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Results for “Uranium Immobilization”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots

Biogeochemistry of uranium in wetlands plays important roles in U immobilization in storage ponds of U mining and processing facilities but has not been well understood. The objective of this work was to study molecular mechanisms responsible for high U retention by Savannah River Site (SRS) wetland sediments under varying redox and acidic (pH = 2.6–5.8) conditions using U L₃-edge X-ray absorption spectroscopy. Uranium in the SRS wetland sediments existed primarily as U(VI) bonded as a bidentate to carboxylic sites (U–C bond distance at ~2.88 Å), rather than phenolic or other sites of natural organic matter (NOM). In microcosms simulating the SRS wetland processes, U immobilization on roots was two orders of magnitude higher than on the adjacent brown or more distant white sands in which U was U(VI). Uranium on the roots were both U(IV) and U(VI), which were bonded as a bidentate to carbon, but the U(VI) may also form a U phosphate mineral. After 140 days of air exposure, all U(IV) was re-oxidized to U(VI) but remained as a bidentate bonding to carbon. This study demonstrated NOM and plant roots can highly immobilize U(VI) in the SRS acidic sediments, which has significant implication for the long-term stewardship of U-contaminated wetlands.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

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

Phosphate amendments can be added to U(VI)-contaminated subsurface environments to promote in situ remediation. The primary objective of this study was to evaluate the impacts of phosphate addition on the transport of U(VI) through contaminated sediments. In batch experiments using sediments (<2 mm size fraction) from a site in Rifle, Colorado, U(VI) only weakly adsorbed due to the dominance of the aqueous speciation by CaeU(VI)-carbonate complexes. Column experiments with these sediments were performed with flow rates that correspond to a groundwater velocity of 1.1 m/day. In the absence of phosphate, the sediments took up 1.68e1.98 mg U/g of sediments when the synthetic groundwater influent contained 4 mM U(VI). When U(VI)-free influents were then introduced with and without phosphate, substantially more uranium was retained within the column when phosphate was present in the influent. Sequential extractions of sediments from the columns revealed that uranium was uniformly distributed along the length of the columns and was primarily in forms that could be extracted by ion exchange and contact with a weak acid. Laser induced fluorescence spectroscopy (LIFS) analysis along with sequential extraction results suggest adsorption as the dominant uranium uptake mechanism. The response of dissolved uranium concentrations to stopped-flow events and the comparison of experimental data with simulations from a simple reactive transport model indicated that uranium adsorption to and desorption from the sediments was not always at local equilibrium.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Modeling Substrate Utilization, Metabolite Production, and Uranium Immobilization in Shewanella oneidensis Biofilms

In this study, we developed a two-dimensional mathematical model to predict substrate utilization and metabolite production rates in Shewanella oneidensis MR-1 biofilm in the presence and absence of uranium (U). In our model, lactate and fumarate are used as the electron donor and the electron acceptor, respectively. The model includes the production of extracellular polymeric substances (EPS). The EPS bound to the cell surface and the EPS distributed in the biofilm were considered bound EPS (bEPS) and loosely associated EPS (laEPS), respectively. COMSOL ® Multiphysics finite element analysis software was used to solve the model numerically (model file provided in the Supplementary Material). The input variables of the model were the lactate and fumarate concentrations, cell density, EPS density, half saturation constant for fumarate, and diffusion coefficients of the substrates and metabolites. To estimate unknown parameters and calibrate the model, we used a custom designed biofilm reactor placed inside a nuclear magnetic resonance (NMR) microimaging and spectroscopy system and measured substrate utilization and metabolite production rates. From these data we estimated the yield coefficients, maximum substrate utilization rate, half saturation constant for lactate, stoichiometric ratio of fumarate and acetate to lactate and stoichiometric ratio of succinate to fumarate. These parameters are critical to predicting the activity of biofilms and are not available in the literature. Lastly, the model was used to predict uranium immobilization in S. oneidensis MR-1 biofilms by considering reduction and adsorption processes in the cells and in the EPS. We found that the majority of immobilization was due to cells, and that EPS were less efficient at immobilizing U. Furthermore, most of the immobilization occurred within the top 10 µm of the biofilm. To the best of our knowledge, this research is one of the first biofilm immobilization mathematical models based on experimental observation. It has the ability to predict the relative contributions to U immobilization of laEPS, bEPS and cells.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Ammonia gas Treatment for Uranium Immobilization at DOE Hanford Site - 17067

