Genome-scale dynamic modeling of the competition between Rhodoferax and Geobacter in anoxic subsurface environments

PubMed Central

Zhuang, Kai; Izallalen, Mounir; Mouser, Paula; Richter, Hanno; Risso, Carla; Mahadevan, Radhakrishnan; Lovley, Derek R

2011-01-01

The advent of rapid complete genome sequencing, and the potential to capture this information in genome-scale metabolic models, provide the possibility of comprehensively modeling microbial community interactions. For example, Rhodoferax and Geobacter species are acetate-oxidizing Fe(III)-reducers that compete in anoxic subsurface environments and this competition may have an influence on the in situ bioremediation of uranium-contaminated groundwater. Therefore, genome-scale models of Geobacter sulfurreducens and Rhodoferax ferrireducens were used to evaluate how Geobacter and Rhodoferax species might compete under diverse conditions found in a uranium-contaminated aquifer in Rifle, CO. The model predicted that at the low rates of acetate flux expected under natural conditions at the site, Rhodoferax will outcompete Geobacter as long as sufficient ammonium is available. The model also predicted that when high concentrations of acetate are added during in situ bioremediation, Geobacter species would predominate, consistent with field-scale observations. This can be attributed to the higher expected growth yields of Rhodoferax and the ability of Geobacter to fix nitrogen. The modeling predicted relative proportions of Geobacter and Rhodoferax in geochemically distinct zones of the Rifle site that were comparable to those that were previously documented with molecular techniques. The model also predicted that under nitrogen fixation, higher carbon and electron fluxes would be diverted toward respiration rather than biomass formation in Geobacter, providing a potential explanation for enhanced in situ U(VI) reduction in low-ammonium zones. These results show that genome-scale modeling can be a useful tool for predicting microbial interactions in subsurface environments and shows promise for designing bioremediation strategies. PMID:20668487

Genome-Based Models to Optimize In Situ Bioremediation of Uranium and Harvesting Electrical Energy from Waste Organic Matter

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

Lovley, Derek R

2012-12-28

The goal of this research was to provide computational tools to predictively model the behavior of two microbial communities of direct relevance to Department of Energy interests: 1) the microbial community responsible for in situ bioremediation of uranium in contaminated subsurface environments; and 2) the microbial community capable of harvesting electricity from waste organic matter and renewable biomass. During this project the concept of microbial electrosynthesis, a novel form of artificial photosynthesis for the direct production of fuels and other organic commodities from carbon dioxide and water was also developed and research was expanded into this area as well.

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

Catalano, Jeffrey G.; Giammar, Daniel E.; Wang, Zheming

Phosphate addition is an in situ remediation approach that may enhance the sequestration of uranium without requiring sustained reducing conditions. However, the geochemical factors that determine the dominant immobilization mechanisms upon phosphate addition are insufficiently understood to design efficient remediation strategies or accurately predict U(VI) transport. The overall objective of our project is to determine the dominant mechanisms of U(VI)-phosphate reactions in subsurface environments. Our research approach seeks to determine the U(VI)-phosphate solid that form in the presence of different groundwater cations, characterize the effects of phosphate on U(VI) adsorption and precipitation on smectite and iron oxide minerals, examples ofmore » two major reactive mineral phases in contaminated sediments, and investigate how phosphate affects U(VI) speciation and fate during water flow through sediments from contaminated sites. The research activities conducted for this project have generated a series of major findings. U(VI) phosphate solids from the autunite mineral family are the sole phases to form during precipitation, with uranyl orthophosphate not occurring despite its predicted greater stability. Calcium phosphates may take up substantial quantities of U(VI) through three different removal processes (adsorption, coprecipitation, and precipitation) but the dominance of each process varies with the pathway of reaction. Phosphate co-adsorbs with U(VI) onto smectite mineral surfaces, forming a mixed uranium-phosphate surface complex over a wide range of conditions. However, this molecular-scale association of uranium and phosphate has not effect on the overall extent of uptake. In contrast, phosphate enhanced U(VI) adsorption to iron oxide minerals at acidic pH conditions but suppresses such adsorption at neutral and alkaline pH, despite forming mixed uranium-phosphate surface complexes during adsorption. Nucleation barriers exist that inhibit U(VI) phosphate solids from precipitating in the presence of smectite and iron oxide minerals as well as sediments from contaminated sites. Phosphate addition enhances retention of U(VI) by sediments from the Rifle, CO and Hanford, WA field research sites, areas containing substantial uranium contamination of groundwater. This enhanced retention is through adsorption processes. Both fast and slow uptake and release behavior is observed, indicating that diffusion of uranium between sediment grains has a substantial effect of U(VI) fate in flowing groundwater systems. This project has revealed the complexity of U(VI)-phosphate reactions in subsurface systems. Distinct chemical processes occur in acidic and alkaline groundwater systems. For the latter, calcium phosphate formation, solution complexation, and competition between phosphate and uranium for adsorption sites may serve to either enhance or inhibit U(VI) removal from groundwater. Under the groundwater conditions present at many contaminated sites in the U.S., phosphate appears to general enhance U(VI) retention and limit transport. However, formation of low-solubility uranium phosphate solids does not occur under field-relevant conditions, despite this being the desired product of phosphate-based remediation approaches. In addition, simple equilibrium approaches fail to well-predict uranium fate in contaminated sediments amended with phosphate, with reactive transport models that include reaction rates and mass transport through occluded domains needed to properly describe the system. Phosphate addition faces challenges to being effective as a stand-alone groundwater treatment approach but would prove beneficial as an add-on to other treatment methods that will further limit uranium migration in the subsurface.« less

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.

Uranium Biomineralization by Natural Microbial Phosphatase Activities in the Subsurface

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

Sobecky, Patricia A.

2015-04-06

In this project, inter-disciplinary research activities were conducted in collaboration among investigators at The University of Alabama (UA), Georgia Institute of Technology (GT), Lawrence Berkeley National Laboratory (LBNL), Brookhaven National Laboratory (BNL), the DOE Joint Genome Institute (JGI), and the Stanford Synchrotron Radiation Light source (SSRL) to: (i) confirm that phosphatase activities of subsurface bacteria in Area 2 and 3 from the Oak Ridge Field Research Center result in solid U-phosphate precipitation in aerobic and anaerobic conditions; (ii) investigate the eventual competition between uranium biomineralization via U-phosphate precipitation and uranium bioreduction; (iii) determine subsurface microbial community structure changes of Areamore » 2 soils following organophosphate amendments; (iv) obtain the complete genome sequences of the Rahnella sp. Y9-602 and the type-strain Rahnella aquatilis ATCC 33071 isolated from these soils; (v) determine if polyphosphate accumulation and phytate hydrolysis can be used to promote U(VI) biomineralization in subsurface sediments; (vi) characterize the effect of uranium on phytate hydrolysis by a new microorganism isolated from uranium-contaminated sediments; (vii) utilize positron-emission tomography to label and track metabolically-active bacteria in soil columns, and (viii) study the stability of the uranium phosphate mineral product. Microarray analyses and mineral precipitation characterizations were conducted in collaboration with DOE SBR-funded investigators at LBNL. Thus, microbial phosphorus metabolism has been shown to have a contributing role to uranium immobilization in the subsurface.« less

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

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

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

2011-06-15

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

Microbial physiology-based model of ethanol metabolism in subsurface sediments

NASA Astrophysics Data System (ADS)

Jin, Qusheng; Roden, Eric E.

2011-07-01

A biogeochemical reaction model was developed based on microbial physiology to simulate ethanol metabolism and its influence on the chemistry of anoxic subsurface environments. The model accounts for potential microbial metabolisms that degrade ethanol, including those that oxidize ethanol directly or syntrophically by reducing different electron acceptors. Out of the potential metabolisms, those that are active in the environment can be inferred by fitting the model to experimental observations. This approach was applied to a batch sediment slurry experiment that examined ethanol metabolism in uranium-contaminated aquifer sediments from Area 2 at the U.S. Department of Energy Field Research Center in Oak Ridge, TN. According to the simulation results, complete ethanol oxidation by denitrification, incomplete ethanol oxidation by ferric iron reduction, ethanol fermentation to acetate and H 2, hydrogenotrophic sulfate reduction, and acetoclastic methanogenesis: all contributed significantly to the degradation of ethanol in the aquifer sediments. The assemblage of the active metabolisms provides a frame work to explore how ethanol amendment impacts the chemistry of the environment, including the occurrence and levels of uranium. The results can also be applied to explore how diverse microbial metabolisms impact the progress and efficacy of bioremediation strategies.

The effect of uranium on bacterial viability and cell surface morphology using atomic force microscopy in the presence of bicarbonate ions

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

Sepulveda-Medina, Paola; Katsenovich, Yelena; Musaramthota, Vishal

Nuclear production facilities during the Cold War have caused liquid waste to leak and soak into the ground creating multiple radionuclide plumes. The Arthrobacter bacteria are one of the most common groups in soils and are found in large numbers in subsurface environments contaminated with radionuclides. This study experimentally analyzed changes on the bacteria surface after uranium exposure and evaluated the effect of bicarbonate ions on U(VI) toxicity of a less uranium tolerant Arthrobacter strain, G968, by investigating changes in adhesion forces and cells dimensions via atomic force microscopy (AFM). AFM and viability studies showed that samples containing bicarbonate aremore » able to acclimate and withstand uranium toxicity. Samples containing no bicarbonate exhibited deformed surfaces and a low height profile, which might be an indication that the cells are not alive.« less

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)

Influence of acidic and alkaline waste solution properties on uranium migration in subsurface sediments.

PubMed

Szecsody, Jim E; Truex, Mike J; Qafoku, Nikolla P; Wellman, Dawn M; Resch, Tom; Zhong, Lirong

2013-08-01

This study shows that acidic and alkaline wastes co-disposed with uranium into subsurface sediments have significant impact on changes in uranium retardation, concentration, and mass during downward migration. For uranium co-disposal with acidic wastes, significant rapid (i.e., hours) carbonate and slow (i.e., 100 s of hours) clay dissolution resulted, releasing significant sediment-associated uranium, but the extent of uranium release and mobility change was controlled by the acid mass added relative to the sediment proton adsorption capacity. Mineral dissolution in acidic solutions (pH2) resulted in a rapid (<10 h) increase in aqueous carbonate (with Ca(2+), Mg(2+)) and phosphate and a slow (100 s of hours) increase in silica, Al(3+), and K(+), likely from 2:1 clay dissolution. Infiltration of uranium with a strong acid resulted in significant shallow uranium mineral dissolution and deeper uranium precipitation (likely as phosphates and carbonates) with downward uranium migration of three times greater mass at a faster velocity relative to uranium infiltration in pH neutral groundwater. In contrast, mineral dissolution in an alkaline environment (pH13) resulted in a rapid (<10h) increase in carbonate, followed by a slow (10 s to 100 s of hours) increase in silica concentration, likely from montmorillonite, muscovite, and kaolinite dissolution. Infiltration of uranium with a strong base resulted in not only uranium-silicate precipitation (presumed Na-boltwoodite) but also desorption of natural uranium on the sediment due to the high ionic strength solution, or 60% greater mass with greater retardation compared with groundwater. Overall, these results show that acidic or alkaline co-contaminant disposal with uranium can result in complex depth- and time-dependent changes in uranium dissolution/precipitation reactions and uranium sorption, which alter the uranium migration mass, concentration, and velocity. Copyright © 2013 Elsevier B.V. All rights reserved.

Performance Indicators for Uranium Bioremediation in the Subsurface: Basis and Assessment

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

Long, Philip E.; Yabusaki, Steven B.

2006-12-29

The purpose of this letter report is to identify performance indicators for in situ engineered bioremediation of subsurface uranium (U) contamination. This report focuses on in situ treatment of groundwater by biostimulation of extant in situ microbial populations (see http://128.3.7.51/NABIR/generalinfo/primers_guides/03_NABIR_primer.pdf for background information on bioremediation of metals and radionuclides). The treatment process involves amendment of the subsurface with an electron donor such as acetate, lactate, ethanol or other organic compound such that in situ microorganisms mediate the reduction of U(VI) to U(IV). U(VI) precipitates as uraninite or other insoluble U phase. Uranium is thus immobilized in place by such processesmore » and is subject to reoxidation that may remobilize the reduced uranium. Related processes include augmenting the extant subsurface microbial populations, addition of electron acceptors, and introduction of chemically reducing materials such as zero-valent Fe. While metrics for such processes may be similar to those for in situ biostimulation, these related processes are not directly in the scope of this letter report.« less

Subsurface Nitrogen-Cycling Microbial Communities at Uranium Contaminated Sites in the Colorado River Basin

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.

In situ remediation of uranium contaminated groundwater

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

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

1997-02-01

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

In situ remediation of uranium contaminated groundwater

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

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

1997-12-31

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

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

PubMed Central

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

2011-01-01

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

Evaluation of positron emission tomography as a method to visualize subsurface microbial processes

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

Kinsella K.; Schlyer D.; Kinsella, K.

2012-01-18

Positron emission tomography (PET) provides spatiotemporal monitoring in a nondestructive manner and has higher sensitivity and resolution relative to other tomographic methods. Therefore, this technology was evaluated for its application to monitor in situ subsurface bacterial activity. To date, however, it has not been used to monitor or image soil microbial processes. In this study, PET imaging was applied as a 'proof-of-principle' method to assess the feasibility of visualizing a radiotracer labeled subsurface bacterial strain (Rahnella sp. Y9602), previously isolated from uranium contaminated soils and shown to promote uranium phosphate precipitation. Soil columns packed with acid-purified simulated mineral soils weremore » seeded with 2-deoxy-2-[{sup 18}F]fluoro-d-glucose ({sup 18}FDG) labeled Rahnella sp. Y9602. The applicability of [{sup 18}F]fluoride ion as a tracer for measuring hydraulic conductivity and {sup 18}FDG as a tracer to identify subsurface metabolically active bacteria was successful in our soil column studies. Our findings indicate that positron-emitting isotopes can be utilized for studies aimed at elucidating subsurface microbiology and geochemical processes important in contaminant remediation.« less

GROUNDWATER REMEDIATION SOLUTIONS AT HANFORD

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

Gilmore, Tyler J.; Truex, Michael J.; Williams, Mark D.

2007-02-26

In 2006, Congress provided funding to the U. S. Department of Energy (DOE) to study new technologies that could be used to treat contamination from the Hanford Site that might impact the Columbia River. The contaminants of concern are primarily metals and radionuclides, which are byproducts of Hanford’s cold war mission to produce plutonium for atomic weapons. The DOE asked Pacific Northwest National Laboratory (PNNL) to consider this problem and develop approaches to address the contamination that threatens the river. DOE identified three high priority sites that had groundwater contamination migrating towards the Columbia river for remediation. The contaminants includedmore » strontium-90, uranium and chromium. Remediation techniques for metals and radionuclides focus primarily on altering the oxidation state of the contaminant chemically or biologically, isolating the contaminants from the environment through adsorption or encapsulation or concentrating the contaminants for removal. A natural systems approach was taken that uses a mass balance concept to frame the problem and determine the most appropriate remedial approach. This approach provides for a scientifically based remedial decision. The technologies selected to address these contaminants included an apatite adsorption barrier coupled with a phytoremediation to address the strontium-90 contamination, injection of polyphosphate into the subsurface to sequester uranium, and a bioremediation approach to reduce chromium contamination in the groundwater. The ability to provide scientifically based approaches is in large part due to work developed under previous DOE Office of Science and Office of Environmental Management projects. For example, the polyphosphate and the bioremediation techniques, were developed by PNNL under the EMSP and NABIR programs. Contaminated groundwater under the Hanford Site poses a potential risk to humans and the Columbia River. These new technologies holds great promise for effectively remediating the residual waste that threatens the environment.« less

Influence of microorganisms on the oxidation state distribution of multivalent actinides under anoxic conditions

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

Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean - Francois

2010-12-10

The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity.more » Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.« less

Identification of Mn(II)-oxidizing bacteria from a low-pH contaminated former uranium mine.

PubMed

Akob, Denise M; Bohu, Tsing; Beyer, Andrea; Schäffner, Franziska; Händel, Matthias; Johnson, Carol A; Merten, Dirk; Büchel, Georg; Totsche, Kai Uwe; Küsel, Kirsten

2014-08-01

Biological Mn oxidation is responsible for producing highly reactive and abundant Mn oxide phases in the environment that can mitigate metal contamination. However, little is known about Mn oxidation in low-pH environments, where metal contamination often is a problem as the result of mining activities. We isolated two Mn(II)-oxidizing bacteria (MOB) at pH 5.5 (Duganella isolate AB_14 and Albidiferax isolate TB-2) and nine strains at pH 7 from a former uranium mining site. Isolate TB-2 may contribute to Mn oxidation in the acidic Mn-rich subsoil, as a closely related clone represented 16% of the total community. All isolates oxidized Mn over a small pH range, and isolates from low-pH samples only oxidized Mn below pH 6. Two strains with different pH optima differed in their Fe requirements for Mn oxidation, suggesting that Mn oxidation by the strain found at neutral pH was linked to Fe oxidation. Isolates tolerated Ni, Cu, and Cd and produced Mn oxides with similarities to todorokite and birnessite, with the latter being present in subsurface layers where metal enrichment was associated with Mn oxides. This demonstrates that MOB can be involved in the formation of biogenic Mn oxides in both moderately acidic and neutral pH environments. Copyright © 2014, American Society for Microbiology. All Rights Reserved.

Identification of Mn(II)-Oxidizing Bacteria from a Low-pH Contaminated Former Uranium Mine

PubMed Central

Bohu, Tsing; Beyer, Andrea; Schäffner, Franziska; Händel, Matthias; Johnson, Carol A.; Merten, Dirk; Büchel, Georg; Totsche, Kai Uwe; Küsel, Kirsten

2014-01-01

Biological Mn oxidation is responsible for producing highly reactive and abundant Mn oxide phases in the environment that can mitigate metal contamination. However, little is known about Mn oxidation in low-pH environments, where metal contamination often is a problem as the result of mining activities. We isolated two Mn(II)-oxidizing bacteria (MOB) at pH 5.5 (Duganella isolate AB_14 and Albidiferax isolate TB-2) and nine strains at pH 7 from a former uranium mining site. Isolate TB-2 may contribute to Mn oxidation in the acidic Mn-rich subsoil, as a closely related clone represented 16% of the total community. All isolates oxidized Mn over a small pH range, and isolates from low-pH samples only oxidized Mn below pH 6. Two strains with different pH optima differed in their Fe requirements for Mn oxidation, suggesting that Mn oxidation by the strain found at neutral pH was linked to Fe oxidation. Isolates tolerated Ni, Cu, and Cd and produced Mn oxides with similarities to todorokite and birnessite, with the latter being present in subsurface layers where metal enrichment was associated with Mn oxides. This demonstrates that MOB can be involved in the formation of biogenic Mn oxides in both moderately acidic and neutral pH environments. PMID:24928873

Identification of Mn(II)-oxidizing bacteria from a low-pH contaminated former uranium mine

USGS Publications Warehouse

Akob, Denise M.; Bohu, Tsing; Beyer, Andrea; Schäffner, Franziska; Händel, Matthias; Johnson, Carol A.; Merten, Dirk; Büchel, Georg; Totsche, Kai Uwe; Küsel, Kirsten

2014-01-01

Biological Mn oxidation is responsible for producing highly reactive and abundant Mn oxide phases in the environment that can mitigate metal contamination. However, little is known about Mn oxidation in low-pH environments, where metal contamination often is a problem as the result of mining activities. We isolated two Mn(II)-oxidizing bacteria (MOB) at pH 5.5 (Duganella isolate AB_14 and Albidiferax isolate TB-2) and nine strains at pH 7 from a former uranium mining site. Isolate TB-2 may contribute to Mn oxidation in the acidic Mn-rich subsoil, as a closely related clone represented 16% of the total community. All isolates oxidized Mn over a small pH range, and isolates from low-pH samples only oxidized Mn below pH 6. Two strains with different pH optima differed in their Fe requirements for Mn oxidation, suggesting that Mn oxidation by the strain found at neutral pH was linked to Fe oxidation. Isolates tolerated Ni, Cu, and Cd and produced Mn oxides with similarities to todorokite and birnessite, with the latter being present in subsurface layers where metal enrichment was associated with Mn oxides. This demonstrates that MOB can be involved in the formation of biogenic Mn oxides in both moderately acidic and neutral pH environments.

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

NASA Astrophysics Data System (ADS)

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

2004-05-01

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

THE INTERPLAY BETWEEN GEOCHEMICAL REACTIONS AND ADVECTION-DISPERSION IN CONTAMINANT TRANSPORT AT A URANIUM MILL TAILINGS SITE

EPA Science Inventory

It is well known that the fate and transport of contaminants in the subsurface are controlled by complex processes including advection, dispersion-diffusion, and chemical reactions. However, the interplay between the physical transport processes and chemical reactions, and their...

The effect of uranium on bacterial viability and cell surface morphology using atomic force microscopy in the presence of bicarbonate ions.

PubMed

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.

The Study of Microbial Environmental Processes Related to the Natural Attenuation of Uranium at the Rifle Site using Systems-level Biology

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

Effect of Reaction Pathway on the Extent and Mechanism of Uranium(VI) Immobilization with Calcium and Phosphate

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

Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming

Phosphate addition to subsurface environments contaminated with uranium can be used as an in situ remediation approach. Batch experiments were conducted to evaluate the dependence of the extent and mechanism of uranium uptake on the pathway for reaction with calcium phosphates. At pH 4.0 and 6.0 uranium uptake occurred via autunite (Ca(UO2)(PO4)3) precipitation irrespective of the starting forms of calcium and phosphate. At pH 7.5, the uptake mechanism depended on the nature of the calcium and phosphate. When dissolved uranium, calcium, and phosphate were added simultaneously, uranium was structurally incorporated into a newly formed amorphous calcium phosphate solid. Adsorption wasmore » the dominant removal mechanism for uranium contacted with pre-formed amorphous calcium phosphate solids,. When U(VI) was added to a suspension containing amorphous calcium phosphate solids as well as dissolved calcium and phosphate, then removal occurred through precipitation (57±4 %) of autunite and adsorption (43±4 %) onto calcium phosphate. The solid phase speciation of the uranium was determined using X-ray absorption spectroscopy and laser induced fluorescence spectroscopy. Dissolved uranium, calcium, and phosphate concentrations with saturation index calculations helped identify removal mechanisms and determine thermodynamically favorable solid phases.« less

Enrichment of specific protozoan populations during in situ bioremediation of uranium-contaminated groundwater.

PubMed

Holmes, Dawn E; Giloteaux, Ludovic; Williams, Kenneth H; Wrighton, Kelly C; Wilkins, Michael J; Thompson, Courtney A; Roper, Thomas J; Long, Philip E; Lovley, Derek R

2013-07-01

The importance of bacteria in the anaerobic bioremediation of groundwater polluted with organic and/or metal contaminants is well recognized and in some instances so well understood that modeling of the in situ metabolic activity of the relevant subsurface microorganisms in response to changes in subsurface geochemistry is feasible. However, a potentially significant factor influencing bacterial growth and activity in the subsurface that has not been adequately addressed is protozoan predation of the microorganisms responsible for bioremediation. In field experiments at a uranium-contaminated aquifer located in Rifle, CO, USA, acetate amendments initially promoted the growth of metal-reducing Geobacter species, followed by the growth of sulfate reducers, as observed previously. Analysis of 18S rRNA gene sequences revealed a broad diversity of sequences closely related to known bacteriovorous protozoa in the groundwater before the addition of acetate. The bloom of Geobacter species was accompanied by a specific enrichment of sequences most closely related to the ameboid flagellate, Breviata anathema, which at their peak accounted for over 80% of the sequences recovered. The abundance of Geobacter species declined following the rapid emergence of B. anathema. The subsequent growth of sulfate-reducing Peptococcaceae was accompanied by another specific enrichment of protozoa, but with sequences most similar to diplomonadid flagellates from the family Hexamitidae, which accounted for up to 100% of the sequences recovered during this phase of the bioremediation. These results suggest a prey-predator response with specific protozoa responding to increased availability of preferred prey bacteria. Thus, quantifying the influence of protozoan predation on the growth, activity and composition of the subsurface bacterial community is essential for predictive modeling of in situ uranium bioremediation strategies.

Enrichment of specific protozoan populations during in situ bioremediation of uranium-contaminated groundwater

PubMed Central

Holmes, Dawn E; Giloteaux, Ludovic; Williams, Kenneth H; Wrighton, Kelly C; Wilkins, Michael J; Thompson, Courtney A; Roper, Thomas J; Long, Philip E; Lovley, Derek R

2013-01-01

The importance of bacteria in the anaerobic bioremediation of groundwater polluted with organic and/or metal contaminants is well recognized and in some instances so well understood that modeling of the in situ metabolic activity of the relevant subsurface microorganisms in response to changes in subsurface geochemistry is feasible. However, a potentially significant factor influencing bacterial growth and activity in the subsurface that has not been adequately addressed is protozoan predation of the microorganisms responsible for bioremediation. In field experiments at a uranium-contaminated aquifer located in Rifle, CO, USA, acetate amendments initially promoted the growth of metal-reducing Geobacter species, followed by the growth of sulfate reducers, as observed previously. Analysis of 18S rRNA gene sequences revealed a broad diversity of sequences closely related to known bacteriovorous protozoa in the groundwater before the addition of acetate. The bloom of Geobacter species was accompanied by a specific enrichment of sequences most closely related to the ameboid flagellate, Breviata anathema, which at their peak accounted for over 80% of the sequences recovered. The abundance of Geobacter species declined following the rapid emergence of B. anathema. The subsequent growth of sulfate-reducing Peptococcaceae was accompanied by another specific enrichment of protozoa, but with sequences most similar to diplomonadid flagellates from the family Hexamitidae, which accounted for up to 100% of the sequences recovered during this phase of the bioremediation. These results suggest a prey–predator response with specific protozoa responding to increased availability of preferred prey bacteria. Thus, quantifying the influence of protozoan predation on the growth, activity and composition of the subsurface bacterial community is essential for predictive modeling of in situ uranium bioremediation strategies. PMID:23446832

Enrichment of specific protozoan populations during in situ bioremediation of uranium-contaminated groundwater

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

Holmes, Dawn; Giloteaux, L.; Williams, Kenneth H.

2013-07-28

The importance of bacteria in the anaerobic bioremediation of groundwater polluted with organic and/or metal contaminants is well-recognized and in some instances so well understood that modeling of the in situ metabolic activity of the relevant subsurface microorganisms in response to changes in subsurface geochemistry is feasible. However, a potentially significant factor influencing bacterial growth and activity in the subsurface that has not been adequately addressed is protozoan predation of the microorganisms responsible for bioremediation. In field experiments at a uranium-contaminated aquifer located in Rifle, CO, acetate amendments initially promoted the growth of metal-reducing Geobacter species followed by the growthmore » of sulfate-reducers, as previously observed. Analysis of 18S rRNA gene sequences revealed a broad diversity of sequences closely related to known bacteriovorous protozoa in the groundwater prior to the addition of acetate. The bloom of Geobacter species was accompanied by a specific enrichment of sequences most closely related to the amoeboid flagellate, Breviata anathema, which at their peak accounted for over 80% of the sequences recovered. The abundance of Geobacter species declined following the rapid emergence of B. anathema. The subsequent growth of sulfate-reducing Peptococcaceae was accompanied by another specific enrichment of protozoa, but with sequences most similar to diplomonadid flagellates from the family Hexamitidae, which accounted for up to 100% of the sequences recovered during this phase of the bioremediation. These results suggest a prey-predator response with specific protozoa responding to increased availability of preferred prey bacteria. Thus, quantifying the influence of protozoan predation on the growth, activity, and composition of the subsurface bacterial community is essential for predictive modeling of in situ uranium bioremediation strategies.« less

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

PubMed

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

2015-02-01

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

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

NASA Astrophysics Data System (ADS)

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

2013-11-01

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

Uranium Bioreduction and Biomineralization.

PubMed

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

2017-01-01

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

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

PubMed

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

2011-07-01

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

Non-enzymatic U(VI) interactions with biogenic mackinawite

NASA Astrophysics Data System (ADS)

Veeramani, H.; Qafoku, N. P.; Kukkadapu, R. K.; Murayama, M.; Hochella, M. F.

2011-12-01

Reductive immobilization of hexavalent uranium [U(VI)] by stimulation of dissimilatory metal and/or sulfate reducing bacteria (DMRB or DSRB) has been extensively researched as a remediation strategy for subsurface U(VI) contamination. These bacteria derive energy by reducing oxidized metals as terminal electron acceptors, often utilizing organic substrates as electron donors. Thus, when evaluating the potential for in-situ uranium remediation in heterogeneous subsurface media, it is important to understand how the presence of alternative electron acceptors such as Fe(III) and sulfate affect U(VI) remediation and the long term behavior and reactivity of reduced uranium. Iron, an abundant subsurface element, represents a substantial sink for electrons from DMRB, and the reduction of Fe(III) leads to the formation of dissolved Fe(II) or to reactive biogenic Fe(II)- and mixed Fe(II)/Fe(III)- mineral phases. Consequently, abiotic U(VI) reduction by reactive forms of biogenic Fe(II) minerals could be a potentially important process for uranium immobilization. In our study, the DMRB Shewanella putrefaciens CN32 was used to synthesize a biogenic Fe(II)-bearing sulfide mineral: mackinawite, that has been characterized by XRD, SEM, HRTEM and Mössbauer spectroscopy. Batch experiments involving treated biogenic mackinawite and uranium (50:1 molar ratio) were carried out at room temperature under strict anoxic conditions. Following complete removal of uranium from solution, the biogenic mackinawite was analyzed by a suite of analytical techniques including XAS, HRTEM and Mössbauer spectroscopy to determine the speciation of uranium and investigate concomitant Fe(II)-phase transformation. Determining the speciation of uranium is critical to success of a remediation strategy. The present work elucidates non-enzymatic/abiotic molecular scale redox interactions between biogenic mackinawite and uranium.

Identification and Removal of Contaminant Sequences From Ribosomal Gene Databases: Lessons From the Census of Deep Life

PubMed Central

Sheik, Cody S.; Reese, Brandi Kiel; Twing, Katrina I.; Sylvan, Jason B.; Grim, Sharon L.; Schrenk, Matthew O.; Sogin, Mitchell L.; Colwell, Frederick S.

2018-01-01

Earth’s subsurface environment is one of the largest, yet least studied, biomes on Earth, and many questions remain regarding what microorganisms are indigenous to the subsurface. Through the activity of the Census of Deep Life (CoDL) and the Deep Carbon Observatory, an open access 16S ribosomal RNA gene sequence database from diverse subsurface environments has been compiled. However, due to low quantities of biomass in the deep subsurface, the potential for incorporation of contaminants from reagents used during sample collection, processing, and/or sequencing is high. Thus, to understand the ecology of subsurface microorganisms (i.e., the distribution, richness, or survival), it is necessary to minimize, identify, and remove contaminant sequences that will skew the relative abundances of all taxa in the sample. In this meta-analysis, we identify putative contaminants associated with the CoDL dataset, recommend best practices for removing contaminants from samples, and propose a series of best practices for subsurface microbiology sampling. The most abundant putative contaminant genera observed, independent of evenness across samples, were Propionibacterium, Aquabacterium, Ralstonia, and Acinetobacter. While the top five most frequently observed genera were Pseudomonas, Propionibacterium, Acinetobacter, Ralstonia, and Sphingomonas. The majority of the most frequently observed genera (high evenness) were associated with reagent or potential human contamination. Additionally, in DNA extraction blanks, we observed potential archaeal contaminants, including methanogens, which have not been discussed in previous contamination studies. Such contaminants would directly affect the interpretation of subsurface molecular studies, as methanogenesis is an important subsurface biogeochemical process. Utilizing previously identified contaminant genera, we found that ∼27% of the total dataset were identified as contaminant sequences that likely originate from DNA extraction and DNA cleanup methods. Thus, controls must be taken at every step of the collection and processing procedure when working with low biomass environments such as, but not limited to, portions of Earth’s deep subsurface. Taken together, we stress that the CoDL dataset is an incredible resource for the broader research community interested in subsurface life, and steps to remove contamination derived sequences must be taken prior to using this dataset. PMID:29780369

Identification and Removal of Contaminant Sequences From Ribosomal Gene Databases: Lessons From the Census of Deep Life.

PubMed

Sheik, Cody S; Reese, Brandi Kiel; Twing, Katrina I; Sylvan, Jason B; Grim, Sharon L; Schrenk, Matthew O; Sogin, Mitchell L; Colwell, Frederick S

2018-01-01

Earth's subsurface environment is one of the largest, yet least studied, biomes on Earth, and many questions remain regarding what microorganisms are indigenous to the subsurface. Through the activity of the Census of Deep Life (CoDL) and the Deep Carbon Observatory, an open access 16S ribosomal RNA gene sequence database from diverse subsurface environments has been compiled. However, due to low quantities of biomass in the deep subsurface, the potential for incorporation of contaminants from reagents used during sample collection, processing, and/or sequencing is high. Thus, to understand the ecology of subsurface microorganisms (i.e., the distribution, richness, or survival), it is necessary to minimize, identify, and remove contaminant sequences that will skew the relative abundances of all taxa in the sample. In this meta-analysis, we identify putative contaminants associated with the CoDL dataset, recommend best practices for removing contaminants from samples, and propose a series of best practices for subsurface microbiology sampling. The most abundant putative contaminant genera observed, independent of evenness across samples, were Propionibacterium , Aquabacterium , Ralstonia , and Acinetobacter . While the top five most frequently observed genera were Pseudomonas , Propionibacterium , Acinetobacter , Ralstonia , and Sphingomonas . The majority of the most frequently observed genera (high evenness) were associated with reagent or potential human contamination. Additionally, in DNA extraction blanks, we observed potential archaeal contaminants, including methanogens, which have not been discussed in previous contamination studies. Such contaminants would directly affect the interpretation of subsurface molecular studies, as methanogenesis is an important subsurface biogeochemical process. Utilizing previously identified contaminant genera, we found that ∼27% of the total dataset were identified as contaminant sequences that likely originate from DNA extraction and DNA cleanup methods. Thus, controls must be taken at every step of the collection and processing procedure when working with low biomass environments such as, but not limited to, portions of Earth's deep subsurface. Taken together, we stress that the CoDL dataset is an incredible resource for the broader research community interested in subsurface life, and steps to remove contamination derived sequences must be taken prior to using this dataset.

The Use of Phosphate Amendments for Chemical Immobilization of Uranium in Contaminated Soil.

NASA Astrophysics Data System (ADS)

Baker, M.; Coutelot, F.; Seaman, J. C.

2017-12-01

Past Department of Energy (DOE) production of nuclear materials has resulted in uranium (U) contaminated soil and groundwater posing a significant risk to the environment and human health. In situ remediation strategies are typically less expensive and rely on the introduction of chemical additives in order to reduce contaminant migration and ultimately the associated exposure hazard. Phosphate addition to U-contaminated subsurface environments has been proposed as a U remediation strategy. Saturated and unsaturated batch experiments were performed to investigate the ability of three different phosphate source treatments: hydroxyapatite (HA), phytic acid (IP6) and sodium tripolyphosphate (TPP) to chemically immobilize U in contaminated Savannah River Site (SRS) soil (2,040 mg U/kg soil). Amendment treatments ranged from 925 to 4620 mg P /kg soil. Unsaturated test samples were equilibrated for 3 weeks at 60% of the soil's field capacity, followed by pore-water extraction by centrifugation to provide an indication of the remaining mobile U fraction. Saturated batch experiments were equilibrated on an orbital shaker for 30 days under both oxic and anoxic conditions, with aliquots taken at specific intervals for chemical analysis. In the saturated microcosms, HA decreased the mobile U concentration by 98% in both redox environments and at all treatment levels. IP6 and TPP were able to decrease the soluble U concentration at low treatment levels, but tended to release U at higher treatment levels compared to the control. Unsaturated microcosms also showed HA to be the most effective treatment for immobilizing U, but IP6 and TPP were as effective as HA at the lowest treatment level. The limited contaminant immobilization following TPP and IP6 amendments correlated with the dispersion of organic matter and organo-mineral colloids. For both experiment types, TPP and IP6 samples showed a very limited ortho-phosphate (PO4-) in the solution, indicating the slow mineralization of TPP and IP6.

Environmental and taxonomic bacterial diversity of anaerobic uranium(IV) bio-oxidation.

PubMed

Weber, Karrie A; Thrash, J Cameron; Van Trump, J Ian; Achenbach, Laurie A; Coates, John D

2011-07-01

Microorganisms in diverse terrestrial surface and subsurface environments can anaerobically catalyze the oxidative dissolution of uraninite. While a limited quantity (∼5 to 12 μmol liter(-1)) of uranium is oxidatively dissolved in pure culture studies, the metabolism is coupled to electron transport, providing the potential of uraninite to support indigenous microbial populations and to solubilize uranium.

Deep Vadose Zone Treatability Test of Soil Desiccation for the Hanford Central Plateau: Final Report

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

Truex, Michael J.; Chronister, Glen B.; Strickland, Christopher E.

Some of the inorganic and radionuclide contaminants in the deep vadose zone at the Hanford Site are at depths where direct exposure pathways are not of concern, but may need to be remediated to protect groundwater. The Department of Energy developed a treatability test program for technologies to address Tc-99 and uranium in the deep vadose zone. These contaminants are mobile in the subsurface environment, have been detected at high concentrations deep in the vadose zone, and at some locations have reached groundwater. The treatability test of desiccation described herein was conducted as an element of the deep vadose zonemore » treatability test program. Desiccation was shown to be a potentially effective vadose zone remediation technology to protect groundwater when used in conjunction with a surface infiltration barrier.« less

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

NASA Astrophysics Data System (ADS)

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

2003-12-01

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

National Uranium Resource Evaluation: Newcastle Quadrangle, Wyoming and South Dakota

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

Santos, E S; Robinson, K; Geer, K A

1982-09-01

Uranium resources of the Newcastle 1/sup 0/x2/sup 0/ Quadrangle, Wyoming and South Dakota were evaluated to a depth of 1500 m (5000 ft) using available surface and subsurface geologic information. Many of the uranium occurrences reported in the literature and in reports of the US Atomic Energy Commission were located, sampled and described. Areas of anomalous radioactivity, interpreted from an aerial radiometric survey, were outlined. Areas favorable for uranium deposits in the subsurface were evaluated using gamma-ray logs. Based on surface and subsurface data, two areas have been delineated which are underlain by rocks deemed favorable as hosts for uraniummore » deposits. One of these is underlain by rocks that contain fluvial arkosic facies in the Wasatch and Fort Union Formations of Tertiary age; the other is underlain by rocks containing fluvial quartzose sandstone facies of the Inyan Kara Group of Early Cretaceous age. Unfavorable environments characterize all rock units of Tertiary age above the Wasatch Formation, all rock units of Cretaceous age above the Inyan Kara Group, and most rock units of Mesozoic and Paleozoic age below the Inyan Kara Group. Unfavorable environments characterize all rock units of Cretaceous age above the Inyan Kara Group, and all rock units of Mesozoic and Paleozoic age below the Inyan Kara Group.« less

Effect of rapidly changing river stage on uranium flux through the hyporheic zone.

PubMed

Fritz, Brad G; Arntzen, Evan V

2007-01-01

Measurement of ground water/surface water interaction within the hyporheic zone is increasingly recognized as an important aspect of subsurface contaminant fate and transport. Understanding the interaction between ground water and surface water is critical in developing a complete conceptual model of contaminant transport through the hyporheic zone. At the Hanford Site near Richland, Washington, ground water contaminated with uranium discharges to the Columbia River through the hyporheic zone. Ground water flux varies according to changes in hydraulic gradient caused by fluctuating river stage, which changes in response to operation of dams on the Columbia River. Piezometers and continuous water quality monitoring probes were installed in the hyporheic zone to provide long-term, high-frequency measurement of hydraulic gradient and estimated uranium concentrations. Subsequently, the flux of water and uranium was calculated for each half-hour time period over a 15-month study period. In addition, measurement of water levels in the near-shore unconfined aquifer enhanced the understanding of the relationship between river stage, aquifer elevation, and uranium flux. Changing river stage resulted in fluctuating hydraulic gradient within the hyporheic zone. Further, influx of river water caused lower uranium concentrations as a result of dilution. The methods employed in this study provide a better understanding of the interaction between surface and ground water in a situation with a dynamically varying vertical hydraulic gradient and illustrate how the combination of relatively standard methods can be used to derive an accurate estimation of water and contaminant flux through the hyporheic zone.

Groundwater remediation solutions at hanford

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

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

2007-07-01

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

National Uranium Resource Evaluation: Palestine Quadrangle, Texas and Louisiana

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

McGowen, M.; Basciano, J.; Fose, F.G. Jr.

1982-09-01

The uranium resource potential of the Palestine Quadrangle, Texas and Louisiana, was evaluated to a depth of 1500 m (5000 ft) using criteria established for the National Uranium Resource Evaluation program. Data derived from geochemical analyses of surface samples (substrate, soil, and stream sediment) in conjunction with hydrochemical data from water wells were used to evaluate geologic environments as being favorable or unfavorable for the occurrence of uranium deposits. Two favorable environments have been identified in the Palestine Quadrangle: potential deposits of modified Texas roll-type in fluvial channels and associated facies within the Yegua Formation, and potential occurrences along mineralizationmore » fronts associated with the Elkhart Graben and Mount Enterprise fault system. Unfavorable environments include: Cretaceous shales and limestones, Tertiary fine-grained marine sequences, Tertiary sandstone units that exhibit favorable host-rock characteristics but fail to show significant syngenetic or epigenetic mineralization, and Quaternary sands and gravels. Unevaluated units include the Woodbine Group (Upper Cretaceous), Jackson Group (Tertiary), and Catahoula Formation (Tertiary). The subsurface interval of the Jackson Group and Catahoula Formation contains depositional facies that may represent favorable environments; however, the evaluation of these units is inconclusive because of the general lack of shallow subsurface control and core material. The Woodbine Group, restricted to the subsurface except for a small exposure over Palestine Dome, occurs above 1500 m (5000 ft) in the northwest quarter of the quadrangle. The unit exhibits favorable host-rock characteristics, but the paucity of gamma logs and cores, as well as the lack of hydrogeochemical and stream-sediment reconnaissance data, makes evaluation of the unit difficult.« less

Characterization and reclamation assessment for the Central Shops Diesel Storage Facility, Savannah River Site, Aiken, South Carolina

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

Fliermans, C.B.; Hazen, T.C.; Bledsoe, H.

1993-10-01

The contamination of subsurface terrestrial environments by organic contaminants is a global phenomenon. The remediation of such environments requires innovative assessment techniques and strategies for successful clean-ups. Central Shops Diesel Storage Facility at Savannah River Site was characterized to determine the extent of subsurface diesel fuel contamination using innovative approaches and effective bioremediation techniques for clean-up of the contaminant plume have been established.

Molecular-Scale Characterization of Natural Organic Matter From A Uranium Contaminated Aquifer and its Utilization by Native Microbial Communities

NASA Astrophysics Data System (ADS)

Mouser, P. J.; Wilkins, M. J.; Williams, K. H.; Smith, D. F.; Paša-Tolić, L.

2011-12-01

The availability and form of natural organic matter (NOM) strongly influences rates of microbial metabolism and associated redox processes in subsurface environments. This is an important consideration in metal-contaminated aquifers, such as the DOE's Rifle Integrated Field Research Challenge (IFRC) site, where naturally occurring suboxic conditions in groundwater may play an important function in controlling uranium mobility, and therefore the long-term stewardship of the site. Currently, the biophysiochemical processes surrounding the nature of the aquifer and its role in controlling the fate and transport of uranium are poorly understood. Using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) with electrospray ionization (ESI), we characterized dissolved organic matter (DOM) chemistry for three surface and groundwater sources at Rifle and assessed microbial utilization in batch incubation experiments. FT-ICR-MS uniquely offers ultrahigh mass measurement accuracy and resolving power for polar organics, in addition to enabling elemental composition assignments of these compounds. Samples were collected from the Colorado River, a shallow groundwater aquifer adjacent to the river, and a spring/seep discharge point upgradient from the aquifer. DOM was concentrated and purified from each source and analyzed using FT-ICR-MS with ESI. We identified between 6,000 and 7,000 formulae at each location, with the river sample having the smallest and the spring sample having the largest number of identified peaks. The groundwater and spring samples contained DOM with a large percentage of formulae containing nitrogen and sulfur species, while the river sample was dominated by carbon, hydrogen, and oxygen species. Less than 38% of the formulae were shared between any two samples, indicating a significant level of uniqueness across the samples. Unsaturated hydrocarbons, cellulose, and lipids were rapidly utilized by indigenous bacteria during a 24-day incubation period, and presumably transformed to more recalcitrant lignins and protein-type molecules. These findings indicate that FT-ICR-MS with ESI is an effective method for characterizing molecular-scale differences in DOM from complex environments. We also provide preliminary evidence that certain DOM fractions are more efficiently utilized by indigenous microbial communities and likely play an important role in controlling reducing conditions in heterogeneous subsurface environments.

Dissolution Kinetics of Meta-Torbernite under Circum-neutral to Alkaline Conditions

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

Wellman, Dawn M.; McNamara, Bruce K.; Bacon, Diana H.

2009-12-21

Autunite group minerals have been identified in contaminated sediments as the long-term controlling phase of uranium. Meta-torbernite, has been identified in subsurface environments which were subjected to co-contaminant disposal practices from past nuclear weapons and fuel operations. Under these conditions the mobility of uranium in subsurface pore waters is limited by the rate of meta-torbernite dissolution; however, there are no known investigations which report the dissolution behavior of meta-torbernite. The purpose of this investigation was to conduct a series of single-pass flow-through (SPFT) tests to 1) quantify the effect of temperature (23 - 90oC) and pH (6 -10) on meta-torbernitemore » dissolution, 2) compare the dissolution of meta-torbernite to other autunite-group minerals, and 3) evaluate the effect of aqueous phosphate on the dissolution kinetics of meta-torbernite. Results presented here illustrate meta-torbernite dissolution rates increase by ~100X over the pH interval of 6 to 10 (eta = 0.59 ± 0.07), irrespective of temperature. The power law coefficient for meta-torbernite, eta = 0.59 ± 0.07, is greater than that quantified for Ca-meta-autunite, eta = 0.42 ± 0.12. This suggests the stability of meta-torbernite is greater than that of meta-autunite, which is reflected in the predicted stability constants. The rate equation for the dissolution of meta-torbernite as a function of aqueous phosphate concentration is log rdissol (mol m-2 sec-1) = -4.7 x 10-13 + 4.1 x 10-10 [PO43-].« less

The long-term effect of uranium and pH on the community composition of an artificial consortium.

PubMed

Brzoska, Ryann M; Bollmann, Annette

2016-01-01

In the environment, microorganisms are living in diverse communities, which are impacted by the prevailing environmental conditions. Here, we present a study investigating the effect of low pH and elevated uranium concentration on the dynamics of an artificial microbial consortium. The members (Caulobacter sp. OR37, Asinibacterium sp. OR53, Ralstonia sp. OR214 and Rhodanobacter sp. OR444) were isolated from a uranium contaminated and acidic subsurface sediment. In pure culture, Ralstonia sp. OR214 had the highest growth rate at neutral and low pH and only Caulobacter sp. OR37 and Asinibacterium sp. OR53 grew in the presence uranium. The four strains were mixed in equal ratios, incubated at neutral and low pH and in the presence uranium and transferred to fresh medium once per week for 30 weeks. After 30 weeks, Ralstonia sp. OR214 was dominant at low and neutral pH and Caulobacter sp. OR37 and Asinibacterium sp. OR53 were dominant in the presence of uranium. After 12 weeks, the cultures were also transferred to new conditions to access the response of the consortia to changing conditions. The transfers showed an irreversible effect of uranium, but not of low pH on the consortia. Overall, the strains initially tolerant to the respective conditions persisted over time in high abundances in the consortia. © FEMS 2015. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

Model-based Analysis of Mixed Uranium(VI) Reduction by Biotic and Abiotic Pathways During in Situ Bioremediation

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

Zhao, Jiao; Scheibe, Timothy D.; Mahadevan, Radhakrishnan

2013-10-24

Uranium bioremediation has emerged as a potential strategy of cleanup of radionuclear contamination worldwide. An integrated geochemical & microbial community model is a promising approach to predict and provide insights into the bioremediation of a complicated natural subsurface. In this study, an integrated column-scale model of uranium bioremediation was developed, taking into account long-term interactions between biotic and abiotic processes. It is also combined with a comprehensive thermodynamic analysis to track the fate and cycling of biogenic species. As compared with other bioremediation models, the model increases the resolution of the connection of microbial community to geochemistry and establishes directmore » quantitative correlation between overall community evolution and geochemical variation, thereby accurately predicting the community dynamics under different sedimentary conditions. The thermodynamic analysis examined a recently identified homogeneous reduction of U(VI) by Fe(II) under dynamic sedimentary conditions across time and space. It shows that the biogenic Fe(II) from Geobacter metabolism can be removed rapidly by the biogenic sulphide from sulfate reducer metabolism, hence constituting one of the reasons that make the abiotic U(VI) reduction thermodynamically infeasible in the subsurface. Further analysis indicates that much higher influent concentrations of both Fe(II) and U(VI) than normal are required to for abiotic U(VI) reduction to be thermodynamically feasible, suggesting that the abiotic reduction cannot be an alternative to the biotic reduction in the remediation of uranium contaminated groundwater.« less

Carbon Characteristics and Biogeochemical Processes of Uranium Accumulating Organic Matter Rich Sediments in the Upper Colorado River Basin

NASA Astrophysics Data System (ADS)

Boye, K.; Noel, V.; Tfaily, M. M.; Dam, W. L.; Bargar, J.; Fendorf, S. E.

2015-12-01

Uranium plume persistence in groundwater aquifers is a problem on several former ore processing sites on floodplains in the upper Colorado River Basin. Earlier observations by our group and others at the Old Rifle Site, CO, have noted that U concentrations are highest in organic rich, fine-grained, and, therefore, diffusion limited sediment material. Due to the constantly evolving depositional environments of floodplains, surficial organic matter may become buried at various stages of decomposition, through sudden events such as overbank flooding and through the slower progression of river meandering. This creates a discontinuous subsurface distribution of organic-rich sediments, which are hotspots for microbial activity and thereby central to the subsurface cycling of contaminants (e.g. U) and biologically relevant elements (e.g. C, N, P, Fe). However, the organic matter itself is poorly characterized. Consequently, little is known about its relevance in driving biogeochemical processes that control U fate and transport in the subsurface. In an investigation of soil/sediment cores from five former uranium ore processing sites on floodplains distributed across the Upper Colorado River Basin we confirmed consistent co-enrichment of U with organic-rich layers in all profiles. However, using C K-edge X-ray Absorption Spectroscopy (XAS) coupled with Fourier-Transformed Ion-Cyclotron-Resonance Mass-Spectroscopy (FT-ICR-MS) on bulk sediments and density-separated organic matter fractions, we did not detect any chemical difference in the organic rich sediments compared to the surrounding coarser-grained aquifer material within the same profile, even though there were differences in organic matter composition between the 5 sites. This suggests that U retention and reduction to U(IV) is independent of C chemical composition on the bulk scale. Instead it appears to be the abundance of organic matter in combination with a limited O2 supply in the fine-grained material that stimulate anaerobic microbial processes responsible for U enrichment. Thus, the chemical composition of organic matter is subordinate to the physical environment and total organic matter content in controlling U reduction and retention processes.

