224
STRIPPING OF URANIUM FROM ORGANIC EXTRACTANTS
Crouse, D.J. Jr.
1962-09-01
A liquid-liquid extraction method is given for recovering uranium values from uranium-containing solutions. Uranium is removed from a uranium-containing organic solution by contacting said organic solution with an aqueous ammonium carbonate solution substantially saturated in uranium values. A uranium- containing precipitate is thereby formed which is separated from the organic and aqueous phases. Uranium values are recovered from this separated precipitate. (AE C)
Process for electroslag refining of uranium and uranium alloys
Lewis, P.S. Jr.; Agee, W.A.; Bullock, J.S. IV; Condon, J.B.
1975-07-22
A process is described for electroslag refining of uranium and uranium alloys wherein molten uranium and uranium alloys are melted in a molten layer of a fluoride slag containing up to about 8 weight percent calcium metal. The calcium metal reduces oxides in the uranium and uranium alloys to provide them with an oxygen content of less than 100 parts per million. (auth)
Herlory, Olivier; Bonzom, Jean-Marc; Gilbin, Rodolphe
2013-09-15
Although ecotoxicological studies tend to address the toxicity thresholds of uranium in freshwaters, there is a lack of information on the effects of the metal on physiological processes, particularly in aquatic plants. Knowing that uranium alters photosynthesis via impairment of the water photo-oxidation process, we determined whether pulse amplitude modulated (PAM) fluorometry was a relevant tool for assessing the impact of uranium on the green alga Chlamydomonas reinhardtii and investigated how and to what extent uranium hampered photosynthetic performance. Photosynthetic activity and quenching were assessed from fluorescence induction curves generated by PAM fluorometry, after 1 and 5h of uranium exposure in controlled conditions. The oxygen-evolving complex (OEC) of PSII was identified as the primary action site of uranium, through alteration of the water photo-oxidation process as revealed by F0/Fv. Limiting re-oxidation of the plastoquinone pool, uranium impaired the electron flux between the photosystems until almost complete inhibition of the PSII quantum efficiency ( [Formula: see text] , EC50=303 ± 64 μg UL(-1) after 5h of exposure) was observed. Non-photochemical quenching (qN) was identified as the most sensitive fluorescence parameter (EC50=142 ± 98 μg UL(-1) after 5h of exposure), indicating that light energy not used in photochemistry was dissipated in non-radiative processes. It was shown that parameters which stemmed from fluorescence induction kinetics are valuable indicators for evaluating the impact of uranium on PSII in green algae. PAM fluorometry provided a rapid and reasonably sensitive method for assessing stress response to uranium in microalgae. Copyright © 2013 Elsevier B.V. All rights reserved.
Preliminary study of radioactive limonite localities in Colorado, Utah, and Wyoming
Lovering, T.G.; Beroni, E.P.
1956-01-01
Nine radioactive limonite localities of different types were sampled during the spring and fall of 1953 in an effort to establish criteria for differentiating limonite outcrops associated with uranium or thorium deposits from limonite outcrops not associated with such deposits. The samples were analyzed for uranium and thorium by standard chemical methods, for equivalent uranium by the radiometric method, and for a number of common metals by semiquantitative geochemical methods. Correlation coefficients were then calculated for each of the metals with respect to equivalent uranium, and to uranium where present, for all of the samples from each locality. The correlation coefficients may indicate a significant association between uranium or thorium and certain metals. Occurrences of specific that are interpreted as significant very considerably for different uranium localities but are more consistent for the thorium localities. Samples taken from radioactive outcrops in the vicinity of uranium or thorium deposits can be quickly analyzed by geochemical methods for various elements. Correlation coefficients can then be determined for the various elements with respect to uranium or thorium; if any significant correlations are obtained, the elements showing such correlation may be indicators of uranium or thorium. Soil samples of covered areas in the vicinity of the radioactive outcrop may then be analyzed for the indicator elements and any resulting anomalies used as a guide for prospecting where the depth of overburden is too great to allow the use of radiation-detecting instruments. Correlation coefficients of the associated indicator elements, used in conjunction with petrographic evidence, may also be useful in interpreting the origin and paragenesis of radioactive deposits. Changes in color of limonite stains on the outcrop may also be a useful guide to ore in some areas.