Ammonia gas is a potential uranium (U) remediation technique for the vadose zone at the Department of Energy's (DOE) Hanford Site in Washington State via pH manipulation. The objective of this work was to investigate U removal from the aqueous phase and mineral dissolution with either NaOH or NH{sub 4}OH in order to understand ammonia as a remediation technique for the vadose zone. Batch experiments were designed to investigate the fate of U and mineral dissolution upon treatment with either NaOH or NH{sub 4}OH. These experiments investigated mineral dissolution and U partitioning in the presence of pure minerals (quartz, kaolinite, illite, montmorillonite, muscovite) and sediments relevant to the Hanford site in either NaCl or synthetic groundwater formulated based on the Hanford site groundwater components. Analysis of mineral dissolution via measurement of major cations has demonstrated that there is a significant increase in dissolution of minerals with basic treatment and likely greater secondary precipitation for the NH{sub 4}OH as compared to NaOH treatment for clay minerals and Hanford sediments. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Base Treatment for Uranium Immobilization at DOE's Hanford Site - 18279

Ammonia gas injection is currently being field tested for uranium remediation in the vadose zone at the Department of Energy's Hanford site in Washington State. U is a significant risk driver for the site because of its high mobility in the subsurface and the significant mass released due to Manhattan Project activities. In this research, we conducted laboratory batch experiments to evaluate the changes in mobility of U with different base treatments. Based on our current body of work, base treatment is a promising technique for U immobilization with ammonia gas being the optimal choice because (1) it increases partitioning coefficients for U and results in significant removal from the aqueous phase and (2) it does not add liquid to the vadose zone which could initially increase the flux of U into groundwater. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Uranium Immobilization through Fe(II) bio-oxidation: A Column study

Current research on the bioremediation of heavy metals and radionuclides is focused on the ability of reducing organisms to use these metals as alternative electron acceptors in the absence of oxygen and thus precipitate them out of solution. However, many aspects of this proposed scheme need to be resolved, not the least of which is the time frame of the treatment process. Once treatment is complete and the electron donor addition is halted, the system will ultimately revert back to an oxic state and potentially result in the abiotic reoxidation and remobilization of the immobilized metals. In addition, the possibility exists that the presence of more electropositive electron acceptors such as nitrate or oxygen will also stimulate the biological oxidation and remobilization of these contaminants. The selective nitrate-dependent biooxidation of added Fe(II) may offer an effective means of “capping off” and completing the attenuation of these contaminants in a reducing environment making the contaminants less accessible to abiotic and biotic reactions and allowing the system to naturally revert to an oxic state. Our previous DOE-NABIR funded studies demonstrated that radionuclides such as uranium and cobalt are rapidly removed from solution during the biogenic formation of Fe(III)-oxides. In the case of uranium, X-ray spectroscopy analysis indicated that the uranium was in the hexavalent form (normally soluble) and was bound to the precipitated Fe(III)-oxides thus demonstrating the bioremediative potential of this process. We also demonstrated that nitrate-dependent Fe(II)-oxidizing bacteria are prevalent in the sediment and groundwater samples collected from sites 1 and 2 and the background site of the NABIR FRC in Oakridge, TN. However, all of these studies were performed in batch experiments in the laboratory with pure cultures and although a significant amount was learned about the microbiology of nitrate-dependent bio-oxidation of Fe(II), the effects of complex processes (such as advective flow) present in the natural environment are unknown. The objective of the current studies was to address some of these short-comings in an attempt to develop this bioremediative strategy into a robust, field applicable technology. This objective was approached by both pure culture studies investigating the mechanism of Fe(II) oxidation by nitrate reducing bacteria and examining the flow dynamics and microbial processes in advective flow columns amended with Fe(II) and nitrate over an extended period.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Linking AS, SE, V, and MN Behavior to Natural Biostimulated Uranium Cycling

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 mobilization 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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Phosphate can be added to subsurface environments to immobilize U(VI) contamination. The efficacy of immobilization depends on the site-specific groundwater chemistry and aquifer sediment properties. Batch and column experiments were performed with sediments from the Hanford 300 Area in Washington State and artificial groundwater prepared to emulate the conditions at the site. Batch experiments revealed enhanced U(VI) sorption with increasing phosphate addition. X-ray absorption spectroscopy measurements of samples from the batch experiments found that U(VI) was predominantly adsorbed at conditions relevant to the column experiments and most field sites (low U(VI) loadings, <25 μM), and U(VI) phosphate precipitation occurred only at high initial U(VI) (>25μM) and phosphate loadings. While batch experiments showed the transition of U(VI) uptake from adsorption to precipitation, the column study was more directly relevant to the subsurface environment because of the high solid:water ratio in the column and the advective flow of water. In column experiments, nearly six times more U(VI) was retained in sediments when phosphate-containing groundwater was introduced to U(VI)-loaded sediments than when the groundwater did not contain phosphate. This enhanced retention persisted for at least one month after cessation of phosphate addition to the influent fluid. Sequential extractions and laser-induced fluorescence spectroscopy of sediments from the columns suggested that the retained U(VI) was primarily in adsorbed forms. These results indicate that in situ remediation of groundwater by phosphate addition provides lasting benefit beyond the treatment period via enhanced U(VI) adsorption to sediments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Experimental assessment of antimony (Sb) in pure uranium for immobilizing fission product lanthanides