Bound Flavin-Cytochrome Model of Extracellular Electron Transfer in Shewanella oneidensis: Analysis by Free Energy Molecular (Postprint)

DTIC Science & Technology

2016-06-06

toxic chemicals,4 protection of steel from corrosion,5 or in bioremediation .6 Of special interest is the potential use of the exoelectrogens in... Bioremediation of Uranium-Contaminated Groundwater: A Systems Approach to Subsurface Biogeochemistry. Curr. Opin. Biotechnol. 2013, 24, 489−497. (7

Using Geophysical Signatures to Investigate Temporal Changes Due to Source Reduction in the Subsurface Contaminated with Hydrocarbons

EPA Science Inventory

We investigated the geophysical response to subsurface hydrocarbon contamination source removal. Source removal by natural attenuation or by engineered bioremediation is expected to change the biological, chemical, and physical environment associated with the contaminated matrix....

MURMoT. Design and Application of Microbial Uranium Reduction Monitoring Tools

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

Loeffler, Frank E.

2014-12-31

Uranium (U) contamination in the subsurface is a major remediation challenge at many DOE sites. Traditional site remedies present enormous costs to DOE; hence, enhanced bioremediation technologies (i.e., biostimulation and bioaugmentation) combined with monitoring efforts are being considered as cost-effective corrective actions to address subsurface contamination. This research effort improved understanding of the microbial U reduction process and developed new tools for monitoring microbial activities. Application of these tools will promote science-based site management decisions that achieve contaminant detoxification, plume control, and long-term stewardship in the most efficient manner. The overarching hypothesis was that the design, validation and application ofmore » a suite of new molecular and biogeochemical tools advance process understanding, and improve environmental monitoring regimes to assess and predict in situ U immobilization. Accomplishments: This project (i) advanced nucleic acid-based approaches to elucidate the presence, abundance, dynamics, spatial distribution, and activity of metal- and radionuclide-detoxifying bacteria; (ii) developed proteomics workflows for detection of metal reduction biomarker proteins in laboratory cultures and contaminated site groundwater; (iii) developed and demonstrated the utility of U isotopic fractionation using high precision mass spectrometry to quantify U(VI) reduction for a range of reduction mechanisms and environmental conditions; and (iv) validated the new tools using field samples from U-contaminated IFRC sites, and demonstrated their prognostic and diagnostic capabilities in guiding decision making for environmental remediation and long-term site stewardship.« less

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

Mehta, Vrajesh; Maillot, Fabien; Wang, Zheming

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

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

NASA Astrophysics Data System (ADS)

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

2007-10-01

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

Subsurface Environment Sampler for Improved In Situ Characterization of Subsurface Microbial Communities

NASA Astrophysics Data System (ADS)

Barnhart, E. P.; Ruppert, L. F.; Orem, W. H.; McIntosh, J. C.; Cunningham, A. B.; Fields, M. W.; Hiebert, R.; Hyatt, R.

2016-12-01

There is an increasing threat that deep aquifers, an important drinking water resource, may be contaminated by the extraction and transport of fossil fuels. This threat increases the need for improved groundwater monitoring and the ability to predict the extent to which microbial activity may remediate such contamination. The characterization of subsurface microbial communities could provide an ideal biomonitoring tool for the assessment of subsurface contamination due to prokaryotes environmental ubiquity, rapidity of response to environmental perturbation and the important role they play in hydrocarbon degradation and bioremediation. New DNA sequencing technologies provide the opportunity to cost-effectively identify the vast subsurface microbial ecosystem, but use of this new technology is restricted due to issues with sampling. Prior subsurface microbiology studies have relied on core samples that are expensive to obtain hard to collect aseptically and/or ground water samples that do not reflect in situ microbial densities or activities. The development of down-well incubation of sterile sediment with a Diffusive Microbial Sampler (DMS) has emerged as an alternative method to sample subsurface microbial communities that minimizes cost and contamination issues associated with traditional methods. We have designed a Subsurface Environment Sampler with a DMS module that could enable the anaerobic transport of the in situ microbial community from the field for laboratory bioremediation studies. This sampler could provide an inexpensive and standard method for subsurface microbial sampling which would make this tool useful for Federal, State, private and local agencies interested in monitoring contamination or the effectiveness of bioremediation activities in subsurface aquifers.

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

PubMed

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

2012-07-01

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

Multivariate analysis of subsurface radiometric data in Rongsohkham area, East Khasi Hills district, Meghalaya (India): implication on uranium exploration.

PubMed

Kukreti, B M; Pandey, Pradeep; Singh, R V

2012-08-01

Non-coring based exploratory drilling was under taken in the sedimentary environment of Rangsohkham block, East Khasi Hills district to examine the eastern extension of existing uranium resources located at Domiasiat and Wakhyn in the Mahadek basin of Meghalaya (India). Although radiometric survey and radiometric analysis of surface grab/channel samples in the block indicate high uranium content but the gamma ray logging results of exploratory boreholes in the block, did not obtain the expected results. To understand this abrupt discontinuity between the two sets of data (surface and subsurface) multivariate statistical analysis of primordial radioactive elements (K(40), U(238) and Th(232)) was performed using the concept of representative subsurface samples, drawn from the randomly selected 11 boreholes of this block. The study was performed to a high confidence level (99%), and results are discussed for assessing the U and Th behavior in the block. Results not only confirm the continuation of three distinct geological formations in the area but also the uranium bearing potential in the Mahadek sandstone of the eastern part of Mahadek Basin. Copyright © 2012 Elsevier Ltd. All rights reserved.

Tackling the Challenge of Deep Vadose Zone Remediation at the Hanford Site

NASA Astrophysics Data System (ADS)

Morse, J. G.; Wellman, D. M.; Gephart, R.

2010-12-01

The Central Plateau of the Hanford Site in Washington State contains some 800 waste disposal sites where 1.7 trillion liters of contaminated water was once discharged into the subsurface. Most of these sites received liquids from the chemical reprocessing of spent uranium fuel to recover plutonium. In addition, 67 single shell tanks have leaked or are suspected to have leaked 3.8 million liters of high alkali and aluminate rich cesium-contaminated liquids into the sediment. Today, this inventory of subsurface contamination contains an estimated 550,000 curies of radioactivity and 150 million kg (165,000 tons) of metals and hazardous chemicals. Radionuclides range from mobile 99Tc to more immobilized 137Cs, 241Am, uranium, and plutonium. A significant fraction of these contaminants likely remain within the deep vadose zone. Plumes of groundwater containing tritium, nitrate, 129I and other contaminants have migrated through the vadose zone and now extend outward from the Central Plateau to the Columbia River. During most of Hanford Site history, subsurface studies focused on groundwater monitoring and characterization to support waste management decisions. Deep vadose zone studies were not a priority because waste practices relied upon that zone to buffer contaminant releases into the underlying aquifer. Remediation of the deep vadose zone is now central to Hanford Site cleanup because these sediments can provide an ongoing source of contamination to the aquifer and therefore to the Columbia River. However, characterization and remediation of the deep vadose zone pose some unique challenges. These include sediment thickness; contaminant depth; coupled geohydrologic, geochemical, and microbial processes controlling contaminant spread; limited availability and effectiveness of traditional characterization tools and cleanup remedies; and predicting contaminant behavior and remediation performance over long time periods and across molecular to field scales. The U.S Department of Energy recognizes these challenges and is committed to a sustained, focused effort of continuing to apply existing technologies where feasible while investing and developing in new innovative, field-demonstrated capabilities supporting longer-term basic and applied research to establish the technical underpinning for solving intractable deep vadose zone problems and implementing final remedies. This approach will rely upon Multi-Project Teams focusing on coordinated projects across multiple DOE offices, programs, and site contractors plus the facilitation of basic and applied research investments through implementing a Deep Vadose Zone Applied Field Research Center and other scientific studies.

Mobilization of radionuclides from uranium mill tailings and related waste materials in anaerobic environments

USGS Publications Warehouse

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.

Environmental Remediation

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

None

2017-04-11

At Pacific Northwest National Laboratory, we are a leader in subsurface science and remediation. We use our expertise in these areas to characterize subsurface contaminants and assess contaminant transport. We're also using our capabilities to restore the Hanford Site in southeastern Washington State to a safe, clean environment.

Processes affecting transport of uranium in a suboxic aquifer

USGS Publications Warehouse

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

2006-01-01

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

Enhanced uranium immobilization and reduction by Geobacter sulfurreducens biofilms.

PubMed

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

2014-11-01

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

Enhanced Uranium Immobilization and Reduction by Geobacter sulfurreducens Biofilms

PubMed Central

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

2014-01-01

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

A Multifaceted Sampling Approach to Better Understanding Biogeochemical and Hydrogeological Controls on Uranium Mobility at a Former Uranium Mill Tailings Site in Riverton, Wyoming

NASA Astrophysics Data System (ADS)

Dam, W. L.; Johnson, R. H.; Campbell, S.; Bone, S. E.; Noel, V.; Bargar, J.

2015-12-01

Understanding uranium mobility in subsurface environments is not trivial. Obtaining sufficient data to accurately represent soil and aquifer characteristics can require unique approaches that evolve with added site knowledge. At Riverton, the primary source of uranium mill tailings remaining from ore processing was removed but contaminant plumes have persisted longer than predicted by groundwater modeling. What are the primary mechanisms controlling plume persistence? DOE is conducting new characterization studies to assist our understanding of underlying biogeochemical and hydrogeological mechanisms affecting secondary sources. A variety of field sampling techniques are being sequentially employed including augering, trenching, pore water sampling, and installing multi-level wells. In August 2012, vadose zone soil samples from 34 locations and groundwater from 103 boreholes were collected with Geoprobe ® direct push rods. Lower than expected uranium concentrations in composited shallow soils indicated the need for more focused and deeper samples. In May 2014, soil samples containing evaporites were collected along the bank of the Little Wind River; elevated uranium concentrations in evaporite minerals correlated with plume configurations and reflect contaminated groundwater discharge at the river. In September 2014, hand anger samples collected by the river and oxbow lake also indicated the presence of organic rich zones containing elevated uranium (>50 mg/kg). Subsequent samples collected from five backhoe trenches in May 2015 revealed a highly heterogeneous vadose zone composed of clay, silt, sand and cobbles containing evaporites and organic rich zones which may interact with groundwater plumes.Plans for August 2015 include sonic drilling to obtain continuous cores from the surface down to the base of the surficial aquifer with multi-level monitoring wells constructed in each borehole to assess vertical variation in groundwater chemistry. Temporary well-points will be installed adjacent to the river to assess geochemical and flow controls in the area of plume stagnation. Analyses include critical element speciation (C, S, Fe, and U), microbes, isotopes, diffusivity and flow characteristics. These activities support a dramatically improved understanding of plume persistence.

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

NASA Astrophysics Data System (ADS)

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

2015-12-01

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

Contaminated environments in the subsurface and bioremediation: organic contaminants.

PubMed

Holliger, C; Gaspard, S; Glod, G; Heijman, C; Schumacher, W; Schwarzenbach, R P; Vazquez, F

1997-07-01

Due to leakages, spills, improper disposal and accidents during transport, organic compounds have become subsurface contaminants that threaten important drinking water resources. One strategy to remediate such polluted subsurface environments is to make use of the degradative capacity of bacteria. It is often sufficient to supply the subsurface with nutrients such as nitrogen and phosphorus, and aerobic treatments are still dominating. However, anaerobic processes have advantages such as low biomass production and good electron acceptor availability, and they are sometimes the only possible solution. This review will focus on three important groups of environmental organic contaminants: hydrocarbons, chlorinated and nitroaromatic compounds. Whereas hydrocarbons are oxidized and completely mineralized under anaerobic conditions in the presence of electron acceptors such as nitrate, iron, sulfate and carbon dioxide, chlorinated and nitroaromatic compounds are reductively transformed. For the aerobic often persistent polychlorinated compounds, reductive dechlorination leads to harmless products or to compounds that are aerobically degradable. The nitroaromatic compounds are first reductively transformed to the corresponding amines and can subsequently be bound to the humic fraction in an aerobic process. Such new findings and developments give hope that in the near future contaminated aquifers can efficiently be remediated, a prerequisite for a sustainable use of the precious-subsurface drinking water resources.

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

PubMed

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

2014-10-01

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

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

DOE PAGES

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

2014-06-07

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

Bioremediation of contaminated groundwater

DOEpatents

Hazen, T.C.; Fliermans, C.B.

1994-01-01

Disclosed is an apparatus and method for in situ remediation of contaminated subsurface soil or groundwater contaminated by chlorinated hydrocarbons. A nutrient fluid (NF) is selected to simulated the growth and reproduction of indigenous subsurface microorganisms capable of degrading the contaminants; an oxygenated fluid (OF) is selected to create an aerobic environment with anaerobic pockets. NF is injected periodically while OF is injected continuously and both are extracted so that both are drawn across the plume. NF stimulates microbial colony growth; withholding it periodically forces the larger, healthy colony of microbes to degrade the contaminants. Treatment is continued until the subsurface concentration of contaminants is acceptable. NF can be methane and OF be air, for stimulating production of methanotrophs to break down chlorohydrocarbons, especially TCE and tetrachloroethylene.

Detection of biological uranium reduction using magnetic resonance.

PubMed

Vogt, Sarah J; Stewart, Brandy D; Seymour, Joseph D; Peyton, Brent M; Codd, Sarah L

2012-04-01

The conversion of soluble uranyl ions (UO₂²⁺) by bacterial reduction to sparingly soluble uraninite (UO₂(s)) is being studied as a way of immobilizing subsurface uranium contamination. Under anaerobic conditions, several known types of bacteria including iron and sulfate reducing bacteria have been shown to reduce U (VI) to U (IV). Experiments using a suspension of uraninite (UO₂(s)) particles produced by Shewanella putrefaciens CN32 bacteria show a dependence of both longitudinal (T₁) and transverse (T₂) magnetic resonance (MR) relaxation times on the oxidation state and solubility of the uranium. Gradient echo and spin echo MR images were compared to quantify the effect caused by the magnetic field fluctuations (T*₂) of the uraninite particles and soluble uranyl ions. Since the precipitate studied was suspended in liquid water, the effects of concentration and particle aggregation were explored. A suspension of uraninite particles was injected into a polysaccharide gel, which simulates the precipitation environment of uraninite in the extracellular biofilm matrix. A reduction in the T₂ of the gel surrounding the particles was observed. Tests done in situ using three bioreactors under different mixing conditions, continuously stirred, intermittently stirred, and not stirred, showed a quantifiable T₂ magnetic relaxation effect over the extent of the reaction. Copyright © 2011 Wiley Periodicals, Inc.

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

PubMed Central

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

2013-01-01

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

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

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

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

In-Situ Contained And Of Volatile Soil Contaminants

DOEpatents

Varvel, Mark Darrell

2005-12-27

The invention relates to a novel approach to containing and removing toxic waste from a subsurface environment. More specifically the present invention relates to a system for containing and removing volatile toxic chemicals from a subsurface environment using differences in surface and subsurface pressures. The present embodiment generally comprises a deep well, a horizontal tube, at least one injection well, at least one extraction well and a means for containing the waste within the waste zone (in-situ barrier). During operation the deep well air at the bottom of well (which is at a high pressure relative to the land surface as well as relative to the air in the contaminated soil) flows upward through the deep well (or deep well tube). This stream of deep well air is directed into the horizontal tube, down through the injection tube(s) (injection well(s)) and into the contaminate plume where it enhances volatization and/or removal of the contaminants.

In-Situ Containment and Extraction of Volatile Soil Contaminants

DOEpatents

Varvel, Mark Darrell

2005-12-27

The invention relates to a novel approach to containing and removing toxic waste from a subsurface environment. More specifically the present invention relates to a system for containing and removing volatile toxic chemicals from a subsurface environment using differences in surface and subsurface pressures. The present embodiment generally comprises a deep well, a horizontal tube, at least one injection well, at least one extraction well and a means for containing the waste within the waste zone (in-situ barrier). During operation the deep well air at the bottom of well (which is at a high pressure relative to the land surface as well as relative to the air in the contaminated soil) flows upward through the deep well (or deep well tube). This stream of deep well air is directed into the horizontal tube, down through the injection tube(s) (injection well(s)) and into the contaminate plume where it enhances volatization and/or removal of the contaminants.

Conceptual Model of Iodine Behavior in the Subsurface at the Hanford Site

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

Truex, Michael J.; Lee, Brady D.; Johnson, Christian D.

The fate and transport of 129I in the environment and potential remediation technologies are currently being studied as part of environmental remediation activities at the Hanford Site. A conceptual model describing the nature and extent of subsurface contamination, factors that control plume behavior, and factors relevant to potential remediation processes is needed to support environmental remedy decisions. Because 129I is an uncommon contaminant, relevant remediation experience and scientific literature are limited. Thus, the conceptual model also needs to both describe known contaminant and biogeochemical process information and to identify aspects about which additional information needed to effectively support remedy decisions.more » this document summarizes the conceptual model of iodine behavior relevant to iodine in the subsurface environment at the Hanford site.« less

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

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

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

2008-01-31

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

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

Microbial populations in contaminant plumes

USGS Publications Warehouse

Haack, S.K.; Bekins, B.A.

2000-01-01

Efficient biodegradation of subsurface contaminants requires two elements: (1) microbial populations with the necessary degradative capabilities, and (2) favorable subsurface geochemical and hydrological conditions. Practical constraints on experimental design and interpretation in both the hydrogeological and microbiological sciences have resulted in limited knowledge of the interaction between hydrogeological and microbiological features of subsurface environments. These practical constraints include: (1) inconsistencies between the scales of investigation in the hydrogeological and microbiological sciences, and (2) practical limitations on the ability to accurately define microbial populations in environmental samples. However, advances in application of small-scale sampling methods and interdisciplinary approaches to site investigations are beginning to significantly improve understanding of hydrogeological and microbiological interactions. Likewise, culture-based and molecular analyses of microbial populations in subsurface contaminant plumes have revealed significant adaptation of microbial populations to plume environmental conditions. Results of recent studies suggest that variability in subsurface geochemical and hydrological conditions significantly influences subsurface microbial-community structure. Combined investigations of site conditions and microbial-community structure provide the knowledge needed to understand interactions between subsurface microbial populations, plume geochemistry, and contaminant biodegradation.

Uranium redox transition pathways in acetate-amended sediments

USGS Publications Warehouse

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.

Functional environmental proteomics: elucidating the role of a c-type cytochrome abundant during uranium bioremediation

PubMed Central

Yun, Jiae; Malvankar, Nikhil S; Ueki, Toshiyuki; Lovley, Derek R

2016-01-01

Studies with pure cultures of dissimilatory metal-reducing microorganisms have demonstrated that outer-surface c-type cytochromes are important electron transfer agents for the reduction of metals, but previous environmental proteomic studies have typically not recovered cytochrome sequences from subsurface environments in which metal reduction is important. Gel-separation, heme-staining and mass spectrometry of proteins in groundwater from in situ uranium bioremediation experiments identified a putative c-type cytochrome, designated Geobacter subsurface c-type cytochrome A (GscA), encoded within the genome of strain M18, a Geobacter isolate previously recovered from the site. Homologs of GscA were identified in the genomes of other Geobacter isolates in the phylogenetic cluster known as subsurface clade 1, which predominates in a diversity of Fe(III)-reducing subsurface environments. Most of the gscA sequences recovered from groundwater genomic DNA clustered in a tight phylogenetic group closely related to strain M18. GscA was most abundant in groundwater samples in which Geobacter sp. predominated. Expression of gscA in a strain of Geobacter sulfurreducens that lacked the gene for the c-type cytochrome OmcS, thought to facilitate electron transfer from conductive pili to Fe(III) oxide, restored the capacity for Fe(III) oxide reduction. Atomic force microscopy provided evidence that GscA was associated with the pili. These results demonstrate that a c-type cytochrome with an apparent function similar to that of OmcS is abundant when Geobacter sp. are abundant in the subsurface, providing insight into the mechanisms for the growth of subsurface Geobacter sp. on Fe(III) oxide and suggesting an approach for functional analysis of other Geobacter proteins found in the subsurface. PMID:26140532

Functional environmental proteomics: elucidating the role of a c-type cytochrome abundant during uranium bioremediation.

PubMed

Yun, Jiae; Malvankar, Nikhil S; Ueki, Toshiyuki; Lovley, Derek R

2016-02-01

Studies with pure cultures of dissimilatory metal-reducing microorganisms have demonstrated that outer-surface c-type cytochromes are important electron transfer agents for the reduction of metals, but previous environmental proteomic studies have typically not recovered cytochrome sequences from subsurface environments in which metal reduction is important. Gel-separation, heme-staining and mass spectrometry of proteins in groundwater from in situ uranium bioremediation experiments identified a putative c-type cytochrome, designated Geobacter subsurface c-type cytochrome A (GscA), encoded within the genome of strain M18, a Geobacter isolate previously recovered from the site. Homologs of GscA were identified in the genomes of other Geobacter isolates in the phylogenetic cluster known as subsurface clade 1, which predominates in a diversity of Fe(III)-reducing subsurface environments. Most of the gscA sequences recovered from groundwater genomic DNA clustered in a tight phylogenetic group closely related to strain M18. GscA was most abundant in groundwater samples in which Geobacter sp. predominated. Expression of gscA in a strain of Geobacter sulfurreducens that lacked the gene for the c-type cytochrome OmcS, thought to facilitate electron transfer from conductive pili to Fe(III) oxide, restored the capacity for Fe(III) oxide reduction. Atomic force microscopy provided evidence that GscA was associated with the pili. These results demonstrate that a c-type cytochrome with an apparent function similar to that of OmcS is abundant when Geobacter sp. are abundant in the subsurface, providing insight into the mechanisms for the growth of subsurface Geobacter sp. on Fe(III) oxide and suggesting an approach for functional analysis of other Geobacter proteins found in the subsurface.

Geobacter daltonii sp. nov., an Fe(III)- and uranium(VI)-reducing bacterium isolated from a shallow subsurface exposed to mixed heavy metal and hydrocarbon contamination.

PubMed

Prakash, Om; Gihring, Thomas M; Dalton, Dava D; Chin, Kuk-Jeong; Green, Stefan J; Akob, Denise M; Wanger, Greg; Kostka, Joel E

2010-03-01

An Fe(III)- and uranium(VI)-reducing bacterium, designated strain FRC-32(T), was isolated from a contaminated subsurface of the USA Department of Energy Oak Ridge Field Research Center (ORFRC) in Oak Ridge, Tennessee, where the sediments are exposed to mixed waste contamination of radionuclides and hydrocarbons. Analyses of both 16S rRNA gene and the Geobacteraceae-specific citrate synthase (gltA) mRNA gene sequences retrieved from ORFRC sediments indicated that this strain was abundant and active in ORFRC subsurface sediments undergoing uranium(VI) bioremediation. The organism belonged to the subsurface clade of the genus Geobacter and shared 92-98 % 16S rRNA gene and 75-81 % rpoB gene sequence similarities with other recognized species of the genus. In comparison to its closest relative, Geobacter uraniireducens Rf4(T), according to 16S rRNA gene sequence similarity, strain FRC-32(T) showed a DNA-DNA relatedness value of 21 %. Cells of strain FRC-32(T) were Gram-negative, non-spore-forming, curved rods, 1.0-1.5 microm long and 0.3-0.5 microm in diameter; the cells formed pink colonies in a semisolid cultivation medium, a characteristic feature of the genus Geobacter. The isolate was an obligate anaerobe, had temperature and pH optima for growth at 30 degrees C and pH 6.7-7.3, respectively, and could tolerate up to 0.7 % NaCl although growth was better in the absence of NaCl. Similar to other members of the Geobacter group, strain FRC-32(T) conserved energy for growth from the respiration of Fe(III)-oxyhydroxide coupled with the oxidation of acetate. Strain FRC-32(T) was metabolically versatile and, unlike its closest relative, G. uraniireducens, was capable of utilizing formate, butyrate and butanol as electron donors and soluble ferric iron (as ferric citrate) and elemental sulfur as electron acceptors. Growth on aromatic compounds including benzoate and toluene was predicted from preliminary genomic analyses and was confirmed through successive transfer with fumarate as the electron acceptor. Thus, based on genotypic, phylogenetic and phenotypic differences, strain FRC-32(T) is considered to represent a novel species of the genus Geobacter, for which the name Geobacter daltonii sp. nov. is proposed. The type strain is FRC-32(T) (=DSM 22248(T)=JCM 15807(T)).

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

PubMed

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

2016-10-01

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

Uranium ores and depleted uranium in the environment, with a reference to uranium in the biosphere from the Erzgebirge/Sachsen, Germany.

PubMed

Meinrath, A; Schneider, P; Meinrath, G

2003-01-01

The Erzgebirge ('Ore Mountains') area in the eastern part of Germany was a major source of uranium for Soviet nuclear programs between 1945 and 1989. During this time, the former German Democratic Republic became the third largest uranium producer in the world. The high abundance of uranium in the geological formations of the Erzgebirge are mirrored in the discovery of uranium by M. Klaproth close to Freiberg City in 1789 and the description of the so-called 'Schneeberg' disease, lung cancer caused in miners by the accumulation of the uranium decay product, radon, in the subsurfaces of shafts. Since 1991, remediation and mitigation of uranium at production facilities, rock piles and mill tailings has taken place. In parallel, efforts were initiated to assess the likely adverse effects of uranium mining to humans. The costs of these activities amount to about 6.5 10(9) Euro. A comparison with concentrations of depleted uranium at certain sites is given.

Bioremediation of contaminated groundwater

DOEpatents

Hazen, Terry C.; Fliermans, Carl B.

1995-01-01

An apparatus and method for in situ remediation of contaminated subsurface soil or groundwater contaminated by chlorinated hydrocarbons. A nutrient fluid is selected to stimulate the growth and reproduction of indigenous subsurface microorganisms that are capable of degrading the contaminants; an oxygenated fluid is selected to create a generally aerobic environment for these microorganisms to degrade the contaminants, leaving only pockets that are anaerobic. The nutrient fluid is injected periodically while the oxygenated fluid is injected continuously and both are extracted so that both are drawn across the plume. The nutrient fluid stimulates microbial colony growth; withholding it periodicially forces the larger, healthy colony of microbes to degrade the contaminants. Treatment is continued until the subsurface concentration of contaminants is reduced to an acceptable, preselected level. The nutrient fluid can be methane and the oxygenated fluid air for stimulating production of methanotrophs to break down chlorohydrocarbons, especially trichloroethylene (TCE) and tetrachloroethylene.

Bioremediation of contaminated groundwater

DOEpatents

Hazen, T.C.; Fliermans, C.B.

1995-01-24

An apparatus and method are described for in situ remediation of contaminated subsurface soil or groundwater contaminated by chlorinated hydrocarbons. A nutrient fluid is selected to stimulate the growth and reproduction of indigenous subsurface microorganisms that are capable of degrading the contaminants. An oxygenated fluid is selected to create a generally aerobic environment for these microorganisms to degrade the contaminants, leaving only pockets that are anaerobic. The nutrient fluid is injected periodically while the oxygenated fluid is injected continuously and both are extracted so that both are drawn across the plume. The nutrient fluid stimulates microbial colony growth. Withholding it periodically forces the larger, healthy colony of microbes to degrade the contaminants. Treatment is continued until the subsurface concentration of contaminants is reduced to an acceptable, preselected level. The nutrient fluid can be methane and the oxygenated fluid air for stimulating production of methanotrophs to break down chlorohydrocarbons, especially trichloroethylene (TCE) and tetrachloroethylene. 3 figures.

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.

Distribution of uranium and thorium in dolomitic gravel fill and shale saprolite

DOE PAGES

Phillips, D. H.; Watson, D. B.

2014-12-05

The objectives of this study were to examine (1) the distribution of U and Th in dolomitic gravel fill and shale saprolite, and (2) the removal of uranium from acidic groundwater by dolomitic gravel through precipitation with amorphous basaluminite at the U.S. DOE Oak Ridge Integrated Field Research Challenge (ORIFRC) field site west of the Oak Ridge Y-12 National Security Complex in East Tennessee. Media reactivity and sustainability are a technical concern with the deployment of any subsurface reactive media. Because the gravel was placed in the subsurface and exposed to contaminated groundwater for over 20 years, it provided amore » unique opportunity to study the solid and water phase geochemical conditions within the media after this length of exposure. This study illustrates that dolomite gravel can remove U from acidic contaminated groundwater with high levels of Al 3+, Ca 2+, NO 3-, and SO 4 2- over the long term. As the groundwater flows through high pH carbonate gravel, U containing amorphous basaluminite precipitates as the pH increases. This is due to an increase in groundwater pH from 3.2 to ~6.5 as it comes in contact with the gravel. Therefore, carbonate gravel could be considered as a possible treatment medium for removal and sequestration ofUand otherpHsensitive metals from acidic contaminated groundwater. Thorium concentrations are also high in the carbonate gravel. Thorium generally shows an inverse relationship with U from the surface down into the deeper saprolite. Barite precipitated in the shallow saprolite directly below the dolomitic gravel from barium present in the acidic contaminated groundwater.« less

Abundance and Distribution of Microbial Cells and Viruses in an Alluvial Aquifer

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

Pan, Donald; Nolan, Jason; Williams, Kenneth H.

Viruses are the most abundant biological entity on Earth and their interactions with microbial communities are recognized to influence microbial ecology and impact biogeochemical cycling in various ecosystems. While the factors that control the distribution of viruses in surface aquatic environments are well-characterized, the abundance and distribution of continental subsurface viruses with respect to microbial abundance and biogeochemical parameters have not yet been established. In order to begin to understand the factors governing virus distribution in subsurface environments, we assessed microbial cell and virus abundance in groundwater concurrent with groundwater chemistry in a uranium impacted alluvial aquifer adjoining the Coloradomore » River near Rifle, CO. Virus abundance ranged from 8.0 × 10 4 to 1.0 × 10 6 mL -1 and exceeded cell abundance in all samples (cell abundance ranged from 5.8 × 10 4 to 6.1 × 10 5 mL -1). The virus to microbial cell ratio ranged from 1.1 to 8.1 and averaged 3.0 ± 1.6 with virus abundance most strongly correlated to cell abundance (Spearman's ρ = 0.73, p < 0.001). Both viruses and cells were positively correlated to dissolved organic carbon (DOC) with cells having a slightly stronger correlation (Spearman's ρ = 0.46, p < 0.05 and ρ = 0.54, p < 0.05; respectively). Groundwater uranium was also strongly correlated with DOC and virus and cell abundance (Spearman's ρ = 0.62, p < 0.05; ρ = 0.46, p < 0.05; and ρ = 0.50, p < 0.05; respectively). Together the data indicate that microbial cell and virus abundance are correlated to the geochemical conditions in the aquifer. As such local geochemical conditions likely control microbial host cell abundance which in turn controls viral abundance. Given the potential impacts of viral-mediated cell lysis such as liberation of labile organic matter from lysed cells and changes in microbial community structure, viral interactions with the microbiota should be considered in an effort to understand subsurface biogeochemical cycling and contaminant mobility.« less

Abundance and Distribution of Microbial Cells and Viruses in an Alluvial Aquifer

DOE PAGES

Pan, Donald; Nolan, Jason; Williams, Kenneth H.; ...

2017-07-11

Viruses are the most abundant biological entity on Earth and their interactions with microbial communities are recognized to influence microbial ecology and impact biogeochemical cycling in various ecosystems. While the factors that control the distribution of viruses in surface aquatic environments are well-characterized, the abundance and distribution of continental subsurface viruses with respect to microbial abundance and biogeochemical parameters have not yet been established. In order to begin to understand the factors governing virus distribution in subsurface environments, we assessed microbial cell and virus abundance in groundwater concurrent with groundwater chemistry in a uranium impacted alluvial aquifer adjoining the Coloradomore » River near Rifle, CO. Virus abundance ranged from 8.0 × 10 4 to 1.0 × 10 6 mL -1 and exceeded cell abundance in all samples (cell abundance ranged from 5.8 × 10 4 to 6.1 × 10 5 mL -1). The virus to microbial cell ratio ranged from 1.1 to 8.1 and averaged 3.0 ± 1.6 with virus abundance most strongly correlated to cell abundance (Spearman's ρ = 0.73, p < 0.001). Both viruses and cells were positively correlated to dissolved organic carbon (DOC) with cells having a slightly stronger correlation (Spearman's ρ = 0.46, p < 0.05 and ρ = 0.54, p < 0.05; respectively). Groundwater uranium was also strongly correlated with DOC and virus and cell abundance (Spearman's ρ = 0.62, p < 0.05; ρ = 0.46, p < 0.05; and ρ = 0.50, p < 0.05; respectively). Together the data indicate that microbial cell and virus abundance are correlated to the geochemical conditions in the aquifer. As such local geochemical conditions likely control microbial host cell abundance which in turn controls viral abundance. Given the potential impacts of viral-mediated cell lysis such as liberation of labile organic matter from lysed cells and changes in microbial community structure, viral interactions with the microbiota should be considered in an effort to understand subsurface biogeochemical cycling and contaminant mobility.« less

National Uranium Resource Evaluation: Wells Quadrangle, Nevada, Idaho, and Utah

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

Proffitt, J.L.; Mayerson, D.L.; Parker, D.P.

1982-08-01

The Wells 2/sup 0/ Quadrangle, Nevada, Idaho, and Utah, was evaluated using National Uranium Resource Evaluation criteria to delineate areas favorable for uranium deposits. Our investigation has resulted in the delineation of areas that contain Tertiary sedimentary rocks favorable for hydroallogenic deposits in the Mountain City area (Favorable Area A) and in the Oxley Peak area north of Wells (Favorable Area B). Environments considered to be unfavorable for uranium deposits include Tertiary felsic volcanic, felsic plutonic, intermediate to mafic volcanic, Paleozoic and Mesozoic sedimentary rocks, Precambrian rocks, and most Tertiary sedimentary rocks located outside the favorable areas. Present-day basins aremore » unevaluated environments because of a paucity of adequate outcrop and subsurface data. However, the scarce data indicate that some characteristics favorable for uranium deposits are present in the Susie Creek-Tule Valley-Wild Horse basin, the Contact-Granite Range-Tijuana John stocks area, the Charleston Reservoir area, and the Wells-Marys River basin.« less

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

PubMed

Durante, Marco; Pugliese, Mariagabriella

2002-01-01

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

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

PubMed

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

2016-08-01

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

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

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

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

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

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

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

Sepulveda, Paola; Katsenovich, Yelena; Lagos, Leonel

2013-07-01

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

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.

Influence Of pH On The Transport Of Nanoscale Zinc Oxide In Saturated Porous Media

EPA Science Inventory

Widespread use of nanoscale zinc oxide (nZnO) in various fields causes subsurface environment contamination. Even though the transport of dissolved zinc ions in subsurface environments such as soils and sediments has been widely studied, the transport mechanism of nZnO in such e...

Redox behavior of uranium at the nanoporous aluminum oxide-water interface: implications for uranium remediation.

PubMed

Jung, Hun Bok; Boyanov, Maxim I; Konishi, Hiromi; Sun, Yubing; Mishra, Bhoopesh; Kemner, Kenneth M; Roden, Eric E; Xu, Huifang

2012-07-03

Sorption-desorption experiments show that the majority (ca. 80-90%) of U(VI) presorbed to mesoporous and nanoporous alumina could not be released by extended (2 week) extraction with 50 mM NaHCO(3) in contrast with non-nanoporous α alumina. The extent of reduction of U(VI) presorbed to aluminum oxides was semiquantitatively estimated by comparing the percentages of uranium desorbed by anoxic sodium bicarbonate between AH(2)DS-reacted and unreacted control samples. X-ray absorption spectroscopy confirmed that U(VI) presorbed to non-nanoporous alumina was rapidly and completely reduced to nanoparticulate uraninite by AH(2)DS, whereas reduction of U(VI) presorbed to nanoporous alumina was slow and incomplete (<5% reduction after 1 week). The observed nanopore size-dependent redox behavior of U has important implications in developing efficient remediation techniques for the subsurface uranium contamination because the efficiency of in situ bioremediation depends on how effectively and rapidly U(VI) bound to sediment or soil can be converted to an immobile phase.

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

PubMed

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

2015-06-16

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

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.

Integrated geophysical investigations for the delineation of source and subsurface structure associated with hydro-uranium anomaly: A case study from South Purulia Shear Zone (SPSZ), India

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.

Mineral transformation and biomass accumulation associated with uranium bioremediation at Rifle, Colorado

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

Li, L.; Steefel, C.I.; Williams, K.H.

2009-04-20

Injection of organic carbon into the subsurface as an electron donor for bioremediation of redox-sensitive contaminants like uranium often leads to mineral transformation and biomass accumulation, both of which can alter the flow field and potentially bioremediation efficacy. This work combines reactive transport modeling with a column experiment and field measurements to understand the biogeochemical processes and to quantify the biomass and mineral transformation/accumulation during a bioremediation experiment at a uranium contaminated site near Rifle, Colorado. We use the reactive transport model CrunchFlow to explicitly simulate microbial community dynamics of iron and sulfate reducers, and their impacts on reaction rates.more » The column experiment shows clear evidence of mineral precipitation, primarily in the form of calcite and iron monosulfide. At the field scale, reactive transport simulations suggest that the biogeochemical reactions occur mostly close to the injection wells where acetate concentrations are highest, with mineral precipitate and biomass accumulation reaching as high as 1.5% of the pore space. This work shows that reactive transport modeling coupled with field data can be an effective tool for quantitative estimation of mineral transformation and biomass accumulation, thus improving the design of bioremediation strategies.« less

Mineral transformation and biomass accumulation associated with uranium bioremediation at Rifle, Colorado.

PubMed

Li, Li; Steefel, Carl I; Williams, Kenneth H; Wilkins, Michael J; Hubbard, Susan S

2009-07-15

Injection of organic carbon into the subsurface as an electron donor for bioremediation of redox-sensitive contaminants like uranium often leads to mineral transformation and biomass accumulation, both of which can alter the flow field and potentially bioremediation efficacy. This work combines reactive transport modeling with a column experiment and field measurements to understand the biogeochemical processes and to quantify the biomass and mineral transformation/accumulation during a bioremediation experiment at a uranium contaminated site near Rifle, Colorado. We use the reactive transport model CrunchFlow to explicitly simulate microbial community dynamics of iron and sulfate reducers, and their impacts on reaction rates. The column experiment shows clear evidence of mineral precipitation, primarily in the form of calcite and iron monosulfide. At the field scale, reactive transport simulations suggest that the biogeochemical reactions occur mostly close to the injection wells where acetate concentrations are highest, with mineral precipitate and biomass accumulation reaching as high as 1.5% of the pore space. This work shows that reactive transport modeling coupled with field data can bean effective tool for quantitative estimation of mineral transformation and biomass accumulation, thus improving the design of bioremediation strategies.

A Limited Microbial Consortium Is Responsible for Extended Bioreduction of Uranium in a Contaminated Aquifer ▿†

PubMed Central

Gihring, Thomas M.; Zhang, Gengxin; Brandt, Craig C.; Brooks, Scott C.; Campbell, James H.; Carroll, Susan; Criddle, Craig S.; Green, Stefan J.; Jardine, Phil; Kostka, Joel E.; Lowe, Kenneth; Mehlhorn, Tonia L.; Overholt, Will; Watson, David B.; Yang, Zamin; Wu, Wei-Min; Schadt, Christopher W.

2011-01-01

Subsurface amendments of slow-release substrates (e.g., emulsified vegetable oil [EVO]) are thought to be a pragmatic alternative to using short-lived, labile substrates for sustained uranium bioimmobilization within contaminated groundwater systems. Spatial and temporal dynamics of subsurface microbial communities during EVO amendment are unknown and likely differ significantly from those of populations stimulated by soluble substrates, such as ethanol and acetate. In this study, a one-time EVO injection resulted in decreased groundwater U concentrations that remained below initial levels for approximately 4 months. Pyrosequencing and quantitative PCR of 16S rRNA from monitoring well samples revealed a rapid decline in groundwater bacterial community richness and diversity after EVO injection, concurrent with increased 16S rRNA copy levels, indicating the selection of a narrow group of taxa rather than a broad community stimulation. Members of the Firmicutes family Veillonellaceae dominated after injection and most likely catalyzed the initial oil decomposition. Sulfate-reducing bacteria from the genus Desulforegula, known for long-chain fatty acid oxidation to acetate, also dominated after EVO amendment. Acetate and H2 production during EVO degradation appeared to stimulate NO3−, Fe(III), U(VI), and SO42− reduction by members of the Comamonadaceae, Geobacteriaceae, and Desulfobacterales. Methanogenic archaea flourished late to comprise over 25% of the total microbial community. Bacterial diversity rebounded after 9 months, although community compositions remained distinct from the preamendment conditions. These results demonstrated that a one-time EVO amendment served as an effective electron donor source for in situ U(VI) bioreduction and that subsurface EVO degradation and metal reduction were likely mediated by successive identifiable guilds of organisms. PMID:21764967

A limited microbial consortium is responsible for extended bioreduction of uranium in a contaminated aquifer.

PubMed

Gihring, Thomas M; Zhang, Gengxin; Brandt, Craig C; Brooks, Scott C; Campbell, James H; Carroll, Susan; Criddle, Craig S; Green, Stefan J; Jardine, Phil; Kostka, Joel E; Lowe, Kenneth; Mehlhorn, Tonia L; Overholt, Will; Watson, David B; Yang, Zamin; Wu, Wei-Min; Schadt, Christopher W

2011-09-01

Subsurface amendments of slow-release substrates (e.g., emulsified vegetable oil [EVO]) are thought to be a pragmatic alternative to using short-lived, labile substrates for sustained uranium bioimmobilization within contaminated groundwater systems. Spatial and temporal dynamics of subsurface microbial communities during EVO amendment are unknown and likely differ significantly from those of populations stimulated by soluble substrates, such as ethanol and acetate. In this study, a one-time EVO injection resulted in decreased groundwater U concentrations that remained below initial levels for approximately 4 months. Pyrosequencing and quantitative PCR of 16S rRNA from monitoring well samples revealed a rapid decline in groundwater bacterial community richness and diversity after EVO injection, concurrent with increased 16S rRNA copy levels, indicating the selection of a narrow group of taxa rather than a broad community stimulation. Members of the Firmicutes family Veillonellaceae dominated after injection and most likely catalyzed the initial oil decomposition. Sulfate-reducing bacteria from the genus Desulforegula, known for long-chain fatty acid oxidation to acetate, also dominated after EVO amendment. Acetate and H(2) production during EVO degradation appeared to stimulate NO(3)(-), Fe(III), U(VI), and SO(4)(2-) reduction by members of the Comamonadaceae, Geobacteriaceae, and Desulfobacterales. Methanogenic archaea flourished late to comprise over 25% of the total microbial community. Bacterial diversity rebounded after 9 months, although community compositions remained distinct from the preamendment conditions. These results demonstrated that a one-time EVO amendment served as an effective electron donor source for in situ U(VI) bioreduction and that subsurface EVO degradation and metal reduction were likely mediated by successive identifiable guilds of organisms.

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

Code of Federal Regulations, 2013 CFR

2013-07-01

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

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

Code of Federal Regulations, 2012 CFR

2012-07-01

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

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

Code of Federal Regulations, 2014 CFR

2014-07-01

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

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

Code of Federal Regulations, 2011 CFR

2011-07-01

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

Deep Vadose Zone Treatability Test for the Hanford Central Plateau: Interim Post-Desiccation Monitoring Results, Fiscal Year 2014

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

Truex, Michael J.; Strickland, Christopher E.; Johnson, Christian D.

Over decades of operation, the U.S. Department of Energy (DOE) and its predecessors have released nearly 2 trillion L (450 billion gal.) of liquid into the vadose zone at the Hanford Site. Much of this discharge of liquid waste into the vadose zone occurred in the Central Plateau, a 200 km 2 (75 mi 2) area that includes approximately 800 waste sites. Some of the inorganic and radionuclide contaminants in the deep vadose zone at the Hanford Site are at depths below the limit of direct exposure pathways, but may need to be remediated to protect groundwater. The Tri-Party Agenciesmore » (DOE, U.S. Environmental Protection Agency, and Washington State Department of Ecology) established Milestone M 015 50, which directed DOE to submit a treatability test plan for remediation of technetium-99 (Tc-99) and uranium in the deep vadose zone. These contaminants are mobile in the subsurface environment and have been detected at high concentrations deep in the vadose zone, and at some locations have reached groundwater. Testing technologies for remediating Tc-99 and uranium will also provide information relevant for remediating other contaminants in the vadose zone. A field test of desiccation is being conducted as an element of the DOE test plan published in March 2008 to meet Milestone M 015 50. The active desiccation portion of the test has been completed. Monitoring data have been collected at the field test site during the post-desiccation period and are reported herein. This is an interim data summary report that includes about 3 years of post-desiccation monitoring data. The DOE field test plan proscribes a total of 5 years of post-desiccation monitoring.« less

Remediation of subsurface and groundwater contamination with uranium from fuel fabrication facilities at Hanau (Germany)

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

Nitzsche, Olaf; Thierfeldt, Stefan; Hummel, Lothar

2013-07-01

This paper presents aspects of site decommissioning and clearance of a former fuel fabrication facility (development and production of fuel assemblies for research reactors and HTR) at Hanau (Germany). The main pathways for environmental contamination were deposition on soil surface and topsoil and pollution of deep soil and the aquifer by waste water channel leakage. Soil excavation could be done by classical excavator techniques. An effective removal of material from the saturated zone was possible by using advanced drilling techniques. A large amount of demolished building structure and excavated soil had to be classified. Therefore the use of conveyor detectormore » was necessary. Nearly 100000 Mg of material (excavated soil and demolished building material) were disposed of at an underground mine. A remaining volume of 700 m{sup 3} was classified as radioactive waste. Site clearance started in 2006. Groundwater remediation and monitoring is still ongoing, but has already provided excellent results by reducing the remaining Uranium considerably. (authors)« less

INNOVATIVE PROCESSES FOR RECLAMATION OF CONTAMINATED SUBSURFACE ENVIRONMENTS

EPA Science Inventory

Research to better assess the capabilities and limitations of fixed-film bioreactors for removing selected organic contaminants from ground water or from contaminated vapor streams produced by air stripping of polluted ground water and by soil venting operations is described. ...

Controls on radium transport by adsorption to iron minerals

NASA Astrophysics Data System (ADS)

Chen, M.; Wang, T.; Kocar, B. D.

2015-12-01

Radium is a naturally occurring radioactive metal found in many subsurface environments. Radium isotopes are generated by uranium and thorium decay, and are particularly abundant within groundwaters where minimal porewater flux leads to accumulation. These isotopes are used as natural tracers for estimating submarine groundwater discharge (SGD) [1], allowing for large scale estimation of GW fluxes into and out of the ocean [2]. They also represent a substantial hazard in wastewater produced after hydraulic fracturing for natural gas extraction [3], resulting in a significant risk of environmental release to surface and near-surface waters, and increased cost for water treatment or disposal. Adsorption to mineral surfaces represents a dominant pathway of radium retention in subsurface environments. For SGD studies, adsorption processes impact estimates of GW fluxes, while in hydraulic fracturing, radium adsorption to aquifer solids mediates wastewater radium activities. Analysis of past sorption studies revealed large variability in partition coefficients [4], while examination of radium adsorption kinetics and surface complexation have only recently started [5]. Accordingly, we present the results of sorption and column experiments of radium with a suite of iron minerals representative of those found within deep saline and near-surface (freshwater) aquifers, and evaluate impacts of varying salinity solutions through artificial waters. Further, we explore the impacts of pyrite oxidation and ferrihydrite transformation to other iron-bearing secondary minerals on the transport and retention of radium. These results will provide critical information on the mineralogical controls on radium retention in subsurface environments, and will therefore improve predictions of radium groundwater transport in natural and contaminated systems. [1] Charette, M.A., Buesseler, K.O. & Andrews, J.E., Limnol. Oceanogr. (2001). [2] Moore, W.S., Ann. Rev. Mar. Sci. (2010). [3] Vengosh, A. et al. Environ. Sci. Technol., (2014). [4] Beck, A., Cochran, M., Marine Chem., (2013). [5] Sajih, M. et al. Geochim. Cosmochim. AC. (2014).

In-situ evidence for uranium immobilization and remobilization

USGS Publications Warehouse

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.

Deep subsurface microbial processes

USGS Publications Warehouse

Lovley, D.R.; Chapelle, F.H.

1995-01-01

Information on the microbiology of the deep subsurface is necessary in order to understand the factors controlling the rate and extent of the microbially catalyzed redox reactions that influence the geophysical properties of these environments. Furthermore, there is an increasing threat that deep aquifers, an important drinking water resource, may be contaminated by man's activities, and there is a need to predict the extent to which microbial activity may remediate such contamination. Metabolically active microorganisms can be recovered from a diversity of deep subsurface environments. The available evidence suggests that these microorganisms are responsible for catalyzing the oxidation of organic matter coupled to a variety of electron acceptors just as microorganisms do in surface sediments, but at much slower rates. The technical difficulties in aseptically sampling deep subsurface sediments and the fact that microbial processes in laboratory incubations of deep subsurface material often do not mimic in situ processes frequently necessitate that microbial activity in the deep subsurface be inferred through nonmicrobiological analyses of ground water. These approaches include measurements of dissolved H2, which can predict the predominant microbially catalyzed redox reactions in aquifers, as well as geochemical and groundwater flow modeling, which can be used to estimate the rates of microbial processes. Microorganisms recovered from the deep subsurface have the potential to affect the fate of toxic organics and inorganic contaminants in groundwater. Microbial activity also greatly influences 1 the chemistry of many pristine groundwaters and contributes to such phenomena as porosity development in carbonate aquifers, accumulation of undesirably high concentrations of dissolved iron, and production of methane and hydrogen sulfide. Although the last decade has seen a dramatic increase in interest in deep subsurface microbiology, in comparison with the study of other habitats, the study of deep subsurface microbiology is still in its infancy.