Technical Basis for Assessing Uranium Bioremediation Performance
DOE Office of Scientific and Technical Information (OSTI.GOV)
PE Long; SB Yabusaki; PD Meyer
2008-04-01
In situ bioremediation of uranium holds significant promise for effective stabilization of U(VI) from groundwater at reduced cost compared to conventional pump and treat. This promise is unlikely to be realized unless researchers and practitioners successfully predict and demonstrate the long-term effectiveness of uranium bioremediation protocols. Field research to date has focused on both proof of principle and a mechanistic level of understanding. Current practice typically involves an engineering approach using proprietary amendments that focuses mainly on monitoring U(VI) concentration for a limited time period. Given the complexity of uranium biogeochemistry and uranium secondary minerals, and the lack of documentedmore » case studies, a systematic monitoring approach using multiple performance indicators is needed. This document provides an overview of uranium bioremediation, summarizes design considerations, and identifies and prioritizes field performance indicators for the application of uranium bioremediation. The performance indicators provided as part of this document are based on current biogeochemical understanding of uranium and will enable practitioners to monitor the performance of their system and make a strong case to clients, regulators, and the public that the future performance of the system can be assured and changes in performance addressed as needed. The performance indicators established by this document and the information gained by using these indicators do add to the cost of uranium bioremediation. However, they are vital to the long-term success of the application of uranium bioremediation and provide a significant assurance that regulatory goals will be met. The document also emphasizes the need for systematic development of key information from bench scale tests and pilot scales tests prior to full-scale implementation.« less
High pressure elasticity and thermal properties of depleted uranium
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jacobsen, M. K., E-mail: mjacobsen@lanl.gov; Velisavljevic, N., E-mail: nenad@lanl.gov
2016-04-28
Studies of the phase diagram of uranium have revealed a wealth of high pressure and temperature phases. Under ambient conditions the crystal structure is well defined up to 100 gigapascals (GPa), but very little information on thermal conduction or elasticity is available over this same range. This work has applied ultrasonic interferometry to determine the elasticity, mechanical, and thermal properties of depleted uranium to 4.5 GPa. Results show general strengthening with applied load, including an overall increase in acoustic thermal conductivity. Further implications are discussed within. This work presents the first high pressure studies of the elasticity and thermal properties ofmore » depleted uranium metal and the first real-world application of a previously developed containment system for making such measurements.« less
NASA Astrophysics Data System (ADS)
Long, Zhong; Zeng, Rongguang; Hu, Yin; Liu, Jing; Wang, Wenyuan; Zhao, Yawen; Luo, Zhipeng; Bai, Bin; Wang, Xiaofang; Liu, Kezhao
2018-06-01
Oxide formation on surface of nitrogen-rich uranium nitride film/particles was investigated using X-ray photoelectron spectroscopy (XPS), auger electron spectroscopy (AES), aberration-corrected transmission electron microscopy (TEM), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) coupled with electron energy-loss spectroscopy (EELS). XPS and AES studies indicated that the oxidized layer on UN2-x film is ternary compound uranium oxynitride (UNxOy) in 5-10 nm thickness. TEM/HAADF-STEM and EELS studies revealed the UNxOy crystallizes in the FCC CaF2-type structure with the lattice parameter close to the CaF2-type UN2-x matrix. The work can provide further information to the oxidation mechanism of uranium nitride.
High pressure elasticity and thermal properties of depleted uranium
Jacobsen, M. K.; Velisavljevic, N.
2016-04-28
Studies of the phase diagram of uranium have revealed a wealth of high pressure and temperature phases. Under ambient conditions the crystal structure is well defined up to 100 gigapascals (GPa), but very little information on thermal conduction or elasticity is available over this same range. This work has applied ultrasonic interferometry to determine the elasticity, mechanical, and thermal properties of depleted uranium to 4.5 GPa. Results show general strengthening with applied load, including an overall increase in acoustic thermal conductivity. Further implications are discussed within. Lastly, this work presents the first high pressure studies of the elasticity and thermalmore » properties of depleted uranium metal and the first real-world application of a previously developed containment system for making such measurements.« less
Detection of depleted uranium in urine of veterans from the 1991 Gulf War.
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.
Groundwater uranium and cancer incidence in South Carolina
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
31 CFR 540.317 - Uranium feed; natural uranium feed.
Code of Federal Regulations, 2013 CFR
2013-07-01
... 31 Money and Finance:Treasury 3 2013-07-01 2013-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The...
31 CFR 540.317 - Uranium feed; natural uranium feed.
Code of Federal Regulations, 2012 CFR
2012-07-01
... 31 Money and Finance:Treasury 3 2012-07-01 2012-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The...
31 CFR 540.317 - Uranium feed; natural uranium feed.
Code of Federal Regulations, 2014 CFR
2014-07-01
... 31 Money and Finance:Treasury 3 2014-07-01 2014-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The...
Arsenic and uranium in private wells in Connecticut, 2013-15
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.