The use of fuel additives is one of the concepts to mitigate fuel cladding chemical interaction (FCCI) for metallic fuel because fission product lanthanides are expected to be immobilized by the additive. Antimony (Sb) has been discovered to be a good candidate in UZr fuel. The present study focuses on its mechanism for immobilization in pure uranium, U–4Sb alloy was fabricated to understand the Sb behavior, while U–4Sb–4Ce was fabricated to simulate the case when lanthanides are generated. Both of the as-cast and annealed samples were characterized by scanning electron microscope (SEM) and energy dispersive spectrometer (EDS). U–Sb precipitates are formed in U–4Sb alloy, while U–Sb and Ce–Sb were found in U–4Sb–4Ce alloy, thermal exposure does not change the Sb-precipitation morphologies or chemical composition. Furthermore, diffusion couple tests between those alloys and cladding materials (Fe or HT9) under 650 °C for 500 h were performed and analyzed using SEM/EDS. Diffusion couple tests demonstrate the reaction between cladding and uranium, while no reaction between Sb-precipitations and cladding materials was found.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Uranium redistribution due to water table fluctuations in sandy wetland mesocosms

In order to better understand the fate and stability of immobilized uranium (U) in wetland sediments, and how intermittent dry periods affect U stability, we dosed saturated wetland mesocosms planted with Scirpus acutus with low levels of uranyl acetate for 4 months before imposing a short drying and rewetting period. Concentrations of U in mesocosm effluent increased after drying and rewetting, but the cumulative amount of U released following the dry period constituted less than 1% of the total U immobilized in the soil during the 4 months prior. This low level of remobilization suggests, and XAS analyses confirm, that microbial reduction was not the primary means of U immobilization, as the U immobilized in mesocosms was primarily U(VI) rather than U(IV). Drying followed by re-wetting caused a redistribution of U downward in the soil profile and on to root surfaces. While the U on roots before drying was primarily associated with minerals, the U that relocated to the roots during drying and rewetting was bound diffusely to root surfaces. Results show that short periods of drought conditions in a wetland, which expose reduced sediments to air, may impact U distribution, but these conditions may not cause large releases of soil-bound U from planted wetlands to surface waters.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2021

Immobilization of Uranium in a Wetland 8-km Downstream from an Industrial Source (Report)

A three-day walk-over survey with portable gamma detecting equipment was conducted over a uranium-contaminated wetland located 8-km downstream from a former fuel fabrication facility. 97,000 spectra were collected, individually processed to extract uranium activity data, and then integrated with topographical information (LIDAR) to create maps. These maps reveal that 50 years after being released into the environment, 11% of the uranium is retained in the 9-ha wetland area. Combined with measurement collected closer to the source, it was determined that 94% of the released uranium is presently being held in downstream wetlands. This demonstrates that wetlands can be very effective at immobilizing contaminants for long durations. The survey also showed that previous flyover maps overestimated the size of the contaminated areas by 140% but had the advantage of being completed in orders-of-magnitude fewer labor hours. Depending on project needs, the walk-over technique may be useful to include in tandem with flyover measurements to acquire maps with greater sensitivity and spatial resolution.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Phosphate amendments for chemical immobilization of uranium in contaminated soil

Uranium (U) contamination is a major environmental problem associated with the mining and processing of nuclear materials for both weapons and power production. When possible, in situ soil remediation techniques are preferable for reducing the risk associated with diffuse low-level U contamination. Uranium is known to form sparingly soluble phosphate compounds that persist in the environment. Therefore, batch experiments were performed to evaluate the efficacy of three phosphate amendments, hydroxyapatite (HA), sodium phytate (IP6) and sodium tripolyphosphate (TPP), to immobilize U in contaminated sediments. The amendments were added at equivalent phosphorus (P) concentrations and then equilibrated under a range of test conditions, with changes in soluble U and Ptotal monitored at pre-set time intervals. Only HA was effective at reducing the soluble U soil fraction when compared to the control, with IP6 and TPP increasing the soluble U soil fraction. After equilibration, changes in contaminant partitioning in the amended sediments were evaluated using operational extraction methods. Sequential extraction results for HA generally indicated a transfer of U from labile to more recalcitrant phases, while the results for IP6 and TPP were more ambiguous.

Uranyl↗