Microfluidic Experiments Studying Pore Scale Interactions of Microbes and Geochemistry

NASA Astrophysics Data System (ADS)

Chen, M.; Kocar, B. D.

2016-12-01

Understanding how physical phenomena, chemical reactions, and microbial behavior interact at the pore-scale is crucial to understanding larger scale trends in groundwater chemistry. Recent studies illustrate the utility of microfluidic devices for illuminating pore-scale physical-biogeochemical processes and their control(s) on the cycling of iron, uranium, and other important elements 1-3. These experimental systems are ideal for examining geochemical reactions mediated by microbes, which include processes governed by complex biological phenomenon (e.g. biofilm formation, etc.)4. We present results of microfluidic experiments using a model metal reducing bacteria and varying pore geometries, exploring the limitations of the microorganisms' ability to access tight pore spaces, and examining coupled biogeochemical-physical controls on the cycling of redox sensitive metals. Experimental results will provide an enhanced understanding of coupled physical-biogeochemical processes transpiring at the pore-scale, and will constrain and compliment continuum models used to predict and describe the subsurface cycling of redox-sensitive elements5. 1. Vrionis, H. A. et al. Microbiological and geochemical heterogeneity in an in situ uranium bioremediation field site. Appl. Environ. Microbiol. 71, 6308-6318 (2005). 2. Pearce, C. I. et al. Pore-scale characterization of biogeochemical controls on iron and uranium speciation under flow conditions. Environ. Sci. Technol. 46, 7992-8000 (2012). 3. Zhang, C., Liu, C. & Shi, Z. Micromodel investigation of transport effect on the kinetics of reductive dissolution of hematite. Environ. Sci. Technol. 47, 4131-4139 (2013). 4. Ginn, T. R. et al. Processes in microbial transport in the natural subsurface. Adv. Water Resour. 25, 1017-1042 (2002). 5. Scheibe, T. D. et al. Coupling a genome-scale metabolic model with a reactive transport model to describe in situ uranium bioremediation. Microb. Biotechnol. 2, 274-286 (2009).

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.

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

NASA Astrophysics Data System (ADS)

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

2012-12-01

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

STATE WATER RESOURCES RESEARCH INSTITUTE PROGRAM: GROUND WATER RESEARCH.

USGS Publications Warehouse

Burton, James S.; ,

1985-01-01

This paper updates a review of the accomplishments of the State Water Resources Research Program in ground water contamination research. The aim is to assess the progress made towards understanding the mechanisms of ground water contamination and based on this understanding, to suggest procedures for the prevention and control of ground water contamination. The following research areas are covered: (1) mechanisms of organic contaminant transport in the subsurface environment; (2) bacterial and viral contamination of ground water from landfills and septic tank systems; (3) fate and persistence of pesticides in the subsurface; (4) leachability and transport of ground water pollutants from coal production and utilization; and (5) pollution of ground water from mineral mining activities.

Viral Tracer Studies Indicate Contamination of Marine Waters by Sewage Disposal Practices in Key Largo, Florida

PubMed Central

Paul, J. H.; Rose, J. B.; Brown, J.; Shinn, E. A.; Miller, S.; Farrah, S. R.

1995-01-01

Domestic wastewater disposal practices in the Florida Keys are primarily limited to on-site disposal systems such as septic tanks, injection wells, and illegal cesspits. Poorly treated sewage is thus released into the highly porous subsurface Key Largo limestone matrix. To investigate the fate and transport of sewage in the subsurface environment and the potential for contamination of marine surface waters, we employed bacteriophages as tracers in a domestic septic system and a simulated injection well in Key Largo, Florida. Transport of bacteriophage (Phi)HSIC-1 from the septic tank to adjacent surface canal waters and outstanding marine waters occurred in as little as 11 and 23 h, respectively. Transport of the Salmonella phage PRD1 from the simulated injection well to a canal adjacent to the injection site occurred in 11.2 h. Estimated rates of migration of viral tracers ranged from 0.57 to 24.2 m/h, over 500-fold greater than flow rates measured previously by subsurface flow meters in similar environments. These results suggest that current on-site disposal practices can lead to contamination of the subsurface and surface marine waters in the Keys. PMID:16535046

Viral tracer studies indicate contamination of marine waters by sewage disposal practices in key largo, Florida.

PubMed

Paul, J H; Rose, J B; Brown, J; Shinn, E A; Miller, S; Farrah, S R

1995-06-01

Domestic wastewater disposal practices in the Florida Keys are primarily limited to on-site disposal systems such as septic tanks, injection wells, and illegal cesspits. Poorly treated sewage is thus released into the highly porous subsurface Key Largo limestone matrix. To investigate the fate and transport of sewage in the subsurface environment and the potential for contamination of marine surface waters, we employed bacteriophages as tracers in a domestic septic system and a simulated injection well in Key Largo, Florida. Transport of bacteriophage (Phi)HSIC-1 from the septic tank to adjacent surface canal waters and outstanding marine waters occurred in as little as 11 and 23 h, respectively. Transport of the Salmonella phage PRD1 from the simulated injection well to a canal adjacent to the injection site occurred in 11.2 h. Estimated rates of migration of viral tracers ranged from 0.57 to 24.2 m/h, over 500-fold greater than flow rates measured previously by subsurface flow meters in similar environments. These results suggest that current on-site disposal practices can lead to contamination of the subsurface and surface marine waters in the Keys.

Time series analysis of contaminant transport in the subsurface: applications to conservative tracer and engineered nanomaterials.

PubMed

Bai, Chunmei; Li, Yusong

2014-08-01

Accurately predicting the transport of contaminants in the field is subject to multiple sources of uncertainty due to the variability of geological settings, the complexity of field measurements, and the scarcity of data. Such uncertainties can be amplified when modeling some emerging contaminants, such as engineered nanomaterials, when a fundamental understanding of their fate and transport is lacking. Typical field work includes collecting concentration at a certain location for an extended period of time, or measuring the movement of plume for an extended period time, which would result in a time series of observation data. This work presents an effort to evaluate the possibility of applying time series analysis, particularly, autoregressive integrated moving average (ARIMA) models, to forecast contaminant transport and distribution in the subsurface environment. ARIMA modeling was first assessed in terms of its capability to forecast tracer transport at two field sites, which had different levels of heterogeneity. After that, this study evaluated the applicability of ARIMA modeling to predict the transport of engineered nanomaterials at field sites, including field measured data of nanoscale zero valent iron and (nZVI) and numerically generated data for the transport of nano-fullerene aggregates (nC60). This proof-of-concept effort demonstrates the possibility of applying ARIMA to predict the contaminant transport in the subsurface environment. Like many other statistical models, ARIMA modeling is only descriptive and not explanatory. The limitation and the challenge associated with applying ARIMA modeling to contaminant transport in the subsurface are also discussed. Copyright © 2014 Elsevier B.V. All rights reserved.

Time series analysis of contaminant transport in the subsurface: Applications to conservative tracer and engineered nanomaterials

NASA Astrophysics Data System (ADS)

Bai, Chunmei; Li, Yusong

2014-08-01

Accurately predicting the transport of contaminants in the field is subject to multiple sources of uncertainty due to the variability of geological settings, the complexity of field measurements, and the scarcity of data. Such uncertainties can be amplified when modeling some emerging contaminants, such as engineered nanomaterials, when a fundamental understanding of their fate and transport is lacking. Typical field work includes collecting concentration at a certain location for an extended period of time, or measuring the movement of plume for an extended period time, which would result in a time series of observation data. This work presents an effort to evaluate the possibility of applying time series analysis, particularly, autoregressive integrated moving average (ARIMA) models, to forecast contaminant transport and distribution in the subsurface environment. ARIMA modeling was first assessed in terms of its capability to forecast tracer transport at two field sites, which had different levels of heterogeneity. After that, this study evaluated the applicability of ARIMA modeling to predict the transport of engineered nanomaterials at field sites, including field measured data of nanoscale zero valent iron and (nZVI) and numerically generated data for the transport of nano-fullerene aggregates (nC60). This proof-of-concept effort demonstrates the possibility of applying ARIMA to predict the contaminant transport in the subsurface environment. Like many other statistical models, ARIMA modeling is only descriptive and not explanatory. The limitation and the challenge associated with applying ARIMA modeling to contaminant transport in the subsurface are also discussed.

Monitoring radionuclides in subsurface drinking water sources near unconventional drilling operations: a pilot study.

PubMed

Nelson, Andrew W; Knight, Andrew W; Eitrheim, Eric S; Schultz, Michael K

2015-04-01

Unconventional drilling (the combination of hydraulic fracturing and horizontal drilling) to extract oil and natural gas is expanding rapidly around the world. The rate of expansion challenges scientists and regulators to assess the risks of the new technologies on drinking water resources. One concern is the potential for subsurface drinking water resource contamination by naturally occurring radioactive materials co-extracted during unconventional drilling activities. Given the rate of expansion, opportunities to test drinking water resources in the pre- and post-fracturing setting are rare. This pilot study investigated the levels of natural uranium, lead-210, and polonium-210 in private drinking wells within 2000 m of a large-volume hydraulic fracturing operation--before and approximately one-year following the fracturing activities. Observed radionuclide concentrations in well waters tested did not exceed maximum contaminant levels recommended by state and federal agencies. No statistically-significant differences in radionuclide concentrations were observed in well-water samples collected before and after the hydraulic fracturing activities. Expanded monitoring of private drinking wells before and after hydraulic fracturing activities is needed to develop understanding of the potential for drinking water resource contamination from unconventional drilling and gas extraction activities. Copyright © 2015 Elsevier Ltd. All rights reserved.

Armored Enzyme Nanoparticles for Remediation of Subsurface

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

Grate, Jay W.

2005-09-01

The remediation of subsurface contaminants is a critical problem for the Department of Energy, other government agencies, and our nation. Severe contamination of soil and groundwater exists at several DOE sites due to various methods of intentional and unintentional release. Given the difficulties involved in conventional removal or separation processes, it is vital to develop methods to transform contaminants and contaminated earth/water to reduce risks to human health and the environment. Transformation of the contaminants themselves may involve conversion to other immobile species that do not migrate into well water or surface waters, as is proposed for metals and radionuclides;more » or degradation to harmless molecules, as is desired for organic contaminants. Transformation of contaminated earth (as opposed to the contaminants themselves) may entail reductions in volume or release of bound contaminants for remediation.« less

RESEARCH ACTIVITIES AT U.S. GOVERNMENT AGENCIES IN SUBSURFACE REACTIVE TRANSPORT MODELING

EPA Science Inventory

The fate of contaminants in the environment is controlled by both chemical reactions and transport phenomena in the subsurface. Our ability to understand the significance of these processes over time requires an accurate conceptual model that incorporates the various mechanisms ...

Integrated Geophysical Measurements for Bioremediation Monitoring: Combining Spectral Induced Polarization, Nuclear Magnetic Resonance and Magnetic Methods

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

Keating, Kristina; Slater, Lee; Ntarlagiannis, Dimitris

2015-02-24

This documents contains the final report for the project "Integrated Geophysical Measurements for Bioremediation Monitoring: Combining Spectral Induced Polarization, Nuclear Magnetic Resonance and Magnetic Methods" (DE-SC0007049) Executive Summary: Our research aimed to develop borehole measurement techniques capable of monitoring subsurface processes, such as changes in pore geometry and iron/sulfur geochemistry, associated with remediation of heavy metals and radionuclides. Previous work has demonstrated that geophysical method spectral induced polarization (SIP) can be used to assess subsurface contaminant remediation; however, SIP signals can be generated from multiple sources limiting their interpretation value. Integrating multiple geophysical methods, such as nuclear magnetic resonance (NMR)more » and magnetic susceptibility (MS), with SIP, could reduce the ambiguity of interpretation that might result from a single method. Our research efforts entails combining measurements from these methods, each sensitive to different mineral forms and/or mineral-fluid interfaces, providing better constraints on changes in subsurface biogeochemical processes and pore geometries significantly improving our understanding of processes impacting contaminant remediation. The Rifle Integrated Field Research Challenge (IFRC) site was used as a test location for our measurements. The Rifle IFRC site is located at a former uranium ore-processing facility in Rifle, Colorado. Leachate from spent mill tailings has resulted in residual uranium contamination of both groundwater and sediments within the local aquifer. Studies at the site include an ongoing acetate amendment strategy, native microbial populations are stimulated by introduction of carbon intended to alter redox conditions and immobilize uranium. To test the geophysical methods in the field, NMR and MS logging measurements were collected before, during, and after acetate amendment. Next, laboratory NMR, MS, and SIP measurements were collected on columns of Rifle sediments during acetate amendment. The laboratory experiments were designed to simulate the field experiments; changes in geophysical signals were expected to correlate with changes in redox conditions and iron speciation. Field MS logging measurements revealed vertically stratified magnetic mineralization, likely the result of detrital magnetic fraction within the bulk alluvium. Little to no change was observed in the MS data suggesting negligible production of magnetic phases (e.g. magnetite, pyrrhotite) as a result of sulfidogenesis. Borehole NMR measurements contained high levels of noise contamination requiring significant signal processing, and analysis suggests that any changes may be difficult to differentiate from simultaneous changes in water content. Laboratory MS and NMR measurements remained relatively stable throughout the course of the acetate amendment experiment, consistent with field measurements. However, SIP measurements changed during the acetate amendment associated with the formation of iron-sulfide mineral phases; a finding that is consistent with chemical analysis of the solid phase materials in the columns.« less

Effects of nitrate on the stability of uranium in a bioreduced region of the subsurface.

PubMed

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.

Characterization of Uranium Contamination, Transport, and Remediation at Rocky Flats - Across Remediation into Post-Closure

NASA Astrophysics Data System (ADS)

Janecky, D. R.; Boylan, J.; Murrell, M. T.

2009-12-01

The Rocky Flats Site is a former nuclear weapons production facility approximately 16 miles northwest of Denver, Colorado. Built in 1952 and operated by the Atomic Energy Commission and then Department of Energy, the Site was remediated and closed in 2005, and is currently undergoing long-term surveillance and monitoring by the DOE Office of Legacy Management. Areas of contamination resulted from roughly fifty years of operation. Of greatest interest, surface soils were contaminated with plutonium, americium, and uranium; groundwater was contaminated with chlorinated solvents, uranium, and nitrates; and surface waters, as recipients of runoff and shallow groundwater discharge, have been contaminated by transport from both regimes. A region of economic mineralization that has been referred to as the Colorado Mineral Belt is nearby, and the Schwartzwalder uranium mine is approximately five miles upgradient of the Site. Background uranium concentrations are therefore elevated in many areas. Weapons-related activities included work with enriched and depleted uranium, contributing anthropogenic content to the environment. Using high-resolution isotopic analyses, Site-related contamination can be distinguished from natural uranium in water samples. This has been instrumental in defining remedy components, and long-term monitoring and surveillance strategies. Rocky Flats hydrology interlinks surface waters and shallow groundwater (which is very limited in volume and vertical and horizontal extent). Surface water transport pathways include several streams, constructed ponds, and facility surfaces. Shallow groundwater has no demonstrated connection to deep aquifers, and includes natural preferential pathways resulting primarily from porosity in the Rocky Flats alluvium, weathered bedrock, and discontinuous sandstones. In addition, building footings, drains, trenches, and remedial systems provide pathways for transport at the site. Removal of impermeable surfaces (buildings, roads, and so on) during the Site closure efforts resulted in major changes to surface and shallow groundwater flow. Consistent with previous documentation of uranium operations and contamination, only very small amounts of highly enriched uranium are found in a small number of water samples, generally from the former Solar Ponds complex and central Industrial Area. Depleted uranium is more widely distributed at the site, and water samples exhibit the full range of depleted plus natural uranium mixtures. However, one third of the samples are found to contain only natural uranium, and three quarters of the samples are found to contain more than 90% natural uranium - substantial fractions given that the focus of these analyses was on evaluating potentially contaminated waters. Following site closure, uranium concentrations have increased at some locations, particularly for surface water samples. Overall, isotopic ratios at individual locations have been relatively consistent, indicating that the increases in concentrations are due to decreases in dilution flow following removal of impermeable surfaces and buildings.

76 FR 5370 - Potential Addition of Vapor Intrusion Component to the Hazard Ranking System

Federal Register 2010, 2011, 2012, 2013, 2014

2011-01-31

... structures through the subsurface environment and thus, enabling sites with vapor intrusion contamination to... contamination to be included in an HRS evaluation. Presented below is background information on the HRS, its... facility, the potential for contamination of drinking water supplies, direct human contact, destruction of...

Final Technical Report

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

Sobecky, Patricia A; Taillefert, Martial

This final technical report describes results and findings from a research project to examine the role of microbial phosphohydrolase enzymes in naturally occurring subsurface microorganisms for the purpose of promoting the immobilization of the radionuclide uranium through the production of insoluble uranium phosphate minerals. The research project investigated the microbial mechanisms and the physical and chemical processes promoting uranium biomineralization and sequestration in oxygenated subsurface soils. Uranium biomineralization under aerobic conditions can provide a secondary biobarrier strategy to immobilize radionuclides should the metal precipitates formed by microbial dissimilatory mechanisms remobilize due to a change in redox state.

Molybdenum Availability Is Key to Nitrate Removal in Contaminated Groundwater Environments

PubMed Central

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

2015-01-01

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

Pore-scale characterization of biogeochemical controls on iron and uranium speciation under flow conditions.

PubMed

Pearce, Carolyn I; Wilkins, Michael J; Zhang, Changyong; Heald, Steve M; Fredrickson, Jim K; Zachara, John M

2012-08-07

Etched silicon microfluidic pore network models (micromodels) with controlled chemical and redox gradients, mineralogy, and microbiology under continuous flow conditions are used for the incremental development of complex microenvironments that simulate subsurface conditions. We demonstrate the colonization of micromodel pore spaces by an anaerobic Fe(III)-reducing bacterial species (Geobacter sulfurreducens) and the enzymatic reduction of a bioavailable Fe(III) phase within this environment. Using both X-ray microprobe and X-ray absorption spectroscopy, we investigate the combined effects of the precipitated Fe(III) phases and the microbial population on uranium biogeochemistry under flow conditions. Precipitated Fe(III) phases within the micromodel were most effectively reduced in the presence of an electron shuttle (AQDS), and Fe(II) ions adsorbed onto the precipitated mineral surface without inducing any structural change. In the absence of Fe(III), U(VI) was effectively reduced by the microbial population to insoluble U(IV), which was precipitated in discrete regions associated with biomass. In the presence of Fe(III) phases, however, both U(IV) and U(VI) could be detected associated with biomass, suggesting reoxidation of U(IV) by localized Fe(III) phases. These results demonstrate the importance of the spatial localization of biomass and redox active metals, and illustrate the key effects of pore-scale processes on contaminant fate and reactive transport.

Transformation of zinc-concentrate in surface and subsurface environments: Implications for assessing zinc mobility/toxicity and choosing an optimal remediation strategy.

PubMed

Kwon, Man Jae; Boyanov, Maxim I; Yang, Jung-Seok; Lee, Seunghak; Hwang, Yun Ho; Lee, Ju Yeon; Mishra, Bhoopesh; Kemner, Kenneth M

2017-07-01

Zinc contamination in near- and sub-surface environments is a serious threat to many ecosystems and to public health. Sufficient understanding of Zn speciation and transport mechanisms is therefore critical to evaluating its risk to the environment and to developing remediation strategies. The geochemical and mineralogical characteristics of contaminated soils in the vicinity of a Zn ore transportation route were thoroughly investigated using a variety of analytical techniques (sequential extraction, XRF, XRD, SEM, and XAFS). Imported Zn-concentrate (ZnS) was deposited in a receiving facility and dispersed over time to the surrounding roadside areas and rice-paddy soils. Subsequent physical and chemical weathering resulted in dispersal into the subsurface. The species identified in the contaminated areas included Zn-sulfide, Zn-carbonate, other O-coordinated Zn-minerals, and Zn species bound to Fe/Mn oxides or clays, as confirmed by XAFS spectroscopy and sequential extraction. The observed transformation from S-coordinated Zn to O-coordinated Zn associated with minerals suggests that this contaminant can change into more soluble and labile forms as a result of weathering. For the purpose of developing a soil washing remediation process, the contaminated samples were extracted with dilute acids. The extraction efficiency increased with the increase of O-coordinated Zn relative to S-coordinated Zn in the sediment. This study demonstrates that improved understanding of Zn speciation in contaminated soils is essential for well-informed decision making regarding metal mobility and toxicity, as well as for choosing an appropriate remediation strategy using soil washing. Copyright © 2017 Elsevier Ltd. All rights reserved.

Transformation of zinc-concentrate in surface and subsurface environments: Implications for assessing zinc mobility/toxicity and choosing an optimal remediation strategy

DOE PAGES

Kwon, Man Jae; Boyanov, Maxim I.; Yang, Jung -Seok; ...

2017-03-24

Zinc contamination in near- and sub-surface environments is a serious threat to many ecosystems and to public health. Sufficient understanding of Zn speciation and transport mechanisms is therefore critical to evaluating its risk to the environment and to developing remediation strategies. The geochemical and mineralogical characteristics of contaminated soils in the vicinity of a Zn ore transportation route were thoroughly investigated using a variety of analytical techniques (sequential extraction, XRF, XRD, SEM, and XAFS). Imported Zn-concentrate (ZnS) was deposited in a receiving facility and dispersed over time to the surrounding roadside areas and rice-paddy soils. Subsequent physical and chemical weatheringmore » resulted in dispersal into the subsurface. The species identified in the contaminated areas included Zn-sulfide, Zn-carbonate, other O-coordinated Zn-minerals, and Zn species bound to Fe/Mn oxides or clays, as confirmed by XAFS spectroscopy and sequential extraction. The observed transformation from S-coordinated Zn to O-coordinated Zn associated with minerals suggests that this contaminant can change into more soluble and labile forms as a result of weathering. For the purpose of developing a soil washing remediation process, the contaminated samples were extracted with dilute acids. The extraction efficiency increased with the increase of O-coordinated Zn relative to S-coordinated Zn in the sediment. Furthermore, this study demonstrates that improved understanding of Zn speciation in contaminated soils is essential for well-informed decision making regarding metal mobility and toxicity, as well as for choosing an appropriate remediation strategy using soil washing.« less

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

PubMed

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

2017-09-01

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

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

Microplastics and Nanoplastics in Aquatic Environments: Aggregation, Deposition, and Enhanced Contaminant Transport.

PubMed

Alimi, Olubukola S; Farner Budarz, Jeffrey; Hernandez, Laura M; Tufenkji, Nathalie

2018-02-20

Plastic litter is widely acknowledged as a global environmental threat, and poor management and disposal lead to increasing levels in the environment. Of recent concern is the degradation of plastics from macro- to micro- and even to nanosized particles smaller than 100 nm in size. At the nanoscale, plastics are difficult to detect and can be transported in air, soil, and water compartments. While the impact of plastic debris on marine and fresh waters and organisms has been studied, the loads, transformations, transport, and fate of plastics in terrestrial and subsurface environments are largely overlooked. In this Critical Review, we first present estimated loads of plastics in different environmental compartments. We also provide a critical review of the current knowledge vis-à-vis nanoplastic (NP) and microplastic (MP) aggregation, deposition, and contaminant cotransport in the environment. Important factors that affect aggregation and deposition in natural subsurface environments are identified and critically analyzed. Factors affecting contaminant sorption onto plastic debris are discussed, and we show how polyethylene generally exhibits a greater sorption capacity than other plastic types. Finally, we highlight key knowledge gaps that need to be addressed to improve our ability to predict the risks associated with these ubiquitous contaminants in the environment by understanding their mobility, aggregation behavior and their potential to enhance the transport of other pollutants.

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

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

GANDER MJ; LEARY KD; LEVITT MT

2011-01-14

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

Subsurface Contamination Control

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

Y. Yuan

There are two objectives of this report, ''Subsurface Contamination Control''. The first is to provide a technical basis for recommending limiting radioactive contamination levels (LRCL) on the external surfaces of waste packages (WP) for acceptance into the subsurface repository. The second is to provide an evaluation of the magnitude of potential releases from a defective WP and the detectability of the released contents. The technical basis for deriving LRCL has been established in ''Retrieval Equipment and Strategy for Wp on Pallet'' (CRWMS M and O 2000g, 6.3.1). This report updates the derivation by incorporating the latest design information of themore » subsurface repository for site recommendation. The derived LRCL on the external surface of WPs, therefore, supercede that described in CRWMS M and O 2000g. The derived LRCL represent the average concentrations of contamination on the external surfaces of each WP that must not be exceeded before the WP is to be transported to the subsurface facility for emplacement. The evaluation of potential releases is necessary to control the potential contamination of the subsurface repository and to detect prematurely failed WPs. The detection of failed WPs is required in order to provide reasonable assurance that the integrity of each WP is intact prior to MGR closure. An emplaced WP may become breached due to manufacturing defects or improper weld combined with failure to detect the defect, by corrosion, or by mechanical penetration due to accidents or rockfall conditions. The breached WP may release its gaseous and volatile radionuclide content to the subsurface environment and result in contaminating the subsurface facility. The scope of this analysis is limited to radioactive contaminants resulting from breached WPs during the preclosure period of the subsurface repository. This report: (1) documents a method for deriving LRCL on the external surfaces of WP for acceptance into the subsurface repository; (2) provides a table of derived LRCL for nuclides of radiological importance; (3) Provides an as low as is reasonably achievable (ALARA) evaluation of the derived LRCL by comparing potential onsite and offsite doses to documented ALARA requirements; (4) Provides a method for estimating potential releases from a defective WP; (5) Provides an evaluation of potential radioactive releases from a defective WP that may become airborne and result in contamination of the subsurface facility; and (6) Provides a preliminary analysis of the detectability of a potential WP leak to support the design of an airborne release monitoring system.« less

Advances in Multiphase Flow and Transport in the Subsurface Environment

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

Shi, Xiaoqing; Finsterle, Stefan; Zhang, Keni

Multiphase flow and transport processes in the subsurface environment are extremely important in a number of industrial and environmental applications at various spatial and temporal scales. Thus, it is necessary to identify, understand, and predict these processes to improve the production of conventional and unconventional oil and gas, to increase the safety of geological sequestration of carbon dioxide and nuclear waste disposal, and to make remediation of contaminated aquifers more effective.

Advances in Multiphase Flow and Transport in the Subsurface Environment

DOE PAGES

Shi, Xiaoqing; Finsterle, Stefan; Zhang, Keni; ...

2018-03-04

Multiphase flow and transport processes in the subsurface environment are extremely important in a number of industrial and environmental applications at various spatial and temporal scales. Thus, it is necessary to identify, understand, and predict these processes to improve the production of conventional and unconventional oil and gas, to increase the safety of geological sequestration of carbon dioxide and nuclear waste disposal, and to make remediation of contaminated aquifers more effective.

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2013 CFR

2013-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2012 CFR

2012-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

40 CFR 141.55 - Maximum contaminant level goals for radionuclides.

Code of Federal Regulations, 2014 CFR

2014-07-01

... radionuclides. 141.55 Section 141.55 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) WATER PROGRAMS (CONTINUED) NATIONAL PRIMARY DRINKING WATER REGULATIONS Maximum Contaminant Level Goals and... and radium-228 Zero. 2. Gross alpha particle activity (excluding radon and uranium) Zero. 3. Beta...

Iron Mineralogy and Uranium-Binding Environment in the Rhizosphere of a Wetland Soil

EPA Science Inventory

Wetlands mitigate the migration of groundwater contaminants through a series of biogeochemical gradients that enhance multiple contaminant-binding processes. The hypothesis of this study was that wetland plant roots contribute organic carbon and release O₂ within the ...

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

PubMed

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

2017-05-01

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

Molybdenum Availability Is Key to Nitrate Removal in Contaminated Groundwater Environments

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

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

2015-05-15

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

Phytoforensics—Using trees to find contamination

USGS Publications Warehouse

Wilson, Jordan L.

2017-09-28

The water we drink, air we breathe, and soil we come into contact with have the potential to adversely affect our health because of contaminants in the environment. Environmental samples can characterize the extent of potential contamination, but traditional methods for collecting water, air, and soil samples below the ground (for example, well drilling or direct-push soil sampling) are expensive and time consuming. Trees are closely connected to the subsurface and sampling tree trunks can indicate subsurface pollutants, a process called phytoforensics. Scientists at the Missouri Water Science Center were among the first to use phytoforensics to screen sites for contamination before using traditional sampling methods, to guide additional sampling, and to show the large cost savings associated with tree sampling compared to traditional methods. 

Molecular analysis of phosphate limitation in Geobacteraceae during the bioremediation of a uranium-contaminated aquifer

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

N'Guessan, L.A.; Elifantz, H.; Nevin, K.P.

2009-09-01

Nutrient limitation is an environmental stress that may reduce the effectiveness of bioremediation strategies, especially when the contaminants are organic compounds or when organic compounds are added to promote microbial activities such as metal reduction. Genes indicative of phosphate-limitation were identified via microarray analysis of chemostat cultures of Geobacter sulfureducens. This analysis revealed that genes in the pst-pho operon, which is associated with a high affinity phosphate uptake system in other microorganisms, had significantly higher transcript abundance under phosphate-limiting conditions, with the genes pstB and phoU the most up-regulated. Quantitative PCR analysis of pstB and phoU transcript levels in G.more » sulfurreducens grown in chemostats demonstrated that the expression of these genes increased when phosphate was removed from the culture medium. Transcripts of pstB and phoU within the subsurface Geobacter species predominating during an in situ uranium bioremediation field experiment were more abundant than in chemostat cultures of G. sulfurreducens that were not limited for phosphate. Addition of phosphate to incubations of subsurface sediments did not stimulate dissimilatory metal reduction. The added phosphate was rapidly adsorbed onto the sediments. The results demonstrate that Geobacter species can effectively reduce U(VI) even when experiencing suboptimal phosphate concentrations and that increasing phosphate availability with phosphate additions is difficult to achieve due to the high reactivity of this compound. This transcript-based approach developed for diagnosing phosphate limitation should be applicable to assessing the potential need for additional phosphate in other bioremediation processes.« less

Molecular Analysis of Phosphate Limitation in Geobacteraceae During the Bioremediation of a Uranium-Contaminated Aquifer

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

N'Guessan, A. Lucie; Elifantz, H.; Nevin, Kelly P.

2010-02-01

Nutrient limitation is an environmental stress that may reduce the effectiveness of bioremediation strategies, especially when the contaminants are organic compounds or when organic compounds are added to promote microbial activities such as metal reduction. Genes indicative of phosphate-limitation were identified via microarray analysis of chemostat cultures of Geobacter sulfureducens. This analysis revealed that genes in the pst-pho operon, which is associated with a high affinity phosphate uptake system in other microorganisms, had significantly higher transcript abundance under phosphate-limiting conditions, with the genes pstB and phoU the most up-regulated. Quantitative PCR analysis of pstB and phoU transcript levels in G.more » sulfurreducens grown in chemostats demonstrated that the expression of these genes increased when phosphate was removed from the culture medium. Transcripts of pstB and phoU within the subsurface Geobacter species predominating during an in situ uranium bioremediation field experiment were more abundant than in chemostat cultures of G. sulfurreducens that were not limited for phosphate. Addition of phosphate to incubations of subsurface sediments did not stimulate dissimilatory metal reduction. The added phosphate was rapidly adsorbed onto the sediments. The results demonstrate that Geobacter species can effectively reduce U(VI) even when experiencing suboptimal phosphate concentrations and that increasing phosphate availability with phosphate additions is difficult to achieve due to the high reactivity of this compound. This transcript-based approach developed for diagnosing phosphate limitation should be applicable to assessing the potential need for additional phosphate in other bioremediation processes.« less

Molecular analysis of phosphate limitation in Geobacteraceae during the bioremediation of a uranium-contaminated aquifer

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

N'Guessan, A. Lucie; Elifantz, H.; Nevin, Kelly P.

2010-01-10

Nutrient limitation is an environmental stress that may reduce the effectiveness of bioremediation strategies, especially when the contaminants are organic compounds or when organic compounds are added to promote microbial activities such as metal reduction. Genes indicative of phosphatelimitation were identified by microarray analysis of chemostat cultures of Geobacter sulfureducens. This analysis revealed that genes in the pst-pho operon, which is associated with a high-affinity phosphate uptake system in other microorganisms, had significantly higher transcript abundance under phosphate-limiting conditions, with the genes pstB and phoU upregulated the most. Quantitative PCR analysis of pstB and phoU transcript levels in G. sulfurreducensmore » grown in chemostats demonstrated that the expression of these genes increased when phosphate was removed from the culture medium. Transcripts of pstB and phoU within the subsurface Geobacter species predominating during an in situ uranium-bioremediation field experiment were more abundant than in chemostat cultures of G. sulfurreducens that were not limited for phosphate. Addition of phosphate to incubations of subsurface sediments did not stimulate dissimilatory metal reduction. The added phosphate was rapidly adsorbed onto the sediments. The results demonstrate that Geobacter species can effectively reduce U(VI) even when experiencing suboptimal phosphate concentrations and that increasing phosphate availability with phosphate additions is difficult to achieve because of the high reactivity of this compound. This transcript-based approach developed for diagnosing phosphate limitation should be applicable to assessing the potential need for additional phosphate in other bioremediation processes.« less

Microbial Communities in Contaminated Sediments, Associated with Bioremediation of Uranium to Submicromolar Levels▿

PubMed Central

Cardenas, Erick; Wu, Wei-Min; Leigh, Mary Beth; Carley, Jack; Carroll, Sue; Gentry, Terry; Luo, Jian; Watson, David; Gu, Baohua; Ginder-Vogel, Matthew; Kitanidis, Peter K.; Jardine, Philip M.; Zhou, Jizhong; Criddle, Craig S.; Marsh, Terence L.; Tiedje, James M.

2008-01-01

Microbial enumeration, 16S rRNA gene clone libraries, and chemical analysis were used to evaluate the in situ biological reduction and immobilization of uranium(VI) in a long-term experiment (more than 2 years) conducted at a highly uranium-contaminated site (up to 60 mg/liter and 800 mg/kg solids) of the U.S. Department of Energy in Oak Ridge, TN. Bioreduction was achieved by conditioning groundwater above ground and then stimulating growth of denitrifying, Fe(III)-reducing, and sulfate-reducing bacteria in situ through weekly injection of ethanol into the subsurface. After nearly 2 years of intermittent injection of ethanol, aqueous U levels fell below the U.S. Environmental Protection Agency maximum contaminant level for drinking water and groundwater (<30 μg/liter or 0.126 μM). Sediment microbial communities from the treatment zone were compared with those from a control well without biostimulation. Most-probable-number estimations indicated that microorganisms implicated in bioremediation accumulated in the sediments of the treatment zone but were either absent or in very low numbers in an untreated control area. Organisms belonging to genera known to include U(VI) reducers were detected, including Desulfovibrio, Geobacter, Anaeromyxobacter, Desulfosporosinus, and Acidovorax spp. The predominant sulfate-reducing bacterial species were Desulfovibrio spp., while the iron reducers were represented by Ferribacterium spp. and Geothrix spp. Diversity-based clustering revealed differences between treated and untreated zones and also within samples of the treated area. Spatial differences in community structure within the treatment zone were likely related to the hydraulic pathway and to electron donor metabolism during biostimulation. PMID:18456853

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

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

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, particle size, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population andmore » composition, which mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfatereducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. The results of this study suggest that reductive immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

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

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

DOE PAGES

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.; ...

2016-12-29

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy's Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments' mineralogy, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population and composition, whichmore » mainly determines the system's performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of sulfate-reducing bacteria, and the sediments' propensity to sequester aqueous uranium. In contrast, no obvious connections were observed between the abundance of common iron-reducing bacteria, e.g., Geobacter spp., and the sediments' ability to sequester uranium. In the sediments with low bacterial biomass and the absence of sulfate-reducing conditions, abiotic adsorption onto mineral surfaces such as phyllosilicates likely played a relatively major role in the attenuation of aqueous uranium; however, in these scenarios, acetate amendment induced detectable rebounds in the effluent uranium concentrations. Lastly, the results of this study suggest that immobilization of uranium can be achieved under predominantly sulfate-reducing conditions, and provide insight into the integrated roles of various biogeochemical components in long-term uranium sequestration.« less

Mobility of Source Zone Heavy Metals and Radionuclides: The Mixed Roles of Fermentative Activity on Fate and Transport of U and Cr. Final Report

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

Gerlach, Robin; Peyton, Brent M.; Apel, William A.

2014-01-29

Various U. S. Department of Energy (DOE) low and medium-level radioactive waste sites contain mixtures of heavy metals, radionuclides and assorted organic materials. In addition, there are numerous sites around the world that are contaminated with a mixture of organic and inorganic contaminants. In most sites, over time, water infiltrates the wastes, and releases metals, radionuclides and other contaminants causing transport into the surrounding environment. We investigated the role of fermentative microorganisms in such sites that may control metal, radionuclide and organics migration from source zones. The project was initiated based on the following overarching hypothesis: Metals, radionuclides and othermore » contaminants can be mobilized by infiltration of water into waste storage sites. Microbial communities of lignocellulose degrading and fermenting microorganisms present in the subsurface of contaminated DOE sites can significantly impact migration by directly reducing and immobilizing metals and radionuclides while degrading complex organic matter to low molecular weight organic compounds. These low molecular weight organic acids and alcohols can increase metal and radionuclide mobility by chelation (i.e., certain organic acids) or decrease mobility by stimulating respiratory metal reducing microorganisms. We demonstrated that fermentative organisms capable of affecting the fate of Cr6+, U6+ and trinitrotoluene can be isolated from organic-rich low level waste sites as well as from less organic rich subsurface environments. The mechanisms, pathways and extent of contaminant transformation depend on a variety of factors related to the type of organisms present, the aqueous chemistry as well as the geochemistry and mineralogy. This work provides observations and quantitative data across multiple scales that identify and predict the coupled effects of fermentative carbon and electron flow on the transport of radionuclides, heavy metals and organic contaminants in the subsurface; a primary concern of the DOE Environmental Remediation Science Division (ERSD) and Subsurface Geochemical Research (SBR) Program.« less

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

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

Not Available

1991-12-01

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

Carbon-free induction furnace

DOEpatents

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

1985-01-01

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

Non-carbon induction furnace

DOEpatents

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

1984-01-06

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

DETERMINATION OF TRANSFORMATION RATES OF CHIRAL PESTICIDES AND PCBS IN SOIL AND SEDIMENT MICROCOSMS

EPA Science Inventory

Risk Based Corrective Action (RBCA) has gained widespread acceptance as a favorable approach to remediating contaminated sites. The use of RBCA methods often requires computer-based modeling to assess the fate and transport of hazardous contaminants in subsurface environments, a...

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

Qafoku, Nikolla; Sahajpal, Rahul

Chromium-contaminated subsurface sites are common throughout the globe. In this chapter the discussion will be focused on one Cr-contaminated, i.e., Hanford site, WA, USA. The chapter summarizes the work conducted at this site to study contaminant Cr6+ fate and behavior under conditions imposed by different waste chemistries ranging from acidic to hyperalkaline. The objectives of this chapter are to present an overview of different aspects of Cr interaction with minerals; present evidence of similar and contrasting Cr6+ reactions, processes and attenuation mechanisms operating in subsurface environments under different conditions imposed by acidic, neutral and alkaline waste liquids; provide inputs tomore » conceptual Cr geochemical models (either site specific or general and suitable for many contaminated sites); present ideas on potential remedial measures. The insights presented and discussed in this chapter should be useful for other Cr contaminated sites across the world.« less

Final Report, University of California Merced: Uranium and strontium fate in waste-weathered sediments: Scaling of molecular processes to predict reactive transport

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

Chorover, Jon; Mueller, Karl; O'Day, Peggy Anne

2016-06-30

Objectives of the Project: 1. Determine the process coupling that occurs between mineral transformation and contaminant (U and Sr) speciation in acid-uranium waste weathered Hanford sediments. 2. Establish linkages between molecular-scale contaminant speciation and meso-scale contaminant lability, release and reactive transport. 3. Make conjunctive use of molecular- to bench-scale data to constrain the development of a mechanistic, reactive transport model that includes coupling of contaminant sorption-desorption and mineral transformation reactions. Hypotheses Tested: Uranium and strontium speciation in legacy sediments from the U-8 and U-12 Crib sites can be reproduced in bench-scale weathering experiments conducted on unimpacted Hanford sediments from themore » same formations; Reactive transport modeling of future uranium and strontium releases from the vadose zone of acid-waste weathered sediments can be effectively constrained by combining molecular-scale information on contaminant bonding environment with grain-scale information on contaminant phase partitioning, and meso-scale kinetic data on contaminant release from the waste-weathered porous media; Although field contamination and laboratory experiments differ in their diagenetic time scales (decades for field vs. months to years for lab), sediment dissolution, neophase nucleation, and crystal growth reactions that occur during the initial disequilibrium induced by waste-sediment interaction leave a strong imprint that persists over subsequent longer-term equilibration time scales and, therefore, give rise to long-term memory effects. Enabling Capabilities Developed: Our team developed an iterative measure-model approach that is broadly applicable to elucidate the mechanistic underpinnings of reactive contaminant transport in geomedia subject to active weathering.« less

National Uranium Resource Evaluation: Marfa Quadrangle, Texas

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

Henry, C D; Duex, T W; Wilbert, W P

1982-09-01

The uranium favorability of the Marfa 1/sup 0/ by 2/sup 0/ Quadrangle, Texas, was evaluated in accordance with criteria established for the National Uranium Resource Evaluation. Surface and subsurface studies, to a 1500 m (5000 ft) depth, and chemical, petrologic, hydrogeochemical, and airborne radiometric data were employed. The entire quadrangle is in the Basin and Range Province and is characterized by Tertiary silicic volcanic rocks overlying mainly Cretaceous carbonate rocks and sandstones. Strand-plain sandstones of the Upper Cretaceous San Carlos Formation and El Picacho Formation possess many favorable characteristics and are tentatively judged as favorable for sandstone-type deposits. The Tertiarymore » Buckshot Ignimbrite contains uranium mineralization at the Mammoth Mine. This deposit may be an example of the hydroauthigenic class; alternatively, it may have formed by reduction of uranium-bearing ground water produced during diagenesis of tuffaceous sediments of the Vieja Group. Although the presence of the deposit indicates favorability, the uncertainty in the process that formed the mineralization makes delineation of a favorable environment or area difficult. The Allen intrusions are favorable for authigenic deposits. Basin fill in several bolsons possesses characteristics that suggest favorability but which are classified as unevaluated because of insufficient data. All Precambrian, Paleozoic, other Mesozoic, and other Cenozoic environments are unfavorable.« less

Small-scale geochemical cycles and the distribution of uranium in central and north Florida organic deposits

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

Bond, P.A.

1993-03-01

The global geochemical cycle for an element tracks its path from its various sources to its sinks via processes of weathering and transportation. The cycle may then be quantified in a necessarily approximate manner. The geochemical cycle (thus quantified) reveals constraints (known and unknown) on an element's behavior imposed by the various processes which act on it. In the context of a global geochemical cycle, a continent becomes essentially a source term. If, however, an element's behavior is examined in a local or regional context, sources and their related sinks may be identified. This suggests that small-scale geochemical cycles maymore » be superimposed on global geochemical cycles. Definition of such sub-cycles may clarify the distribution of an element in the earth's near-surface environment. In Florida, phosphate minerals of the Hawthorn Group act as a widely distributed source of uranium. Uranium is transported by surface- and ground-waters. Florida is the site of extensive wetlands and peatlands. The organic matter associated with these deposits adsorbs uranium and may act as a local sink depending on its hydrogeologic setting. This work examines the role of organic matter in the distribution of uranium in the surface and shallow subsurface environments of central and north Florida.« less

Phosphate-Induced Immobilization of Uranium in Hanford Sediments.

PubMed

Pan, Zezhen; Giammar, Daniel E; Mehta, Vrajesh; Troyer, Lyndsay D; Catalano, Jeffrey G; Wang, Zheming

2016-12-20

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) (>25 μM) 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.

Phosphate-Induced Immobilization of Uranium in Hanford Sediments

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

Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh

2016-12-20

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 onlymore » at high initial U(VI) (>25 μM) 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.« less

Phosphate-Induced Immobilization of Uranium in Hanford Sediments

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

Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh

2016-12-20

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 onlymore » 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.« less

Bacterial community succession during in situ uranium bioremediation: spatial similarities along controlled flow paths.

PubMed

Hwang, Chiachi; Wu, Weimin; Gentry, Terry J; Carley, Jack; Corbin, Gail A; Carroll, Sue L; Watson, David B; Jardine, Phil M; Zhou, Jizhong; Criddle, Craig S; Fields, Matthew W

2009-01-01

Bacterial community succession was investigated in a field-scale subsurface reactor formed by a series of wells that received weekly ethanol additions to re-circulating groundwater. Ethanol additions stimulated denitrification, metal reduction, sulfate reduction and U(VI) reduction to sparingly soluble U(IV). Clone libraries of SSU rRNA gene sequences from groundwater samples enabled tracking of spatial and temporal changes over a 1.5-year period. Analyses showed that the communities changed in a manner consistent with geochemical variations that occurred along temporal and spatial scales. Canonical correspondence analysis revealed that the levels of nitrate, uranium, sulfide, sulfate and ethanol were strongly correlated with particular bacterial populations. As sulfate and U(VI) levels declined, sequences representative of sulfate reducers and metal reducers were detected at high levels. Ultimately, sequences associated with sulfate-reducing populations predominated, and sulfate levels declined as U(VI) remained at low levels. When engineering controls were compared with the population variation through canonical ordination, changes could be related to dissolved oxygen control and ethanol addition. The data also indicated that the indigenous populations responded differently to stimulation for bioreduction; however, the two biostimulated communities became more similar after different transitions in an idiosyncratic manner. The strong associations between particular environmental variables and certain populations provide insight into the establishment of practical and successful remediation strategies in radionuclide-contaminated environments with respect to engineering controls and microbial ecology.

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

NASA Astrophysics Data System (ADS)

Wang, Qing; Cheng, Tao; Wu, Yang

2014-12-01

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

Pore-Scale Characterization of Biogeochemical Controls on Iron and Uranium Speciation under Flow Conditions

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

Pearce, Carolyn I.; Wilkins, Michael J.; Zhang, Changyong

2012-09-17

Etched silicon microfluidic pore network models (micromodels) with controlled chemical and redox gradients, mineralogy, and microbiology under continuous flow conditions are used for the incremental development of complex microenvironments that simulate subsurface conditions. We demonstrate the colonization of micromodel pore spaces by an anaerobic Fe(III)-reducing bacterial species (Geobacter sulfurreducens) and the enzymatic reduction of a bioavailable Fe(III) phase within this environment. Using both X-ray Microprobe and X-ray Absorption Spectroscopy, we investigate the combined effects of the precipitated Fe(III) phases and the microbial population on uranium biogeochemistry under flow conditions. Precipitated Fe(III) phases within the micromodel were most effectively reduced inmore » the presence of an electron shuttle (AQDS), and Fe(II) ions adsorbed onto the precipitated mineral surface without inducing any structural change. In the absence of Fe(III), U(VI) was effectively reduced by the microbial population to insoluble U(IV), which was precipitated in discrete regions associated with biomass. In the presence of Fe(III) phases, however, both U(IV) and U(VI) could be detected associated with biomass, suggesting re-oxidation of U(IV) by localized Fe(III) phases. These results demonstrate the importance of the spatial localization of biomass and redox active metals, and illustrate the key effects of pore-scale processes on contaminant fate and reactive transport.« less

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

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

NONE

1995-09-01

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

A trench study to assess transfer of pesticides in subsurface lateral flow for a soil with contrasting texture on a sloping vineyard in Beaujolais.

PubMed

Peyrard, X; Liger, L; Guillemain, C; Gouy, V

2016-01-01

Subsurface lateral flow in both texture-contrast soils and catchments with shallow bedrock is suspected to be a non-point source of contamination of watercourses by pesticides used in agriculture. As a case study, the north of the Beaujolais region (eastern France) provides a favorable environment for such contamination due to its agro-pedo-climatic conditions. Environments seen in the Beaujolais region include intense viticulture, permeable and shallow soils, steep hillslopes, and storms that occur during the periods of pesticide application. Watercourse contamination by pesticides has been widely observed in this region, and offsite pesticide transport by subsurface lateral flow is suspected to be involved in diffuse and chronic presence of pesticides in surface water. In order to confirm and quantify the potential role of such processes in pesticide transfer, an automated trench system has been designed. The trench was set up on a steep farmed hillslope in a texture-contrast soil. It was equipped with a tipping bucket flow meter and an automatic sampler to monitor pesticide concentrations in lateral flow at fine resolution, by means of a flow-dependent sampling strategy. Four pesticides currently used in vine growing were studied to provide a range of mobility properties: one insecticide (chlorpyrifos-methyl) and three fungicides (spiroxamine, tebuconazole, and dimethomorph). With this system, it was possible to study pesticide concentration dynamics in the subsurface lateral flow, generated by substantial rainfall events following pesticide applications. The experimental design ascertained to be a suitable method in which to monitor subsurface lateral flow and related transfer of pesticides.

Composition, stability, and measurement of reduced uranium phases for groundwater bioremediation at Old Rifle, CO

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

Campbell, K. M.; Davis, J. A.; Bargar, J.

2011-10-15

Reductive biostimulation is currently being explored as a possible remediation strategy for uranium (U) contaminated groundwater, and is currently being investigated at a field site in Rifle, CO, USA. The long-term stability of the resulting U(IV) phases is a key component of the overall performance and depends upon a variety of factors, including rate and mechanism of reduction, mineral associations in the subsurface, and propensity for oxidation. To address these factors, several approaches were used to evaluate the redox sensitivity of U: measurement of the rate of oxidative dissolution of biogenic uraninite (UO{sub 2(s)}) deployed in groundwater at Rifle, characterizationmore » of a zone of natural bioreduction exhibiting relevant reduced mineral phases, and laboratory studies of the oxidative capacity of Fe(III) and reductive capacity of Fe(II) with regard to U(IV) and U(VI), respectively.« less

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

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

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

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

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

USGS Publications Warehouse

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

2000-01-01

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

Development of experimental approach to examine U occurrence continuity over the extended area reconnoitory boreholes: Lostoin Block, West Khasi Hills district, Meghalaya (India).

PubMed

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.

Monitoring of Water and Contaminant Migration at the Groundwater-Surface Water Interface

DTIC Science & Technology

2008-08-01

seepage is occurring in a freshwater lake environment and to map the lateral extent of any subsurface contamination at the groundwater –surface water ...and Contaminant Migration at the Groundwater -Surface Water Interface August 2008 Report Documentation Page Form ApprovedOMB No. 0704-0188 Public...4. TITLE AND SUBTITLE Monitoring of Water and Contaminant Migration at the Groundwater -Surface Water Interface 5a. CONTRACT NUMBER 5b. GRANT NUMBER

Single cell genomic study of Dehalococcoidites in deep sea sediments of Peru Margin 1230

NASA Astrophysics Data System (ADS)

Kaster, A.; Meyer-Blackwell, K.; Spormann, A. M.

2013-12-01

Dehalogenating Chloroflexi, such as Dehalococcoidites Dhc were originally discovered as the key microorganisms mediating reductive dehalogenation of the prevalent groundwater contaminants tetrachloroethene and trichloroethene. Molecular and genomic studies on their key enzymes for energy conservation, reductive dehalogenases rdh, have provided evidence for ubiquitous horizontal gene transfer. A pioneering study by Futagami et al. discovered novel putative rdh phylotypes in sediments from the Pacific, revealing an unknown and surprising abundance of rdh genes in pristine habitats. The frequent detection of Dhc-related 16S rRNA genes from these environments implied the occurrence of dissimilatory dehalorespiration in marine subsurface sediments, however, pristine Dhc could never be linked to this activity. Despite being ubiquitous in those environments, metabolic life style or ecological function of Dhc in the absence of anthropogenic contaminants is still completely unknown. We therefore analyzed a non-contaminated deep sea sediment sample of the Peru Margin 1230 site by a single cell genomic (SGC) approach. We present for the first time data on three single Dhc cells, helping to elucidate their role in the poorly understood oligotrophic marine sub-surface environment.

Efficacy of acetate-amended biostimulation for uranium sequestration: Combined analysis of sediment/groundwater geochemistry and bacterial community structure

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

Xu, Jie; Veeramani, Harish; Qafoku, Nikolla P.

Systematic flow-through column experiments were conducted using sediments and ground water collected from different subsurface localities at the U.S. Department of Energy’s Integrated Field Research Challenge site in Rifle, Colorado. The principal purpose of this study is to gain a better understanding of the interactive effects of groundwater geochemistry, sediment mineralogy, and indigenous bacterial community structures on the efficacy of uranium removal from the groundwater with/without acetate amendment. Overall, we find that the subtle variations in the sediments’ mineralogy, particle size, redox conditions, as well as contents of metal(loid) co-contaminants showed a pronounced effect on the associated bacterial population andmore » composition, which mainly determines the system’s performance with respect to uranium removal. Positive relationship was identified between the abundance of dissimilatory sulfate-reduction genes (i.e., drsA), markers of 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

Bioengineered Chimeric Spider Silk-Uranium Binding Proteins

PubMed Central

Krishnaji, Sreevidhya Tarakkad; Kaplan, David L.

2014-01-01

Heavy metals constitute a source of environmental pollution. Here, novel functional hybrid biomaterials for specific interactions with heavy metals are designed by bioengineering consensus sequence repeats from spider silk of Nephila clavipes with repeats of a uranium peptide recognition motif from a mutated 33-residue of calmodulin protein from Paramecium tetraurelia. The self-assembly features of the silk to control nanoscale organic/inorganic material interfaces provides new biomaterials for uranium recovery. With subsequent enzymatic digestion of the silk to concentrate the sequestered metals, options can be envisaged to use these new chimeric protein systems in environmental engineering, including to remediate environments contaminated by uranium. PMID:23212989

Uranium (VI) transport in saturated heterogeneous media: Influence of kaolinite and humic acid.

PubMed

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.

AN EVALUATION OF HANFORD SITE TANK FARM SUBSURFACE CONTAMINATION FY2007

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

MANN, F.M.

2007-07-10

The Tank Farm Vadose Zone (TFVZ) Project conducts activities to characterize and analyze the long-term environmental and human health impacts from tank waste releases to the vadose zone. The project also implements interim measures to mitigate impacts, and plans the remediation of waste releases from tank farms and associated facilities. The scope of this document is to report data needs that are important to estimating long-term human health and environmental risks. The scope does not include technologies needed to remediate contaminated soils and facilities, technologies needed to close tank farms, or management and regulatory decisions that will impact remediation andmore » closure. This document is an update of ''A Summary and Evaluation of Hanford Site Tank Farm Subsurface Contamination''. That 1998 document summarized knowledge of subsurface contamination beneath the tank farms at the time. It included a preliminary conceptual model for migration of tank wastes through the vadose zone and an assessment of data and analysis gaps needed to update the conceptual model. This document provides a status of the data and analysis gaps previously defined and discussion of the gaps and needs that currently exist to support the stated mission of the TFVZ Project. The first data-gaps document provided the basis for TFVZ Project activities over the previous eight years. Fourteen of the nineteen knowledge gaps identified in the previous document have been investigated to the point that the project defines the current status as acceptable. In the process of filling these gaps, significant accomplishments were made in field work and characterization, laboratory investigations, modeling, and implementation of interim measures. The current data gaps are organized in groups that reflect Components of the tank farm vadose zone conceptual model: inventory, release, recharge, geohydrology, geochemistry, and modeling. The inventory and release components address residual wastes that will remain in the tanks and tank-farm infrastructure after closure and potential losses from leaks during waste retrieval. Recharge addresses the impacts of current conditions in the tank farms (i.e. gravel covers that affect infiltration and recharge) as well as the impacts of surface barriers. The geohydrology and geochemistry components address the extent of the existing subsurface contaminant inventory and drivers and pathways for contaminants to be transported through the vadose zone and groundwater. Geochemistry addresses the mobility of key reactive contaminants such as uranium. Modeling addresses conceptual models and how they are simulated in computers. The data gaps will be used to provide input to planning (including the upcoming C Farm Data Quality Objective meetings scheduled this year).« less

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

PubMed

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

2005-09-01

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

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

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

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

1996-12-31

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

Analysis of Tank 38H (HTF-38-16-80, 81) and Tank 43H (HTF-43-16-82, 83) Samples for Support of the Enrichment Control and Corrosion Control Programs

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

Hay, M.

2016-10-24

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H surface sample was 57.6 mg/L, while the sub-surface sample was 106 mg/L. The Tank 43H samples ranged from 50.0 to 51.9 mg/L total uranium. The U-235 percentage was consistent for all four samples at 0.62%. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The Tank 38H plutonium results show a large difference between the surface and sub-surface sample concentrations and somewhat higher concentrations than previous samples. The Pu-238 concentrationmore » is more than forty times higher in the Tank 38H sub-surface sample than the surface sample. The surface and sub-surface Tank 43H samples contain similar plutonium concentrations and are within the range of values measured on previous samples. The four samples analyzed show silicon concentrations somewhat higher than the previous sample with values ranging from 104 to 213 mg/L.« less

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

PubMed Central

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

2001-01-01

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

Model-Based Analysis of the Role of Biological, Hydrological and Geochemical Factors Affecting Uranium Bioremediation

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

Zhao, Jiao; Scheibe, Timothy D.; Mahadevan, Radhakrishnan

2011-01-24

Uranium contamination is a serious concern at several sites motivating the development of novel treatment strategies such as the Geobacter-mediated reductive immobilization of uranium. However, this bioremediation strategy has not yet been optimized for the sustained uranium removal. While several reactive-transport models have been developed to represent Geobacter-mediated bioremediation of uranium, these models often lack the detailed quantitative description of the microbial process (e.g., biomass build-up in both groundwater and sediments, electron transport system, etc.) and the interaction between biogeochemical and hydrological process. In this study, a novel multi-scale model was developed by integrating our recent model on electron capacitancemore » of Geobacter (Zhao et al., 2010) with a comprehensive simulator of coupled fluid flow, hydrologic transport, heat transfer, and biogeochemical reactions. This mechanistic reactive-transport model accurately reproduces the experimental data for the bioremediation of uranium with acetate amendment. We subsequently performed global sensitivity analysis with the reactive-transport model in order to identify the main sources of prediction uncertainty caused by synergistic effects of biological, geochemical, and hydrological processes. The proposed approach successfully captured significant contributing factors across time and space, thereby improving the structure and parameterization of the comprehensive reactive-transport model. The global sensitivity analysis also provides a potentially useful tool to evaluate uranium bioremediation strategy. The simulations suggest that under difficult environments (e.g., highly contaminated with U(VI) at a high migration rate of solutes), the efficiency of uranium removal can be improved by adding Geobacter species to the contaminated site (bioaugmentation) in conjunction with the addition of electron donor (biostimulation). The simulations also highlight the interactive effect of initial cell concentration and flow rate on U(VI) reduction.« less

Preliminary biological sampling of GT3 and BT1 cores and the microbial community dynamics of existing subsurface wells

NASA Astrophysics Data System (ADS)

Kraus, E. A.; Stamps, B. W.; Rempfert, K. R.; Ellison, E. T.; Nothaft, D. B.; Boyd, E. S.; Templeton, A. S.; Spear, J. R.

2017-12-01

Subsurface microbial life is poorly understood but potentially very important to the search for life on other planets as well as increasing our understanding of Earth's geobiological processes. Fluids and rocks of actively serpentinizing subsurface environments are a recent target of biological study due to their apparent ubiquity across the solar system. Areas of serpentinization can contain high concentrations of molecular hydrogen, H2, that can serve as the dominant fuel source for subsurface microbiota. Working with the Oman Drilling Project, DNA and RNA were extracted from fluids of seven alkaline wells and two rock cores from drill sites GT3 and BT1 within the Samail ophiolite. DNA and cDNA (produced via reverse transcription from the recovered RNA) were sequenced using universal primers to identify microbial life across all three domains. Alkaline subsurface fluids support a microbial community that changes with pH and host-rock type. In peridotite with pH values of >11, wells NSHQ 14 and WAB 71 have high relative abundances of Meiothermus, Methanobacterium, the family Nitrospiraceae, and multiple types of the class Dehalococcoidia. While also hosted in peridotite but at pH 8.5, wells WAB 104 and 105 have a distinct, more diverse microbial community. This increased variance in community make-up is seen in wells that sit near/at the contact of gabbro and peridotite formations as well. Core results indicate both sampled rock types host a very low biomass environment subject to multiple sources of contamination during the drilling process. Suggestions for contaminant reduction, such as having core handlers wear nitrile gloves and flame-sterilizing the outer surfaces of core rounds for biological sampling, would have minimal impact to overall ODP coreflow and maximize the ability to better understand in situ microbiota in this low-biomass serpentinizing subsurface environment. While DNA extraction was successful with gram amounts of crushed rock, much can be done to improve yields and reduce contamination sources for Phase II drilling.

Sustained removal of uranium from contaminated groundwater following stimulation of dissimilatory metal reduction.

PubMed

N'Guessan, A Lucie; Vrionis, Helen A; Resch, Charles T; Long, Philip E; Lovley, Derek R

2008-04-15

Previous field studies on in situ bioremediation of uranium-contaminated groundwater in an aquifer in Rifle, Colorado identified two distinct phases following the addition of acetate to stimulate microbial respiration. In phase I, Geobacter species are the predominant organisms, Fe(III) is reduced, and microbial reduction of soluble U(VI) to insoluble U(IV) removes uranium from the groundwater. In phase II, Fe(III) is depleted, sulfate is reduced, and sulfate-reducing bacteria predominate. Long-term monitoring revealed an unexpected third phase during which U(VI) removal continues even after acetate additions are stopped. All three of these phases were successfully reproduced in flow-through sediment columns. When sediments from the third phase were heat sterilized, the capacity for U(VI) removal was lost. In the live sediments U(VI) removed from the groundwater was recovered as U(VI) in the sediments. This contrasts to the recovery of U(IV) in sediments resulting from the reduction of U(VI) to U(IV) during the Fe(III) reduction phase in acetate-amended sediments. Analysis of 16S rRNA gene sequences in the sediments in which U(VI) was being adsorbed indicated that members of the Firmicutes were the predominant organisms whereas no Firmicutes sequences were detected in background sediments which did not have the capacity to sorb U(VI), suggesting that the U(VI) adsorption might be due to the presence of these living organisms or at least their intact cell components. This unexpected enhanced adsorption of U(VI) onto sediments following the stimulation of microbial growth in the subsurface may potentially enhance the cost effectiveness of in situ uranium bioremediation.

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

USGS Publications Warehouse

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

2015-01-01

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

Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 415: Project 57 No. 1 Plutonium Dispersion (NTTR), Nevada, Revision 0

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

Matthews, Patrick; Burmeister, Mark

2014-04-01

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 415, Project 57 No. 1 Plutonium Dispersion (NTTR). CAU 415 is located on Range 4808A of the Nevada Test and Training Range (NTTR) and consists of one corrective action site: NAFR-23-02, Pu Contaminated Soil. The CAU 415 site consists of the atmospheric release of radiological contaminants to surface soil from the Project 57 safety experiment conducted in 1957. The safety experiment released plutonium (Pu), uranium (U), and americium (Am) to the surface soil over an area of approximately 1.9 squaremore » miles. This area is currently fenced and posted as a radiological contamination area. Vehicles and debris contaminated by the experiment were subsequently buried in a disposal trench within the surface-contaminated, fenced area and are assumed to have released radiological contamination to subsurface soils. Potential source materials in the form of pole-mounted electrical transformers were also identified at the site and will be removed as part of closure activities.« less

Environmental Electrokinetics for a sustainable subsurface.

PubMed

Lima, A T; Hofmann, A; Reynolds, D; Ptacek, C J; Van Cappellen, P; Ottosen, L M; Pamukcu, S; Alshawabekh, A; O'Carroll, D M; Riis, C; Cox, E; Gent, D B; Landis, R; Wang, J; Chowdhury, A I A; Secord, E L; Sanchez-Hachair, A

2017-08-01

Soil and groundwater are key components in the sustainable management of the subsurface environment. Source contamination is one of its main threats and is commonly addressed using established remediation techniques such as in-situ chemical oxidation (ISCO), in-situ chemical reduction (ISCR; most notably using zero-valent iron [ZVI]), enhanced in-situ bioremediation (EISB), phytoremediation, soil-washing, pump-and-treat, soil vapour extraction (SVE), thermal treatment, and excavation and disposal. Decades of field applications have shown that these techniques can successfully treat or control contaminants in higher permeability subsurface materials such as sands, but achieve only limited success at sites where low permeability soils, such as silts and clays, prevail. Electrokinetics (EK), a soil remediation technique mostly recognized in in-situ treatment of low permeability soils, has, for the last decade, been combined with more conventional techniques and can significantly enhance the performance of several of these remediation technologies, including ISCO, ISCR, EISB and phytoremediation. Herein, we discuss the use of emerging EK techniques in tandem with conventional remediation techniques, to achieve improved remediation performance. Furthermore, we highlight new EK applications that may come to play a role in the sustainable treatment of the contaminated subsurface. Copyright © 2017 Elsevier Ltd. All rights reserved.

Characterization of subsurface geologic structure for potential water resources near the Villages of Moenkopi, Arizona, 2009--2010

USGS Publications Warehouse

Macy, Jamie P.

2012-01-01

The Hopi Tribe depends on groundwater as their primary drinking-water source in the area of the Villages of Moenkopi, in northeastern Arizona. Growing concerns of the potential for uranium contamination at the Moenkopi water supply wells from the Tuba City Landfill prompted the need for an improved understanding of subsurface geology and groundwater near Moenkopi. Information in this report provides the Hopi Tribe with new hydrogeologic information that provides a better understanding of groundwater resources near the Villages of Moenkopi. The U.S. Geological Survey in cooperation with the U.S. Bureau of Reclamation and the Hopi Tribe used the controlled source audio-frequency magnetotelluric (CSAMT) geophysical technique to characterize the subsurface near Moenkopi from December 2009 to September 2010. A total of six CSAMT profiles were surveyed to identify possible fracturing and faulting in the subsurface that provides information about the occurrence and movement of groundwater. Inversion results from the six CSAMT lines indicated that north to south trending fractures are more prevalent than east to west. CSAMT Lines A and C showed multiple areas in the Navajo Sandstone where fractures are present. Lines B, D, E, and F did not show the same fracturing as Lines A and C.

Phytosiderophore effects on subsurface actinide contaminants: potential for phytostabilization and phytoextraction.

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

Ruggiero, C. E.; Twary, S. N.; Deladurantaye, E.

2003-01-01

In recognition of the need for a safe, effective technology for long term Pu/Th/Actinide stabilization or removal from soils, we have begun an investigation of the potential for phytoremediation (phytostabilization and/or phytoextraction) of Pu and other actinide soil contaminants at DOE sites using phytosiderophore producing plants, and are investigating the contribution of phytosiderophores to actinide mobility in the subsurface environment. Phytoremediation and Phytostabilization have been proven to be a cost-effective, safe, efficient, and publicly acceptable technology for clean up and/or stabilization of contaminant metals . However, no phyto-based technologies have been developed for stabilization or removal of plutonium from soilsmore » and groundwater, and very few have been investigated for other actinides . Current metal-phytostabilization and phytoremediation techniques, predominately based around lead, nickel, and other soft-metal phytoextraction, will almost certainly be inadequate for plutonium due its distinct chemical properties . Phytosiderophore-based phytoremediation may provide technically and financially practical methods for remediation and long-term stewardship of soils that have low to moderate, near surface actinide contamination . We plan to demonstrate potential benefits of phytosiderophore-producing plants for long-term actinide contaminant stabilization by the plant's prevention of soil erosion and actinide migration through hydraulic control and/or through actinide removal through phytoextraction . We may also show possible harm caused by these plants through increased presence of actinide chelators that could increase actinide mobilization and migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or be used to develop plant-based soil stabilization/remediation technologies .« less

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

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

Not Available

1994-06-01

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

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.

IMPACT OF REDOX DISEQUILIBRIA ON CONTAMINANT TRANSPORT AND REMEDIATION IN SUBSURFACE SYSTEMS

EPA Science Inventory

Partitioning to mineral surfaces exerts significant control on inorganic contaminant transport in subsurface systems. Remedial technologies for in-situ treatment of subsurface contamination are frequently designed to optimize the efficiency of contaminant partitioning to solid s...

Novel tools for in situ detection of biodiversity and function of dechlorinating and uranium-reducing bacteria in contaminated environments

USDA-ARS?s Scientific Manuscript database

Toxic heavy metals and radionuclides pose a growing, global threat to the environment. For an intelligent remediation design, reliable analytical tools for detection of relevant species are needed, such as PCR. However, PCR cannot visualize its targets and thus provide information about the morpholo...

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

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

Not Available

1994-09-01

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

Reduced Uranium Phases Produced from Anaerobic Reaction with Nanoscale Zerovalent Iron.

PubMed

Tsarev, Sergey; Collins, Richard N; Fahy, Adam; Waite, T David

2016-03-01

Nanoscale zerovalent iron (nZVI) has shown potential to be an effective remediation agent for uranium-contaminated subsurface environments, however, the nature of the reaction products and their formation kinetics have not been fully elucidated over a range of environmentally relevant conditions. In this study, the oxygen-free reaction of U(VI) with varying quantities of nZVI was examined at pH 7 in the presence of both calcium and carbonate using a combination of X-ray absorption spectroscopy, X-ray diffraction and transmission electron microscopy. It was observed that the structure of the reduced U solid phases was time dependent and largely influenced by the ratio of nZVI to U in the system. At the highest U:Fe molar ratio examined (1:4), nanoscale uraninite (UO2) was predominantly formed within 1 day of reaction. At lower U:Fe molar ratios (1:21), evidence was obtained for the formation of sorbed U(IV) and U(V) surface complexes which slowly transformed to UO2 nanoparticles that were stable for up to 1 year of anaerobic incubation. After 8 days of reaction at the lowest U:Fe molar ratio examined (1:110), sorbed U(IV) was still the major form of U associated with the solid phase. Regardless of the U:Fe molar ratio, the anaerobic corrosion of nZVI resulted in the slow formation of micron-sized fibrous chukanovite (Fe2(OH)2CO3) particles.

Bacterial Community Succession During in situ Uranium Bioremediation: Spatial Similarities Along Controlled Flow Paths

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

Hwang, Chiachi; Wu, Weimin; Gentry, Terry J.

2009-05-22

Bacterial community succession was investigated in a field-scale subsurface reactor formed by a series of wells that received weekly ethanol additions to re-circulating groundwater. Ethanol additions stimulated denitrification, metal reduction, sulfate reduction, and U(VI) reduction to sparingly soluble U(IV). Clone libraries of SSU rRNA gene sequences from groundwater samples enabled tracking of spatial and temporal changes over a 1.5 y period. Analyses showed that the communities changed in a manner consistent with geochemical variations that occurred along temporal and spatial scales. Canonical correspondence analysis revealed that the levels of nitrate, uranium, sulfide, sulfate, and ethanol strongly correlated with particular bacterialmore » populations. As sulfate and U(VI) levels declined, sequences representative of sulfate-reducers and metal-reducers were detected at high levels. Ultimately, sequences associated with sulfate-reducing populations predominated, and sulfate levels declined as U(VI) remained at low levels. When engineering controls were compared to the population variation via canonical ordination, changes could be related to dissolved oxygen control and ethanol addition. The data also indicated that the indigenous populations responded differently to stimulation for bio-reduction; however, the two bio-stimulated communities became more similar after different transitions in an idiosyncratic manner. The strong associations between particular environmental variables and certain populations provide insight into the establishment of practical and successful remediation strategies in radionuclide-contaminated environments with respect to engineering controls and microbial ecology.« less

Construction of a naturally occurring radioactive material project in the BeAAT hazardous waste facilities.

PubMed

Abuahmad, H

2015-06-01

This paper does not necessarily reflect the views of the International Commission on Radiological Protection. Naturally occurring radioactive material (NORM) is produced during exploration and production operations of subsidiaries of the Abu Dhabi National Oil Company (ADNOC) in the United Arab Emirates, and accumulates in drilling tubulars, plant equipment, and components. These NORM hazardous wastes need to be managed in such a way that they do not damage human health and the environment. The primary radionuclides of concern in the oil and gas industries are radium-226 and radium-228. These radioisotopes are the decay products of uranium and thorium isotopes that are present in subsurface formations from which hydrocarbons are produced. While uranium and thorium are largely immobile, radium is slightly more soluble and may become mobilised in the fluid phases of the formation (International Association of Oil & Gas Producers, 2008). In order to treat and dispose of NORM waste products safely, ADNOC's subsidiary 'TAKREER' is developing a new facility, on behalf of all ADNOC subsidiaries, within the existing Central Environmental Protection Facilities (BeAAT) in Ruwais city. The NORM plant is envisaged to treat, handle, and dispose of NORM waste in the forms of scale, sludge, and contaminated equipment. The NORM treatment facility will cover activities such as decontamination, volume reduction, NORM handling, and concrete immobilisation of NORM waste into packages for designated landfilling. © The International Society for Prosthetics and Orthotics Reprints and permissions: sagepub.co.uk/journalsPermissions.nav.

Microanalytical X-ray imaging of depleted uranium speciation in environmentally aged munitions residues.

PubMed

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

2014-01-01

Use of depleted uranium (DU) munitions has resulted in contamination of the near-surface environment with penetrator residues. Uncertainty in the long-term environmental fate of particles produced by impact of DU penetrators with hard targets is a specific concern. In this study DU particles produced in this way and exposed to the surface terrestrial environment for longer than 30 years at a U.K. firing range were characterized using synchrotron X-ray chemical imaging. Two sites were sampled: a surface soil and a disposal area for DU-contaminated wood, and the U speciation was different between the two areas. Surface soil particles showed little extent of alteration, with U speciated as oxides U3O7 and U3O8. Uranium oxidation state and crystalline phase mapping revealed these oxides occur as separate particles, reflecting heterogeneous formation conditions. Particles recovered from the disposal area were substantially weathered, and U(VI) phosphate phases such as meta-ankoleite (K(UO2)(PO4) · 3H2O) were dominant. Chemical imaging revealed domains of contrasting U oxidation state linked to the presence of both U3O7 and meta-ankoleite, indicating growth of a particle alteration layer. This study demonstrates that substantial alteration of DU residues can occur, which directly influences the health and environmental hazards posed by this contamination.

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

NASA Astrophysics Data System (ADS)

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

2017-07-01

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

Newly recognized hosts for uranium in the Hanford Site vadose zone

USGS Publications Warehouse

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

2009-01-01

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

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

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

Taillefert, Martial; Van Cappellen, Philippe

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

Analysis of Tank 38H (HTF-38-16-26, 27) and Tank 43H (HTF-43-16-28, 29) Samples for Support of the Enrichment Control and Corrosion Control Programs

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

Hay, M. S.

Savannah River National Laboratory analyzed samples from Tank 38H and Tank 43H to support Enrichment Control Program and Corrosion Control Program. The total uranium in the Tank 38H samples ranged from 20.5 to 34.0 mg/L while the Tank 43H samples ranged from 47.6 to 50.6 mg/L. The U-235 percentage ranged from 0.62% to 0.64% over the four samples. The total uranium and percent U-235 results appear consistent with previous Tank 38H and Tank 43H uranium measurements. The Tank 38H plutonium results show a large difference between the surface and sub-surface sample concentrations and a somewhat higher concentration than previous sub-surfacemore » samples. The two Tank 43H samples show similar plutonium concentrations and are within the range of values measured on previous samples. The plutonium results may be biased high due to the presence of plutonium contamination in the blank samples from the cell sample preparations. The four samples analyzed show silicon concentrations ranging from 47.9 to 105 mg/L.« less

Characterization and transcription of arsenic respiration and resistance genes during in situ uranium bioremediation

PubMed Central

Giloteaux, Ludovic; Holmes, Dawn E; Williams, Kenneth H; Wrighton, Kelly C; Wilkins, Michael J; Montgomery, Alison P; Smith, Jessica A; Orellana, Roberto; Thompson, Courtney A; Roper, Thomas J; Long, Philip E; Lovley, Derek R

2013-01-01

The possibility of arsenic release and the potential role of Geobacter in arsenic biogeochemistry during in situ uranium bioremediation was investigated because increased availability of organic matter has been associated with substantial releases of arsenic in other subsurface environments. In a field experiment conducted at the Rifle, CO study site, groundwater arsenic concentrations increased when acetate was added. The number of transcripts from arrA, which codes for the α-subunit of dissimilatory As(V) reductase, and acr3, which codes for the arsenic pump protein Acr3, were determined with quantitative reverse transcription-PCR. Most of the arrA (>60%) and acr3-1 (>90%) sequences that were recovered were most similar to Geobacter species, while the majority of acr3-2 (>50%) sequences were most closely related to Rhodoferax ferrireducens. Analysis of transcript abundance demonstrated that transcription of acr3-1 by the subsurface Geobacter community was correlated with arsenic concentrations in the groundwater. In contrast, Geobacter arrA transcript numbers lagged behind the major arsenic release and remained high even after arsenic concentrations declined. This suggested that factors other than As(V) availability regulated the transcription of arrA in situ, even though the presence of As(V) increased the transcription of arrA in cultures of Geobacter lovleyi, which was capable of As(V) reduction. These results demonstrate that subsurface Geobacter species can tightly regulate their physiological response to changes in groundwater arsenic concentrations. The transcriptomic approach developed here should be useful for the study of a diversity of other environments in which Geobacter species are considered to have an important influence on arsenic biogeochemistry. PMID:23038171

Characterization and Transcription of Arsenic Respiration and Resistance Genes During In Situ Uranium Bioremediation

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

Giloteaux, L.; Holmes, Dawn E.; Williams, Kenneth H.

2013-02-04

The possibility of arsenic release and the potential role of Geobacter in arsenic biogeochemistry during in situ uranium bioremediation was investigated because increased availability of organic matter has been associated with substantial releases of arsenic in other subsurface environments. In a field experiment conducted at the Rifle, CO study site, groundwater arsenic concentrations increased when acetate was added. The number of transcripts from arrA, which codes for the alpha subunit of dissimilatory As(V) reductase, and acr3, which codes for the arsenic pump protein Acr3, were determined with quantitative RT-PCR. Most of the arrA (> 60%) and acr3-1 (> 90%) sequencesmore » that were recovered were most similar to Geobacter species, while the majority of acr3-2 (>50%) sequences were most closely related to Rhodoferax ferrireducens. Analysis of transcript abundance demonstrated that transcription of acr3-1 by the subsurface Geobacter community was correlated with arsenic concentrations in the groundwater. In contrast, Geobacter arrA transcript numbers lagged behind the major arsenic release and remained high even after arsenic concentrations declined. This suggested that factors other than As(V) availability regulated transcription of arrA in situ even though the presence of As(V) increased transcription of arrA in cultures of G. lovleyi, which was capable of As(V) reduction. These results demonstrate that subsurface Geobacter species can tightly regulate their physiological response to changes in groundwater arsenic concentrations. The transcriptomic approach developed here should be useful for the study of a diversity of other environments in which Geobacter species are considered to have an important influence on arsenic biogeochemistry.« less

Assessment of a Hydroxyapatite Permeable Reactive Barrier to Remediate Uranium at the Old Rifle Site Colorado.

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

3D Inversion of Induced Polarization Data From Borehole Measurements to Map Subsurface Contaminations of Tetrachloroethylene and Trichloroethylene.

NASA Astrophysics Data System (ADS)

Briggs, V. A.; Sogade, J.; Minsley, B.; Lambert, M.; Coles, D.; Repert, P.; Morgan, F.; Rossabi, J.; Riha, B.

2003-12-01

The purpose of this study is to image contaminant plumes of tetrachloroethylene (PCE) and Trichloroethylene (TCE) in a subsurface environment. PCE and TCE have been used in the metals fabrication industry since the start of the second word war and subsequently millions of tons of these chemicals have been released in to the environment. Once in the water supply these contaminants are difficult to remove and can be toxic at the part per billion level. Remediation at the source of many of these contaminated sites, in the form of vapour extraction, can effectively remove alot of the chemicals but without techniques to delineate the size and shape of the contaminated zone, or to monitor the effectiveness of the remediation effort, it is difficult to quantify the remediation success. Using complex resistivity methods it is possible to determine the spatial extent and concentration of these chemicals due to their effect on the pore space chemistry. Even at parts per billion the contaminantas can significantly alter the IP signature enabling detection. Data were collected from a site in South Carolina where these chemcals are known to have been released in large quantities from the 1950's through to the 1980's. Induced Polarization data were measured in a multi-borehole environment to ensure good data coverage. Data is inverted using a 3D finite difference bi-conjugate gradient method and correlated to ground truth boreholes within the region of interest.

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

Exogenous contamination of uranium in human scalp hair.

PubMed

Muikku, Maarit; Heikkinen, Tarja

2012-06-01

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

Uranium Biomineralization by Natural Microbial Phosphatase Activities in the Subsurface

NASA Astrophysics Data System (ADS)

Martinez, R.; Wu, C. H.; Beazley, M. J.; Andersen, G. L.; Hazen, T. C.; Taillefert, M.; Sobecky, P. A.

2011-12-01

Soils and groundwater contaminated with heavy metals and radionuclides remain a legacy of Cold War nuclear weapons development. Due to the scale of environmental contamination, in situ sequestration of heavy metals and radionuclides remain the most cost-effective strategy for remediation. We are currently investigating a remediation approach that utilizes periplasmic and extracellular microbial phosphatase activity of soil bacteria capable promoting in situ uranium phosphate sequestration. Our studies focus on the contaminated soils from the DOE Field Research Center (ORFRC) in Oak Ridge, TN. We have previously demonstrated that ORFRC strains with phosphatase-positive phenotypes were capable of promoting the precpitation of >95% U(VI) as a low solubility phosphate mineral during growth on glycerol phosphate as a sole carbon and phosphorus source. Here we present culture-independent soil slurry studies aimed at understanding microbial community dynamics resulting from exogenous organophosphate additions. Soil slurries containing glycerol-2-phosphate (G2P) or glycerol-3-phosphate (G3P) and nitrate as the sole C, P and N sources were incubated under oxic growth conditions at pH 5.5 or pH 6.8. Following treatments, total DNA was extracted and prokaryotic diversity was assessed using high-density 16S oligonucleotide microarray (PhyloChip) analysis. Treatments at pH 5.5 and pH 6.8 amended with G2P required 36 days to accumulate 4.8mM and 2.2 mM phosphate, respectively. In contrast, treatments at pH 5.5 and pH 6.8 amended with G3P accumulated 8.9 mM and 8.7 mM phosphate, respectively, after 20 days. A total of 2120 unique taxa representing 46 phyla, 66 classes, 110 orders, and 186 families were detected among all treatment conditions. The phyla that significantly (P<0.05) increased in abundance relative to incubations lacking organophosphate amendments included: Crenarchaeota, Euryarchaeota, Bacteroidetes, and Proteobacteria. Members from the classes Bacteroidetes, Sphingobacteria, α-proteobacteria, and γ-proteobacteria increased in relative abundance by 10 to 406-fold. These are the first PhyloChip studies that identify unique subsurface community responses to organophosphate substrates as well as demonstrate the diversity of the extant ORFRC microbial community capable of promoting in situ uranium phosphate sequestration. These studies also indicate that concentrations of phosphate released into extracellular space can be controlled by the type of substrate supplied to soil microbial communities. Additionally, we will present data summarizing the two Rahnella genome sequencing projects (Rahnella sp. Y9602 and the Rahnella aquatilis ATCC 33071) completed by the Joint Genome Institute.

Chromium Chemistry in the Subsurface

EPA Science Inventory

Chromium (VI) (Cr) is carcinogenic and a threat to human and ecological health. There are adequate and acceptable methods to characterize and assess Cr contaminated sites. Cr chemistry in the environment is well understood. There are documented methods to address Cr contaminat...

Final OSWER Vapor Intrusion Guidance

EPA Science Inventory

EPA is preparing to finalize its guidance on assessing and addressing vapor intrusion, which is defined as migration of volatile constituents from contaminated media in the subsurface (soil or groundwater) into the indoor environment. In November 2002, EPA issued draft guidance o...

MASS BALANCE ANALYSIS FOR MICROBIAL DECHLORINATION OF TETRACHLOROETHENE

EPA Science Inventory

Contamination of subsurface environments by chlorinated aliphatic solvents and petroleum hydrocarbons is a significant public health concern because groundwater is one of the major drinking water resources in the United States. Biotic and abiotic techniques have been widely exam...

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.

Research Spotlight: Potential pathways of radioactive contaminants to surface waters

NASA Astrophysics Data System (ADS)

Kumar, Mohi

2011-02-01

From the 1940s to the end of the Cold War, the U.S. Department of Energy maintained production facilities for manufacturing nuclear weapons along the Columbia River north of Richland, Wash. Known as the Hanford Site, the Rhode Island-sized area contains more than 53 million gallons of radioactive waste and is the location of a massive environmental cleanup. Of particular concern is that when the facility was active, fluids containing 33-59 tons of uranium were discharged into the shallow subsurface aquifer underneath Hanford. Studies suggest that this pollution is pervasively moving with the groundwater in the direction of the Columbia River. (Water Resources Research, doi:10.1029/2010WR009110, 2010)

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium

PubMed Central

Thorgersen, Michael P.; Lancaster, W. Andrew; Rajeev, Lara; Ge, Xiaoxuan; Vaccaro, Brian J.; Poole, Farris L.; Arkin, Adam P.; Mukhopadhyay, Aindrila

2016-01-01

ABSTRACT Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC had an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. IMPORTANCE Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Herein, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. While other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments. PMID:27913415

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium

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

Thorgersen, Michael P.; Lancaster, W. Andrew; Rajeev, Lara

Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC hadmore » an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Here in this paper, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. Finally, while other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments.« less

A Highly Expressed High-Molecular-Weight S-Layer Complex of Pelosinus sp. Strain UFO1 Binds Uranium.

PubMed

Thorgersen, Michael P; Lancaster, W Andrew; Rajeev, Lara; Ge, Xiaoxuan; Vaccaro, Brian J; Poole, Farris L; Arkin, Adam P; Mukhopadhyay, Aindrila; Adams, Michael W W

2017-02-15

Cell suspensions of Pelosinus sp. strain UFO1 were previously shown, using spectroscopic analysis, to sequester uranium as U(IV) complexed with carboxyl and phosphoryl group ligands on proteins. The goal of our present study was to characterize the proteins involved in uranium binding. Virtually all of the uranium in UFO1 cells was associated with a heterodimeric protein, which was termed the uranium-binding complex (UBC). The UBC was composed of two S-layer domain proteins encoded by UFO1_4202 and UFO1_4203. Samples of UBC purified from the membrane fraction contained 3.3 U atoms/heterodimer, but significant amounts of phosphate were not detected. The UBC had an estimated molecular mass by gel filtration chromatography of 15 MDa, and it was proposed to contain 150 heterodimers (UFO1_4203 and UFO1_4202) and about 500 uranium atoms. The UBC was also the dominant extracellular protein, but when purified from the growth medium, it contained only 0.3 U atoms/heterodimer. The two genes encoding the UBC were among the most highly expressed genes within the UFO1 genome, and their expressions were unchanged by the presence or absence of uranium. Therefore, the UBC appears to be constitutively expressed and is the first line of defense against uranium, including by secretion into the extracellular medium. Although S-layer proteins were previously shown to bind U(VI), here we showed that U(IV) binds to S-layer proteins, we identified the proteins involved, and we quantitated the amount of uranium bound. Widespread uranium contamination from industrial sources poses hazards to human health and to the environment. Herein, we identified a highly abundant uranium-binding complex (UBC) from Pelosinus sp. strain UFO1. The complex makes up the primary protein component of the S-layer of strain UFO1 and binds 3.3 atoms of U(IV) per heterodimer. While other bacteria have been shown to bind U(VI) on their S-layer, we demonstrate here an example of U(IV) bound by an S-layer complex. The UBC provides a potential tool for the microbiological sequestration of uranium for the cleaning of contaminated environments. Copyright © 2017 American Society for Microbiology.

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

PubMed

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

2010-09-01

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

Evapotranspiration And Geochemical Controls On Groundwater Plumes At Arid Sites: Toward Innovative Alternate End-States For Uranium Processing And Tailings Facilities

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

Looney, Brian B.; Denham, Miles E.; Eddy-Dilek, Carol A.

2014-01-08

Management of legacy tailings/waste and groundwater contamination are ongoing at the former uranium milling site in Tuba City AZ. The tailings have been consolidated and effectively isolated using an engineered cover system. For the existing groundwater plume, a system of recovery wells extracts contaminated groundwater for treatment using an advanced distillation process. The ten years of pump and treat (P&T) operations have had minimal impact on the contaminant plume – primarily due to geochemical and hydrological limits. A flow net analysis demonstrates that groundwater contamination beneath the former processing site flows in the uppermost portion of the aquifer and exitsmore » the groundwater as the plume transits into and beneath a lower terrace in the landscape. The evaluation indicates that contaminated water will not reach Moenkopi Wash, a locally important stream. Instead, shallow groundwater in arid settings such as Tuba City is transferred into the vadose zone and atmosphere via evaporation, transpiration and diffuse seepage. The dissolved constituents are projected to precipitate and accumulate as minerals such as calcite and gypsum in the deep vadose zone (near the capillary fringe), around the roots of phreatophyte plants, and near seeps. The natural hydrologic and geochemical controls common in arid environments such as Tuba City work together to limit the size of the groundwater plume, to naturally attenuate and detoxify groundwater contaminants, and to reduce risks to humans, livestock and the environment. The technical evaluation supports an alternative beneficial reuse (“brownfield”) scenario for Tuba City. This alternative approach would have low risks, similar to the current P&T scenario, but would eliminate the energy and expense associated with the active treatment and convert the former uranium processing site into a resource for future employment of local citizens and ongoing benefit to the Native American Nations.« less

Arsenic Detoxification by Geobacter Species.

PubMed

Dang, Yan; Walker, David J F; Vautour, Kaitlin E; Dixon, Steven; Holmes, Dawn E

2017-02-15

Insight into the mechanisms for arsenic detoxification by Geobacter species is expected to improve the understanding of global cycling of arsenic in iron-rich subsurface sedimentary environments. Analysis of 14 different Geobacter genomes showed that all of these species have genes coding for an arsenic detoxification system (ars operon), and several have genes required for arsenic respiration (arr operon) and methylation (arsM). Genes encoding four arsenic repressor-like proteins were detected in the genome of G. sulfurreducens; however, only one (ArsR1) regulated transcription of the ars operon. Elimination of arsR1 from the G. sulfurreducens chromosome resulted in enhanced transcription of genes coding for the arsenic efflux pump (Acr3) and arsenate reductase (ArsC). When the gene coding for Acr3 was deleted, cells were not able to grow in the presence of either the oxidized or reduced form of arsenic, while arsC deletion mutants could grow in the presence of arsenite but not arsenate. These studies shed light on how Geobacter influences arsenic mobility in anoxic sediments and may help us develop methods to remediate arsenic contamination in the subsurface. This study examines arsenic transformation mechanisms utilized by Geobacter, a genus of iron-reducing bacteria that are predominant in many anoxic iron-rich subsurface environments. Geobacter species play a major role in microbially mediated arsenic release from metal hydroxides in the subsurface. This release raises arsenic concentrations in drinking water to levels that are high enough to cause major health problems. Therefore, information obtained from studies of Geobacter should shed light on arsenic cycling in iron-rich subsurface sedimentary environments, which may help reduce arsenic-associated illnesses. These studies should also help in the development of biosensors that can be used to detect arsenic contaminants in anoxic subsurface environments. We examined 14 different Geobacter genomes and found that all of these species possess genes coding for an arsenic detoxification system (ars operon), and some also have genes required for arsenic respiration (arr operon) and arsenic methylation (arsM). Copyright © 2017 American Society for Microbiology.

Arsenic Detoxification by Geobacter Species

PubMed Central

Walker, David J. F.; Vautour, Kaitlin E.; Dixon, Steven

2016-01-01

ABSTRACT Insight into the mechanisms for arsenic detoxification by Geobacter species is expected to improve the understanding of global cycling of arsenic in iron-rich subsurface sedimentary environments. Analysis of 14 different Geobacter genomes showed that all of these species have genes coding for an arsenic detoxification system (ars operon), and several have genes required for arsenic respiration (arr operon) and methylation (arsM). Genes encoding four arsenic repressor-like proteins were detected in the genome of G. sulfurreducens; however, only one (ArsR1) regulated transcription of the ars operon. Elimination of arsR1 from the G. sulfurreducens chromosome resulted in enhanced transcription of genes coding for the arsenic efflux pump (Acr3) and arsenate reductase (ArsC). When the gene coding for Acr3 was deleted, cells were not able to grow in the presence of either the oxidized or reduced form of arsenic, while arsC deletion mutants could grow in the presence of arsenite but not arsenate. These studies shed light on how Geobacter influences arsenic mobility in anoxic sediments and may help us develop methods to remediate arsenic contamination in the subsurface. IMPORTANCE This study examines arsenic transformation mechanisms utilized by Geobacter, a genus of iron-reducing bacteria that are predominant in many anoxic iron-rich subsurface environments. Geobacter species play a major role in microbially mediated arsenic release from metal hydroxides in the subsurface. This release raises arsenic concentrations in drinking water to levels that are high enough to cause major health problems. Therefore, information obtained from studies of Geobacter should shed light on arsenic cycling in iron-rich subsurface sedimentary environments, which may help reduce arsenic-associated illnesses. These studies should also help in the development of biosensors that can be used to detect arsenic contaminants in anoxic subsurface environments. We examined 14 different Geobacter genomes and found that all of these species possess genes coding for an arsenic detoxification system (ars operon), and some also have genes required for arsenic respiration (arr operon) and arsenic methylation (arsM). PMID:27940542

Analysis of Tank 38H (HTF-38-17-52, -53) and Tank 43H (HTF-43-17-54, -55) Samples for Support of the Enrichment Control and Corrosion Control Programs

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

Hay, M.; Coleman, C.; Diprete, D.

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H surface sample was 41.3 mg/L while the sub-surface sample was 43.5 mg/L. The Tank 43H samples contained total uranium concentrations of 28.5 mg/L in the surface sample and 28.1 mg/L in the sub-surface sample. The U-235 percentage ranged from 0.62% to 0.63% for the Tank 38H samples and Tank 43H samples. The total uranium and percent U-235 results in the table appear slightly lower than recent Tank 38H and Tank 43H uranium measurements. The plutonium results in the tablemore » show a large difference between the surface and sub-surface sample concentrations for Tank 38H. The Tank 43H plutonium results closely match the range of values measured on previous samples. The Cs-137 results for the Tank 38H surface and sub-surface samples show similar concentrations slightly higher than the concentrations measured in recent samples. The Cs-137 results for the two Tank 43H samples also show similar concentrations within the range of values measured on previous samples. The four samples show silicon concentrations somewhat lower than the previous samples with values ranging from 124 to 168 mg/L.« less

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

PubMed

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

2013-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2013-04-01

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

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

USGS Publications Warehouse

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

1995-01-01

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

MICROBIAL ECOLOGY OF THE SUBSURFACE AT AN ABANDONED CREOSOTE WASTE SITE

EPA Science Inventory

The microbial ecology of pristine, slightly contaminated, and heavily contaminated subsurface materials, and four subsurface materials on the periphery of the plume at an abandoned creosote waste site was investigated. Except for the unsaturated zone of the heavily contaminated m...

Process for removing carbon from uranium

DOEpatents

Powell, George L.; Holcombe, Jr., Cressie E.

1976-01-01

Carbon contamination is removed from uranium and uranium alloys by heating in inert atmosphere to 700.degree.-1900.degree.C in effective contact with yttrium to cause carbon in the uranium to react with the yttrium. The yttrium is either in direct contact with the contaminated uranium or in indirect contact by means of an intermediate transport medium.

Chemical aspects of uranium behavior in soils: A review

NASA Astrophysics Data System (ADS)

Vodyanitskii, Yu. N.

2011-08-01

Uranium has varying degrees of oxidation (+4 and +6) and is responsive to changes in the redox potential of the environment. It is deposited at the reduction barrier with the participation of biota and at the sorption barrier under oxidative conditions. Iron (hydr)oxides are the strongest sorbents of uranium. Uranium, being an element of medium biological absorption, can accumulate (relative to thorium) in the humus horizons of some soils. The high content of uranium in uncontaminated soils is most frequently inherited from the parent rocks in the regions of positive U anomalies: in the soils developed on oil shales and in the marginal zone of bogs at the reduction barrier. The development of nuclear and coal-fired power engineering resulted in the environmental contamination with uranium. The immobilization of anthropogenic uranium at artificial geochemical barriers is based on two preconditions: the stimulation of on-site metal-reducing bacteria or the introduction of strong mineral reducers, e.g., Fe at low degrees of oxidation.

Conceptual Model of Iodine Behavior in the Subsurface at the Hanford Site

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

Truex, Michael J.; Lee, Brady D.; Johnson, Christian D.

Isotopes of iodine were generated during plutonium production within the nine production reactors at the U.S. Department of Energy Hanford Site. The short half-life 131I that was released from the fuel into the atmosphere during the dissolution process (when the fuel was dissolved) in the Hanford Site 200 Area is no longer present at concentrations of concern in the environment. The long half-life 129I generated at the Hanford Site during reactor operations was (1) stored in single-shell and double-shell tanks, (2) discharged to liquid disposal sites (e.g., cribs and trenches), (3) released to the atmosphere during fuel reprocessing operations, ormore » (4) captured by off-gas absorbent devices (silver reactors) at chemical separations plants (PUREX, B-Plant, T-Plant, and REDOX). Releases of 129I to the subsurface have resulted in several large, though dilute, plumes in the groundwater. There is also 129I remaining in the vadose zone beneath disposal or leak locations. The fate and transport of 129I in the environment and potential remediation technologies are currently being studied as part of environmental remediation activities at the Hanford Site. A conceptual model describing the nature and extent of subsurface contamination, factors that control plume behavior, and factors relevant to potential remediation processes is needed to support environmental remedy decisions. Because 129I is an uncommon contaminant, relevant remediation experience and scientific literature are limited. In addition, its behavior in subsurface is different from that of other more common and important contaminants (e.g., U, Cr and Tc) in terms of sorption (adsorption and precipitation), and aqueous phase species transformation via redox reactions. Thus, the conceptual model also needs to both describe known contaminant and biogeochemical process information and identify aspects about which additional information is needed to effectively support remedy decisions.« less

Selective phylogenetic analysis targeting 16S rRNA genes of hyperthermophilic archaea in the deep-subsurface hot biosphere.

PubMed

Kimura, Hiroyuki; Ishibashi, Jun-Ichiro; Masuda, Harue; Kato, Kenji; Hanada, Satoshi

2007-04-01

International drilling projects for the study of microbial communities in the deep-subsurface hot biosphere have been expanded. Core samples obtained by deep drilling are commonly contaminated with mesophilic microorganisms in the drilling fluid, making it difficult to examine the microbial community by 16S rRNA gene clone library analysis. To eliminate mesophilic organism contamination, we previously developed a new method (selective phylogenetic analysis [SePA]) based on the strong correlation between the guanine-plus-cytosine (G+C) contents of the 16S rRNA genes and the optimal growth temperatures of prokaryotes, and we verified the method's effectiveness (H. Kimura, M. Sugihara, K. Kato, and S. Hanada, Appl. Environ. Microbiol. 72:21-27, 2006). In the present study we ascertained SePA's ability to eliminate contamination by archaeal rRNA genes, using deep-sea hydrothermal fluid (117 degrees C) and surface seawater (29.9 degrees C) as substitutes for deep-subsurface geothermal samples and drilling fluid, respectively. Archaeal 16S rRNA gene fragments, PCR amplified from the surface seawater, were denatured at 82 degrees C and completely digested with exonuclease I (Exo I), while gene fragments from the deep-sea hydrothermal fluid remained intact after denaturation at 84 degrees C because of their high G+C contents. An examination using mixtures of DNAs from the two environmental samples showed that denaturation at 84 degrees C and digestion with Exo I completely eliminated archaeal 16S rRNA genes from the surface seawater. Our method was quite useful for culture-independent community analysis of hyperthermophilic archaea in core samples recovered from deep-subsurface geothermal environments.

Depleted uranium investigation at missile impact sites in White Sands Missile Range

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

Van Etten, D.M.; Purtymun, W.D.

1994-01-01

An investigation for residual depleted uranium was conducted at Pershing missile impact sites on the White Sands Missile Range. Subsurface core soil samples were taken at Chess, Salt Target, and Mine Impact Sites. A sampling pump was installed in a monitoring well at Site 65 where a Pershing earth penetrator was not recovered. Pumping tests and water samples were taken at this site. Chess Site, located in a gypsum flat, was the only location showing elevated levels of depleted uranium in the subsurface soil or perched groundwater. Small fragments can still be found on the surface of the impact sites.more » The seasonal flooding and near surface water has aided in the movement of surface fragments.« less

Iron mineralogy and uranium-binding environment in the rhizosphere of a wetland soil

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

Kaplan, Daniel I.; Kukkadapu, Ravi; Seaman, John C.

Wetlands mitigate the migration of groundwater contaminants through the creation of biogeochemical gradients that enhance multiple contaminant-binding processes. Our hypothesis was that wetland plants not only contribute organic carbon, produce strong redox gradients, and elevate microbial populations to soils, but together these conditions also promote the formation of Fe (oxyhydr)oxides within the plant rhizosphere that may also contribute to contaminant immobilization. Mineralogy and U binding environments of the rhizosphere (plant-impacted soil zone) were evaluated in samples collected from contaminated and non-contaminated areas of a wetland on the Savannah River Site in South Carolina. Based on Mossbauer spectroscopy, rhizosphere soil collectedmore » from the field study site was greatly enriched with poorly crystalline nanoparticulate Fe-oxide/ferrihydrite-like materials and nano-goethite (<15-nm). X-ray computed tomography or various microscopy techniques showed that root plaques, tens-of microns thick, were consisted of highly oriented nanoparticles in an orientation suggestive that the roots were involved in the Fe-nanoparticle formation. Because of detection limits, SEM/EDS could not confirm whether U was enriched in the rhizosphere but did demonstrate that U was enriched on root plaques. Uranium in the plaques was always found in association with P and frequently with Fe. Together these findings suggest that plants may not only alter soil microbial and chemical conditions, but also mineralogical conditions that may be conducive to aqueous contaminant immobilization in wetlands.« less

Effects of organic carbon supply rates on uranium mobility in a previously bioreduced contaminated sediment.

PubMed

Wan, Jiamin; Tokunaga, Tetsu K; Kim, Yongman; Brodie, Eoin; Daly, Rebecca; Hazen, Terry C; Firestone, Mary K

2008-10-15

Bioreduction-based strategies for remediating uranium (U)-contaminated sediments face the challenge of maintaining the reduced status of U for long times. Because groundwater influxes continuously bring in oxidizing terminal electron acceptors (O2, NO3(-)), it is necessary to continue supplying organic carbon (OC) to maintain the reducing environment after U bioreduction is achieved. We tested the influence of OC supply rates on mobility of previously microbial reduced uranium U(IV) in contaminated sediments. We found that high degrees of U mobilization occurred when OC supply rates were high, and when the sediment still contained abundant Fe(III). Although 900 days with low levels of OC supply minimized U mobilization, the sediment redox potential increased with time as did extractable U(VI) fractions. Molecular analyses of total microbial activity demonstrated a positive correlation with OC supply and analyses of Geobacteraceae activity (RT-qPCR of 16S rRNA) indicated continued activity even when the effluent Fe(II) became undetectable. These data support our hypothesis on the mechanisms responsible for remobilization of U under reducing conditions; that microbial respiration caused increased (bi)carbonate concentration and formation of stable uranyl carbonate complexes, thereby shifted U(IV)/U(VI) equilibrium to more reducing potentials. The data also suggested that low OC concentrations could not sustain the reducing condition of the sediment for much longer time. Bioreduced U(IV) is not sustainable in an oxidizing environment for a very long time.

Review on subsurface colloids and colloid-associated contaminant transport in saturated porous media.

PubMed

Kanti Sen, Tushar; Khilar, Kartic C

2006-02-28

In this review article, the authors present up-to-date developments on experimental, modeling and field studies on the role of subsurface colloidal fines on contaminant transport in saturated porous media. It is a complex phenomenon in porous media involving several basic processes such as colloidal fines release, dispersion stabilization, migration and fines entrapment/plugging at the pore constrictions and adsorption at solid/liquid interface. The effects of these basic processes on the contaminant transport have been compiled. Here the authors first present the compilation on in situ colloidal fines sources, release, stabilization of colloidal dispersion and migration which are a function of physical and chemical conditions of subsurface environment and finally their role in inorganic and organic contaminants transport in porous media. The important aspects of this article are as follows: (i) it gives not only complete compilation on colloidal fines-facilitated contaminant transport but also reviews the new role of colloidal fines in contaminant retardation due to plugging of pore constrictions. This plugging phenomenon also depends on various factors such as concentration of colloidal fines, superficial velocity and bead-to-particle size ratio. This plugging-based contaminant transport can be used to develop containment technique in soil and groundwater remediation. (ii) It also presents the importance of critical salt concentration (CSC), critical ionic strength for mixed salt, critical shear stressor critical particle concentration (CPC) on in situ colloidal fines release and migration and consequently their role on contaminant transport in porous media. (iii) It also reviews another class of colloidal fines called biocolloids and their transport in porous media. Finally, the authors highlight the future research based on their critical review on colloid-associated contaminant transport in saturated porous media.

Reduction of uranium by cytochrome c3 of Desulfovibrio vulgaris

USGS Publications Warehouse

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

1993-01-01

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

US Air Force 1989 Research Initiation Program . Volume 1.

DTIC Science & Technology

1992-06-25

microbial ecology of contaminated soils. 27-5 Thomas and coworkers (1989) studied microbial activity at a creosote waste site and demonstrated that...provide information essential for an understanding of the microbial ecology of contaminated soils, they do not address the microbiology of...substrates. Appl. Environ. Microbiol. 49:711-713. Thomas, J. M., M. D. Lee, M. J. Scott and C. H. Ward. 1989. Microbial ecology of the subsurface Lt an

MINERALOGICAL PRESERVATION OF SOLID SAMPLES COLLECTED FROM ANOXIC SUBSURFACE ENVIRONMENTS

EPA Science Inventory

Remedial technologies utilized at hazardous waste sites for the treatment of metal and metalloid contaminants often take advantage of reduction-oxidation (redox) processes to reach ground water clean up goals. This is because redox reactions, in many cases, govern the biogeochem...

IN-SITU BIOREMEDIATION OF GROUND WATER AND GEOLOGICAL MATERIAL: A REVIEW OF TECHNOLOGIES

EPA Science Inventory

In situ bioremediation of subsurface environments involve the use of microorganisms to convert contaminants to less harmful products and sometimes offers significant potential advantages over other remediation technologies. n order for these biodegradative processes to occur, icr...

ENGINEERING CONCEPTS FOR IN SITU BIOREMEDIATION. (R825689C051)

EPA Science Inventory

Abstract

Most organic materials that contaminate soil and the subsurface environment are readily degraded by natural biological processes. Thus, bioremediation can be thought of as a highly successful purification process. However, some organic molecules are naturally ...

Geochemistry and migration of contaminants at the Weldon Spring chemical plant site, St. Charles County, Missouri, 1989-91

USGS Publications Warehouse

Schumacher, John G.

1993-01-01

The geochemistry of the shallow aquifer and geochemical controls on the migration of uranium and other constituents from raffinate pits were determined at the Weldon Spring chemical plant site. Surface-water samples from the raffinate pits con- tained large concentrations of calcium, magnesium, sodium, potassium, sulfate, nitrite, lithium, moly- bdenum, strontium, vanadium, and uranium. Analyses of interstitial-water samples from raffinate pit 3 indicated that concentrations of most constituents increased with increasing depth below the water- sediment interface. Nitrate and uranium were not chemically reduced and attenuated within the raffinate pits and can be expected to migrate into the overburden. Laboratory sorption experiments were performed to evaluate the effect of pH value on the sorption of several raffinate constituents by the overburden. No sorption of calcium, sodium, sulfate, nitrate, or lithium was observed. Sorption of molybdenum was dependent on solution pH and sorption of uranium was dependent on solution pH and carbonate concentration. The sorption of uranium and molybdenum was consistent with sorption controlled by oxyhydroxides. The quality of water collected in overburden lysimeters near raffinate pit 4 can be modeled as a mixture of water from raffinate pits 3 and 4, and an uncontaminated com- ponent in a system at equilibrium with ferrihydrite and calcite. Increased constituent concentrations in a perennial spring north of the site were the result of a subsurface connection between the spring and several losing stream segments receiving runoff from the site, in addition to seepage from the raffinate pits.

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

PubMed

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

2013-02-01

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

Aseptically Sampled Organics in Subsurface Rocks From the Mars Analog Rio Tinto Experiment: An Analog For The Search for Deep Subsurface Life on Mars.}

NASA Astrophysics Data System (ADS)

Bonaccorsi, R.; Stoker, C. R.

2005-12-01

The subsurface is the key environment for searching for life on planets lacking surface life. Subsurface ecosystems are of great relevance to astrobiology including the search for past/present life on Mars. The surface of Mars has conditions preventing current life but the subsurface might preserve organics and even host some life [1]. The Mars-Analog-Rio-Tinto-Experiment (MARTE) is performing a simulation of a Mars drilling experiment. This comprises conventional and robotic drilling of cores in a volcanically-hosted-massive-pyrite deposit [2] from the Iberian Pyritic Belt (IBP) and life detection experiments applying anti-contamination protocols (e.g., ATP Luminometry assay). The RT is considered an important analog of the Sinus Meridiani site on Mars and an ideal model analog for a deep subsurface Martian environment. Former results from MARTE suggest the existence of a relatively complex subsurface life including aerobic and anaerobic chemoautotrophs and strict anaerobic methanogens sustained by Fe and S minerals in anoxic conditions. A key requirement for the analysis of a subsurface sample on Mars is a set of simple tests that can help determine if the sample contains organic material of biological origin, and its potential for retaining definitive biosignatures. We report here on the presence of bulk organic matter Corg (0.03-0.05 Wt%), and Ntot (0.01-0.04 Wt%) and amount of measured ATP (Lightning MVP, Biocontrol) in weathered rocks (tuffs, gossan, pyrite stockwork from Borehole #8; >166m). This provides key insight on the type of trophic system sustaining the subsurface biosphere (i.e., heterotrophs vs. autotrophs) at RT. ATP data (Relative-Luminosity-Units, RLU) provide information on possible contamination and distribution of viable biomass with core depth (BH#8, and BH#7, ~3m). Avg. 153 RLU, i.e., surface vs. center of core, suggest that cleaness/sterility can be maintained when using a simple sterile protocol under field conditions. Results from this research will support future drilling mission planned on Mars. [1] Boston, P.J., et al., 1992. Icarus 95,300-308; [2] Leistel et al., 1998.

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

PubMed

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

2016-06-07

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

Movement and fate of crude-oil in contaminants in the subsurface environment at Bemidji, Minnesota: Chapter C in U.S. Geological Survey program on toxic waste--ground-water contamination: Proceedings of the Third technical meeting, Pensacola, Florida, March 23-27, 1987

USGS Publications Warehouse

Hult, Marc F.

1987-01-01

Predictions of the evolution and ultimate geometry of contaminant plumes resulting from spills require quantitative descriptions of the rate of mass transfer from the organic fluid to ground water. Pfannkuch presents laboratory and field work that describe how the the rate of oil dissolution, and therefore the strength of the contaminant source, is controlled by fluctuations in ground-water velocity and water-table fluctuations.

Bioimmobilization of uranium-practical tools for field applications

NASA Astrophysics Data System (ADS)

Istok, J. D.

2011-12-01

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

Geologic report on the San Rafael Swell Drilling Project, San Rafael Swell, Utah

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

Bluhm, C.T.; Rundle, J.G.

1981-08-01

Twenty-two holes totaling 34,874 feet (10,629.6 meters) were rotary and core drilled on the northern and western flanks of the San Rafael Swell to test fluvial-lacustrine sequences of the Morrison Formation and the lower part of the Chinle Formation. The objective of the project was to obtain subsurface data so that improved uranium resource estimates could be determined for the area. Although the Brushy Basin and the Salt Wash Members of the Morrison Formation are not considered favorable in this area for the occurrence of significant uranium deposits, uranium minerals were encountered in several of the holes. Some spotty ormore » very low-grade mineralization was also encountered in the White Star Trunk area. The lower part of the Chinle Formation is considered to be favorable for potentially significant uranium deposits along the west flank of the San Rafael Swell. One hole (SR-202) east of Ferron, Utah, intersected uranium, silver, molybdenum, and copper mineralization. More exploratory drilling in the vicinity of this hole is recommended. As a result of the study of many geochemical analyses and a careful determination of the lithology shown by drilling, a sabkha environment is suggested for the concentration of uranium, zinc, iron, lead, copper, silver, and perhaps other elements in parts of the Moody Canyon Member of the Moenkopi Formation.« less

PRELIMINARY DATA REPORT: HUMATE INJECTION AS AN ENHANCED ATTENUATION METHOD AT THE F-AREA SEEPAGE BASINS, SAVANNAH RIVER SITE

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

Millings, M.

2013-09-16

A field test of a humate technology for uranium and I-129 remediation was conducted at the F-Area Field Research Site as part of the Attenuation-Based Remedies for the Subsurface Applied Field Research Initiative (ABRS AFRI) funded by the DOE Office of Soil and Groundwater Remediation. Previous studies have shown that humic acid sorbed to sediments strongly binds uranium at mildly acidic pH and potentially binds iodine-129 (I-129). Use of humate could be applicable for contaminant stabilization at a wide variety of DOE sites however pilot field-scale tests and optimization of this technology are required to move this technical approach frommore » basic science to actual field deployment and regulatory acceptance. The groundwater plume at the F-Area Field Research Site contains a large number of contaminants, the most important from a risk perspective being strontium-90 (Sr-90), uranium isotopes, I-129, tritium, and nitrate. Groundwater remains acidic, with pH as low as 3.2 near the basins and increasing to the background pH of approximately 5at the plume fringes. The field test was conducted in monitoring well FOB 16D, which historically has shown low pH and elevated concentrations of Sr-90, uranium, I-129 and tritium. The field test included three months of baseline monitoring followed by injection of a potassium humate solution and approximately four and half months of post monitoring. Samples were collected and analyzed for numerous constituents but the focus was on attenuation of uranium, Sr-90, and I-129. This report provides background information, methodology, and preliminary field results for a humate field test. Results from the field monitoring show that most of the excess humate (i.e., humate that did not sorb to the sediments) has flushed through the surrounding formation. Furthermore, the data indicate that the test was successful in loading a band of sediment surrounding the injection point to a point where pH could return to near normal during the study timeframe. Future work will involve a final report, which will include data trends, correlations and interpretations of laboratory data.« less

Calixarene-entrapped nanoemulsion for uranium extraction from contaminated solutions.

PubMed

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

2010-03-01

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

INTERLABORATORY METHODS COMPARISON FOR THE TOTAL ORGANIC CARBON ANALYSIS OF AQUIFER MATERIALS

EPA Science Inventory

The total organic carbon (TOC) content of aquifer materials has been found to have significant effects on the movement of pollutants in the subsurface environment. Accurate quantification of TOC is therefore of great im- portance to research in groundwater contamination. However,...

Uncertainty analysis of multi-rate kinetics of uranium desorption from sediments

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

Zhang, Xiaoying; Liu, Chongxuan; Hu, Bill X.

2014-01-01

A multi-rate expression for uranyl [U(VI)] surface complexation reactions has been proposed to describe diffusion-limited U(VI) sorption/desorption in heterogeneous subsurface sediments. An important assumption in the rate expression is that its rate constants follow a certain type probability distribution. In this paper, a Bayes-based, Differential Evolution Markov Chain method was used to assess the distribution assumption and to analyze parameter and model structure uncertainties. U(VI) desorption from a contaminated sediment at the US Hanford 300 Area, Washington was used as an example for detail analysis. The results indicated that: 1) the rate constants in the multi-rate expression contain uneven uncertaintiesmore » with slower rate constants having relative larger uncertainties; 2) the lognormal distribution is an effective assumption for the rate constants in the multi-rate model to simualte U(VI) desorption; 3) however, long-term prediction and its uncertainty may be significantly biased by the lognormal assumption for the smaller rate constants; and 4) both parameter and model structure uncertainties can affect the extrapolation of the multi-rate model with a larger uncertainty from the model structure. The results provide important insights into the factors contributing to the uncertainties of the multi-rate expression commonly used to describe the diffusion or mixing-limited sorption/desorption of both organic and inorganic contaminants in subsurface sediments.« less

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

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

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

1978-12-31

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

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

PubMed Central

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

2018-01-01

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

Post-test evaluation of the geology, geochemistry, microbiology, and hydrology of the in situ air stripping demonstration site at the Savannah River Site

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

Eddy Dilek, C.A.; Looney, B.B.; Hazen, T.C.

A full-scale demonstration of the use of horizontal wells for in situ air stripping for environment restoration was completed as part of the Savannah River Integrated Demonstration Program. The demonstration of in situ air stripping was the first in a series of demonstrations of innovative remediation technologies for the cleanup of sites contaminated with volatile organic contaminants. The in situ air stripping system consisted of two directionally drilled wells that delivered gases to and extract contamination from the subsurface. The demonstration was designed to remediate soils and sediments in the unsaturated and saturated zones as well as groundwater contaminated withmore » volatile organic compounds. The demonstration successfully removed significant quantities of solvent from the subsurface. The field site and horizontal wells were subsequently used for an in situ bioremediation demonstration during which methane was added to the injected air. The field conditions documented herein represent the baseline status of the site for evaluating the in situ bioremediation as well as the post-test conditions for the in situ air stripping demonstration. Characterization activities focused on documenting the nature and distribution of contamination in the subsurface. The post-test characterization activities discussed herein include results from the analysis of sediment samples, three-dimensional images of the pretest and post-test data, contaminant inventories estimated from pretest and post-test models, a detailed lithologic cross sections of the site, results of aquifer testing, and measurements of geotechnical parameters of undisturbed core sediments.« less

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

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

PubMed

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

2015-12-01

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

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

PubMed

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

2009-01-01

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

Impact of natural organic matter on uranium transport through saturated geologic materials: from molecular to column scale.

PubMed

Yang, Yu; Saiers, James E; Xu, Na; Minasian, Stefan G; Tyliszczak, Tolek; Kozimor, Stosh A; Shuh, David K; Barnett, Mark O

2012-06-05

The risk stemming from human exposure to actinides via the groundwater track has motivated numerous studies on the transport of radionuclides within geologic environments; however, the effects of waterborne organic matter on radionuclide mobility are still poorly understood. In this study, we compared the abilities of three humic acids (HAs) (obtained through sequential extraction of a peat soil) to cotransport hexavalent uranium (U) within water-saturated sand columns. Relative breakthrough concentrations of U measured upon elution of 18 pore volumes increased from undetectable levels (<0.001) in an experiment without HAs to 0.17 to 0.55 in experiments with HAs. The strength of the HA effect on U mobility was positively correlated with the hydrophobicity of organic matter and NMR-detected content of alkyl carbon, which indicates the possible importance of hydrophobic organic matter in facilitating U transport. Carbon and uranium elemental maps collected with a scanning transmission X-ray microscope (STXM) revealed uneven microscale distribution of U. Such molecular- and column-scale data provide evidence for a critical role of hydrophobic organic matter in the association and cotransport of U by HAs. Therefore, evaluations of radionuclide transport within subsurface environments should consider the chemical characteristics of waterborne organic substances, especially hydrophobic organic matter.

Salmon Site Remedial Investigation Report, Exhibit 5

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

USDOE /NV

1999-09-01

This Salmon Site Remedial Investigation Report provides the results of activities initiated by the U.S. Department of Energy (DOE) to determine if contamination at the Salmon Site poses a current or future risk to human health and the environment. These results were used to develop and evaluate a range of risk-based remedial alternatives. Located in Lamar County, Mississippi, the Salmon Site was used by the U.S. Atomic Energy Commission (predecessor to the DOE) between 1964 and 1970 for two nuclear and two gas explosions conducted deep underground in a salt dome. The testing resulted in the release of radionuclides intomore » the salt dome. During reentry drilling and other site activities, liquid and solid wastes containing radioactivity were generated resulting in surface soil and groundwater contamination. Most of the waste and contaminated soil and water were disposed of in 1993 during site restoration either in the cavities left by the tests or in an injection well. Other radioactive wastes were transported to the Nevada Test Site for disposal. Nonradioactive wastes were disposed of in pits at the site and capped with clean soil and graded. The preliminary investigation showed residual contamination in the Surface Ground Zero mud pits below the water table. Remedial investigations results concluded the contaminant concentrations detected present no significant risk to existing and/or future land users, if surface institutional controls and subsurface restrictions are maintained. Recent sampling results determined no significant contamination in the surface or shallow subsurface. The test cavity resulting from the experiments is contaminated and cannot be economically remediated with existing technologies. The ecological sampling did not detect biological uptake of contaminants in the plants or animals sampled. Based on the current use of the Salmon Site, the following remedial actions were identified to protect both human health and the environment: (1) the installation of a water supply system that will provide potable water to the site and residence in the proximity to the site; (2) continued maintenance of surface institutional controls and subsurface restrictions; and (3) continue to implement the long-term hydrologic monitoring program. The Salmon Site will be relinquished the State of Mississippi as mandated by Public Law 104-201-September 23, 1996, to be used as a demonstration forest/wildlife refuge. Should the land use change in the future and/or monitoring information indicates a change in the site conditions, the DOE will reassess the risk impacts to human health and the environment.« less

Salmon Site Remedial Investigation Report, Main Body

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

US DOE /NV

1999-09-01

This Salmon Site Remedial Investigation Report provides the results of activities initiated by the U.S. Department of Energy (DOE) to determine if contamination at the Salmon Site poses a current or future risk to human health and the environment. These results were used to develop and evaluate a range of risk-based remedial alternatives. Located in Lamar County, Mississippi, the Salmon Site was used by the U.S. Atomic Energy Commission (predecessor to the DOE) between 1964 and 1970 for two nuclear and two gas explosions conducted deep underground in a salt dome. The testing resulted in the release of radionuclides intomore » the salt dome. During reentry drilling and other site activities, liquid and solid wastes containing radioactivity were generated resulting in surface soil and groundwater contamination. Most of the waste and contaminated soil and water were disposed of in 1993 during site restoration either in the cavities left by the tests or in an injection well. Other radioactive wastes were transported to the Nevada Test Site for disposal. Nonradioactive wastes were disposed of in pits at the site and capped with clean soil and graded. The preliminary investigation showed residual contamination in the Surface Ground Zero mud pits below the water table. Remedial investigations results concluded the contaminant concentrations detected present no significant risk to existing and/or future land users, if surface institutional controls and subsurface restrictions are maintained. Recent sampling results determined no significant contamination in the surface or shallow subsurface. The test cavity resulting from the experiments is contaminated and cannot be economically remediated with existing technologies. The ecological sampling did not detect biological uptake of contaminants in the plants or animals sampled. Based on the current use of the Salmon Site, the following remedial actions were identified to protect both human health and the environment: (1) the installation of a water supply system that will provide potable water to the site and residence in the proximity to the site; (2) continued maintenance of surface institutional controls and subsurface restrictions; and (3) continue to implement the long-term hydrologic monitoring program. The Salmon Site will be relinquished the State of Mississippi as mandated by Public Law 104-201-September 23, 1996, to be used as a demonstration forest/wildlife refuge. Should the land use change in the future and/or monitoring information indicates a change in the site conditions, the DOE will reassess the risk impacts to human health and the environment.« less

Salmon Site Remedial Investigation Report, Exhibit 2

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

USDOE NV

1999-09-01

This Salmon Site Remedial Investigation Report provides the results of activities initiated by the U.S. Department of Energy (DOE) to determine if contamination at the Salmon Site poses a current or future risk to human health and the environment. These results were used to develop and evaluate a range of risk-based remedial alternatives. Located in Lamar County, Mississippi, the Salmon Site was used by the U.S. Atomic Energy Commission (predecessor to the DOE) between 1964 and 1970 for two nuclear and two gas explosions conducted deep underground in a salt dome. The testing resulted in the release of radionuclides intomore » the salt dome. During reentry drilling and other site activities, liquid and solid wastes containing radioactivity were generated resulting in surface soil and groundwater contamination. Most of the waste and contaminated soil and water were disposed of in 1993 during site restoration either in the cavities left by the tests or in an injection well. Other radioactive wastes were transported to the Nevada Test Site for disposal. Nonradioactive wastes were disposed of in pits at the site and capped with clean soil and graded. The preliminary investigation showed residual contamination in the Surface Ground Zero mud pits below the water table. Remedial investigations results concluded the contaminant concentrations detected present no significant risk to existing and/or future land users, if surface institutional controls and subsurface restrictions are maintained. Recent sampling results determined no significant contamination in the surface or shallow subsurface. The test cavity resulting from the experiments is contaminated and cannot be economically remediated with existing technologies. The ecological sampling did not detect biological uptake of contaminants in the plants or animals sampled. Based on the current use of the Salmon Site, the following remedial actions were identified to protect both human health and the environment: (1) the installation of a water supply system that will provide potable water to the site and residence in the proximity to the site; (2) continued maintenance of surface institutional controls and subsurface restrictions; and (3) continue to implement the long-term hydrologic monitoring program. The Salmon Site will be relinquished the State of Mississippi as mandated by Public Law 104-201-September 23, 1996, to be used as a demonstration forest/wildlife refuge. Should the land use change in the future and/or monitoring information indicates a change in the site conditions, the DOE will reassess the risk impacts to human health and the environment.« less

Spatially variable stage-driven groundwater-surface water interaction inferred from time-frequency analysis of distributed temperature sensing data

USGS Publications Warehouse

Mwakanyamale, Kisa; Slater, Lee; Day-Lewis, Frederick D.; Elwaseif, Mehrez; Johnson, Carole D.

2012-01-01

Characterization of groundwater-surface water exchange is essential for improving understanding of contaminant transport between aquifers and rivers. Fiber-optic distributed temperature sensing (FODTS) provides rich spatiotemporal datasets for quantitative and qualitative analysis of groundwater-surface water exchange. We demonstrate how time-frequency analysis of FODTS and synchronous river stage time series from the Columbia River adjacent to the Hanford 300-Area, Richland, Washington, provides spatial information on the strength of stage-driven exchange of uranium contaminated groundwater in response to subsurface heterogeneity. Although used in previous studies, the stage-temperature correlation coefficient proved an unreliable indicator of the stage-driven forcing on groundwater discharge in the presence of other factors influencing river water temperature. In contrast, S-transform analysis of the stage and FODTS data definitively identifies the spatial distribution of discharge zones and provided information on the dominant forcing periods (≥2 d) of the complex dam operations driving stage fluctuations and hence groundwater-surface water exchange at the 300-Area.

Enhancement of in situ microbial remediation of aquifers

DOEpatents

Fredrickson, James K.; Brockman, Fred J.; Streile, Gary P.; Cary, John W.; McBride, John F.

1993-01-01

Methods are provided for remediating subsurface areas contaminated by toxic organic compounds. An innocuous oil, such as vegetable oil, mineral oil, or other immiscible organic liquid, is introduced into the contaminated area and permitted to move therethrough. The oil concentrates or strips the organic contaminants, such that the concentration of the contaminants is reduced and such contaminants are available to be either pumped out of the subsurface area or metabolized by microorganisms. Microorganisms may be introduced into the contaminated area to effect bioremediation of the contamination. The methods may be adapted to deliver microorganisms, enzymes, nutrients and electron donors to subsurface zones contaminated by nitrate in order to stimulate or enhance denitrification.

Enhancement of in situ microbial remediation of aquifers

DOEpatents

Fredrickson, J.K.; Brockman, F.J.; Streile, G.P.; Cary, J.W.; McBride, J.F.

1993-11-30

Methods are provided for remediating subsurface areas contaminated by toxic organic compounds. An innocuous oil, such as vegetable oil, mineral oil, or other immiscible organic liquid, is introduced into the contaminated area and permitted to move therethrough. The oil concentrates or strips the organic contaminants, such that the concentration of the contaminants is reduced and such contaminants are available to be either pumped out of the subsurface area or metabolized by microorganisms. Microorganisms may be introduced into the contaminated area to effect bioremediation of the contamination. The methods may be adapted to deliver microorganisms, enzymes, nutrients and electron donors to subsurface zones contaminated by nitrate in order to stimulate or enhance denitrification. 4 figures.

Method to remove uranium/vanadium contamination from groundwater

DOEpatents

Metzler, Donald R.; Morrison, Stanley

2004-07-27

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

Fractal topography and subsurface water flows from fluvial bedforms to the continental shield

USGS Publications Warehouse

Worman, A.; Packman, A.I.; Marklund, L.; Harvey, J.W.; Stone, S.H.

2007-01-01

Surface-subsurface flow interactions are critical to a wide range of geochemical and ecological processes and to the fate of contaminants in freshwater environments. Fractal scaling relationships have been found in distributions of both land surface topography and solute efflux from watersheds, but the linkage between those observations has not been realized. We show that the fractal nature of the land surface in fluvial and glacial systems produces fractal distributions of recharge, discharge, and associated subsurface flow patterns. Interfacial flux tends to be dominated by small-scale features while the flux through deeper subsurface flow paths tends to be controlled by larger-scale features. This scaling behavior holds at all scales, from small fluvial bedforms (tens of centimeters) to the continental landscape (hundreds of kilometers). The fractal nature of surface-subsurface water fluxes yields a single scale-independent distribution of subsurface water residence times for both near-surface fluvial systems and deeper hydrogeological flows. Copyright 2007 by the American Geophysical Union.

Remediation of TCE-contaminated groundwater using nanocatalyst and bacteria.

PubMed

Kang, Ser Ku; Seo, Hyunhee; Sun, Eunyoung; Kim, Inseon; Roh, Yul

2011-08-01

The objective of this study was to develop and evaluate the remediation of trichloroethene (TCE)-contaminated groundwater using both a nanocatalyst (bio-Zn-magnetite) and bacterium (similar to Clostridium quinii) in anoxic environments. Of the 7 nanocatalysts tested, bio-Zn-magnetite showed the highest TCE dechlorination efficiency, with an average of ca. 90% within 8 days in a batch experiment. The column tests confirmed that the application of bio-Zn-magnetite in combination with the bacterium achieved high degradation efficiency (ca. 90%) of TCE within 5 days compared to the nanocatalyst only, which degraded only 30% of the TCE. These results suggest that the application of a nanocatalyst and the bacterium have potential for the remediation of TCE-contaminated groundwater in subsurface environments.

FLUORIDE VOLATILITY PROCESS FOR THE RECOVERY OF URANIUM

DOEpatents

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

1958-04-15

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

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

PubMed

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

2013-09-25

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

Microbial Functional Gene Diversity with a Shift of Subsurface Redox Conditions during In Situ Uranium Reduction

PubMed Central

Liang, Yuting; Van Nostrand, Joy D.; N′Guessan, Lucie A.; Peacock, Aaron D.; Deng, Ye; Long, Philip E.; Resch, C. Tom; Wu, Liyou; He, Zhili; Li, Guanghe; Hazen, Terry C.; Lovley, Derek R.

2012-01-01

To better understand the microbial functional diversity changes with subsurface redox conditions during in situ uranium bioremediation, key functional genes were studied with GeoChip, a comprehensive functional gene microarray, in field experiments at a uranium mill tailings remedial action (UMTRA) site (Rifle, CO). The results indicated that functional microbial communities altered with a shift in the dominant metabolic process, as documented by hierarchical cluster and ordination analyses of all detected functional genes. The abundance of dsrAB genes (dissimilatory sulfite reductase genes) and methane generation-related mcr genes (methyl coenzyme M reductase coding genes) increased when redox conditions shifted from Fe-reducing to sulfate-reducing conditions. The cytochrome genes detected were primarily from Geobacter sp. and decreased with lower subsurface redox conditions. Statistical analysis of environmental parameters and functional genes indicated that acetate, U(VI), and redox potential (Eh) were the most significant geochemical variables linked to microbial functional gene structures, and changes in microbial functional diversity were strongly related to the dominant terminal electron-accepting process following acetate addition. The study indicates that the microbial functional genes clearly reflect the in situ redox conditions and the dominant microbial processes, which in turn influence uranium bioreduction. Microbial functional genes thus could be very useful for tracking microbial community structure and dynamics during bioremediation. PMID:22327592

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

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

He, Zhili; Zhang, Ping; Wu, Linwei

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

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning

DOE PAGES

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

2018-02-20

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

Spatial Distribution of an Uranium-Respiring Betaproteobacterium at the Rifle, CO Field Research Site

PubMed Central

Koribanics, Nicole M.; Tuorto, Steven J.; Lopez-Chiaffarelli, Nora; McGuinness, Lora R.; Häggblom, Max M.; Williams, Kenneth H.; Long, Philip E.; Kerkhof, Lee J.

2015-01-01

The Department of Energy’s Integrated Field-Scale Subsurface Research Challenge Site (IFRC) at Rifle, Colorado was created to address the gaps in knowledge on the mechanisms and rates of U(VI) bioreduction in alluvial sediments. Previous studies at the Rifle IFRC have linked microbial processes to uranium immobilization during acetate amendment. Several key bacteria believed to be involved in radionuclide containment have been described; however, most of the evidence implicating uranium reduction with specific microbiota has been indirect. Here, we report on the cultivation of a microorganism from the Rifle IFRC that reduces uranium and appears to utilize it as a terminal electron acceptor for respiration with acetate as electron donor. Furthermore, this bacterium constitutes a significant proportion of the subsurface sediment community prior to biostimulation based on TRFLP profiling of 16S rRNA genes. 16S rRNA gene sequence analysis indicates that the microorganism is a betaproteobacterium with a high similarity to Burkholderia fungorum. This is, to our knowledge, the first report of a betaproteobacterium capable of uranium respiration. Our results indicate that this microorganism occurs commonly in alluvial sediments located between 3-6 m below ground surface at Rifle and may play a role in the initial reduction of uranium at the site. PMID:25874721

Spatial distribution of an uranium-respiring betaproteobacterium at the Rifle, CO field research site

DOE PAGES

Koribanics, Nicole M.; Tuorto, Steven J.; Lopez-Chiaffarelli, Nora; ...

2015-04-13

The Department of Energy’s Integrated Field-Scale Subsurface Research Challenge Site (IFRC) at Rifle, Colorado was created to address the gaps in knowledge on the mechanisms and rates of U(VI) bioreduction in alluvial sediments. Previous studies at the Rifle IFRC have linked microbial processes to uranium immobilization during acetate amendment. Several key bacteria believed to be involved in radionuclide containment have been described; however, most of the evidence implicating uranium reduction with specific microbiota has been indirect. Here, we report on the cultivation of a microorganism from the Rifle IFRC that reduces uranium and appears to utilize it as a terminalmore » electron acceptor for respiration with acetate as electron donor. Furthermore, this bacterium constitutes a significant proportion of the subsurface sediment community prior to biostimulation based on TRFLP profiling of 16S rRNA genes. 16S rRNA gene sequence analysis indicates that the microorganism is a betaproteobacterium with a high similarity to Burkholderia fungorum. This is, to our knowledge, the first report of a betaproteobacterium capable of uranium respiration. Our results indicate that this microorganism occurs commonly in alluvial sediments located between 3-6 m below ground surface at Rifle and may play a role in the initial reduction of uranium at the site.« less

Bioremediation of uranium contamination with enzymatic uranium reduction

USGS Publications Warehouse

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

1992-01-01

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

The genome of Geobacter bemidjiensis, exemplar for the subsurface clade of Geobacter species that predominate in Fe(III)-reducing subsurface environments

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

Aklujkar, Muktak; Young, Nelson D; Holmes, Dawn

2010-01-01

Background. Geobacter species in a phylogenetic cluster known as subsurface clade 1 are often the predominant microorganisms in subsurface environments in which Fe(III) reduction is the primary electron-accepting process. Geobacter bemidjiensis, a member of this clade, was isolated from hydrocarbon-contaminated subsurface sediments in Bemidji, Minnesota, and is closely related to Geobacter species found to be abundant at other subsurface sites. This study examines whether there are significant differences in the metabolism and physiology of G. bemidjiensis compared to non-subsurface Geobacter species. Results. Annotation of the genome sequence of G. bemidjiensis indicates several differences in metabolism compared to previously sequenced non-subsurfacemore » Geobacteraceae, which will be useful for in silico metabolic modeling of subsurface bioremediation processes involving Geobacter species. Pathways can now be predicted for the use of various carbon sources such as propionate by G. bemidjiensis. Additional metabolic capabilities such as carbon dioxide fixation and growth on glucose were predicted from the genome annotation. The presence of different dicarboxylic acid transporters and two oxaloacetate decarboxylases in G. bemidjiensis may explain its ability to grow by disproportionation of fumarate. Although benzoate is the only aromatic compound that G. bemidjiensis is known or predicted to utilize as an electron donor and carbon source, the genome suggests that this species may be able to detoxify other aromatic pollutants without degrading them. Furthermore, G. bemidjiensis is auxotrophic for 4-aminobenzoate, which makes it the first Geobacter species identified as having a vitamin requirement. Several features of the genome indicated that G. bemidjiensis has enhanced abilities to respire, detoxify and avoid oxygen. Conclusion. Overall, the genome sequence of G. bemidjiensis offers surprising insights into the metabolism and physiology of Geobacteraceae in subsurface environments, compared to non-subsurface Geobacter species, such as the ability to disproportionate fumarate, more efficient oxidation of propionate, enhanced responses to oxygen stress, and dependence on the environment for a vitamin requirement. Therefore, an understanding of the activity of Geobacter species in the subsurface is more likely to benefit from studies of subsurface isolates such as G. bemidjiensis than from the non-subsurface model species studied so far.« less

Analysis of Tank 13H (HTF-13-14-156, 157) Surface and Subsurface Supernatant Samples in Support of Enrichment Control, Corrosion Control and Sodium Aluminosilicate Formation Potential Programs

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

Oji, L. N.

2015-02-18

The 2H Evaporator system includes mainly Tank 43H (feed tank) and Tank 38H (drop tank) with Tank 22H acting as the DWPF recycle receipt tank. The Tank 13H is being characterized to ensure that it can be transferred to the 2H evaporator. This report provides the results of analyses on Tanks 13H surface and subsurface supernatant liquid samples to ensure compliance with the Enrichment Control Program (ECP), the Corrosion Control Program and Sodium Aluminosilicate Formation Potential in the Evaporator. The U-235 mass divided by the total uranium averaged 0.00799 (0.799 % uranium enrichment) for both the surface and subsurface Tankmore » 13H samples. This enrichment is slightly above the enrichment for Tanks 38H and 43H, where the enrichment normally ranges from 0.59 to 0.7 wt%. The U-235 concentration in Tank 13H samples ranged from 2.01E-02 to 2.63E-02 mg/L, while the U-238 concentration in Tank 13H ranged from 2.47E+00 to 3.21E+00 mg/L. Thus, the U-235/total uranium ratio is in line with the prior 2H-evaporator ECP samples. Measured sodium and silicon concentrations averaged, respectively, 2.46 M and 1.42E-04 M (3.98 mg/L) in the Tank 13H subsurface sample. The measured aluminum concentration in Tanks 13H subsurface samples averaged 2.01E-01 M.« less

MODELING MICROBIAL TRANSPORT IN SOIL AND GROUNDWATER: MICROBIOLOGISTS CAN ASSIST IN THE DEVELOPMENT OF MODELS OF CONTAMINANT TRANSPORT

EPA Science Inventory

A large body of literature describes the processes affecting the fate of microorganisms in the subsurface environment (i.e., soil and groundwater). The fate of microorganisms depends on two main components: survival and transport. other components must be considered when determin...

An explanation for differences in the process of colloid adsorption in batch and column studies

USDA-ARS?s Scientific Manuscript database

It is essential to understand the mechanisms that control virus and bacteria removal in the subsurface environment to assess the risk of groundwater contamination with fecal microorganisms. This study was conducted to explicitly provide a critical and systematic comparison between batch and column e...

GROUNDWATER RECHARGE AND CHEMICAL CONTAMINANTS: CHALLENGES IN COMMUNICATING THE CONNECTIONS AND COLLISIONS OF TWO DISPARATE WORLDS

EPA Science Inventory

The existing knowledge base regarding the presence and significance of chemicals foreign to the subsurface environment is large and growing -the papers in this volume serving as recent testament. But complex questions with few answers surround the unknowns regarding the potenti...

Process for guidance, containment, treatment, and imaging in a subsurface environment utilizing ferro-fluids

DOEpatents

Moridis, George J.; Oldenburg, Curtis M.

2001-01-01

Disclosed are processes for monitoring and control of underground contamination, which involve the application of ferrofluids. Two broad uses of ferrofluids are described: (1) to control liquid movement by the application of strong external magnetic fields; and (2) to image liquids by standard geophysical methods.

Depleted uranium instead of lead in munitions: the lesser evil.

PubMed

Jargin, Sergei V

2014-03-01

Uranium has many similarities to lead in its exposure mechanisms, metabolism and target organs. However, lead is more toxic, which is reflected in the threshold limit values. The main potential hazard associated with depleted uranium is inhalation of the aerosols created when a projectile hits an armoured target. A person can be exposed to lead in similar ways. Accidental dangerous exposures can result from contact with both substances. Encountering uranium fragments is of minor significance because of the low penetration depth of alpha particles emitted by uranium: they are unable to penetrate even the superficial keratin layer of human skin. An additional cancer risk attributable to the uranium exposure might be significant only in case of prolonged contact of the contaminant with susceptible tissues. Lead intoxication can be observed in the wounded, in workers manufacturing munitions etc; moreover, lead has been documented to have a negative impact on the intellectual function of children at very low blood concentrations. It is concluded on the basis of the literature overview that replacement of lead by depleted uranium in munitions would be environmentally beneficial or largely insignificant because both lead and uranium are present in the environment.

Microbial Functional Gene Diversity Predicts Groundwater Contamination and Ecosystem Functioning.

PubMed

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

2018-02-20

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

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

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

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

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

PubMed

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

2006-10-29

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

Compatibility of Surfactants and Thermally Activated Persulfate for Enhanced Subsurface Remediation.

PubMed

Wang, Li; Peng, Libin; Xie, Liling; Deng, Peiyan; Deng, Dayi

2017-06-20

Limited aqueous availability of hydrophobic organic contaminants and nonaqueous phase liquids in subsurface environment may seriously impair the effectiveness of traditional in situ chemical oxidation (ISCO). To tackle the issue, a combination of surfactants and thermally activated persulfate was proposed to enhance the aqueous availability and consequent oxidation of organic contaminants. The compatibility of eight representative nonionic, monovalent anionic, and divalent anionic surfactants with persulfate at various temperatures was first studied, to identify suitable surfactants that have high aqueous stability and low oxidant demands to couple with thermally activated persulfate. C 12 -MADS (sodium dodecyl diphenyl ether disulfonate, a representative divalent anionic surfactant) stands out as the most compatible surfactant. Batch treatability study with coal tar, an example of challenging scenarios for traditional ISCO, was then conducted. The results show that C 12 -MADS can significantly enhance not only the oxidation of polyaromatic hydrocarbons contained in coal tar but also oxidant utilization efficiency, indicating the potential of the proposed coupling process for the treatment of organic contaminants with low aqueous availability.

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

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

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

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

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

DOE PAGES

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

2017-01-09

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

Analytical solutions to dissolved contaminant plume evolution with source depletion during carbon dioxide storage.

PubMed

Yang, Yong; Liu, Yongzhong; Yu, Bo; Ding, Tian

2016-06-01

Volatile contaminants may migrate with carbon dioxide (CO2) injection or leakage in subsurface formations, which leads to the risk of the CO2 storage and the ecological environment. This study aims to develop an analytical model that could predict the contaminant migration process induced by CO2 storage. The analytical model with two moving boundaries is obtained through the simplification of the fully coupled model for the CO2-aqueous phase -stagnant phase displacement system. The analytical solutions are confirmed and assessed through the comparison with the numerical simulations of the fully coupled model. Then, some key variables in the analytical solutions, including the critical time, the locations of the dual moving boundaries and the advance velocity, are discussed to present the characteristics of contaminant migration in the multi-phase displacement system. The results show that these key variables are determined by four dimensionless numbers, Pe, RD, Sh and RF, which represent the effects of the convection, the dispersion, the interphase mass transfer and the retention factor of contaminant, respectively. The proposed analytical solutions could be used for tracking the migration of the injected CO2 and the contaminants in subsurface formations, and also provide an analytical tool for other solute transport in multi-phase displacement system. Copyright © 2016 Elsevier B.V. All rights reserved.

GEOCHEMISTRY OF SUBSURFACE REACTIVE BARRIERS FOR REMEDIATION OF CONTAMINATED GROUND WATER

EPA Science Inventory

Reactive barriers that couple subsurface fluid flow with a passive chemical treatment zone are emerging, cost effective approaches for in-situ remediation of contaminated groundwater. Factors such as the build-up of surface precipitates, bio-fouling, and changes in subsurface tr...

Tree Sampling as a Method to Assess Vapor Intrusion Potential at a Site Characterized by VOC-Contaminated Groundwater and Soil.

PubMed

Wilson, Jordan L; Limmer, Matthew A; Samaranayake, V A; Schumacher, John G; Burken, Joel G

2017-09-19

Vapor intrusion (VI) by volatile organic compounds (VOCs) in the built environment presents a threat to human health. Traditional VI assessments are often time-, cost-, and labor-intensive; whereas traditional subsurface methods sample a relatively small volume in the subsurface and are difficult to collect within and near structures. Trees could provide a similar subsurface sample where roots act as the "sampler' and are already onsite. Regression models were developed to assess the relation between PCE concentrations in over 500 tree-core samples with PCE concentrations in over 50 groundwater and 1000 soil samples collected from a tetrachloroethylene- (PCE-) contaminated Superfund site and analyzed using gas chromatography. Results indicate that in planta concentrations are significantly and positively related to PCE concentrations in groundwater samples collected at depths less than 20 m (adjusted R 2 values greater than 0.80) and in soil samples (adjusted R 2 values greater than 0.90). Results indicate that a 30 cm diameter tree characterizes soil concentrations at depths less than 6 m over an area of 700-1600 m 2 , the volume of a typical basement. These findings indicate that tree sampling may be an appropriate method to detect contamination at shallow depths at sites with VI.

Tree sampling as a method to assess vapor intrusion potential at a site characterized by VOC-contaminated groundwater and soil

USGS Publications Warehouse

Wilson, Jordan L.; Limmer, Matthew A.; Samaranayake, V. A.; Schumacher, John G.; Burken, Joel G.

2017-01-01

Vapor intrusion (VI) by volatile organic compounds (VOCs) in the built environment presents a threat to human health. Traditional VI assessments are often time-, cost-, and labor-intensive; whereas traditional subsurface methods sample a relatively small volume in the subsurface and are difficult to collect within and near structures. Trees could provide a similar subsurface sample where roots act as the “sampler’ and are already onsite. Regression models were developed to assess the relation between PCE concentrations in over 500 tree-core samples with PCE concentrations in over 50 groundwater and 1000 soil samples collected from a tetrachloroethylene- (PCE-) contaminated Superfund site and analyzed using gas chromatography. Results indicate that in planta concentrations are significantly and positively related to PCE concentrations in groundwater samples collected at depths less than 20 m (adjusted R2 values greater than 0.80) and in soil samples (adjusted R2 values greater than 0.90). Results indicate that a 30 cm diameter tree characterizes soil concentrations at depths less than 6 m over an area of 700–1600 m2, the volume of a typical basement. These findings indicate that tree sampling may be an appropriate method to detect contamination at shallow depths at sites with VI.

Immobilization of uranium in contaminated soil by natural apatite addition

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

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

2007-07-01

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

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

PubMed

Mkandawire, Martin

2013-11-01

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

Microbial reduction of uranium

USGS Publications Warehouse

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

1991-01-01

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

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

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

Not Available

1995-02-01

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

Laser removal of loose uranium compound contamination from metal surfaces

NASA Astrophysics Data System (ADS)

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

2007-04-01

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

THE ONSITE ON-LINE CALCULATORS AND TRAINING FOR SUBSURFACE CONTAMINANT TRANSPORT SITE ASSESSMENT

EPA Science Inventory

EPA has developed a suite of on-line calculators called "OnSite" for assessing transport of environmental contaminants in the subsurface. The purpose of these calculators is to provide methods and data for common calculations used in assessing impacts from subsurface contaminatio...

DEVELOPMENT OF A DATA EVALUATION/DECISION SUPPORT SYSTEM FOR REMEDIATION OF SUBSURFACE CONTAMINATION

EPA Science Inventory

Subsurface contamination frequently originates from spatially distributed sources of multi-component nonaqueous phase liquids (NAPLs). Such chemicals are typically persistent sources of ground-water contamination that are difficult to characterize. This work addresses the feasi...

Application of model abstraction techniques to simulate transport in soils

USDA-ARS?s Scientific Manuscript database

Successful understanding and modeling of contaminant transport in soils is the precondition of risk-informed predictions of the subsurface contaminant transport. Exceedingly complex models of subsurface contaminant transport are often inefficient. Model abstraction is the methodology for reducing th...

The effect of bicarbonate on the microbial dissolution of autunite mineral in the presence of gram-positive bacteria.

PubMed

Sepulveda-Medina, Paola M; Katsenovich, Yelena P; Wellman, Dawn M; Lagos, Leonel E

2015-06-01

Bacteria are key players in the processes that govern fate and transport of contaminants. The uranium release from Na and Ca-autunite by Arthrobacter oxydans strain G968 was evaluated in the presence of bicarbonate ions. This bacterium was previously isolated from Hanford Site soil and in earlier prescreening tests demonstrated low tolerance to U(VI) toxicity compared to other A. oxydans isolates. Experiments were conducted using glass serum bottles as mixed bioreactors and sterile 6-well cell culture plates with inserts separating bacteria cells from mineral solids. Reactors containing phosphorus-limiting media were amended with bicarbonate ranging between 0 and 10 mM and meta-autunite solids to provide a U(VI) concentration of 4.4 mmol/L. Results showed that in the presence of bicarbonate, A. oxydans G968 was able to enhance the release of U(VI) from Na and Ca autunite at the same capacity as other A. oxydans isolates with relatively high tolerance to U(VI). The effect of bacterial strains on autunite dissolution decreases as the concentration of bicarbonate increases. The results illustrate that direct interaction between the bacteria and the mineral is not necessary to result in U(VI) biorelease from autunite. The formation of secondary calcium-phosphate mineral phases on the surface of the mineral during the dissolution can ultimately reduce the natural autunite mineral contact area, which bacterial cells can access. This thereby reduces the concentration of uranium released into the solution. This study provides a better understanding of the interactions between meta-autunite and microbes in conditions mimicking arid and semiarid subsurface environments of western U.S. Copyright © 2015 Elsevier Ltd. All rights reserved.

The Effect of Bicarbonate on the Microbial Dissolution of Autunite Mineral in the Presence of Gram-Positive Bacteria

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

Sepulveda-Medina, Paola; Katsenovich, Yelena; Wellman, Dawn M.

Bacteria are key players in the processes that govern fate and transport of contaminants. The uranium release from Na and Ca-autunite by Arthrobacter oxydans strain G968 was evaluated in the presence of bicarbonate ions. This bacterium was previously isolated from Hanford Site soil and in earlier prescreening tests demonstrated low tolerance to U(VI) toxicity compared to other A.oxydans isolates. Experiments were conducted using glass serum bottles as mixed bioreactors and sterile 6-well cell culture plates with inserts separating bacteria cells from mineral solids. Reactors containing phosphorus-limiting media were amended with bicarbonate ranging between 0-10 mM and metaautunite solids to providemore » a U(VI) concentration of 4.4 mmol/L. Results showed that in the presence of bicarbonate, A.oxydans G968 was able to enhance the release of U(VI) from Na and Ca autunite at the same capacity as other A.oxydans isolates with relatively high tolerance to U(VI). The effect of bacterial strains on autunite dissolution decreases as the concentration of bicarbonate increases. The results illustrate that direct interaction between the bacteria and the mineral is not necessary to result in U (VI) biorelease from autunite. The formation of secondary calcium-phosphate mineral phases on the surface of the mineral during the dissolution can ultimately reduce the natural autunite mineral contact area, which bacterial cells can access. This thereby reduces the concentration of uranium released into the solution. This study provides a better understanding of the interactions between meta-autunite and microbes in conditions mimicking arid and semiarid subsurface environments of western U.S.« less

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

Mouser, Paula J.; N'Guessan, A. Lucie; Qafoku, Nikolla

The capacity for subsurface sediments to sequester metal contaminants, such as uranium (U), and retain them after bioremediation efforts are completed is critical to site stewardship. Sediments enriched in natural organic matter are capable of sequestering significant quantities of U, but may also serve as sources to the aquifer, contributing to plume persistence. Two types of sediments were compared to better understand the mechanisms contributing to the sequestration and release of U in the presence of organic matter. Artificially bioreduced sediments were retrieved from a field experimental plot previously stimulated with acetate while naturally bioreduced sediments were collected from amore » location enriched in organic matter but never subject to acetate amendment. Batch incubations demonstrated that the artificially bioreduced sediments were primed to rapidly remove uranium from the groundwater whereas naturally bioreduced sediments initially released a sizeable portion of sediment U before U(VI)-removal commenced. Column experiments confirmed that U release persisted for 65 pore volumes in naturally bioreduced sediments, demonstrating the sink-source behavior of this sediment. Acetate addition to artificially bioreduced sediments shifted the microbial community from one dominated by sulfate-reducing bacteria within Desulfobacteraceae to the iron-reducing family Geobacteraceae and Firmicutes during U(VI) reduction. In contrast, initial Geobacteraceae communities innaturally reduced sediments were replaced by clone sequences with similarity to opportunistic Pseudomonas spp. during U release, while U(VI) removal occurred concurrent with enrichment of Firmicutes. These investigations stress the importance of characterizing zones with heterogeneous carbon pools at U contaminated sites prior to the determination of a remedial strategy.« less

Diversity, metal resistance and uranium sequestration abilities of bacteria from uranium ore deposit in deep earth stratum.

PubMed

Islam, Ekramul; Sar, Pinaki

2016-05-01

Metal resistance and uranium (U) sequestration abilities of bacteria residing in subsurface U ore was investigated using 122 pure culture strains isolated through enrichment. The cumulative frequencies of isolates resistant to each metal tested were as follows: As(V), 74%; Zn, 58%; Ni, 53%; Cd, 47%; Cr(VI), 41%; Co, 40%; Cu, 20%; and Hg, 4%. 16S rRNA gene analysis revealed that isolated bacteria belonged to 14 genera with abundance of Arthrobacter, Microbacterium, Acinetobacter and Stenotrophomonas. Cobalt did not interfere with the growth of most of the bacterial isolates belonging to different groups while U allowed growth of four different genera of which Stenotrophomonas and Microbacterium showed high U tolerance. Interestingly, tolerance to Ni, Zn, Cu, and Hg was observed only in Microbacterium, Arthrobacter, Paenibacillus¸ and Acinetobacter, respectively. However, Microbacterium was found to be dominant when isolated from other five different metal enrichments including U. Uranium removal study showed that 84% of the test bacteria could remove more than 50mgUg(-1) dry weight from 80 or 160mgL(-1) U within 48h. In general, Microbacterium, Arthrobacter and Acinetobacter could remove a higher amount of U. High resolution transmission electron microscopy (HRTEM) study of U exposed cells revealed that accumulated U sequestered mostly around the cell periphery. The study highlights that indigenous U ore deposit bacteria have the potential to interact with U, and thus could be applied for bioremediation of U contaminated sites or wastes. Copyright © 2016 Elsevier Inc. All rights reserved.

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

76 FR 14660 - Public Comment on the Development of Final Guidance for Evaluating the Vapor Intrusion to Indoor...

Federal Register 2010, 2011, 2012, 2013, 2014

2011-03-17

... Groundwater and Soils (Subsurface Vapor Intrusion Guidance) AGENCY: Environmental Protection Agency (EPA... Pathway from Contaminated Groundwater and Soil (Subsurface Vapor Intrusion Guidance). A draft of the... Evaluating Vapor Intrusion to Indoor Air Pathway from Contaminated Groundwater and Soil (Subsurface Vapor...

AN EXPERIMENTAL ASSESSMENT OF THE IMPACTS OF PARTIAL DNAPL SOURCE ZONE DELETION USING SPARGING AS A REMEDIATION TECHNIQUE

EPA Science Inventory

The contamination of the subsurface environment by dense non-aqueous phase liquids (DNAPL) is a wide-spread problem that poses a significant threat to soil and groundwater quality. Implementing different remediation techniques can lead to the removal of a high fraction of the DNA...

Contamination assessment in microbiological sampling of the Eyreville core, Chesapeake Bay impact structure

USGS Publications Warehouse

Gronstal, A.L.; Voytek, M.A.; Kirshtein, J.D.; Von der, Heyde; Lowit, M.D.; Cockell, C.S.

2009-01-01

Knowledge of the deep subsurface biosphere is limited due to difficulties in recovering materials. Deep drilling projects provide access to the subsurface; however, contamination introduced during drilling poses a major obstacle in obtaining clean samples. To monitor contamination during the 2005 International Continental Scientific Drilling Program (ICDP)-U.S. Geological Survey (USGS) deep drilling of the Chesapeake Bay impact structure, four methods were utilized. Fluorescent microspheres were used to mimic the ability of contaminant cells to enter samples through fractures in the core material during retrieval. Drilling mud was infused with a chemical tracer (Halon 1211) in order to monitor penetration of mud into cores. Pore water from samples was examined using excitation-emission matrix (EEM) fl uorescence spectroscopy to characterize dissolved organic carbon (DOC) present at various depths. DOC signatures at depth were compared to signatures from drilling mud in order to identify potential contamination. Finally, microbial contaminants present in drilling mud were identified through 16S ribosomal deoxyribonucleic acid (rDNA) clone libraries and compared to species cultured from core samples. Together, these methods allowed us to categorize the recovered core samples according to the likelihood of contamination. Twenty-two of the 47 subcores that were retrieved were free of contamination by all the methods used and were subsequently used for microbiological culture and culture-independent analysis. Our approach provides a comprehensive assessment of both particulate and dissolved contaminants that could be applied to any environment with low biomass. ?? 2009 The Geological Society of America.

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

PubMed

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

2017-04-01

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

Geological and geochemical investigations of uranium occurrences in the Arrastre Lake area of the Medicine Bow Mountains, Wyoming

USGS Publications Warehouse

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.

Plutonium Decontamination of Uranium using CO2 Cleaning

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

Blau, M

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

Methanogenic degradation of petroleum hydrocarbons in subsurface environments remediation, heavy oil formation, and energy recovery.

PubMed

Gray, N D; Sherry, A; Hubert, C; Dolfing, J; Head, I M

2010-01-01

Hydrocarbons are common constituents of surface, shallow, and deep-subsurface environments. Under anaerobic conditions, hydrocarbons can be degraded to methane by methanogenic microbial consortia. This degradation process is widespread in the geosphere. In comparison with other anaerobic processes, methanogenic hydrocarbon degradation is more sustainable over geological time scales because replenishment of an exogenous electron acceptor is not required. As a consequence, this process has been responsible for the formation of the world's vast deposits of heavy oil, which far exceed conventional oil assets such as those found in the Middle East. Methanogenic degradation is also a potentially important component of attenuation in hydrocarbon contamination plumes. Studies of the organisms, syntrophic partnerships, mechanisms, and geochemical signatures associated with methanogenic hydrocarbon degradation have identified common themes and diagnostic markers for this process in the subsurface. These studies have also identified the potential to engineer methanogenic processes to enhance the recovery of energy assets as biogenic methane from residual oils stranded in petroleum systems. Copyright 2010 Elsevier Inc. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

Design and Practices for Use of Automated Drilling and Sample Handling in MARTE While Minimizing Terrestrial and Cross Contamination

NASA Astrophysics Data System (ADS)

Miller, David P.; Bonaccorsi, Rosalba; Davis, Kiel

2008-10-01

Mars Astrobiology Research and Technology Experiment (MARTE) investigators used an automated drill and sample processing hardware to detect and categorize life-forms found in subsurface rock at Río Tinto, Spain. For the science to be successful, it was necessary for the biomass from other sources -- whether from previously processed samples (cross contamination) or the terrestrial environment (forward contamination) -- to be insignificant. The hardware and practices used in MARTE were designed around this problem. Here, we describe some of the design issues that were faced and classify them into problems that are unique to terrestrial tests versus problems that would also exist for a system that was flown to Mars. Assessment of the biomass at various stages in the sample handling process revealed mixed results; the instrument design seemed to minimize cross contamination, but contamination from the surrounding environment sometimes made its way onto the surface of samples. Techniques used during the MARTE Río Tinto project, such as facing the sample, appear to remove this environmental contamination without introducing significant cross contamination from previous samples.

Design and practices for use of automated drilling and sample handling in MARTE while minimizing terrestrial and cross contamination.

PubMed

Miller, David P; Bonaccorsi, Rosalba; Davis, Kiel

2008-10-01

Mars Astrobiology Research and Technology Experiment (MARTE) investigators used an automated drill and sample processing hardware to detect and categorize life-forms found in subsurface rock at Río Tinto, Spain. For the science to be successful, it was necessary for the biomass from other sources--whether from previously processed samples (cross contamination) or the terrestrial environment (forward contamination)-to be insignificant. The hardware and practices used in MARTE were designed around this problem. Here, we describe some of the design issues that were faced and classify them into problems that are unique to terrestrial tests versus problems that would also exist for a system that was flown to Mars. Assessment of the biomass at various stages in the sample handling process revealed mixed results; the instrument design seemed to minimize cross contamination, but contamination from the surrounding environment sometimes made its way onto the surface of samples. Techniques used during the MARTE Río Tinto project, such as facing the sample, appear to remove this environmental contamination without introducing significant cross contamination from previous samples.

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.

Intrinsic Anaerobic Bioremediation of Hydrocarbons in Contaminated Subsurface Plumes and Marine Sediments

NASA Astrophysics Data System (ADS)

Nanny, M. A.; Nanny, M. A.; Suflita, J. M.; Suflita, J. M.; Davidova, I.; Kropp, K.; Caldwell, M.; Philp, R.; Gieg, L.; Rios-Hernandez, L. A.

2001-05-01

In recent years, several classes of petroleum hydrocarbons contaminating subsurface and marine environments have been found susceptible to anaerobic biodegradation using novel mechanisms entirely distinct from aerobic metabolic pathways. For example, the anaerobic decay of toluene can be initiated by the addition of the aryl methyl group to the double bond of fumarate, resulting in a benzylsuccinic acid metabolite. Our work has shown that an analogous mechanism also occurs with ethylbenzene and the xylene isomers, yielding 3-phenyl-1,2-butane dicarboxylic acid and methylbenzylsuccinic acid, respectively. Moreover, these metabolites have been detected in contaminated environments. Most recently, we have identified metabolites resulting from the initial attack of H26- or D26-n-dodecane during degradation by a sulfate-reducing bacterial culture. Using GC-MS, these metabolites were identified as fatty acids that result from C-H or C-D addition across the double bond of fumarate to give dodecylsuccinic acids in which all 26 protons or deuteriums of the parent alkane were retained. Further, when this enrichment culture was challenged with hexane or decane, hexylsuccinic acid or decylsuccinic acid were identified as resulting metabolites. Similarly, the study of an ethylcyclopentane-degrading sulfate-reducing enrichment produced a metabolite, which is consistent with the addition of fumarate to the parent substrate. These novel anaerobic addition products are characterized by similar, distinctive mass spectral (MS) features (ions specific to the succinic acid portion of the molecule) that can potentially be used to probe contaminated environments for evidence of intrinsic remediation of hydrocarbons. Indeed, analyses of water extracts from two gas condensate-contaminated sites resulted in the tentative detection of alkyl- and cycloalkylsuccinic acids ranging from C3 to C9, including ethylcyclopentyl-succinic acid. In water extracts collected from an area underlying a petroleum production plant, MS profiles consistent with the addition products of methylcycloalkenes were observed. This work helps attests to: 1) the extrapolatability of laboratory results to the field, 2) the unifying metabolic features for the anaerobic destruction of diverse types of hydrocarbons, and 3) how this information can be used to assess the intrinsic bioremediation processes in petroleum-contaminated environments.

INEEL Subregional Conceptual Model Report Volume 3: Summary of Existing Knowledge of Natural and Anthropogenic Influences on the Release of Contaminants to the Subsurface Environment from Waste Source Terms at the INEEL

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

Paul L. Wichlacz

2003-09-01

This source-term summary document is intended to describe the current understanding of contaminant source terms and the conceptual model for potential source-term release to the environment at the Idaho National Engineering and Environmental Laboratory (INEEL), as presented in published INEEL reports. The document presents a generalized conceptual model of the sources of contamination and describes the general categories of source terms, primary waste forms, and factors that affect the release of contaminants from the waste form into the vadose zone and Snake River Plain Aquifer. Where the information has previously been published and is readily available, summaries of the inventorymore » of contaminants are also included. Uncertainties that affect the estimation of the source term release are also discussed where they have been identified by the Source Term Technical Advisory Group. Areas in which additional information are needed (i.e., research needs) are also identified.« less

Methods for microbial filtration of fluids

DOEpatents

Carman, Margaret L.; Jackson, Kenneth J.; Knapp, Richard B.; Knezovich, John P.; Shah, Nilesh N.; Taylor, Robert T.

1996-01-01

Novel methods for purifying contaminated subsurface groundwater are disclosed. The method is involves contacting the contaminated subsurface groundwater with methanotrophic or heterotrophic microorganisms which produce contaminant-degrading enzymes. The microorganisms are derived from surface cultures and are injected into the ground so as to act as a biofilter. The contaminants which may be treated include organic or metallic materials and radionuclides.

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

PubMed

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

2010-11-01

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

Biosorption and biomineralization of uranium(VI) by Saccharomyces cerevisiae-Crystal formation of chernikovite.

PubMed

Zheng, Xin-Yan; Wang, Xiao-Yu; Shen, Yang-Hao; Lu, Xia; Wang, Tie-Shan

2017-05-01

Biosorption of heavy metal elements including radionuclides by microorganisms is a promising and effective method for the remediation of the contaminated places. The responses of live Saccharomyces cerevisiae in the toxic uranium solutions during the biosorption process and the mechanism of uranium biomineralization by cells were investigated in the present study. A novel experimental phenomenon that uranium concentrations have negative correlation with pH values and positive correlation with phosphate concentrations in the supernatant was observed, indicating that hydrogen ions, phosphate ions and uranyl ions were involved in the chernikovite precipitation actively. During the biosorption process, live cells desorb deposited uranium within the equilibrium state of biosorption system was reached and the phosphorus concentration increased gradually in the supernatant. These metabolic detoxification behaviours could significantly alleviate uranium toxicity and protect the survival of the cells better in the environment. The results of microscopic and spectroscopic analysis demonstrated that the precipitate on the cell surface was a type of uranium-phosphate compound in the form of a scale-like substance, and S. cerevisiae could transform the uranium precipitate into crystalline state-tetragonal chernikovite [H 2 (UO 2 ) 2 (PO 4 ) 2 ·8H 2 O]. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

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

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

2017-01-09

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

Leachate plume delineation and lithologic profiling using surface resistivity in an open municipal solid waste dumpsite, Sri Lanka.

PubMed

Wijesekara, Hasintha Rangana; De Silva, Sunethra Nalin; Wijesundara, Dharani Thanuja De Silva; Basnayake, Bendict Francis Antony; Vithanage, Meththika Suharshini

2015-01-01

This study presents the use of direct current resistivity techniques (DCRT) for investigation and characterization of leachate-contaminated subsurface environment of an open solid waste dumpsite at Kandy, Sri Lanka. The particular dumpsite has no liner and hence the leachate flows directly to the nearby river via subsurface and surface channels. For the identification of possible subsurface flow paths and the direction of the leachate, DCRT (two-dimensional, three-dimensional and vertical electrical sounding) have been applied. In addition, the physico-chemical parameters such as pH, electrical conductivity (EC), alkalinity, hardness, chloride, chemical oxygen demand (COD) and total organic carbon (TOC) of leachate collected from different points of the solid waste dumping area and leachate drainage channel were analysed. Resistivity data confirmed that the leachate flow is confined to the near surface and no separate plume is observed in the downstream area, which may be due to the contamination distribution in the shallow overburden thickness. The stratigraphy with leachate pockets and leachate plume movements was well demarcated inside the dumpsite via low resistivity zones (1-3 Ωm). The recorded EC, alkalinity, hardness and chloride contents in leachate were averaged as 14.13 mS cm⁻¹, 3236, 2241 and 320 mg L⁻¹, respectively, which confirmed the possible causes for low resistivity values. This study confirms that DCRT can be effectively utilized to assess the subsurface characteristics of the open dumpsites to decide on corridor placement and depth of permeable reactive barriers to reduce the groundwater contamination.

Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms.

PubMed

Stylo, Malgorzata; Neubert, Nadja; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan

2015-09-01

The prevalent formation of noncrystalline U(IV) species in the subsurface and their enhanced susceptibility to reoxidation and remobilization, as compared to crystalline uraninite, raise concerns about the long-term sustainability of the bioremediation of U-contaminated sites. The main goal of this study was to resolve the remaining uncertainty concerning the formation mechanism of noncrystalline U(IV) in the environment. Controlled laboratory biofilm systems (biotic, abiotic, and mixed biotic-abiotic) were probed using a combination of U isotope fractionation and X-ray absorption spectroscopy (XAS). Regardless of the mechanism of U reduction, the presence of a biofilm resulted in the formation of noncrystalline U(IV). Our results also show that biotic U reduction is the most effective way to immobilize and reduce U. However, the mixed biotic-abiotic system resembled more closely an abiotic system: (i) the U(IV) solid phase lacked a typically biotic isotope signature and (ii) elemental sulfur was detected, which indicates the oxidation of sulfide coupled to U(VI) reduction. The predominance of abiotic U reduction in our systems is due to the lack of available aqueous U(VI) species for direct enzymatic reduction. In contrast, in cases where bicarbonate is present at a higher concentration, aqueous U(VI) species dominate, allowing biotic U reduction to outcompete the abiotic processes.

Mechanisms for Electron Transfer Through Pili to Fe(III) Oxide in Geobacter

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

Lovley, Derek R.

The purpose of these studies was to aid the Department of Energy in its goal of understanding how microorganisms involved in the bioremediation of metals and radionuclides sustain their activity in the subsurface. This information is required in order to incorporate biological processes into decision making for environmental remediation and long-term stewardship of contaminated sites. The proposed research was designed to elucidate the mechanisms for electron transfer to Fe(III) oxides in Geobacter species because Geobacter species are abundant dissimilatory metal-reducing microorganisms in a diversity of sites in which uranium is undergoing natural attenuation via the reduction of soluble U(VI) tomore » insoluble U(IV) or when this process is artificially stimulated with the addition of organic electron donors. This study investigated the novel, but highly controversial, concept that the final conduit for electron transfer to Fe(III) oxides are electrically conductive pili. The specific objectives were to: 1) further evaluate the conductivity along the pili of Geobacter sulfurreducens and related organisms; 2) determine the mechanisms for pili conductivity; and 3) investigate the role of pili in Fe(III) oxide reduction. The studies demonstrated that the pili of G. sulfurreducens are conductive along their length. Surprisingly, the pili possess a metallic-like conductivity similar to that observed in synthetic organic conducting polymers such as polyaniline. Detailed physical analysis of the pili, as well as studies in which the structure of the pili was genetically modified, demonstrated that the metallic-like conductivity of the pili could be attributed to overlapping pi-pi orbitals of aromatic amino acids. Other potential mechanisms for conductivity, such as electron hopping between cytochromes associated with the pili were definitively ruled out. Pili were also found to be essential for Fe(III) oxide reduction in G. metallireducens. Ecological studies demonstrated that electron conduction along pili is a better strategy for Fe(III) oxide reduction under conditions found in the subsurface than producing an electron shuttle. The role of pili in uranium reduction was also elucidated. Our results are the first example of metallic-like conductivity in a biological protein and represent a paradigm shift in the understanding of long-range biological electron transport. The results are of importance not only for understanding subsurface microbial processes involved in the mobility of metal contaminants and carbon cycling, but also make a basic contribution to microbiology and the emerging field of bioelectronics.« less

Genetic Analysis of Stress Responses in Soil Bacteria for Enhanced Bioremediation of Mixed Contaminants

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

Wong, Kwong-Kwok

The purpose of this project is to provide fundamental knowledge on environment stress response of subsurface bacteria and a radiation-resistant bacterium (Deinococcus radiodurans). This information will be particularly useful in the development of successful bioremediation strategies. These organisms represent two phylogenetically distinct groups of soil bacteria, each of which has specific features of interest for bioremediation. The subsurface bacteria, Sphingomonas spp (Savannah River Site), have unique degradative capabilities of organic waste. The study of subsurface bacteria will serve as a model for bioremediation using indigenous bacteria. D. radiodurans exhibits high resistance to external stress such as ionizing radiation and organicmore » solvent. The study of D. radiodurans will serve as a model for the use of genetically engineered bacteria for bioremediation.« less

Methods for microbial filtration of fluids

DOEpatents

Carman, M.L.; Jackson, K.J.; Knapp, R.B.; Knezovich, J.P.; Shah, N.N.; Taylor, R.T.

1996-01-30

Novel methods for purifying contaminated subsurface groundwater are disclosed. The method is involves contacting the contaminated subsurface groundwater with methanotrophic or heterotrophic microorganisms which produce contaminant-degrading enzymes. The microorganisms are derived from surface cultures and are injected into the ground so as to act as a biofilter. The contaminants which may be treated include organic or metallic materials and radionuclides. 8 figs.

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

NASA Astrophysics Data System (ADS)

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

2010-12-01

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

Ground Water Issue. BASIC CONCEPTS OF CONTAMINANT SORPTION AT HAZARDOUS WASTE SITES

EPA Science Inventory

One of the major issues of concern to the Regional Superfund Ground Water Forum is the transport and fate of contaminants in soil and ground water as related to subsurface remediation. Processes which influence the behavior of contaminants in the subsurface must be considered bot...

Uranium mining wastes: The use of the Fish Embryo Acute Toxicity Test (FET) test to evaluate toxicity and risk of environmental discharge.

PubMed

Lourenço, J; Marques, S; Carvalho, F P; Oliveira, J; Malta, M; Santos, M; Gonçalves, F; Pereira, R; Mendo, S

2017-12-15

Active and abandoned uranium mining sites often create environmentally problematic situations, since they cause the contamination of all environmental matrices (air, soil and water) with stable metals and radionuclides. Due to their cytotoxic, genotoxic and teratogenic properties, the exposure to these contaminants may cause several harmful effects in living organisms. The Fish Embryo Acute Toxicity Test (FET) test was employed to evaluate the genotoxic and teratogenic potential of mine liquid effluents and sludge elutriates from a deactivated uranium mine. The aims were: a) to determine the risk of discharge of such wastes in the environment; b) the effectiveness of the chemical treatment applied to the uranium mine water, which is a standard procedure generally applied to liquid effluents from uranium mines and mills, to reduce its toxicological potential; c) the suitability of the FET test for the evaluation the toxicity of such wastes and the added value of including the evaluation of genotoxicity. Results showed that through the FET test it was possible to determine that both elutriates and effluents are genotoxic and also that the mine effluent is teratogenic at low concentrations. Additionally, liquid effluents and sludge elutriates affect other parameters namely, growth and hatching and that water pH alone played an important role in the hatching process. The inclusion of genotoxicity evaluation in the FET test was crucial to prevent the underestimation of the risks posed by some of the tested effluents/elutriates. Finally, it was possible to conclude that care should be taken when using benchmark values calculated for specific stressors to evaluate the risk posed by uranium mining wastes to freshwater ecosystems, due to their chemical complexity. Copyright © 2017 Elsevier B.V. All rights reserved.

Scale-Dependent Solute Dispersion in Variably Saturated Porous Media

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

Rockhold, Mark L.; Zhang, Z. F.; Bott, Yi-Ju

2016-03-29

This work was performed to support performance assessment (PA) calculations for the Integrated Disposal Facility (IDF) at the Hanford Site. PA calculations require defensible estimates of physical, hydraulic, and transport parameters to simulate subsurface water flow and contaminant transport in both the near- and far-field environments. Dispersivity is one of the required transport parameters.

MOBILIZATION AND CHARACTERIZATION OF COLLOIDS GENERATED FROM CEMENT LEACHATES MOVING THROUGH A SRS SANDY SEDIMENT

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

Li, D.; Roberts, K.; Kaplan, D.

Naturally occurring mobile colloids are ubiquitous and are involved in many important processes in the subsurface zone. For example, colloid generation and subsequent mobilization represent a possible mechanism for the transport of contaminants including radionuclides in the subsurface environments. For colloid-facilitated transport to be significant, three criteria must be met: (1) colloids must be generated; (2) contaminants must associate with the colloids preferentially to the immobile solid phase (aquifer); and (3) colloids must be transported through the groundwater or in subsurface environments - once these colloids start moving they become 'mobile colloids'. Although some experimental investigations of particle release inmore » natural porous media have been conducted, the detailed mechanisms of release and re-deposition of colloidal particles within natural porous media are poorly understood. Even though this vector of transport is known, the extent of its importance is not known yet. Colloid-facilitated transport of trace radionuclides has been observed in the field, thus demonstrating a possible radiological risk associated with the colloids. The objective of this study was to determine if cementitious leachate would promote the in situ mobilization of natural colloidal particles from a SRS sandy sediment. The intent was to determine whether cementitious surface or subsurface structure would create plumes that could produce conditions conducive to sediment dispersion and mobile colloid generation. Column studies were conducted and the cation chemistries of influents and effluents were analyzed by ICP-OES, while the mobilized colloids were characterized using XRD, SEM, EDX, PSD and Zeta potential. The mobilization mechanisms of colloids in a SRS sandy sediment by cement leachates were studied.« less

Modern Chemistry Techniques Applied to Metal Behavior and Chelation in Medical and Environmental Systems ? Final Report

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

Sutton, M; Andresen, B; Burastero, S R

2005-02-03

This report details the research and findings generated over the course of a 3-year research project funded by Lawrence Livermore National Laboratory (LLNL) Laboratory Directed Research and Development (LDRD). Originally tasked with studying beryllium chemistry and chelation for the treatment of Chronic Beryllium Disease and environmental remediation of beryllium-contaminated environments, this work has yielded results in beryllium and uranium solubility and speciation associated with toxicology; specific and effective chelation agents for beryllium, capable of lowering beryllium tissue burden and increasing urinary excretion in mice, and dissolution of beryllium contamination at LLNL Site 300; {sup 9}Be NMR studies previously unstudied atmore » LLNL; secondary ionization mass spec (SIMS) imaging of beryllium in spleen and lung tissue; beryllium interactions with aerogel/GAC material for environmental cleanup. The results show that chelator development using modern chemical techniques such as chemical thermodynamic modeling, was successful in identifying and utilizing tried and tested beryllium chelators for use in medical and environmental scenarios. Additionally, a study of uranium speciation in simulated biological fluids identified uranium species present in urine, gastric juice, pancreatic fluid, airway surface fluid, simulated lung fluid, bile, saliva, plasma, interstitial fluid and intracellular fluid.« less

Bacterial Community Shift and Coexisting/Coexcluding Patterns Revealed by Network Analysis in a Uranium-Contaminated Site after Bioreduction Followed by Reoxidation.

PubMed

Li, Bing; Wu, Wei-Min; Watson, David B; Cardenas, Erick; Chao, Yuanqing; Phillips, D H; Mehlhorn, Tonia; Lowe, Kenneth; Kelly, Shelly D; Li, Pengsong; Tao, Huchun; Tiedje, James M; Criddle, Craig S; Zhang, Tong

2018-05-01

A site in Oak Ridge, TN, USA, has sediments that contain >3% iron oxides and is contaminated with uranium (U). The U(VI) was bioreduced to U(IV) and immobilized in situ through intermittent injections of ethanol. It then was allowed to reoxidize via the invasion of low-pH (3.6 to 4.0), high-nitrate (up to 200 mM) groundwater back into the reduced zone for 1,383 days. To examine the biogeochemical response, high-throughput sequencing and network analysis were applied to characterize bacterial population shifts, as well as cooccurrence and coexclusion patterns among microbial communities. A paired t test indicated no significant changes of α-diversity for the bioactive wells. However, both nonmetric multidimensional scaling and analysis of similarity confirmed a significant distinction in the overall composition of the bacterial communities between the bioreduced and the reoxidized sediments. The top 20 major genera accounted for >70% of the cumulative contribution to the dissimilarity in the bacterial communities before and after the groundwater invasion. Castellaniella had the largest dissimilarity contribution (17.7%). For the bioactive wells, the abundance of the U(VI)-reducing genera Geothrix , Desulfovibrio , Ferribacterium , and Geobacter decreased significantly, whereas the denitrifying Acidovorax abundance increased significantly after groundwater invasion. Additionally, seven genera, i.e., Castellaniella , Ignavibacterium , Simplicispira , Rhizomicrobium , Acidobacteria Gp1, Acidobacteria Gp14, and Acidobacteria Gp23, were significant indicators of bioactive wells in the reoxidation stage. Canonical correspondence analysis indicated that nitrate, manganese, and pH affected mostly the U(VI)-reducing genera and indicator genera. Cooccurrence patterns among microbial taxa suggested the presence of taxa sharing similar ecological niches or mutualism/commensalism/synergism interactions. IMPORTANCE High-throughput sequencing technology in combination with a network analysis approach were used to investigate the stabilization of uranium and the corresponding dynamics of bacterial communities under field conditions with regard to the heterogeneity and complexity of the subsurface over the long term. The study also examined diversity and microbial community composition shift, the common genera, and indicator genera before and after long-term contaminated-groundwater invasion and the relationship between the target functional community structure and environmental factors. Additionally, deciphering cooccurrence and coexclusion patterns among microbial taxa and environmental parameters could help predict potential biotic interactions (cooperation/competition), shared physiologies, or habitat affinities, thus, improving our understanding of ecological niches occupied by certain specific species. These findings offer new insights into compositions of and associations among bacterial communities and serve as a foundation for future bioreduction implementation and monitoring efforts applied to uranium-contaminated sites. Copyright © 2018 American Society for Microbiology.

Empirical calibration of uranium releases in the terrestrial environment of nuclear fuel cycle facilities.

PubMed

Pourcelot, Laurent; Masson, Olivier; Saey, Lionel; Conil, Sébastien; Boulet, Béatrice; Cariou, Nicolas

2017-05-01

In the present paper the activity of uranium isotopes measured in plants and aerosols taken downwind of the releases of three nuclear fuel settlements was compared between them and with the activity measured at remote sites. An enhancement of 238 U activity as well as 235 U/ 238 U anomalies and 236 U are noticeable in wheat, grass, tree leaves and aerosols taken at the edge of nuclear fuel settlements, which show the influence of uranium chronic releases. Further plants taken at the edge of the studied sites and a few published data acquired in the same experimental conditions show that the 238 U activity in plants is influenced by the intensity of the U atmospheric releases. Assuming that 238 U in plant is proportional to the intensity of the releases, we proposed empirical relationships which allow to characterize the chronic releases on the ground. Other sources of U contamination in plants such as accidental releases and "delayed source" of uranium in soil are also discussed in the light of uranium isotopes signatures. Copyright © 2017 Elsevier Ltd. All rights reserved.

Plant-Stress Measurements Using Laser-Induced Fluorescence Excitation: Poland Experiment

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

Gene Capelle; Steve Jones

1999-05-01

Bechtel Nevada's Special Technologies Laboratory (STL) has been involved in remote sensing for many years, and in April 1995 STL began to study the use of active remote sensing for detecting plant stress. This work was motivated by the need to detect subsurface contamination, with the supposition that this could be accomplished by remote measurement of optical signatures from the overgrowing vegetation. The project has been a cooperative DOE/Disney effort, in which basic optical signature measurements (primarily fluorescence) were done at the Disney greenhouse facilities at Epcot Center in Florida, using instrumentation developed by STL on DOE funding. The primarymore » instrument is a LIFI system, which had originally been developed for detection of surface uranium contamination at DOE sites. To deal specifically with the plant stress measurements, a LIFS system was built that utilizes the same laser, but captures the complete fluorescence spectrum from blue to red wavelengths. This system had continued to evolve, and the version in existence in September 1997 was sent to Poland, accompanied by two people from STL, for the purpose of making the measurements described in this report.« less

Oxidation of aromatic contaminants coupled to microbial iron reduction

USGS Publications Warehouse

Lovley, D.R.; Baedecker, M.J.; Lonergan, D.J.; Cozzarelli, I.M.; Phillips, E.J.P.; Siegel, D.I.

1989-01-01

THE contamination of sub-surface water supplies with aromatic compounds is a significant environmental concern1,2. As these contaminated sub-surface environments are generally anaerobic, the microbial oxidation of aromatic compounds coupled to nitrate reduction, sulphate reduction and methane production has been studied intensively1-7. In addition, geochemical evidence suggests that Fe(III) can be an important electron acceptor for the oxidation of aromatic compounds in anaerobic groundwater. Until now, only abiological mechanisms for the oxidation of aromatic compounds with Fe(III) have been reported8-12. Here we show that in aquatic sediments, microbial activity is necessary for the oxidation of model aromatic compounds coupled to Fe(III) reduction. Furthermore, a pure culture of the Fe(III)-reducing bacterium GS-15 can obtain energy for growth by oxidizing benzoate, toluene, phenol or p-cresol with Fe(III) as the sole electron acceptor. These results extend the known physiological capabilities of Fe(III)-reducing organisms and provide the first example of an organism of any type which can oxidize an aromatic hydrocarbon anaerobically. ?? 1989 Nature Publishing Group.

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

PubMed

Seltzer, Michael D

2003-09-01

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

Colorimetric detection of uranium in water

DOEpatents

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

2012-03-13

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

Uptake of trace elements and radionuclides from uranium mill tailings by four-wing saltbush (Atriplex canescens) and alkali sacaton (Sporobolus airoides). [Radium 226; Uranium; Molybdenum; Selenium; Vanadium; Astatine

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

Dreesen, D.R.; Marple, M.L.

1979-01-01

A greenhouse experiment was performed to determine the uptake of trace elements and radionuclides from uranium mill tailings by native plant species. Four-wing saltbush and alkali sacaton were grown in alkaline tailings covered with soil and in soil alone as controls. The tailings material was highly enriched in Ra-226, Mo, U, Se, V, and As compared with three local soils. The shrub grown in tailings had elevated concentrations of Mo, Se, Ra-226, U, As, and Na compared with the controls. Alkali sacaton contained high concentrations of Mo, Se, Ra-226, and Ni when grown on tailings. Molybdenum and selenium concentrations inmore » plants grown in tailings are above levels reported to be toxic to grazing animals. These results indicate that the bioavailability of Mo and Se in alkaline environments makes these elements among the most hazardous contaminants present in uranium mill wastes.« less

Directional phytoscreening: contaminant gradients in trees for plume delineation.

PubMed

Limmer, Matt A; Shetty, Mikhil K; Markus, Samantha; Kroeker, Ryan; Parker, Beth L; Martinez, Camilo; Burken, Joel G

2013-08-20

Tree sampling methods have been used in phytoscreening applications to delineate contaminated soil and groundwater, augmenting traditional investigative methods that are time-consuming, resource-intensive, invasive, and costly. In the past decade, contaminant concentrations in tree tissues have been shown to reflect the extent and intensity of subsurface contamination. This paper investigates a new phytoscreening tool: directional tree coring, a concept originating from field data that indicated azimuthal concentrations in tree trunks reflected the concentration gradients in the groundwater around the tree. To experimentally test this hypothesis, large diameter trees were subjected to subsurface contaminant concentration gradients in a greenhouse study. These trees were then analyzed for azimuthal concentration gradients in aboveground tree tissues, revealing contaminant centroids located on the side of the tree nearest the most contaminated groundwater. Tree coring at three field sites revealed sufficiently steep contaminant gradients in trees reflected nearby groundwater contaminant gradients. In practice, trees possessing steep contaminant gradients are indicators of steep subsurface contaminant gradients, providing compass-like information about the contaminant gradient, pointing investigators toward higher concentration regions of the plume.

Modelling dispersal of radioactive contaminants in Arctic waters as a result of potential recovery operations on the dumped submarine K-27.

PubMed

Karcher, M; Hosseini, A; Schnur, R; Kauker, F; Brown, J E; Dowdall, M; Strand, P

2017-03-15

Of the wide variety of dumped objects containing radioactive materials in the Arctic seas, the submarine K-27 constitutes a major risk due to the large amount of highly enriched uranium onboard and its location in shallow waters. As the matter of potential operations involving raising of the submarine have entered the public arena, a priori assessment of the contamination in the Arctic marine environment that could result after a possible accident during such operations is a matter of some interest. The dispersion of contaminants within the Arctic has been assessed using a large scale hydrodynamic model for a series of plausible accident scenarios and locations under different oceanographic regimes. Results indicate that, depending primarily on the nature of a release (i.e. instantaneous or continuous), large areas of the Arctic marine environment will exhibit contamination to varying degrees. Copyright © 2017 Elsevier Ltd. All rights reserved.

Assessing soil and groundwater contamination from biofuel spills.

PubMed

Chen, Colin S; Shu, Youn-Yuen; Wu, Suh-Huey; Tien, Chien-Jung

2015-03-01

Future modifications of fuels should include evaluation of the proposed constituents for their potential to damage environmental resources such as the subsurface environment. Batch and column experiments were designed to simulate biofuel spills in the subsurface environment and to evaluate the sorption and desorption behavior of target fuel constituents (i.e., monoaromatic and polyaromatic hydrocarbons) in soil. The extent and reversibility of the sorption of aromatic biofuel constituents onto soil were determined. When the ethanol content in ethanol-blended gasoline exceeded 25%, enhanced desorption of the aromatic constituents to water was observed. However, when biodiesel was added to diesel fuel, the sorption of target compounds was not affected. In addition, when the organic carbon content of the soil was higher, the desorption of target compounds into water was lower. The empirical relationships between the organic-carbon normalized sorption coefficient (Koc) and water solubility and between Koc and the octanol-water partition coefficient (Kow) were established. Column experiments were carried out for the comparison of column effluent concentration/mass from biofuel-contaminated soil. The dissolution of target components depended on chemical properties such as the hydrophobicity and total mass of biofuel. This study provides a basis for predicting the fate and transport of hydrophobic organic compounds in the event of a biofuel spill. The spill scenarios generated can assist in the assessment of biofuel-contaminated sites.

In-Well Sediment Incubators to Evaluate Microbial Community Stability and Dynamics following Bioimmobilization of Uranium

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

Baldwin, Brett R.; Peacock, Aaron D.; Gan, M.

2009-09-23

An in-situ incubation device (ISI) was developed in order to investigate the stability and dynamics of sediment associated microbial communities to prevailing subsurface oxidizing or reducing conditions. Here we describe the use of these devices at the Old Rifle Uranium Mill Tailings Remedial Action (UMTRA) site. During the 7 month deployment oxidized Rifle aquifer background sediments (RABS) were deployed in previously biostimulated wells under iron reducing conditions, cell densities of known iron reducing bacteria including Geobacteraceae increased significantly showing the microbial community response to local subsurface conditions. PLFA profiles of RABS following in situ deployment were strikingly similar to thosemore » of adjacent sediment cores suggesting ISI results could be extrapolated to the native material of the test plots. Results for ISI deployed reduced sediments showed only slight changes in community composition and pointed toward the ability of the ISIs to monitor microbial community stability and response to subsurface conditions.« less

Analysis of Tank 38H (HTF-38-15-119, 127) Surface, Subsurface and Tank 43H (HTF-43-15-116, 117 and 118) Surface, Feed Pump Suction and Jet Suction Subsurface Supernatant Samples in Support of Enrichment, Corrosion Control and Salt Batch Planning Programs

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

Oji, L.

Compositional feed limits have been established to ensure that a nuclear criticality event for the 2H and 3H Evaporators is not possible. The Enrichment Control Program (ECP) requires feed sampling to determine the equivalent enriched uranium content prior to transfer of waste other than recycle transfers (requires sampling to determine the equivalent enriched uranium at two locations in Tanks 38H and 43H every 26 weeks) The Corrosion Control Program (CCP) establishes concentration and temperature limits for key constituents and periodic sampling and analysis to confirm that waste supernate is within these limits. This report provides the results of analyses onmore » Tanks 38H and 43H surface and subsurface supernatant liquid samples in support of the ECP, the CCP, and the Salt Batch 10 Planning Program.« less

Using electrokinetic phenomena and electrical resistance tomography to characterize the movement of subsurface fluids

DOEpatents

Ramirez, Abelardo L.; Cooper, John F.; Daily, William D.

1996-01-01

This invention relates generally to the remote detections of subsurface liquid contaminants using in combination a geophysical technique known as ERT and an EKS. Electrokinetic transport is used to enhance the ability of electrical resistance tomography (ERT) to detect position and movement of subsurface contaminant liquids, particles or ions. ERT images alone are difficult to interpret because of natural inhomogeneities in soil composition and electrical properties. By subtracting two or more ERT images obtained before and after field induced movement, a high contrast image of a plume of distinct electrokinetic properties can be seen. The invention is applicable to important subsurface characterization problems including, as examples, (1) detection of liquid-saturated plumes of contaminants such as those associated with leaks from underground storage tanks containing hazardous concentrated electrolytes, (2) detection and characterization of soils contaminated with organic pollutants such as droplets of gasoline; and (3) monitoring the progress of electrokinetic containment or clean up of underground contamination.

Using electrokinetic phenomena and electrical resistance tomography to characterize the movement of subsurface fluids

DOEpatents

Ramirez, A.L.; Cooper, J.F.; Daily, W.D.

1996-02-27

This invention relates generally to the remote detections of subsurface liquid contaminants using in combination a geophysical technique known as ERT and an EKS. Electrokinetic transport is used to enhance the ability of electrical resistance tomography (ERT) to detect position and movement of subsurface contaminant liquids, particles or ions. ERT images alone are difficult to interpret because of natural inhomogeneities in soil composition and electrical properties. By subtracting two or more ERT images obtained before and after field induced movement, a high contrast image of a plume of distinct electrokinetic properties can be seen. The invention is applicable to important subsurface characterization problems including, as examples, (1) detection of liquid-saturated plumes of contaminants such as those associated with leaks from underground storage tanks containing hazardous concentrated electrolytes, (2) detection and characterization of soils contaminated with organic pollutants such as droplets of gasoline; and (3) monitoring the progress of electrokinetic containment or clean up of underground contamination. 1 fig.

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

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

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

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

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

DOE PAGES

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

2017-06-01

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

Diagnosis of In Situ Metabolic State and Rates of Microbial Metabolism During In Situ Uranium Bioremediation with Molecular Techniques

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

Lovley, Derek R.

2012-11-28

The goal of these projects was to develop molecule tools to tract the metabolic activity and physiological status of microorganisms during in situ uranium bioremediation. Such information is important in able to design improved bioremediation strategies. As summarized below, the research was highly successful with new strategies developed for estimating in situ rates of metabolism and diagnosing the physiological status of the predominant subsurface microorganisms. This is a first not only for groundwater bioremediation studies, but also for subsurface microbiology in general. The tools and approaches developed in these studies should be applicable to the study of microbial communities inmore » a diversity of soils and sediments.« less

A survey of uranium levels in urine and hair of people living in a coal mining area in Yili, Xinjiang, China.

PubMed

Wufuer, Rehemanjiang; Song, Wenjuan; Zhang, Daoyong; Pan, Xiangliang; Gadd, Geoffrey Michael

2018-09-01

Recent reports have drawn attention to the uranium contamination arising from coal mining activities in the Yili region of Xinjiang, China due to the mixed distribution of uranium and coal mines, and some of the coal mines being associated with a high uranium content. In this study, we have collected water samples, solid samples such as soil, mud, coal, and coal ash, and hair and urine samples from local populations in order to evaluate the uranium level in this environment and its implications for humans in this high uranium coal mining area. Our results showed that uranium concentrations were 8.71-10.91 μg L -1 in underground water, whereas lower levels of uranium occurred in river water. Among the solid samples, coal ash contained fairly high concentrations of uranium (33.1 μg g -1 ) due to enrichment from coal burning. In addition, uranium levels in the other solid samples were around 2.8 μg g -1 (the Earth's average background value). Uranium concentrations in hair and urine samples were 22.2-634.5 ng g -1 (mean: 156.2 ng g -1 ) and 8.44-761.6 ng L -1 (mean: 202.6 ng L -1 ), respectively, which are significantly higher than reference values reported for unexposed subjects in other areas. Therefore, these results indicate that people living in this coal mining area have been subjected to uranium exposure for long periods of time. Copyright © 2018. Published by Elsevier Ltd.

Hydraulic and geochemical framework of the Idaho National Engineering and Environmental Laboratory vadose zone

USGS Publications Warehouse

Nimmo, John R.; Rousseau, Joseph P.; Perkins, Kim S.; Stollenwerk, Kenneth G.; Glynn, Pierre D.; Bartholomay, Roy C.; Knobel, LeRoy L.

2004-01-01

Questions of major importance for subsurface contaminant transport at the Idaho National Engineering and Environmental Laboratory (INEEL) include (i) travel times to the aquifer, both average or typical values and the range of values to be expected, and (ii) modes of contaminant transport, especially sorption processes. The hydraulic and geochemical framework within which these questions are addressed is dominated by extreme heterogeneity in a vadose zone and aquifer consisting of interbedded basalts and sediments. Hydraulically, major issues include diverse possible types of flow pathways, extreme anisotropy, preferential flow, combined vertical and horizontal flow, and temporary saturation or perching. Geochemically, major issues include contaminant mobility as influenced by redox conditions, the concentration of organic and inorganic complexing solutes and other local variables, the interaction with infiltrating waters and with the contaminant source environment, and the aqueous speciation of contaminants such as actinides. Another major issue is the possibility of colloid transport, which inverts some of the traditional concepts of mobility, as sorbed contaminants on mobile colloids may be transported with ease compared with contaminants that are not sorbed. With respect to the goal of minimizing aquifer concentrations of contaminants, some characteristics of the vadose zone are essentially completely favorable. Examples include the great thickness (200 m) of the vadose zone, and the presence of substantial quantities of fine sediments that can retard contaminant transport both hydraulically and chemically. Most characteristics, however, have both favorable and unfavorable aspects. For example, preferential flow, as promoted by several notable features of the vadose zone at the INEEL, can provide fast, minimally sorbing pathways for contaminants to reach the aquifer easily, but it also leads to a wide dispersal of contaminants in a large volume of subsurface material, thus increasing the opportunity for dilution and sorption.

Corrective Action Investigation Plan for Corrective Action Unit 428: Area 3 Septic Waste Systems 1 and 5, Tonopah Test Range, Nevada, REVISION 0, march 1999

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

ITLV.

1999-03-01

The Corrective Action Investigation Plan for Corrective Action Unit 428, Area 3 Septic Waste Systems 1 and 5, has been developed in accordance with the Federal Facility Agreement and Consent Order that was agreed to by the U. S. Department of Energy, Nevada Operations Office; the State of Nevada Division of Environmental Protection; and the U. S. Department of Defense. Corrective Action Unit 428 consists of Corrective Action Sites 03- 05- 002- SW01 and 03- 05- 002- SW05, respectively known as Area 3 Septic Waste System 1 and Septic Waste System 5. This Corrective Action Investigation Plan is used inmore » combination with the Work Plan for Leachfield Corrective Action Units: Nevada Test Site and Tonopah Test Range, Nevada , Rev. 1 (DOE/ NV, 1998c). The Leachfield Work Plan was developed to streamline investigations at leachfield Corrective Action Units by incorporating management, technical, quality assurance, health and safety, public involvement, field sampling, and waste management information common to a set of Corrective Action Units with similar site histories and characteristics into a single document that can be referenced. This Corrective Action Investigation Plan provides investigative details specific to Corrective Action Unit 428. A system of leachfields and associated collection systems was used for wastewater disposal at Area 3 of the Tonopah Test Range until a consolidated sewer system was installed in 1990 to replace the discrete septic waste systems. Operations within various buildings at Area 3 generated sanitary and industrial wastewaters potentially contaminated with contaminants of potential concern and disposed of in septic tanks and leachfields. Corrective Action Unit 428 is composed of two leachfield systems in the northern portion of Area 3. Based on site history collected to support the Data Quality Objectives process, contaminants of potential concern for the site include oil/ diesel range total petroleum hydrocarbons, and Resource Conservation and Recovery Act characteristic volatile organic compounds, semivolatile organic compounds, and metals. A limited number of samples will be analyzed for gamma- emitting radionuclides and isotopic uranium from four of the septic tanks and if radiological field screening levels are exceeded. Additional samples will be analyzed for geotechnical and hydrological properties and a bioassessment may be performed. The technical approach for investigating this Corrective Action Unit consists of the following activities: Perform video surveys of the discharge and outfall lines. Collect samples of material in the septic tanks. Conduct exploratory trenching to locate and inspect subsurface components. Collect subsurface soil samples in areas of the collection system including the septic tanks and outfall end of distribution boxes. Collect subsurface soil samples underlying the leachfield distribution pipes via trenching. Collect surface and near- surface samples near potential locations of the Acid Sewer Outfall if Septic Waste System 5 Leachfield cannot be located. Field screen samples for volatile organic compounds, total petroleum hydrocarbons, and radiological activity. Drill boreholes and collect subsurface soil samples if required. Analyze samples for total volatile organic compounds, total semivolatile organic compounds, total Resource Conservation and Recovery Act metals, and total petroleum hydrocarbons (oil/ diesel range organics). Limited number of samples will be analyzed for gamma- emitting radionuclides and isotopic uranium from particular septic tanks and if radiological field screening levels are exceeded. Collect samples from native soils beneath the distribution system and analyze for geotechnical/ hydrologic parameters. Collect and analyze bioassessment samples at the discretion of the Site Supervisor if total petroleum hydrocarbons exceed field- screening levels.« less

Significant Association between Sulfate-Reducing Bacteria and Uranium-Reducing Microbial Communities as Revealed by a Combined Massively Parallel Sequencing-Indicator Species Approach▿ †

PubMed Central

Cardenas, Erick; Wu, Wei-Min; Leigh, Mary Beth; Carley, Jack; Carroll, Sue; Gentry, Terry; Luo, Jian; Watson, David; Gu, Baohua; Ginder-Vogel, Matthew; Kitanidis, Peter K.; Jardine, Philip M.; Zhou, Jizhong; Criddle, Craig S.; Marsh, Terence L.; Tiedje, James M.

2010-01-01

Massively parallel sequencing has provided a more affordable and high-throughput method to study microbial communities, although it has mostly been used in an exploratory fashion. We combined pyrosequencing with a strict indicator species statistical analysis to test if bacteria specifically responded to ethanol injection that successfully promoted dissimilatory uranium(VI) reduction in the subsurface of a uranium contamination plume at the Oak Ridge Field Research Center in Tennessee. Remediation was achieved with a hydraulic flow control consisting of an inner loop, where ethanol was injected, and an outer loop for flow-field protection. This strategy reduced uranium concentrations in groundwater to levels below 0.126 μM and created geochemical gradients in electron donors from the inner-loop injection well toward the outer loop and downgradient flow path. Our analysis with 15 sediment samples from the entire test area found significant indicator species that showed a high degree of adaptation to the three different hydrochemical-created conditions. Castellaniella and Rhodanobacter characterized areas with low pH, heavy metals, and low bioactivity, while sulfate-, Fe(III)-, and U(VI)-reducing bacteria (Desulfovibrio, Anaeromyxobacter, and Desulfosporosinus) were indicators of areas where U(VI) reduction occurred. The abundance of these bacteria, as well as the Fe(III) and U(VI) reducer Geobacter, correlated with the hydraulic connectivity to the substrate injection site, suggesting that the selected populations were a direct response to electron donor addition by the groundwater flow path. A false-discovery-rate approach was implemented to discard false-positive results by chance, given the large amount of data compared. PMID:20729318

Significant association between sulfate-reducing bacteria and uranium-reducing microbial communities as revealed by a combined massively parallel sequencing-indicator species approach.

PubMed

Cardenas, Erick; Wu, Wei-Min; Leigh, Mary Beth; Carley, Jack; Carroll, Sue; Gentry, Terry; Luo, Jian; Watson, David; Gu, Baohua; Ginder-Vogel, Matthew; Kitanidis, Peter K; Jardine, Philip M; Zhou, Jizhong; Criddle, Craig S; Marsh, Terence L; Tiedje, James M

2010-10-01

Massively parallel sequencing has provided a more affordable and high-throughput method to study microbial communities, although it has mostly been used in an exploratory fashion. We combined pyrosequencing with a strict indicator species statistical analysis to test if bacteria specifically responded to ethanol injection that successfully promoted dissimilatory uranium(VI) reduction in the subsurface of a uranium contamination plume at the Oak Ridge Field Research Center in Tennessee. Remediation was achieved with a hydraulic flow control consisting of an inner loop, where ethanol was injected, and an outer loop for flow-field protection. This strategy reduced uranium concentrations in groundwater to levels below 0.126 μM and created geochemical gradients in electron donors from the inner-loop injection well toward the outer loop and downgradient flow path. Our analysis with 15 sediment samples from the entire test area found significant indicator species that showed a high degree of adaptation to the three different hydrochemical-created conditions. Castellaniella and Rhodanobacter characterized areas with low pH, heavy metals, and low bioactivity, while sulfate-, Fe(III)-, and U(VI)-reducing bacteria (Desulfovibrio, Anaeromyxobacter, and Desulfosporosinus) were indicators of areas where U(VI) reduction occurred. The abundance of these bacteria, as well as the Fe(III) and U(VI) reducer Geobacter, correlated with the hydraulic connectivity to the substrate injection site, suggesting that the selected populations were a direct response to electron donor addition by the groundwater flow path. A false-discovery-rate approach was implemented to discard false-positive results by chance, given the large amount of data compared.

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

PubMed

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

2011-08-15

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

ELUTION OF URANIUM FROM RESIN

DOEpatents

McLEan, D.C.

1959-03-10

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

Thixotropic gel for vadose zone remediation

DOEpatents

Riha, Brian D.

2012-07-03

A thixotropic gel suitable for use in subsurface bioremediation is provided along with a process of using the gel. The thixotropic gel provides a non-migrating injectable substrate that can provide below ground barrier properties. In addition, the gel components provide for a favorable environment in which certain contaminants are preferentially sequestered in the gel and subsequently remediated by either indigenous or introduced microorganisms.

Thixotropic gel for vadose zone remediation

DOEpatents

Rhia, Brian D [Augusta, GA

2011-03-01

A thixotropic gel suitable for use in subsurface bioremediation is provided along with a process of using the gel. The thixotropic gel provides a non-migrating injectable substrate that can provide below ground barrier properties. In addition, the gel components provide for a favorable environment in which certain contaminants are preferentially sequestered in the gel and subsequently remediated by either indigenous or introduced microorganisms.

Thixotropic gel for vadose zone remediation

DOEpatents

Riha, Brian D.; Looney, Brian B.

2015-10-27

A thixotropic gel suitable for use in subsurface bioremediation is provided along with a process of using the gel. The thixotropic gel provides a non-migrating injectable substrate that can provide below ground barrier properties. In addition, the gel components provide for a favorable environment in which certain contaminants are preferentially sequestered in the gel and subsequently remediated by either indigenous or introduced microorganisms.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Overview of environmental and hydrogeologic conditions at Barrow, Alaska

USGS Publications Warehouse

McCarthy, K.A.

1994-01-01

To assist the Federal Aviation Administration (FAA) in evaluating the potential effects of environmental contamination at their facility in Barrow, Alaska, a general assessment was made of the hydrologic system is the vicinity of the installation. The City of Barrow is located approximately 16 kilometers southwest of Point Barrow, the northernmost point in Alaska, and therefore lies within the region of continuous permafrost. Migration of surface or shallow- subsurface chemical releases in this environ- ment would be largely restricted by near-surface permafrost to surface water and the upper, suprapermafrost zone of the subsurface. In the arctic climate and tundra terrain of the Barrow area, this shallow environment has a limited capacity to attenuate the effects of either physical disturbances or chemical contamination and is therefore highly susceptible to degradation. Esatkuat Lagoon, the present drink- ing water supply for the City of Barrow, is located approximately 2 kilometers from the FAA facility. This lagoon is the only practical source of drinking water available to the City of Barrow because alternative sources of water in the area are (1) frozen throughout most of the year, (2) insufficient in volume, (3) of poor quality, or (4) too costly to develop and distribute.

The role of attached phase soil and sediment organic matter physicochemical properties on fullerene (nC60) attachment.

PubMed

McNew, Coy P; LeBoeuf, Eugene J

2015-11-01

Attached phase soil and sediment organic matter is ubiquitous in the subsurface environment, with a tendency to strongly sorb contaminants, and therefore it may play an important role in contaminant transport. In this study, the deposition of C60 nanoparticles onto attached phase Harpeth Humic Acid and Harpeth Fulvic Acid (HHA and HFA) is explored by using a quartz crystal microbalance with dissipation monitoring and systematically varying thermal energy. By comparing the C60 attachment onto HHA and HFA surfaces to that of bare silica and DLVO predictions, we find that the HHA and HFA layers hinder attachment at low temperatures, while HHA enhances attachment at higher temperatures. Based on thermal characterization of the HHA and HFA layers compared to the corresponding attachment trends, the attachment efficiency is strongly correlated with hydration of the layer. Possible mechanisms explaining this phenomenon include water-assisted disruption of polar SOM contacts and hydration-induced swelling of the AP-SOM matrix. Since humic substances typically dominate subsurface organic matter, these results may prove crucial to understanding the complex interactions of engineered nanomaterials in both the natural and engineered environment. Copyright © 2015 Elsevier Ltd. All rights reserved.

Radiological characterization survey of the former Diamond Magnesium Company Company site, 720 Fairport-Nursery Road, Painesville, Ohio (DMP001, DMP002)

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

Foley, R.D.; Carrier, R.F.

1991-12-01

At the request of the US Department of Energy (DOE), a group from Oak Ridge National Laboratory performed an investigative radiological survey at the former Diamond Magnesium Company (DMC) site at 720 Fairport-Nursery Road, Painesville, Ohio, in September 1990. The purpose of the survey was to determine if the site is contaminated with radioactive residues as a result of federal government operation in the development of nuclear energy for defense-related projects. The survey of the site, separate parcels of which are currently owned by the Uniroyal Chemical Company (DMP001) and the Lonza Chemical Company (DMP002), included a gamma scan overmore » the ground surface, determination of gamma exposure rates at the surface and at 1 m above the surface at grid points, collection and radionuclide analysis of soil samples, and directly measured radiation levels inside three buildings used during original DMC processing. Results of the survey revealed widespread radiological contamination outdoors on the Uniroyal property and several isolated spots of elevated radiation levels on the Lonza property. The contaminants consisted of radium, uranium, and thorium in surface and subsurface soil in concentrations exceeding DOE guidelines for the release of property for unrestricted use.« less

Radiological characterization survey of the former Diamond Magnesium Company Company site, 720 Fairport-Nursery Road, Painesville, Ohio (DMP001, DMP002)

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

Foley, R.D.; Carrier, R.F.

At the request of the US Department of Energy (DOE), a group from Oak Ridge National Laboratory performed an investigative radiological survey at the former Diamond Magnesium Company (DMC) site at 720 Fairport-Nursery Road, Painesville, Ohio, in September 1990. The purpose of the survey was to determine if the site is contaminated with radioactive residues as a result of federal government operation in the development of nuclear energy for defense-related projects. The survey of the site, separate parcels of which are currently owned by the Uniroyal Chemical Company (DMP001) and the Lonza Chemical Company (DMP002), included a gamma scan overmore » the ground surface, determination of gamma exposure rates at the surface and at 1 m above the surface at grid points, collection and radionuclide analysis of soil samples, and directly measured radiation levels inside three buildings used during original DMC processing. Results of the survey revealed widespread radiological contamination outdoors on the Uniroyal property and several isolated spots of elevated radiation levels on the Lonza property. The contaminants consisted of radium, uranium, and thorium in surface and subsurface soil in concentrations exceeding DOE guidelines for the release of property for unrestricted use.« less

Optimizing Metalloporphyrin-Catalyzed Reduction Reactions for In Situ Remediation of DOE Contaminants

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

Schlautman, Mark A.

2013-07-14

Past activities have resulted in a legacy of contaminated soil and groundwater at Department of Energy facilities nationwide. Uranium and chromium are among the most frequently encountered and highest-priority metal and radionuclide contaminants at DOE installations. Abiotic chemical reduction of uranium and chromium at contaminated DOE sites can be beneficial because the reduced metal species are less soluble in water, less mobile in the environment, and less toxic to humans and ecosystems. Although direct biological reduction has been reported for U(VI) and Cr(VI) in laboratory studies and at some field sites, the reactions can sometimes be slow or even inhibitedmore » due to unfavorable environmental conditions. One promising approach for the in-situ remediation of DOE contaminants is to develop electron shuttle catalysts that can be delivered precisely to the specific subsurface locations where contaminants reside. Previous research has shown that reduction of oxidized organic and inorganic contaminants often can be catalyzed by electron shuttle systems. Metalloporphyrins and their derivatives are well known electron shuttles for many biogeochemical systems, and thus were selected to study their catalytic capabilities for the reduction of chromium and uranium in the presence of reducing agents. Zero valent iron (ZVI) was chosen as the primary electron donor in most experimental systems. Research proceeded in three phases and the key findings of each phase are reported here. Phase I examined Cr(VI) reduction and utilized micro- and nano-sized ZVI as the electron donors. Electron shuttle catalysts tested were cobalt- and iron-containing metalloporphyrins and Vitamin B12. To aid in the recycle and reuse of the nano-sized ZVI and soluble catalysts, sol-gels and calcium-alginate gel beads were tested as immobilization/support matrices. Although the nano-sized ZVI could be incorporated within the alginate gel beads, preliminary attempts to trap it in sol-gels were not successful. Conversely, the water-soluble catalysts could be trapped within sol-gel matrices but they tended to leach out of the alginate gel beads during use. In general, immobilization of the nano-sized ZVI in gel beads and of the catalysts in sol-gels tended to result in slower rates of Cr(VI) reduction, but these effects could be overcome to some extent by using higher reactant/catalyst concentrations. In addition, the lowering of their effectiveness would likely be offset by the benefits obtained when recycling and reusing the materials because they were immobilized. Addition of the catalytic electron shuttles will be most useful when the micro-sized or nano-sized ZVI becomes less reactive with reaction time. Continued work in Phase II in the area of nano-sized ZVI immobilization led to procedures that were successful in incorporating the iron particles in sol-gel matrices. The water-soluble reductants sodium dithionite and L-ascorbic acid were also tested, but their use appeared to lead to formation of complexes with the uranyl cation which limited their effectiveness. Also, although the sol-gel supported nano-sized ZVI showed some promise at reducing uranium, the fluoride used in the sol-gel synthesis protocol appeared to lead to formation of uranyl-fluoride complexes that were less reactive. Because hexavalent chromium is an anion which does not form complexes with fluoride, it was used to demonstrate the intrinsic reactivity of the sol-gel immobilized nano-sized ZVI. Consistent with our observations in Phase I, the sol-gel matrix once again slowed down the reduction reaction but the expected benefits of recycle/reuse should outweigh this adverse effect. The major emphasis in Phase III of this study was to simultaneously incorporate nano-sized ZVI and water-soluble catalysts in the same sol-gel matrix. The catalysts utilized were cobalt complexes of uroporphyrin and protoporphyrin and Cr(VI) reduction was used to test the efficacy of the combined "catalyst + reductant" sol-gel matrix. When enough catalyst was added to the sol-gels, enhancement of the Cr(VI) reduction reaction was observed. At the lowest levels of catalyst addition, however, the rates of Cr(VI) reduction were similar to those systems which only used sol-gel immobilized nano-sized ZVI without any catalyst present. These findings suggest future areas of research that should be pursued to further optimize abiotic reduction reactions of metals with combined "catalyst + reductant" matrices.« less

The effect of Si and Al concentrations on the removal of U(VI) in the alkaline conditions created by NH3 gas

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

Katsenovich, Yelena P.; Cardona, Claudia; Lapierre, Robert

2016-10-01

Remediation of uranium in the deep unsaturated zone is a challenging task, especially in the presence of oxygenated, high-carbonate alkalinity soil and pore water composition typical for arid and semi-arid environments of the western regions of the U.S. This study evaluates the effect of various pore water constituencies on changes of uranium concentrations in alkaline conditions, created in the presence of reactive gases such as NH3 to effectively mitigate uranium contamination in the vadose zone sediments. This contaminant is a potential source for groundwater pollution through slow infiltration of soluble and highly mobile uranium species towards the water table. Themore » objective of this research was to evaluate uranium sequestration efficiencies in the alkaline synthetic pore water solutions prepared in a broad range of Si, Al, and bicarbonate concentrations typically present in field systems of the western U.S. regions and identify solid uranium-bearing phases that result from ammonia gas treatment. In previous studies (Szecsody et al. 2012; Zhong et al. 2015), although uranium mobility was greatly decreased, solid phases could not be identified at the low uranium concentrations in field-contaminated sediments. The chemical composition of the synthetic pore water used in the experiments varied for silica (5–250 mM), Al3+ (2.8 or 5 mM), HCO3- (0–100 mM) and U(VI) (0.0021–0.0084 mM) in the solution mixture. Experiment results suggested that solutions with Si concentrations higher than 50 mM exhibited greater removal efficiencies of U(VI). Solutions with higher concentrations of bicarbonate also exhibited greater removal efficiencies for Si, Al, and U(VI). Overall, the silica polymerization reaction leading to the formation of Si gel correlated with the removal of U(VI), Si, and Al from the solution. If no Si polymerization was observed, there was no U removal from the supernatant solution. Speciation modeling indicated that the dominant uranium species in the presence of bicarbonate were anionic uranyl carbonate complexes (UO2(CO3)2-2 and UO2(CO3)3-4) and in the absence of bicarbonate in the solution, U(VI) major species appeared as uranyl-hydroxide (UO2(OH)3- and UO2(OH)4-2) species. The model also predicted the formation of uranium solid phases. Uranyl carbonates as rutherfordine [UO2CO3], cejkaite [Na4(UO2)(CO3)3] and hydrated uranyl silicate phases as Na-boltwoodite [Na(UO2)(SiO4)·1.5H2O] were anticipated for most of the synthetic pore water compositions amended from medium (2.9 mM) to high (100 mM) bicarbonate concentrations.« less

Subsurface injection of liquid waste in Florida, United States of America

USGS Publications Warehouse

Vecchioli, John

1981-01-01

In 1979, liquid waste was injected into the subsurface of Florida by 10 injection systems at an aggregate average rate of 165,000 m3/d. All the systems inject into carbonate rocks that contain salty water. Extensive precautions are taken in the construction of the injection wells and in the monitoring of their operation to provide assurance that overlying and laterally contiguous freshwater resources do not become contaminated with either the injected waste or the saltwater displaced by the waste. Several concerns relating to the effectiveness of the confining bed above the injection zone for containing the injected wastes have arisen over the years. These concerns accentuate the value of a well-planned and implemented monitoring program from which one can evaluate the potential impact of waste injection on the subsurface environment.

Final technical report for project titled Quantitative Characterization of Cell Aggregation/Adhesion as Predictor for Distribution and Transport of Microorganisms in Subsurface Environment

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

Gu, April Z.; Wan, Kai-tak

This project aims to explore and develop enabling methodology and techniques for nano-scale characterization of microbe cell surface contact mechanics, interactions and adhesion quantities that allow for identification and quantification of indicative properties related to microorganism migration and transport behavior in porous media and in subsurface environments. Microbe transport has wide impact and therefore is of great interest in various environmental applications such as in situ or enhanced subsurface bioremediation,filtration processes for water and wastewater treatments and protection of drinking water supplies. Although great progress has been made towards understanding the identities and activities of these microorganisms in the subsurface,more » to date, little is known of the mechanisms that govern the mobility and transport of microorganisms in DOE’s contaminated sites, making the outcomes of in situ natural attenuation or contaminant stability enhancement unpredictable. Conventionally, movement of microorganisms was believed to follows the rules governing solute (particle) transport. However, recent studies revealed that cell surface properties, especially those pertaining to cell attachment/adhesion and aggregation behavior, can cause the microbe behavior to deviate from non-viable particles and hence greatly influence the mobility and distribution of microorganisms in porous media.This complexity highlights the need to obtain detailed information of cell-cell and cell-surface interactions in order to improve and refine the conceptual and quantitative model development for fate and transport of microorganisms and contaminant in subsurface. Traditional cell surface characterization methods are not sufficient to fully predict the deposition rates and transport behaviors of microorganism observed. A breakthrough of methodology that would allow for quantitative and molecular-level description of intrinsic cell surface properties indicative for cell-surface interactions is essential for the field. To tackle this, we have developed a number of new Bio-nanomechanical techniques, including reflection interference contrast microscopy (RICM) and bio-AFM (Atomic Force Microscopy), for cell adhesion-detachment measurement of the long-range surface interactions, in combination with mathematical modeling, which would allow us to characterize the mechanical behavior from single cell to multi-cell aggregate, critical thresholds for large scale coaggregation and transportation of cells and aggregates in the presence of long range inter-surface forces etc. Although some technical and mathematical challenges remain, the preliminary results promise great breakthrough potential. In this study, we investigated the cellular surface characteristics of representative bio-remediating microorganisms relevant to DOE IFRC (Integrated Field-Scale Subsurface Research Challenges) sites and their transport behaviors in porous media, aiming to draw a groundbreaking correlation between the micro-scale genetic and biological origin-based cell surface properties, the consequent mechanical adhesion and aggregation behaviors, and the macro-scale microbial mobility and retention in porous media, which are unavailable in the literature. The long-term goal is to significantly improve the mechanistic and quantitative understanding of microbial mobility, sorption, and transport within reactive transport models as needed to manipulate subsurface contaminant fate and transport predictions.« less

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

USGS Publications Warehouse

Goode, Daniel J.; Wilder, Russell J.

1987-01-01

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

Fate of Uranium During Transport Across the Groundwater-Surface Water Interface

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

Jaffe, Peter R.; Kaplan, Daniel I.

Discharge of contaminated groundwater to surface waters is of concern at many DOE facilities. For example, at F-Area and TNX-Area on the Savannah River Site, contaminated groundwater, including uranium, is already discharging into natural wetlands. It is at this interface where contaminants come into contact with the biosphere. These this research addressed a critical knowledge gap focusing on the geochemistry of uranium (or for that matter, any redox-active contaminant) in wetland systems. Understanding the interactions between hydrological, microbial, and chemical processes will make it possible to provide a more accurate conceptual and quantitative understanding of radionuclide fate and transport undermore » these unique conditions. Understanding these processes will permit better long-term management and the necessary technical justification for invoking Monitored Natural Attenuation of contaminated wetland areas. Specifically, this research did provide new insights on how plant-induced alterations to the sediment biogeochemical processes affect the key uranium reducing microorganisms, the uranium reduction, its spatial distribution, the speciation of the immobilized uranium, and its long-term stability. This was achieved by conducting laboratory mesocosm wetland experiments as well as field measurements at the SRNL. Results have shown that uranium can be immobilized in wetland systems. To a degree some of the soluble U(VI) was reduced to insoluble U(IV), but the majority of the immobilized U was incorporated into iron oxyhydroxides that precipitated onto the root surfaces of wetland plants. This U was immobilized mostly as U(VI). Because it was immobilized in its oxidized form, results showed that dry spells, resulting in the lowering of the water table and the exposure of the U to oxic conditions, did not result in U remobilization.« less

U.S. Geological Survey program on toxic waste--ground-water contamination; proceedings of the Third technical meeting, Pensacola, Florida, March 23-27, 1987

USGS Publications Warehouse

Franks, Bernard J.

1987-01-01

Because of the widespread distribution of creosote in the environment, an abandoned wood-treatment plant in Pensacola, Fla., was selected by the U.S. Geological Survey Office of Hazardous Waste Hydrology as one of three national research demonstration areas in order to increase our understanding of hydrologic processes affecting the distributions of contaminants in ground water. The site was selected because of its long, uninterrupted history (1902 81) of discharging wastewaters to unlined surface impoundments, availability of a preliminary data base (Troutman and others, 1984), and the high probability of useful technology transfer from an investigation of the fate of organic compounds associated with wood-preserving wastewaters in the subsurface environment.

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

USGS Publications Warehouse

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

2014-01-01

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

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

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

Wang, Guohui; Um, Wooyong; Wang, Zheming

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

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

PubMed

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

2017-10-03

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

Applying model abstraction techniques to optimize monitoring networks for detecting subsurface contaminant transport

USDA-ARS?s Scientific Manuscript database

Improving strategies for monitoring subsurface contaminant transport includes performance comparison of competing models, developed independently or obtained via model abstraction. Model comparison and parameter discrimination involve specific performance indicators selected to better understand s...

Influence of dissimilatory metal reduction on fate of organic and metal contaminants in the subsurface

USGS Publications Warehouse

Lovely, Derek R.; Anderson, Robert T.

2000-01-01

Geobacter become dominant members of the microbial community when Fe(III)-reducing conditions develop as the result of organic contamination, or when Fe(III) reduction is artificially stimulated. These results suggest that further understanding of the ecophysiology of Geobacter species would aid in better prediction of the natural attenuation of organic contaminants under anaerobic conditions and in the design of strategies for the bioremediation of subsurface metal contamination.

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

Metzler, D.; Gibb, J.P.; Glover, W.A.

Compliance with the mandate of the Uranium Mill Tailings Radiation Control Act (UMTRCA) at Uranium Mill Tailings Remedial Action (UMTRA) Project sites requires implementation of a groundwater remedial action plan that meets the requirements of Subpart B of the US Environmental Protection Agency`s proposed groundwater protection standards (40 CFR 192). The UMTRA Groundwater Project will ensure that unacceptable current risk or potential risk to the public health, safety and the environment resulting from the groundwater contamination attributable to the UMTRA sites, is mitigated in a timely and cost-efficient manner. For each UMTRA processing site and vicinity property where contamination exists,more » a groundwater remedial action plan must be developed that identifies hazardous constituents and establishes acceptable concentration limits for the hazardous constituents as either (a) alternate concentration limits (ACL), (b) maximum concentration limits (MCLs), (c) supplemental standards, or (d) background groundwater quality levels. Project optimization is a strategy that will aggressively work within the current regulatory framework using all available options to meet regulatory requirements. This strategy is outlined within.« less

Near surface geophysical techniques on subsoil contamination: laboratory experiments

NASA Astrophysics Data System (ADS)

Capozzoli, Luigi; Giampaolo, Valeria; Rizzo, Enzo

2016-04-01

Hydrocarbons contamination of soil and groundwater has become a serious environmental problem, because of the increasing number of accidental spills caused by human activities. The starting point of any studies is the reconstruction of the conceptual site model. To make valid predictions about the flow pathways following by hydrocarbons compound is necessary to make a correct reconstruction of their characteristics and the environment in which they move. Near-surface geophysical methods, based on the study of electrical and electromagnetic properties, are proved to be very useful in mapping spatial distribution of the organic contaminants in the subsurface. It is well known, in fact, that electrical properties of the porous media are significantly influenced by hydrocarbons because, when contaminants enter the rock matrix, surface reaction occur between the contaminant and the soil grain surface. The main aim of this work is to investigate the capability of near-surface geophysical methods in mapping and monitoring spatial distribution of contaminants in a controlled setting. A laboratory experiment has been performed at the Hydrogeosite Laboratory of CNR-IMAA (Marsico Nuovo, PZ) where a box-sand has been contaminated by diesel. The used contaminant is a LNAPL, added to the sand through a drilled pipe. Contaminant behaviour and its migration paths have been monitored for one year by Electrical Resistivity measurements. In details, a Cross Borehole Electrical Resistivity Tomography techniques were used to characterize the contamination dynamics after a controlled hydrocarbon spillage occurring in the vadose zone. The approach with cross-borehole resistivity imaging provide a great advantage compared to more conventional surface electrical resistivity tomography, due to the high resolution at high depth (obviously depending on the depth of the well instrumented for the acquisition). This method has been shown to provide good information on the distribution of electrical properties of the subsoil at high depths and, in some cases, a detailed assessment of dynamic processes in the subsurface environment (Binley et al., 2002). Our study confirms the link between hydrocarbons contamination and geoelectrical signal and the capability of cross-hole electrical resistivity tomographies to realize a non-invasive characterization of LNAPL contamination of the media. Although, the electrical behaviour is much more complex and the relation with the contaminants depends also by time of investigation.

Uranium and strontium fate in waste-weathered sediments: Scaling of molecular processes to predict reactive transport

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

Chorover, Jon; Mueller, Karl; O'Day, Peggy

2016-04-02

Objectives of the project: 1. Determine the process coupling that occurs between mineral transformation and contaminant (U and Sr) speciation in acid-uranium waste weathered Hanford sediments. 2. Establish linkages between molecular-scale contaminant speciation and meso-scale contaminant lability, release and reactive transport. 3. Make conjunctive use of molecular- to bench-scale data to constrain the development of a mechanistic, reactive transport model that includes coupling of contaminant sorption-desorption and mineral transformation reactions. Hypotheses tested: - Uranium and strontium speciation in legacy sediments from the U-8 and U-12 Crib sites can be reproduced in bench-scale weathering experiments conducted on unimpacted Hanford sediments frommore » the same formations. - Reactive transport modeling of future uranium and strontium releases from the vadose zone of acid-waste weathered sediments can be effectively constrained by combining molecular-scale information on contaminant bonding environment with grain-scale information on contaminant phase partitioning, and meso-scale kinetic data on contaminant release from the waste-weathered porous media. - Although field contamination and laboratory experiments differ in their diagenetic time scales (decades for field vs. months to years for lab), sediment dissolution, neophase nucleation, and crystal growth reactions that occur during the initial disequilibrium induced by waste-sediment interaction leave a strong imprint that persists over subsequent longer-term equilibration time scales and, therefore, give rise to long-term memory effects. Enabling capabilities developed: Our team developed an iterative measure-model approach that is broadly applicable to elucidate the mechanistic underpinnings of reactive contaminant transport in geomedia subject to active weathering. Experimental design: Hypotheses were tested by comparing (with a similar set of techniques) the geochemical transformations and transport behaviors that occured in bench-scale studies of waste-sediment interaction with parallel model systems studies of homogeneous nucleation and neo-phase dissolution. Initial plans were to compare results with core sample extractions from the acid uranium waste impacted U-8 and U-12 Cribs at Hanford (see original proposal and letter of collaboration from J. Zachara). However, this part of the project was impossible because funding for core extractions were eliminated from the DoE budget. Three distinct crib waste aqueous simulants (whose composition is based on the most up-to-date information from field site investigations) were reacted with Hanford sediments in batch and column systems. Coupling of contaminant uptake to mineral weathering was monitored using a suite of methods both during waste-sediment interaction, and after, when waste-weathered sediments were subjected to infusion with circumneutral background pore water solutions. Our research was designed to adapt as needed to maintain a strong dialogue between laboratory and modeling investigations so that model development was increasingly constrained by emergent data and understanding. Potential impact of the project to DOE: Better prediction of contaminant uranium transport was achieved by employing multi-faceted lines of inquiry to build a strong bridge between molecular- and field-scale information. By focusing multiple lines and scales of observation on a common experimental design, our collaborative team revealed non-linear and emergent behavior in contaminated weathering systems. A goal of the current project was to expand our modeling capabilities, originally focused on hyperalkaline legacy waste streams, to include acidic weathering reactions that, as described above, were expected to result in profoundly different products. We were able to achieve this goal, and showed that these products nonetheless undergo analogous silicate and non-silicate transformation, ripening and aging processes. Our prediction that these weathering reactions would vary with waste stimulant chemistry resulted in data that was incorporated directly into a reactive transport model structure.« less

SITE TECHNOLOGY CAPSULE: SUBSURFACE VOLATILIZATION AND VENTILATION SYSTEM (SVVS)

EPA Science Inventory

The Subsurface Volatilization and Ventilation System is an integrated technology used for attacking all phases of volatile organic compound (VOC) contamination in soil and groundwater. The SVVS technology promotes insitu remediation of soil and groundwater contaminated with or-ga...

BIOPLUME MODEL FOR CONTAMINANT TRANSPORT AFFECTED BY OXYGEN LIMITED BIODEGRADATION

EPA Science Inventory

Many of the organic pollutants entering ground water are potentially biodegradable in the subsurface. This potential has been demonstrated in aquifers contaminated by wood-creosoting process wastes. The persistence of many of these organic compounds in the subsurface indicated ...

Biogeochemical Stability of Contaminants in the Subsurface Following In Situ Treatment

EPA Science Inventory

In recent years, innovative treatment technologies have emerged to meet groundwater cleanup goals. In many cases these methods take advantage of the redox behavior of contaminant species. For example, remedial technologies that strategically manipulate subsurface redox conditio...

PREDICTING SUBSURFACE CONTAMINANT TRANSPORT AND TRANSFORMATION: CONSIDERATIONS FOR MODEL SELECTION AND FIELD VALIDATION

EPA Science Inventory

Predicting subsurface contaminant transport and transformation requires mathematical models based on a variety of physical, chemical, and biological processes. The mathematical model is an attempt to quantitatively describe observed processes in order to permit systematic forecas...

Apparatus for passive removal of subsurface contaminants

DOEpatents

Pemberton, Bradley E.; May, Christopher P.; Rossabi, Joseph

1997-01-01

An apparatus is provided which passively removes contaminated gases from a subsurface. The apparatus includes a riser pipe extending into a subsurface which has an exterior end in fluid communication with a valve. When well pressure is greater than atmospheric pressure, the valve opens to release contaminants into the atmosphere, and when well pressure is less than atmospheric pressure, the valve closes to prevent flow of air into the well. The valve assembly of the invention comprises a lightweight ball which is lifted from its valve seat with a slight pressure drop between the well and the atmosphere.

Apparatus for passive removal of subsurface contaminants

DOEpatents

Pemberton, B.E.; May, C.P.; Rossabi, J.

1997-06-24

An apparatus is provided which passively removes contaminated gases from a subsurface. The apparatus includes a riser pipe extending into a subsurface which has an exterior end in fluid communication with a valve. When well pressure is greater than atmospheric pressure, the valve opens to release contaminants into the atmosphere, and when well pressure is less than atmospheric pressure, the valve closes to prevent flow of air into the well. The valve assembly of the invention comprises a lightweight ball which is lifted from its valve seat with a slight pressure drop between the well and the atmosphere. 7 figs.

In situ chemical degradation of DNAPLS in contaminated soils and sediments

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

Gates, D.D.; Korte, N.E.; Siegrist, R.L.

1996-08-01

An emerging approach to in situ treatment of organic contaminants is chemical degradation. The specific processes discussed in this chapter are in situ chemical oxidation using either hydrogen peroxide (H{sub 2}O{sub 2}) or potassium permanganate (KMnO{sub 4}) and in situ dechlorination of halogenated hydrocarbons using zero-valence base metals such as iron. These technologies are primarily chemical treatment processes, where the treatment goal is to manipulate the chemistry of the subsurface environment in such a manner that the contaminants of interest are destroyed and/or rendered non-toxic. Chemical properties that can be altered include pH, ionic strength, oxidation and reduction potential, andmore » chemical equilibria. In situ contaminant destruction processes alter or destroy contaminants in place and are typically applied to compounds that can be either converted to innocuous species such as CO{sub 2} and water, or can be degraded to species that are non-toxic or amenable to other in situ processes (i.e., bioremediation). With in situ chemical oxidation, the delivery and distribution of chemical reagents are critical to process effectiveness. In contrast, published approaches for the use of zero valence base metals suggest passive approaches in which the metals are used in a permeable reaction wall installed in situ in the saturated zone. Both types of processes are receiving increasing attention and are being applied both in technology demonstration and as final solutions to subsurface contaminant problems. 43 refs., 9 figs., 1 tab.« less

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

PubMed

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

2017-06-01

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

Oxidation of naturally reduced uranium in aquifer sediments by dissolved oxygen and its potential significance to uranium plume persistence

NASA Astrophysics Data System (ADS)

Davis, J. A.; Smith, R. L.; Bohlke, J. K.; Jemison, N.; Xiang, H.; Repert, D. A.; Yuan, X.; Williams, K. H.

2015-12-01

The occurrence of naturally reduced zones is common in alluvial aquifers in the western U.S.A. due to the burial of woody debris in flood plains. Such reduced zones are usually heterogeneously dispersed in these aquifers and characterized by high concentrations of organic carbon, reduced mineral phases, and reduced forms of metals, including uranium(IV). The persistence of high concentrations of dissolved uranium(VI) at uranium-contaminated aquifers on the Colorado Plateau has been attributed to slow oxidation of insoluble uranium(IV) mineral phases found in association with these reducing zones, although there is little understanding of the relative importance of various potential oxidants. Four field experiments were conducted within an alluvial aquifer adjacent to the Colorado River near Rifle, CO, wherein groundwater associated with the naturally reduced zones was pumped into a gas-impermeable tank, mixed with a conservative tracer (Br-), bubbled with a gas phase composed of 97% O2 and 3% CO2, and then returned to the subsurface in the same well from which it was withdrawn. Within minutes of re-injection of the oxygenated groundwater, dissolved uranium(VI) concentrations increased from less than 1 μM to greater than 2.5 μM, demonstrating that oxygen can be an important oxidant for uranium in such field systems if supplied to the naturally reduced zones. Dissolved Fe(II) concentrations decreased to the detection limit, but increases in sulfate could not be detected due to high background concentrations. Changes in nitrogen species concentrations were variable. The results contrast with other laboratory and field results in which oxygen was introduced to systems containing high concentrations of mackinawite (FeS), rather than the more crystalline iron sulfides found in aged, naturally reduced zones. The flux of oxygen to the naturally reduced zones in the alluvial aquifers occurs mainly through interactions between groundwater and gas phases at the water table. Seasonal variations of the water table at the Rifle, CO site may play an important role in introducing oxygen into the system. Although oxygen was introduced directly to the naturally reduced zones in these experiments, delivery of oxidants to the system may also be controlled by other oxidative pathways in which oxygen plays an indirect role.

Analysis of tank 38H (HTF-38-17-18, -19) and tank 43H (HTF-43-17-20, -21) samples for support of the enrichment control and corrosion control programs

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

Hay, M. S.; Coleman, C. J.; Diprete, D. P.

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H samples ranged from 53.7 mg/L for the surface sample to 57.0 mg/L in the sub-surface sample. The Tank 43H samples showed uranium concentrations of 46.2 mg/L for the surface sample and 45.7 mg/L in the sub-surface sample. The U-235 percentage was 0.63% in the Tank 38H samples and 0.62% in the Tank 43H samples. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The plutonium results for the Tank 38Hmore » surface sample are slightly higher than recent sample results, while the Tank 43H plutonium results are within the range of values measured on previous samples. The Cs-137 results for the Tank 38H surface and subsurface samples are slightly higher than the concentrations measured in recent samples. The Cs-137 results for the two Tank 43H samples are within the range of values measured on previous samples. The comparison of the sum of the cations in each sample versus the sum of the anions shows a difference of 23% for the Tank 38H surface sample and 18% for the Tank 43H surface sample. The four samples show silicon concentrations somewhat lower than the previous samples with values ranging from 80.2 to 105 mg/L.« less

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

PubMed

Baumann, Nils; Arnold, Thuro; Haferburg, Götz

2014-01-01

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

ENGINEERING ISSUE: IN SITU BIOREMEDIATION OF CONTAMINATED UNSATURATED SUBSURFACE SOILS

EPA Science Inventory

An emerging technology for the remediation of unsaturated subsurface soils involves the use of microorganisms to degrade contaminants which are present in such soils. Understanding the processes which drive in situ bioremediation, as well as the effectiveness and efficiency of th...

Models Show Subsurface Cracking May Complicate Groundwater Cleanup at Hazardous Waste Sites

EPA Science Inventory

Chlorinated solvents like trichloroethylene contaminate groundwater at numerous sites nationwide. This modeling study, conducted at the Air Force Institute of Technology, shows that subsurface cracks, either natural or due to the presence of the contaminant itself, may result in...

Wireless Sensor Network Based Subsurface Contaminant Plume Monitoring

DTIC Science & Technology

2012-04-16

Sensor Network (WSN) to monitor contaminant plume movement in naturally heterogeneous subsurface formations to advance the sensor networking based...time to assess the source and predict future plume behavior. This proof-of-concept research aimed at demonstrating the use of an intelligent Wireless

Quantification of kinetic rate law parameters for the dissolution of natural autunite in the presence of aqueous bicarbonate ions at high concentrations

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

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn

Uranium is a key contaminant of concern in the groundwater at 91 waste sites at 18 U.S. Department of Energy (DOE) facilities within the United States and is a potential source of groundwater contamination and a risk to human health and the environment through discharges to surface water. Dissolved inorganic carbon (bicarbonate/carbonate) has a high affinity for complexing with uranium that is present as sorbed or unique uranium-bearing mineral phases within the sedimentary matrix. This process can result in the formation of soluble uranyl carbonate aqueous species, which are mobile under circumneutral pH conditions. This study was conducted to quantifymore » the rate of release of uranium from the autunite mineral, (Ca[(UO 2)(PO 4)] 2∙3H 2O), that was formed during polyphosphate injection to remediate uranium; the dissolution of uranium was studied as a function of the aqueous bicarbonate concentration, ranging from 25 to 100 mM. Experiments were carried out in the pH range from 7 to 11 in the temperature range of 23-90°C via single-pass flow-through testing. Consistent with the results of previous studies (Gudavalli et al., 2013 a, b), the rate of uranium release from autunite exhibited minimal dependency on temperature, but was strongly dependent on pH and increasing concentrations of bicarbonate in the solution. Data obtained during these experiments were compared with results of previous experiments conducted using a low-concentration range of bicarbonate solutions (0.5-3.0 mM). An 8- to 30 fold increase in the rate of uranium release was observed in the presence of high bicarbonate concentrations at pH 7-8 compared to low bicarbonate values, while at pH 9-11, there was only a 5-fold increase in uranium rate of release with an increase in bicarbonate concentrations. The rate of uranium release was calculated to be between 5.18 x 10 -8 and 1.69 x 10 -7 mol m -2 s -1. The activation energy values at high and low bicarbonate concentrations were similar, with ratio values in the range of 0.6-1.0.« less

Quantification of kinetic rate law parameters for the dissolution of natural autunite in the presence of aqueous bicarbonate ions at high concentrations.

PubMed

Gudavalli, Ravi; Katsenovich, Yelena; Wellman, Dawn

2018-05-02

Uranium is a key contaminant of concern in the groundwater at U.S. Department of Energy (DOE) facilities within the United States and is a potential source of groundwater contamination and a risk to human health and the environment through discharges to surface water. Dissolved inorganic carbon (bicarbonate/carbonate) has a high affinity for complexing with uranium that is present as sorbed or unique uranium-bearing mineral phases within the sedimentary matrix. This process can result in the formation of soluble uranyl carbonate aqueous species, which are mobile under circumneutral pH conditions. This study was conducted to quantify the rate of release of uranium from the autunite mineral, (Ca[(UO 2 )(PO 4 )] 2 •3H 2 O), that was formed during polyphosphate injection to remediate uranium; the dissolution of uranium was studied as a function of the aqueous bicarbonate concentration, ranging from 25 to 100 mM. Experiments were carried out in the pH range from 7 to 11 in the temperature range of 23-90 °C via single-pass flow-through testing. Consistent with the results of previous studies (Gudavalli et al., 2013a, 2013b), the rate of uranium release from autunite exhibited minimal dependency on temperature, but was strongly dependent on pH and increasing concentrations of bicarbonate in the solution. Data obtained during these experiments were compared with results of previous experiments conducted using a low-concentration range of bicarbonate solutions (0.5-3.0 mM). An 8- to 30-fold increase in the rate of uranium release was observed in the presence of high bicarbonate concentrations at pH 7-8 compared to low bicarbonate values, while at pH 9-11, there was only a 5-fold increase in uranium rate of release with an increase in bicarbonate concentrations. The rate of uranium release was calculated to be between 5.18 × 10 -8 and 1.69 × 10 -7  mol m -2 s -1 . The activation energy values at high and low bicarbonate concentrations were similar, with ratio values in the range of 0.6-1.0. Copyright © 2018 Elsevier Ltd. All rights reserved.

Impact of Ammonium on Syntrophic Organohalide-Respiring and Fermenting Microbial Communities

PubMed Central

Fajardo-Williams, Devyn; Kegerreis, Kylie L.; Parameswaran, Prathap

2016-01-01

ABSTRACT Syntrophic interactions between organohalide-respiring and fermentative microorganisms are critical for effective bioremediation of halogenated compounds. This work investigated the effect of ammonium concentration (up to 4 g liter−1 NH4+-N) on trichloroethene-reducing Dehalococcoides mccartyi and Geobacteraceae in microbial communities fed lactate and methanol. We found that production of ethene by D. mccartyi occurred in mineral medium containing ≤2 g liter−1 NH4+-N and in landfill leachate. For the partial reduction of trichloroethene (TCE) to cis-dichloroethene (cis-DCE) at ≥1 g liter−1 NH4+-N, organohalide-respiring dynamics shifted from D. mccartyi and Geobacteraceae to mainly D. mccartyi. An increasing concentration of ammonium was coupled to lower metabolic rates, longer lag times, and lower gene abundances for all microbial processes studied. The methanol fermentation pathway to acetate and H2 was conserved, regardless of the ammonium concentration provided. However, lactate fermentation shifted from propionic to acetogenic at concentrations of ≥2 g liter−1 NH4+-N. Our study findings strongly support a tolerance of D. mccartyi to high ammonium concentrations, highlighting the feasibility of organohalide respiration in ammonium-contaminated subsurface environments. IMPORTANCE Contamination with ammonium and chlorinated solvents has been reported in numerous subsurface environments, and these chemicals bring significant challenges for in situ bioremediation. Dehalococcoides mccartyi is able to reduce the chlorinated solvent trichloroethene to the nontoxic end product ethene. Fermentative bacteria are of central importance for organohalide respiration and bioremediation to provide D. mccartyi with H2, their electron donor, acetate, their carbon source, and other micronutrients. In this study, we found that high concentrations of ammonium negatively correlated with rates of trichloroethene reductive dehalogenation and fermentation. However, detoxification of trichloroethene to nontoxic ethene occurred even at ammonium concentrations typical of those found in animal waste (up to 2 g liter−1 NH4+-N). To date, hundreds of subsurface environments have been bioremediated through the unique metabolic capability of D. mccartyi. These findings extend our knowledge of D. mccartyi and provide insight for bioremediation of sites contaminated with chlorinated solvents and ammonium. PMID:27303735

Uranium and other contaminants in hair from the parents of children with congenital anomalies in Fallujah, Iraq

PubMed Central

2011-01-01

Background Recent reports have drawn attention to increases in congenital birth anomalies and cancer in Fallujah Iraq blamed on teratogenic, genetic and genomic stress thought to result from depleted Uranium contamination following the battles in the town in 2004. Contamination of the parents of the children and of the environment by Uranium and other elements was investigated using Inductively Coupled Plasma Mass Spectrometry. Hair samples from 25 fathers and mothers of children diagnosed with congenital anomalies were analysed for Uranium and 51 other elements. Mean ages of the parents was: fathers 29.6 (SD 6.2); mothers: 27.3 (SD 6.8). For a sub-group of 6 women, long locks of hair were analysed for Uranium along the length of the hair to obtain information about historic exposures. Samples of soil and water were also analysed and Uranium isotope ratios determined. Results Levels of Ca, Mg, Co, Fe, Mn, V, Zn, Sr, Al, Ba, Bi, Ga, Pb, Hg, Pd and U (for mothers only) were significantly higher than published mean levels in an uncontaminated population in Sweden. In high excess were Ca, Mg, Sr, Al, Bi and Hg. Of these only Hg can be considered as a possible cause of congenital anomaly. Mean levels for Uranium were 0.16 ppm (SD: 0.11) range 0.02 to 0.4, higher in mothers (0.18 ppm SD 0.09) than fathers (0.11 ppm; SD 0.13). The highly unusual non-normal Fallujah distribution mean was significantly higher than literature results for a control population Southern Israel (0.062 ppm) and a non-parametric test (Mann Whitney-Wilcoxon) gave p = 0.016 for this comparison of the distribution. Mean levels in Fallujah were also much higher than the mean of measurements reported from Japan, Brazil, Sweden and Slovenia (0.04 ppm SD 0.02). Soil samples show low concentrations with a mean of 0.76 ppm (SD 0.42) and range 0.1-1.5 ppm; (N = 18). However it may be consistent with levels in drinking water (2.28 μgL-1) which had similar levels to water from wells (2.72 μgL-1) and the river Euphrates (2.24 μgL-1). In a separate study of a sub group of mothers with long hair to investigate historic Uranium excretion the results suggested that levels were much higher in the past. Uranium traces detected in the soil samples and the hair showed slightly enriched isotopic signatures for hair U238/U235 = (135.16 SD 1.45) compared with the natural ratio of 137.88. Soil sample Uranium isotope ratios were determined after extraction and concentration of the Uranium by ion exchange. Results showed statistically significant presence of enriched Uranium with a mean of 129 with SD5.9 (for this determination, the natural Uranium 95% CI was 132.1 < Ratio < 144.1). Conclusions Whilst caution must be exercised about ruling out other possibilities, because none of the elements found in excess are reported to cause congenital diseases and cancer except Uranium, these findings suggest the enriched Uranium exposure is either a primary cause or related to the cause of the congenital anomaly and cancer increases. Questions are thus raised about the characteristics and composition of weapons now being deployed in modern battlefields PMID:21888647

An alternative for cost-effective remediation of depleted uranium (DU) at certain environmental restoration sites.

PubMed

Miller, M; Galloway, B; VanDerpoel, G; Johnson, E; Copland, J; Salazar, M

2000-02-01

Numerous sites in the United States and around the world are contaminated with depleted uranium (DU) in various forms. A prevalent form is fragmented DU originating from various scientific tests involving high explosives and DU during weapon development programs, at firing practice ranges, or war theaters where DU was used in armor-piercing projectiles. The contamination at these sites is typically very heterogeneous, with discreet, visually identifiable DU fragments mixed with native soil. That is, the bulk-averaged DU activity is quite low, while specific DU fragments, which are distinct from the soil matrix, have much higher specific activity. DU is best known as a dark, black metal that is nearly twice as dense as lead, but DU in the environment readily weathers (oxidizes) to a distinctive bright yellow color that is readily visible. While the specific activity (amount of radioactivity per mass of soil) of DU is relatively low and presents only a minor radiological hazard, the fact that it is radioactive and visually identifiable makes it desirable to remove the DU "contamination" from the environment. The typical approach to conducting this DU remediation is to use radiation detection instruments to identify the contaminant and separate it from the adjacent soil, packaging it for disposal as radioactive waste. This process can be performed manually or by specialized, automated equipment. Alternatively, in certain situations a more cost-effective approach might be simple mechanical or gravimetric separation of the DU fragments from the host soil matrix. At SNL/NM, both the automated and simple mechanical approaches have recently been employed. This paper discusses the pros/cons of the two approaches.

Temporary vs. Permanent Sub-slab Ports: A Comparative Performance Study

EPA Science Inventory

Vapor intrusion (VI) is the migration of subsurface vapors, including radon and volatile organic compounds (VOCs), from the subsurface to indoor air. The VI exposure pathway extends from the contaminant source, which can be impacted soil, non-aqueous phase liquid, or contaminated...

Radionuclide Migration through Sediment and Concrete: 16 Years of Investigations

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

Golovich, Elizabeth C.; Mattigod, Shas V.; Snyder, Michelle MV

The Waste Management Project provides safe, compliant, and cost-effective waste management services for the Hanford Site and the U.S. Department of Energy (DOE) complex. Part of these services includes safe disposal of low-level waste and mixed low-level waste at the Hanford Low-Level Waste Burial Grounds in accordance with the requirements of DOE Order 435.1, Radioactive Waste Management. To partially satisfy these requirements, performance assessment analyses were completed and approved. DOE Order 435.1 also requires continuing data collection to increase confidence in the critical assumptions used in these analyses to characterize the operational features of the disposal facility that are reliedmore » on to satisfy the performance objectives identified in the order. Cement-based solidification and stabilization is considered for hazardous waste disposal because it is easily done and cost-efficient. One critical assumption is that concrete will be used as a waste form or container material at the Hanford Site to control and minimize the release of radionuclide constituents in waste into the surrounding environment. Concrete encasement would contain and isolate the waste packages from the hydrologic environment and act as an intrusion barrier. Any failure of concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. The radionuclides iodine-129, selenium-75, technetium-99, and uranium-238 have been identified as long-term dose contributors (Mann et al. 2001; Wood et al. 1995). Because of their anionic nature in aqueous solutions, these constituents of potential concern may be released from the encased concrete by mass flow and/or diffusion and migrate into the surrounding subsurface environment (Serne et al. 1989; 1992; 1993a, b; 1995). Therefore, it is necessary to assess the performance of the concrete encasement structure and the ability of the surrounding soil to retard radionuclide migration. Each of the test methods performed throughout the lifetime of the project has focused on different aspects of the concrete waste form weathering process. Diffusion of different analytes [technetium-99 (Tc-99), iodine-125 (I-125), stable iodine (I), uranium (U), and rhenium (Re)] has been quantified from experiments under both saturated and unsaturated conditions. The water-saturated conditions provide a conservative estimate of the concrete’s performance in situ, and the unsaturated conditions provide a more accurate estimate of the diffusion of contaminants from the concrete.« less

SULFATE REDUCTION IN GROUNDWATER: CHARACTERIZATION AND APPLICATIONS FOR REMEDIATION

PubMed Central

Miao, Z.; Brusseau, M. L.; Carroll, K. C.; Carreón-Diazconti, C.; Johnson, B.

2013-01-01

Sulfate is ubiquitous in groundwater, with both natural and anthropogenic sources. Sulfate reduction reactions play a significant role in mediating redox conditions and biogeochemical processes for subsurface systems. They also serve as the basis for innovative in-situ methods for groundwater remediation. An overview of sulfate reduction in subsurface environments is provided, along with a brief discussion of characterization methods and applications for addressing acid mine drainage. We then focus on two innovative, in-situ methods for remediating sulfate-contaminated groundwater, the use of zero-valent iron (ZVI) and the addition of electron-donor substrates. The advantages and limitations associated with the methods are discussed, with examples of prior applications. PMID:21947714

Adsorption and Retardation of PFASs in Soil

NASA Astrophysics Data System (ADS)

Chen, W.; Yan, N.; Fu, X.; Carroll, K. C.; Holguin, F. O. O.; Brusseau, M. L.

2017-12-01

Per- and poly-fluorinated alkyl substances (PFASs) are emerging contaminants of concern that are present in the subsurface at numerous military and industrial facilities. Knowledge of the retention behavior of these compounds in the subsurface environment is critical for effective risk characterization and remediation. The objective of this research is to investigate the role of adsorption at the air-water interface on PFAS retention in vadose-zone systems. Surface tensions were measured for select PFAS to determine interfacial adsorption coefficients. Column experiments were conducted to characterize retardation and transport under saturated and unsaturated flow conditions. The impact of soil properties and groundwater constituents on surface tension, solid-phase adsorption, and interfacial adsorption was investigated.

Calixarene cleansing formulation for uranium skin contamination.

PubMed

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

2013-10-01

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

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

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

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

2013-06-01

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

JPRS Report, Environmental Issues

DTIC Science & Technology

1990-10-12

IZVESTIYA 18 Sep] 33 UN Mission To Study Chernobyl Effects [TASS 19 Sep] 33 Rumors of’Crack’in Chernobyl Sarcophagus Rebutted [PRAVDA 18...Sep] 33 Russian Parliament Sets Up Chernobyl Committee [TASS 19 Sep] 34 Uranium Wastes Said Contaminating Kirovograd [Moscow TV 18 Sep] 35...following the Chernobyl disaster. The find- ings make it possible to reach conclusions about Cher- nobyl’s impact on the environment in those regions. The

ENVIRONMENTAL IMPACTS AND MONITORING: A HISTORICAL PERSPECTIVE ON THE USE OF NATURAL ATTENUATION FOR SUBSURFACE REMEDIATION

EPA Science Inventory

The collective processes that constitute the broadly used term Anatural attenuation,@ as it relates to subsurface remediation of contaminants, refer to the physical, chemical, and biological interactions that, without human intervention, reduce or contain contaminants in the sub...

Contamination and restoration of groundwater aquifers.

PubMed Central

Piver, W T

1993-01-01

Humans are exposed to chemicals in contaminated groundwaters that are used as sources of drinking water. Chemicals contaminate groundwater resources as a result of waste disposal methods for toxic chemicals, overuse of agricultural chemicals, and leakage of chemicals into the subsurface from buried tanks used to hold fluid chemicals and fuels. In the process, both the solid portions of the subsurface and the groundwaters that flow through these porous structures have become contaminated. Restoring these aquifers and minimizing human exposure to the parent chemicals and their degradation products will require the identification of suitable biomarkers of human exposure; better understandings of how exposure can be related to disease outcome; better understandings of mechanisms of transport of pollutants in the heterogeneous structures of the subsurface; and field testing and evaluation of methods proposed to restore and cleanup contaminated aquifers. In this review, progress in these many different but related activities is presented. PMID:8354172

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

USGS Publications Warehouse

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

2010-01-01

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

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

Phytoremediation removal rates of benzene, toluene, and chlorobenzene.

PubMed

Limmer, Matt A; Wilson, Jordan; Westenberg, David; Lee, Amy; Siegman, Mark; Burken, Joel G

2018-06-07

Phytoremediation is a sustainable remedial approach, although performance efficacy is rarely reported. In this study, we assessed a phytoremediation plot treating benzene, toluene, and chlorobenzene. A comparison of the calculated phytoremediation removal rate with estimates of onsite contaminant mass was used to forecast cleanup periods. The investigation demonstrated that substantial microbial degradation was occurring in the subsurface. Estimates of transpiration indicated that the trees planted were removing approximately 240,000 L of water per year. This large quantity of water removal implies substantial removal of contaminant due to large amounts of contaminants in the groundwater; however, these contaminants extensively sorb to the soil, resulting in large quantities of contaminant mass in the subsurface. The total estimate of subsurface contaminant mass was also complicated by the presence of non-aqueous phase liquids (NAPL), additional contaminant masses that were difficult to quantify. These uncertainties of initial contaminant mass at the site result in large uncertainty in the cleanup period, although mean estimates are on the order of decades. Collectively, the model indicates contaminant removal rates on the order of 10 -2 -10 0 kg/tree/year. The benefit of the phytoremediation system is relatively sustainable cleanup over the long periods necessary due to the presence of NAPL.

Evaluating Potential Exposures to Ecological Receptors Due to Transport of Hydrophobic Organic Contaminants in Subsurface Systems (Final Report)

EPA Science Inventory

EPA's Ecological Risk Assessment Support Center (ERASC) announced the release of the final report, Evaluating Potential Exposures to Ecological Receptors Due to Transport of Hydrophobic Organic Contaminants in Subsurface Systems. This technical paper recommends several ty...

SPECIATION OF SUBSURFACE CONTAMINANTS BY CONE PENETROMETRY GAS CHROMATOGRAPHY/MASS SPECTROMETRY. (R826184)

EPA Science Inventory

A thermal extraction cone penetrometry gas chroma tography/mass spectrometry system (TECP GC/MS) has been developed to detect subsurface contaminants in situ. The TECP can collect soil-bound organics up to depths of 30 m. In contrast to traditional cone penetrometer sample collec...

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

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

B.D. Wood

2007-01-01

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

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

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

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

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

PubMed

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

2015-12-01

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

FY90 R&D Project Descriptions ESL (Engineering & Services Laboratory) Environics Division

DTIC Science & Technology

1989-07-01

and Development Support for Subsurface Monitoring Technology 15 19007048 Pumping and Purging Contaminants 16 19007049 Methods for Selecting In Situ...Decontamination 40 3788VW17 Treatment of Chlorinated Organics with Aboveground Bioreactors 41 3788VW18 Improved Methods for Monitoring Fuel Biodegradation 42 2...Fluoride (HF) Dispersion Model 63 21036093 Solvent Capacity Field Test Method 64 21037097 Volatile Organic Compound (VOC) Control Technology 65 21037102

Improving surface-subsurface water budgeting for Brownfield study sites using high resolution satellite imagery

NASA Astrophysics Data System (ADS)

Dujardin, J.; Boel, S.; Anibas, C.; Batelaan, O.; Canters, F.

2009-04-01

Countries around the world have problems with contaminated brownfield sites as resulting from a relatively anarchic economical and industrial development during the 19th and 20th centuries. Since a few decades policy makers and stakeholders have become more aware of the risk posed by these sites because some of these sites present direct public hazards. Water is often the main vector of the mobility of contaminants. In order to propose remediation measures for the contaminated sites, it is required to describe and to quantify as accurately as possible the surface and subsurface water fluxes in the polluted site. In this research a modelling approach with integrated remote sensing analysis has been developed for accurately calculating water and contaminant fluxes on the polluted sites. Groundwater pollution in urban environments is linked to patterns of land use, so to identify the sources of contamination with great accuracy in urban environments it is essential to characterize the land cover in a detailed way. The use of high resolution spatial information is required because of the complexity of the urban land use. An object-oriented classification approach applied on high resolution satellite data has been adopted. Cluster separability analysis and visual interpretation of the image objects belonging to each cluster resulted in the selection of 8 land-cover categories (water, bare soil, meadow, mixed forest, grey urban surfaces, red roofs, bright roofs and shadow).To assign the image objects to one of the 8 selected classes a multiple layer perceptron (MLP) approach was adopted, using the NeuralWorks Predict software. After a post-classification shadow removal and a rule-based classification enhancement a kappa-value of 0.86 was obtained. Once the land cover was characterized, the groundwater recharge has been simulated using the spatially distributed WetSpass model and the subsurface water flow was simulated with GMS 6.0 in order to identify and budget the water fluxes on the brownfield. The obtained land use map shows to have a strong impact on the groundwater recharge, resulting in a high spatial variability. Simulated groundwater fluxes from brownfield to a receiving river where independently verified by measurements and simulation of groundwater-surface water interaction based on thermal gradients in the river bed. It is concluded that in order to better quantify total fluxes of contaminants from brownfields in the groundwater, remote sensing imagery can be operationally integrated in a modelling procedure. The developed methodology is applied to a case site in Vilvoorde, Brussels (Belgium).

PROCESS FOR SEGREGATING URANIUM FROM PLUTONIUM AND FISSION-PRODUCT CONTAMINATION

DOEpatents

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

1961-06-27

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

Radiochronological Age of a Uranium Metal Sample from an Abandoned Facility

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

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

2012-03-16

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

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

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

Not Available

2011-06-22

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

Health effects of uranium: new research findings.

PubMed

Brugge, Doug; Buchner, Virginia

2011-01-01

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

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

PubMed

Lee, Minhee; Yang, Minjune

2010-01-15

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

SOLVENT EXTRACTION PROCESS FOR URANIUM RECOVERY

DOEpatents

Clark, H.M.; Duffey, D.

1958-06-17

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

User’s guide to the collection and analysis of tree cores to assess the distribution of subsurface volatile organic compounds

USGS Publications Warehouse

Vroblesky, Don A.

2008-01-01

Analysis of the volatile organic compound content of tree cores is an inexpensive, rapid, simple approach to examining the distribution of subsurface volatile organic compound contaminants. The method has been shown to detect several volatile petroleum hydrocarbons and chlorinated aliphatic compounds associated with vapor intrusion and ground-water contamination. Tree cores, which are approximately 3 inches long, are obtained by using an increment borer. The cores are placed in vials and sealed. After a period of equilibration, the cores can be analyzed by headspace analysis gas chromatography. Because the roots are exposed to volatile organic compound contamination in the unsaturated zone or shallow ground water, the volatile organic compound concentrations in the tree cores are an indication of the presence of subsurface volatile organic compound contamination. Thus, tree coring can be used to detect and map subsurface volatile organic compound contamination. For comparison of tree-core data at a particular site, it is important to maintain consistent methods for all aspects of tree-core collection, handling, and analysis. Factors affecting the volatile organic compound concentrations in tree cores include the type of volatile organic compound, the tree species, the rooting depth, ground-water chemistry, the depth to the contaminated horizon, concentration differences around the trunk related to variations in the distribution of subsurface volatile organic compounds, concentration differences with depth of coring related to volatilization loss through the bark and possibly other unknown factors, dilution by rain, seasonal influences, sorption, vapor-exchange rates, and within-tree volatile organic compound degradation.

Radioactivity in Virgin Soils and Soils from Some Areas with Closed Uranium Mining Facilities in Bulgaria

NASA Astrophysics Data System (ADS)

Yordanova, I.; Staneva, D.; Misheva, L.; Bineva, Ts.; Banov, M.

2012-04-01

The soil radioecology is an important part of the environmental research in the country. Since the beginning of the 1970's regular monitoring of the content of different radionuclides in Bulgarian soils has been done. Objective of the studies were virgin soils from high mountain areas, hills and plains (the region of Kozloduy NPP and the Danube river valley). Natural and men-made radionuclides were observed. In the 25-year period after the the contamination with radionuclides due to the 1986 Chernobyl NPP accident a rich data base has been collected, recording the radiation status of the soils in Bulgaria. Special attention has been paid to the contamination with the long-lived technogenic radionuclides caesium-137 and strontium-90. This paper presents a summary of the obtained results. Caesium-137 and strontium-90 were the main men-made radionuclides detected in the examined Bulgarian soils few years after the Chernobyl NPP accident. Their content in the soils from high mountain areas (Rodopa and Rila mountains) is several times higher than that in the soils from North Bulgaria and Sofia fields. High non-homogenity in the pollution within small areas (even as small as several square meters) has been observed. Natural radioactivity was also studied. Averaged values for natural radionuclides like uranium-238, thorium-232, and radium-226 in virgin soils from different areas in the country are presented. A comparison of the dynamics of their behavior throughout the years is done. Bulgaria is a country with intensive uranium mining activities in the past years. That is why radiological monitoring of closed uranium mining facilities in different regions of the country are obligatory and of great interest. This work presents results from such investigations made in regions where remediation has been done. The results have been evaluated according to the Bulgarian radionuclide environment contamination legislation. The necessity of permanent environmental monitoring is assessed.

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

PubMed

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

2010-05-01

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

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

PubMed Central

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

2010-01-01

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

Armored Enzyme Nanoparticles for Remediation of Subsurface Contaminants

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

Jonathan S. Dordick; Jay Grate; Jungbae Kim

2007-02-19

The remediation of subsurface contaminants is a critical problem for the Department of Energy, other government agencies, and our nation. Severe contamination of soil and groundwater exists at several DOE sites due to various methods of intentional and unintentional release. Given the difficulties involved in conventional removal or separation processes, it is vital to develop methods to transform contaminants and contaminated earth/water to reduce risks to human health and the environment. Transformation of the contaminants themselves may involve conversion to other immobile species that do not migrate into well water or surface waters, as is proposed for metals and radionuclides;more » or degradation to harmless molecules, as is desired for organic contaminants. Transformation of contaminated earth (as opposed to the contaminants themselves) may entail reductions in volume or release of bound contaminants for remediation. Research at Rensselaer focused on the development of haloalkane dehalogenase as a critical enzyme in the dehalogenation of contaminated materials (ultimately trichloroethylene and related pollutants). A combination of bioinformatic investigation and experimental work was performed. The bioinformatics was focused on identifying a range of dehalogenase enzymes that could be obtained from the known proteomes of major microorganisms. This work identified several candidate enzymes that could be obtained through relatively straightforward gene cloning and expression approaches. The experimental work focused on the isolation of haloalkane dehalogenase from a Xanthobacter species followed by incorporating the enzyme into silicates to form biocatalytic silicates. These are the precursors of SENs. At the conclusion of the study, dehalogenase was incorporated into SENs, although the loading was low. This work supported a single Ph.D. student (Ms. Philippa Reeder) for two years. The project ended prior to her being able to perform substantive bioinformatics efforts that would identify more promising dehalogenase enzymes. The SEN synthesis, however, was demonstrated to be partially successful with dehalogenases. Further work would provide optimized dehalogenases in SENs for use in pollution remission.« less

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

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

Frederick, Bill; Tandon, Vikas

2013-07-01

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

40 CFR 192.10 - Applicability.

Code of Federal Regulations, 2013 CFR

2013-07-01

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

40 CFR 192.10 - Applicability.

Code of Federal Regulations, 2014 CFR

2014-07-01

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

Uranium Mines and Mills | RadTown USA | US EPA

EPA Pesticide Factsheets

2017-08-07

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

Selective Phylogenetic Analysis Targeted at 16S rRNA Genes of Thermophiles and Hyperthermophiles in Deep-Subsurface Geothermal Environments

PubMed Central

Kimura, Hiroyuki; Sugihara, Maki; Kato, Kenji; Hanada, Satoshi

2006-01-01

Deep-subsurface samples obtained by deep drilling are likely to be contaminated with mesophilic microorganisms in the drilling fluid, and this could affect determination of the community structure of the geothermal microflora using 16S rRNA gene clone library analysis. To eliminate possible contamination by PCR-amplified 16S rRNA genes from mesophiles, a combined thermal denaturation and enzyme digestion method, based on a strong correlation between the G+C content of the 16S rRNA gene and the optimum growth temperatures of most known prokaryotic cultures, was used prior to clone library construction. To validate this technique, hot spring fluid (76°C) and river water (14°C) were used to mimic a deep-subsurface sample contaminated with drilling fluid. After DNA extraction and PCR amplification of the 16S rRNA genes from individual samples separately, the amplified products from river water were observed to be denatured at 82°C and completely digested by exonuclease I (Exo I), while the amplified products from hot spring fluid remained intact after denaturation at 84°C and enzyme digestion with Exo I. DNAs extracted from the two samples were mixed and used as a template for amplification of the 16S rRNA genes. The amplified rRNA genes were denatured at 84°C and digested with Exo I before clone library construction. The results indicated that the 16S rRNA gene sequences from the river water were almost completely eliminated, whereas those from the hot spring fluid remained. PMID:16391020

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

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

Not Available

1980-09-30

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

Impact of Scale-Dependent Coupled Processes on Solute Fate and Transport in the Critical Zone: Case Studies Involving Inorganic and Radioactive Contaminants

NASA Astrophysics Data System (ADS)

Jardine, P. M.; Gentry, R. W.

2011-12-01

Soil, the thin veneer of matter covering the Earths surface that supports a web of living diversity, is often abused through anthropogenic inputs of toxic waste. This subsurface regime, coupled with life sustaining surface water and groundwater is known as the "Critical Zone". The disposal of radioactive and toxic organic and inorganic waste generated by industry and various government agencies has historically involved shallow land burial or the use of surface impoundments in unsaturated soils and sediments. Presently, contaminated sites have been closing rapidly and many remediation strategies have chosen to leave contaminants in-place. As such, contaminants will continue to interact with the geosphere and investigations on long term changes and interactive processes is imperative to verify risks. In this presentation we provide a snap-shot of subsurface science research from the past 25 y that seeks to provide an improved understanding and predictive capability of multi-scale contaminant fate and transport processes in heterogeneous unsaturated and saturated environments. Investigations focus on coupled hydrological, geochemical, and microbial processes that control reactive contaminant transport and that involve multi-scale fundamental research ranging from the molecular scale (e.g. synchrotrons, electron sources, arrays) to in situ plume interrogation strategies at the macroscopic scale (e.g. geophysics, field biostimulation, coupled processes monitoring). We show how this fundamental research is used to provide multi-process, multi-scale predictive monitoring and modeling tools that can be used at contaminated sites to (1) inform and improve the technical basis for decision making, and (2) assess which sites are amenable to natural attenuation and which would benefit from source zone remedial intervention.

PROCESS OF PURIFYING URANIUM

DOEpatents

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

1958-12-23

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

REMOVAL OF URANIUM FROM DRINKING WATER BY CONVENTIONAL TREATMENT METHODS

EPA Science Inventory

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

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

PubMed

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

2013-01-01

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

Mapping Site Remediation with Electrical Resistivity Tomography Explored via Coupled-Model Simulations

NASA Astrophysics Data System (ADS)

Power, C.; Gerhard, J. I.; Tsourlos, P.; Giannopoulos, A.

2011-12-01

Remediation programs for sites contaminated with dense non-aqueous phase liquids (DNAPLs) would benefit from an ability to non-intrusively map the evolving volume and extent of the DNAPL source zone. Electrical resistivity tomography (ERT) is a well-established geophysical tool, widely used outside the remediation industry, that has significant potential for mapping DNAPL source zones. However, that potential has not been realized due to challenges in data interpretation from contaminated sites - in either a qualitative or quantitative way. The objective of this study is to evaluate the potential of ERT to map realistic, evolving DNAPL source zones within complex subsurface environments during remedial efforts. For this purpose, a novel coupled model was developed that integrates a multiphase flow model (DNAPL3D-MT), which generates realistic DNAPL release scenarios, with 3DINV, an ERT model which calculates the corresponding resistivity response. This presentation will describe the developed model coupling methodology, which integrates published petrophysical relationships to generate an electrical resistivity field that accounts for both the spatial heterogeneity of subsurface soils and the evolving spatial distribution of fluids (including permeability, porosity, clay content and air/water/DNAPL saturation). It will also present an example in which the coupled model was employed to explore the ability of ERT to track the remediation of a DNAPL source zone. A field-scale, three-dimensional release of chlorinated solvent DNAPL into heterogeneous clayey sand was simulated, including the subsurface migration and subsequent removal of the DNAPL source zone via dissolution in groundwater. Periodic surveys of this site via ERT applied at the surface were then simulated and inversion programs were used to calculate the subsurface distribution of electrical properties. This presentation will summarize this approach and its potential as a research tool exploring the range of site conditions under which ERT may prove useful in aiding DNAPL site remediation. Moreover, it is expected to provide a cost-effective avenue to test optimum ERT data acquisition, inversion and interpretative tools at contaminated sites.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Microbial biogeochemistry of uranium mill tailings

USGS Publications Warehouse

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.

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

PubMed

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

2016-08-22

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

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

USGS Publications Warehouse

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

2011-01-01

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

Oxidative particle mixtures for groundwater treatment

DOEpatents

Siegrist, Robert L.; Murdoch, Lawrence C.

2000-01-01

The invention is a method and a composition of a mixture for degradation and immobilization of contaminants in soil and groundwater. The oxidative particle mixture and method includes providing a material having a minimal volume of free water, mixing at least one inorganic oxidative chemical in a granular form with a carrier fluid containing a fine grained inorganic hydrophilic compound and injecting the resulting mixture into the subsurface. The granular form of the inorganic oxidative chemical dissolves within the areas of injection, and the oxidative ions move by diffusion and/or advection, therefore extending the treatment zone over a wider area than the injection area. The organic contaminants in the soil and groundwater are degraded by the oxidative ions, which form solid byproducts that can sorb significant amounts of inorganic contaminants, metals, and radionuclides for in situ treatment and immobilization of contaminants. The method and composition of the oxidative particle mixture for long-term treatment and immobilization of contaminants in soil and groundwater provides for a reduction in toxicity of contaminants in a subsurface area of contamination without the need for continued injection of treatment material, or for movement of the contaminants, or without the need for continuous pumping of groundwater through the treatment zone, or removal of groundwater from the subsurface area of contamination.

Molecular Analysis of the In Situ Growth Rates of Subsurface Geobacter Species

PubMed Central

Giloteaux, Ludovic; Barlett, Melissa; Chavan, Milind A.; Smith, Jessica A.; Williams, Kenneth H.; Wilkins, Michael; Long, Philip; Lovley, Derek R.

2013-01-01

Molecular tools that can provide an estimate of the in situ growth rate of Geobacter species could improve understanding of dissimilatory metal reduction in a diversity of environments. Whole-genome microarray analyses of a subsurface isolate of Geobacter uraniireducens, grown under a variety of conditions, identified a number of genes that are differentially expressed at different specific growth rates. Expression of two genes encoding ribosomal proteins, rpsC and rplL, was further evaluated with quantitative reverse transcription-PCR (qRT-PCR) in cells with doubling times ranging from 6.56 h to 89.28 h. Transcript abundance of rpsC correlated best (r2 = 0.90) with specific growth rates. Therefore, expression patterns of rpsC were used to estimate specific growth rates of Geobacter species during an in situ uranium bioremediation field experiment in which acetate was added to the groundwater to promote dissimilatory metal reduction. Initially, increased availability of acetate in the groundwater resulted in higher expression of Geobacter rpsC, and the increase in the number of Geobacter cells estimated with fluorescent in situ hybridization compared well with specific growth rates estimated from levels of in situ rpsC expression. However, in later phases, cell number increases were substantially lower than predicted from rpsC transcript abundance. This change coincided with a bloom of protozoa and increased attachment of Geobacter species to solid phases. These results suggest that monitoring rpsC expression may better reflect the actual rate that Geobacter species are metabolizing and growing during in situ uranium bioremediation than changes in cell abundance. PMID:23275510

Predicting subsurface uranium transport: Mechanistic modeling constrained by experimental data

NASA Astrophysics Data System (ADS)

Ottman, Michael; Schenkeveld, Walter D. C.; Kraemer, Stephan

2017-04-01

Depleted uranium (DU) munitions and their widespread use throughout conflict zones around the world pose a persistent health threat to the inhabitants of those areas long after the conclusion of active combat. However, little emphasis has been put on developing a comprehensive, quantitative tool for use in remediation and hazard avoidance planning in a wide range of environments. In this context, we report experimental data on U interaction with soils and sediments. Here, we strive to improve existing risk assessment modeling paradigms by incorporating a variety of experimental data into a mechanistic U transport model for subsurface environments. 20 different soils and sediments from a variety of environments were chosen to represent a range of geochemical parameters that are relevant to U transport. The parameters included pH, organic matter content, CaCO3, Fe content and speciation, and clay content. pH ranged from 3 to 10, organic matter content from 6 to 120 g kg-1, CaCO3 from 0 to 700 g kg-1, amorphous Fe content from 0.3 to 6 g kg-1 and clay content from 4 to 580 g kg-1. Sorption experiments were then performed, and linear isotherms were constructed. Sorption experiment results show that among separate sets of sediments and soils, there is an inverse correlation between both soil pH and CaCO¬3 concentration relative to U sorptive affinity. The geological materials with the highest and lowest sorptive affinities for U differed in CaCO3 and organic matter concentrations, as well as clay content and pH. In a further step, we are testing if transport behavior in saturated porous media can be predicted based on adsorption isotherms and generic geochemical parameters, and comparing these modeling predictions with the results from column experiments. The comparison of these two data sets will examine if U transport can be effectively predicted from reactive transport modeling that incorporates the generic geochemical parameters. This work will serve to show whether a more mechanistic approach offers an improvement over statistical regression-based risk assessment models.

Impact of mercury on denitrification and denitrifying microbial communities in nitrate enrichments of subsurface sediments.

PubMed

Wang, Yanping; Wiatrowski, Heather A; John, Ria; Lin, Chu-Ching; Young, Lily Y; Kerkhof, Lee J; Yee, Nathan; Barkay, Tamar

2013-02-01

The contamination of groundwater with mercury (Hg) is an increasing problem worldwide. Yet, little is known about the interactions of Hg with microorganisms and their processes in subsurface environments. We tested the impact of Hg on denitrification in nitrate reducing enrichment cultures derived from subsurface sediments from the Oak Ridge Integrated Field Research Challenge site, where nitrate is a major contaminant and where bioremediation efforts are in progress. We observed an inverse relationship between Hg concentrations and onset and rates of denitrification in nitrate enrichment cultures containing between 53 and 1.1 μM of inorganic Hg; higher Hg concentrations increasingly extended the time to onset of denitrification and inhibited denitrification rates. Microbial community complexity, as indicated by terminal restriction fragment length polymorphism (tRFLP) analysis of the 16S rRNA genes, declined with increasing Hg concentrations; at the 312 nM Hg treatment, a single tRFLP peak was detected representing a culture of Bradyrhizobium sp. that possessed the merA gene indicating a potential for Hg reduction. A culture identified as Bradyrhizobium sp. strain FRC01 with an identical 16S rRNA sequence to that of the enriched peak in the tRFLP patterns, reduced Hg(II) to Hg(0) and carried merA whose amino acid sequence has 97 % identity to merA from the Proteobacteria and Firmicutes. This study demonstrates that in subsurface sediment incubations, Hg may inhibit denitrification and that inhibition may be alleviated when Hg resistant denitrifying Bradyrhizobium spp. detoxify Hg by its reduction to the volatile elemental form.

Improving surface-subsurface water budgeting using high resolution satellite imagery applied on a brownfield.

PubMed

Dujardin, J; Batelaan, O; Canters, F; Boel, S; Anibas, C; Bronders, J

2011-01-15

The estimation of surface-subsurface water interactions is complex and highly variable in space and time. It is even more complex when it has to be estimated in urban areas, because of the complex patterns of the land-cover in these areas. In this research a modeling approach with integrated remote sensing analysis has been developed for estimating water fluxes in urban environments. The methodology was developed with the aim to simulate fluxes of contaminants from polluted sites. Groundwater pollution in urban environments is linked to patterns of land use and hence it is essential to characterize the land cover in a detail. An object-oriented classification approach applied on high-resolution satellite data has been adopted. To assign the image objects to one of the land-cover classes a multiple layer perceptron approach was adopted (Kappa of 0.86). Groundwater recharge has been simulated using the spatially distributed WetSpass model and the subsurface water flow using MODFLOW in order to identify and budget water fluxes. The developed methodology is applied to a brownfield case site in Vilvoorde, Brussels (Belgium). The obtained land use map has a strong impact on the groundwater recharge, resulting in a high spatial variability. Simulated groundwater fluxes from brownfield to the receiving River Zenne were independently verified by measurements and simulation of groundwater-surface water interaction based on thermal gradients in the river bed. It is concluded that in order to better quantify total fluxes of contaminants from brownfields in the groundwater, remote sensing imagery can be operationally integrated in a modeling procedure. Copyright © 2010 Elsevier B.V. All rights reserved.

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

DOE PAGES

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

2015-09-18

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

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

PubMed Central

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

2015-01-01

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

A STUDY TO DETERMINE THE FEASIBILITY OF USING A GROUND-PENETRATING RADAR FOR MORE EFFECTIVE REMEDIATION OF SUBSURFACE CONTAMINATION

EPA Science Inventory

A study was conducted (1) to assess the capability of groundpenetrating radar (GPR) to identify natural subsurface features, detect man-made objects burled in the soil, and both detect and define the extent of contaminated soil or ground water due to a toxic spill, and (2) to det...

Actinide removal from spent salts

DOEpatents

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

2002-01-01

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

A comprehensive inventory of radiological and nonradiological contaminants in waste buried or projected to be buried in the subsurface disposal area of the INEL RWMC during the years 1984-2003, Volume 3

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

NONE

1995-05-01

This is the third volume of this comprehensive report of the inventory of radiological and nonradiological contaminants in waste buried or projected to be buried in the subsurface disposal area of the Idaho National Engineering Laboratory. Appendix B contains a complete printout of contaminant inventory and other information from the CIDRA Database and is presented in volumes 2 and 3 of the report.

Assessment of calcium addition on the removal of U(VI) in the alkaline conditions created by NH 3 gas

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

Assessment of calcium addition on the removal of U(VI) in the alkaline conditions created by NH 3 gas

DOE PAGES

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

Radionuclide Concentrations in Terrestrial Vegetation and Soil Samples On and Around the Hanford Site, 1971 Through 2008

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

Simmons, Mary Ann; Poston, Ted M.; Fritz, Brad G.

2011-07-29

Environmental monitoring is conducted on the U.S. Department of Energy (DOE) Hanford Site to comply with DOE Orders and federal and state regulations. Major objectives of the monitoring are to characterize contaminant levels in the environment and to determine site contributions to the contaminant inventory. This report focuses on surface soil and perennial vegetation samples collected between 1971 and 2008 as part of the Pacific Northwest National Laboratory Surface Environmental Surveillance Project performed under contract to DOE. Areas sampled under this program are located on the Hanford Site but outside facility boundaries and on public lands surrounding the Hanford Site.more » Additional samples were collected during the past 8 years under DOE projects that evaluated parcels of land for radiological release. These data were included because the same sampling methodology and analytical laboratory were used for the projects. The spatial and temporal trends of six radionuclides collected over a 38-year period were evaluated. The radionuclides----cobalt-60, cesium-137, strontium-90, plutonium-238, plutonium-239/240, and uranium (reported either as uranium-238 or total uranium)----were selected because they persist in the environment and are still being monitored routinely and reported in Hanford Site environmental reports. All these radionuclides were associated with plutonium production and waste management of activities occurring on the site. Other sources include fallout from atmospheric testing of nuclear weapons, which ended in 1980, and the Chernobyl explosion in 1986. Uranium is also a natural component of the soil. This assessment of soil and vegetation data provides important information on the distribution of radionuclides in areas adjacent to industrial areas, established perimeter locations and buffer areas, and more offsite nearby and distant locations. The concentrations reflect a tendency for detection of some radionuclides close to where they were utilized onsite, but as one moves to unindustrialized areas on the site, surrounding buffer areas and perimeter location into the more distant sites, concentrations of these radionuclides approach background and cannot be distinguished from fallout activity. More importantly, concentrations in soil and vegetation samples did not exceed environmental benchmark concentrations, and associated exposure to human and ecological receptors were well below levels that are demonstratively hazardous to human health and the environment.« less

Final Technical Report: Viral Infection of Subsurface Microorganisms and Metal/Radionuclide Transport

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

Weber, Karrie A.; Bender, Kelly S.; Li, Yusong

Microbially mediated metabolisms have been identified as a significant factor either directly or indirectly impacting the fate and transport of heavy metal/radionuclide contaminants. To date microorganisms have been isolated from contaminated environments. Examination of annotated finished genome sequences of many of these subsurface isolates from DOE sites, revealed evidence of prior viral infection. To date the role that viruses play influencing microbial mortality and the resulting community structure which directly influences biogeochemical cycling in soils and sedimentary environments remains poorly understood. The objective of this exploratory study was to investigate the role of viral infection of subsurface bacteria and themore » formation of contaminant-bearing viral particles. This objective was approached by examining the following working hypotheses: (i) subsurface microorganisms are susceptible to viral infections by the indigenous subsurface viral community, and (ii) viral surfaces will adsorb heavy metals and radionuclides. Our results have addressed basic research needed to accomplish the BER Long Term Measure to provide sufficient scientific understanding such that DOE sites would be able to incorporate coupled physical, chemical and biological processes into decision making for environmental remediation or natural attenuation and long-term stewardship by establishing viral-microbial relationships on the subsequent fate and transport of heavy metals and radionuclides. Here we demonstrated that viruses play a significant role in microbial mortality and community structure in terrestrial subsurface sedimentary systems. The production of viral-like particles within subsurface sediments in response to biostimulation with dissolved organic carbon and a terminal electron acceptor resulted in the production of viral-like particles. Organic carbon alone did not result in significant viral production and required the addition of a terminal electron acceptor (nitrate), indicating that nutrients are not limiting viral production, but rather substrates that can be converted into energy for host metabolism. Our results also revealed that cell abundance was not correlated to the mineralization of organic carbon, but rather viruses were positively correlated with carbon mineralization. This is a result of viral-mediated cell lysis and demonstrates that viruses are sensitive indicators of microbial activity. Viruses as an indicator of microbial activity was not unique to batch culture studies as results obtained from an in situ field experiment conducted at the DOE Old Rifle Field site. This study revealed that viral abundance increased in response to the injection of oxygenated groundwater and influx of dissolved organic carbon whereas cell abundance changes were minimal. However, the extent to which viral-mediated cell lysis alters organic matter pools subsequently influencing microbial community structure and biogeochemical function remains a critical question in subsurface biogeochemical cycling. The production of significant numbers of viruses in groundwater has implications for nanoparticulate metal as well as carbon transport in groundwater. We have demonstrated that the virus surface is reactive and will adsorb heavy metals. Thus viruses can promote colloidal contaminant mobility. Interestingly, the presence of heavy metals has a positive effect on infectivity of the phage, increasing phage infection which could lead to further production of viruses. Together, the results indicate that the sorption of metals to the surface of viruses could not only contribute to nanoparticulate metal as well as carbon transport but could also enhance infectivity further contributing to cell lysis which could subsequently influence biogeochemical cycling. As more viruses infect host microbial populations the high concentration of metals would enhance infection, resulting in cell lysis, and decreasing the metabolically active host population while yielding greater numbers of viruses capable of transporting contaminats. Additional studies will be necessary to further establish the potential relationship(s) between viruses, cells, carbon, and metals/radionuclides to provide sufficient scientific understanding to incorporate coupled physical, chemical, and biological processes into agent based and reactive transport models.« less

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

EPA Pesticide Factsheets

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

XANES and EXAFS investigation of uranium incorporation on nZVI in the presence of phosphate.

PubMed

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.

Biofiltration of Volatile Pollutants: Solubility Effects

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

Davison, Brian H.; Barton, John W.

2001-06-15

This project investigates and collects fundamental partitioning data for a variety of sparingly soluble subsurface contaminants (e.g., TCE, etc.) between vapor, aqueous phase, and matrices containing substantial quantities of biomass and biomass components. Due to the difficulty of obtaining these measurements, environmental models have generally used solubility constants of chemicals in pure water or, in a few rare cases, simple linear models. Our prior EMSP work has shown that the presence of biological material can increase effective solubilities by an order of magnitude for sparingly soluble organics; therefore, the previous simple approaches are not valid and are extremely poor predictorsmore » of actual bio-influenced partitioning. It is likely that environmental contaminants will partition in a similar manner into high-biomass phases (e.g. biobarriers and plants) or humic soils. Biological material in the subsurface can include lipids, fatty acids, humic materials, as well a s the lumped and difficult to estimate 'biomass'. Our measurements include partition into these biological materials to allow better estimation. Fundamental data collected will be used in mathematical models predicting transport and sorption in subsurface environments, with the impacts on bioremediation being evaluated based on this new information. Our 2-D Win95/98 software program, Biofilter 1.0, developed as a part of our prior EMSP efforts for describing biofiltration processes with consideration given to both kinetic and mass transfer factors, will be extended to incorporate and use this information.« less

Biofiltration of Volatile Pollutants: Solubility Effects

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

Davison, Brian H.; Barton, John W.

2002-06-15

This project investigates and collects fundamental partitioning data for a variety of sparingly soluble subsurface contaminants (e.g., TCE, etc.) between vapor, aqueous phase, and matrices containing substantial quantities of biomass and biomass components. Due to the difficulty of obtaining these measurements, environmental models have generally used solubility constants of chemicals in pure water or, in a few rare cases, simple linear models. Our prior EMSP work has shown that the presence of biological material can increase effective solubilities by an order of magnitude for sparingly soluble organics; therefore, the previous simple approaches are not valid and are extremely poor predictorsmore » of actual bio-influenced partitioning. It is likely that environmental contaminants will partition in a similar manner into high-biomass phases (e.g. biobarriers and plants) or humic soils. Biological material in the subsurface can include lipids, fatty acids, humic materials, as well as the lumped and difficult-to-estimate 'biomass'. Our measurements include partition into these biological materials to allow better estimation. Fundamental data collected will be used in mathematical models predicting transport and sorption in subsurface environments, with the impacts on bioremediation being evaluated based on this new information. Our 2-D Win95/98/XP software program, Biofilter 1.0, developed as a part of our prior EMSP efforts for describing biofiltration processes with consideration given to both kinetic and mass transfer factors, is being extended to incorporate and use this information.« less

Radionuclides and heavy metals in Borovac, Southern Serbia.

PubMed

Popovic, Dragana; Todorovic, Dragana; Frontasyeva, Marina; Ajtic, Jelena; Tasic, Mirjana; Rajsic, Slavica

2008-09-01

The paper presents the complex approach to the assessment of the state of the environment in Southern Serbia, surroundings of Bujanovac, the region which is of great concern as being exposed to contamination by depleted uranium (DU) ammunition during the North Atlantic Treaty Organization (NATO) attacks in 1999. It includes studies on concentrations of radionuclides and heavy metals in different environmental samples 5 years after the military actions. In October 2004, samples of soil, grass, lichen, moss, honey, and water were collected at two sites, in the immediate vicinity of the targeted area and 5 km away from it. Radionuclide ((7)Be, (40)K, (137)Cs, (210)Pb, (226)Ra, (232)Th, (235)U, (238)U) activities in solid samples were determined by standard gamma spectrometry and total alpha and beta activity in water was determined by proportional alpha-beta counting. Concentrations of 35 elements were determined in the samples of soil, moss, grass, and lichen by instrumental neutron activation analysis (INAA). The results are discussed in the context of a possible contamination by DU that reached the environment during the attacks as well as in the context of an environmental pollution by radionuclides and heavy metals in Southern Serbia. The results are compared to the state of environment in the region and other parts of the country both prior to and following the attacks. This is the first comprehensive study of the contents of radionuclides and heavy metals in Southern Serbia and consequently highly important for the assessment of the state of environment in this part of the country concerning possible effects of DU ammunition on the environment, as well as anthropogenic source of pollution by radionuclides and heavy metals and other elements. Also, the highly sensitive method of INAA was used for the first time to analyze the environmental samples from this area. The results of the study of radionuclides in the samples of soils, leaves, grass, moss, lichen, honey, and water in Southern Serbia (Bujanovac) gave no evidence of the DU contamination of the environment 5 years after the military actions in 1999. Activities of radionuclides in soils were within the range of the values obtained in the other parts of the country and within the global average. The ratio of uranium isotopes confirmed the natural origin of uranium. In general, concentrations of heavy metals in the samples of soils, plant leaves, mosses, and lichen are found to be less or in the lower range of values found in other parts of the country, in spite of the differences in plant and moss species or soil characteristics. Possible sources of heavy metal contamination were identified as a power coal plant in the vicinity of the sampling sites and wood and waste burning processes. The collected data should provide a base for the health risk assessments on animals and humans in the near future. It should be emphasized that the sampling was carried out 5 years after the military action and that the number of samples was limited; therefore, the conclusions should be accepted only as observed tendencies and a detailed study should be recommended in the future.

Unrefined humic substances as a potential low-cost amendment for the management of acidic groundwater contamination.

PubMed

Gonzalez-Raymat, Hansell; Anagnostopoulos, Vasileios; Denham, Miles; Cai, Yong; Katsenovich, Yelena P

2018-04-15

The present study explores a novel application of Huma-K, a commercially available, unrefined humic substance, as a promising low-cost source of organic matter for in situ remediation of contaminated acidic groundwater plumes. This can be achieved by creating a humic-rich coating on the surface of minerals which can enhance the sorption of contaminants from groundwater. Huma-K was characterized by means of scanning electron microscopy equipped with energy dispersive spectroscopy, Fourier-transform infrared analysis, and potentiometric titrations. Batch experiments were performed to investigate the sorption-desorption behavior of Huma-K and to evaluate what conditions (pH, contact time, and initial Huma-K concentration) affect these processes upon injection into aquifer sediments. As evidenced by potentiometric titrations, Huma-K possesses functional groups that have an acidic nature, with pK values in the range of 4-6 (carboxylic) and 9-10 (phenolic). Sorption, homogeneous precipitation, and surface-induced precipitation seem to be favored in the presence of sediment at pH 4, where there is less deprotonation of acidic functional groups. As the pH is increased, functional groups become negatively charged, leading to electrostatic repulsion and dissolution of Huma-K from sediment. Kinetic experiments indicate that Huma-K sorption is a slow-rate process, most likely governed by film diffusion. The enhanced sorption of Huma-K in acidic conditions suggests that it may be used to create a subsurface treatment zone in acidic aquifers for the sequestration of contaminants such as uranium. The treatment zone will persist as long as the pH does not increase sufficiently to cause soil-bound Huma-K to be released, remobilizing aqueous contaminants. Copyright © 2018 Elsevier Ltd. All rights reserved.

Iron Mineralogy and Uranium-Binding Environment in the ...

EPA Pesticide Factsheets

Wetlands mitigate the migration of groundwater contaminants through a series of biogeochemical gradients that enhance multiple contaminant-binding processes. The hypothesis of this study was that wetland plant roots contribute organic carbon and release O2 within the rhizosphere (plant-impact soil zone) that promote the formation of Fe(III)-(oxyhydr)oxides. In turn, these Fe(III)-(oxyhydr)oxides stabilize organic matter that together contribute to contaminant immobilization. Mineralogy and U binding environments of the rhizosphere were evaluated in samples collected from contaminated and non-contaminated areas of a wetland on the Savannah River Site in South Carolina. Based on Mössbauer spectroscopy, rhizosphere soil was greatly enriched with nanogoethite, ferrihydrite-like nanoparticulates, and hematite, with negligible Fe(II) present. X-ray computed tomography and various microscopy techniques showed that root plaques were tens-of-microns thick and consisted of highly oriented Fe-nanoparticles, suggesting that the roots were involved in creating the biogeochemical conditions conducive to the nanoparticle formation. XAS showed that a majority of the U in the bulk wetland soil was in the +6 oxidation state and was not well correlated spatially to Fe concentrations. SEM/EDS confirm that U was enriched on root plaques, where it was always found in association with P. Together these findings support our hypothesis and suggest that plants can alter mineralo

PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

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

Caldwell, E.; Duff, M.; Ferguson, C.

2010-12-16

The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical andmore » biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.« less

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

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

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

2014-09-01

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

Uranium Interaction with Two Multi-Resistant Environmental Bacteria: Cupriavidus metallidurans CH34 and Rhodopseudomonas palustris

PubMed Central

Llorens, Isabelle; Untereiner, Guillaume; Jaillard, Danielle; Gouget, Barbara; Chapon, Virginie; Carriere, Marie

2012-01-01

Depending on speciation, U environmental contamination may be spread through the environment or inversely restrained to a limited area. Induction of U precipitation via biogenic or non-biogenic processes would reduce the dissemination of U contamination. To this aim U oxidation/reduction processes triggered by bacteria are presently intensively studied. Using X-ray absorption analysis, we describe in the present article the ability of Cupriavidus metallidurans CH34 and Rhodopseudomonas palustris, highly resistant to a variety of metals and metalloids or to organic pollutants, to withstand high concentrations of U and to immobilize it either through biosorption or through reduction to non-uraninite U(IV)-phosphate or U(IV)-carboxylate compounds. These bacterial strains are thus good candidates for U bioremediation strategies, particularly in the context of multi-pollutant or mixed-waste contaminations. PMID:23251623

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.

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

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

Johnson, Raymond; Dam, William; Campbell, Sam

2016-08-01

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

Microscale geochemical gradients in Hanford 300 Area sediment biofilms and influence of uranium

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

Nguyen, Hung D.; Cao, Bin; Mishra, Bhoopesh

2012-01-01

The presence and importance of microenvironments in the subsurface at contaminated sites were suggested by previous geochemical studies. However, no direct quantitative characterization of the geochemical microenvironments had been reported. We quantitatively characterized microscale geochemical gradients (dissolved oxygen (DO), H(2), pH, and redox potential) in Hanford 300A subsurface sediment biofilms. Our results revealed significant differences in geochemical parameters across the sediment biofilm/water interface in the presence and absence of U(VI) under oxic and anoxic conditions. While the pH was relatively constant within the sediment biofilm, the redox potential and the DO and H(2) concentrations were heterogeneous at the microscale (<500-1000more » μm). We found microenvironments with high DO levels (DO hotspots) when the sediment biofilm was exposed to U(VI). On the other hand, we found hotspots (high concentrations) of H(2) under anoxic conditions both in the presence and in the absence of U(VI). The presence of anoxic microenvironments inside the sediment biofilms suggests that U(VI) reduction proceeds under bulk oxic conditions. To test this, we operated our biofilm reactor under air-saturated conditions in the presence of U(VI) and characterized U speciation in the sediment biofilm. U L(III)-edge X-ray absorption spectroscopy (XANES and EXAFS) showed that 80-85% of the U was in the U(IV) valence state.« less

Microscale geochemical gradients in Hanford 300 Area sediment biofilms and influence of uranium.

PubMed

Nguyen, Hung Duc; Cao, Bin; Mishra, Bhoopesh; Boyanov, Maxim I; Kemner, Kenneth M; Fredrickson, Jim K; Beyenal, Haluk

2012-01-01

The presence and importance of microenvironments in the subsurface at contaminated sites were suggested by previous geochemical studies. However, no direct quantitative characterization of the geochemical microenvironments had been reported. We quantitatively characterized microscale geochemical gradients (dissolved oxygen (DO), H(2), pH, and redox potential) in Hanford 300A subsurface sediment biofilms. Our results revealed significant differences in geochemical parameters across the sediment biofilm/water interface in the presence and absence of U(VI) under oxic and anoxic conditions. While the pH was relatively constant within the sediment biofilm, the redox potential and the DO and H(2) concentrations were heterogeneous at the microscale (<500-1000 μm). We found microenvironments with high DO levels (DO hotspots) when the sediment biofilm was exposed to U(VI). On the other hand, we found hotspots (high concentrations) of H(2) under anoxic conditions both in the presence and in the absence of U(VI). The presence of anoxic microenvironments inside the sediment biofilms suggests that U(VI) reduction proceeds under bulk oxic conditions. To test this, we operated our biofilm reactor under air-saturated conditions in the presence of U(VI) and characterized U speciation in the sediment biofilm. U L(III)-edge X-ray absorption spectroscopy (XANES and EXAFS) showed that 80-85% of the U was in the U(IV) valence state. Copyright © 2011 Elsevier Ltd. All rights reserved.

Use of groundwater lifetime expectancy for the performance assessment of a deep geologic radioactive waste repository: 2. Application to a Canadian Shield environment

NASA Astrophysics Data System (ADS)

Park, Y.-J.; Cornaton, F. J.; Normani, S. D.; Sykes, J. F.; Sudicky, E. A.

2008-04-01

F. J. Cornaton et al. (2008) introduced the concept of lifetime expectancy as a performance measure of the safety of subsurface repositories, on the basis of the travel time for contaminants released at a certain point in the subsurface to reach the biosphere or compliance area. The methodologies are applied to a hypothetical but realistic Canadian Shield crystalline rock environment, which is considered to be one of the most geologically stable areas on Earth. In an approximately 10 × 10 × 1.5 km3 hypothetical study area, up to 1000 major and intermediate fracture zones are generated from surface lineament analyses and subsurface surveys. In the study area, mean and probability density of lifetime expectancy are analyzed with realistic geologic and hydrologic shield settings in order to demonstrate the applicability of the theory and the numerical model for optimally locating a deep subsurface repository for the safe storage of spent nuclear fuel. The results demonstrate that, in general, groundwater lifetime expectancy increases with depth and it is greatest inside major matrix blocks. Various sources and aspects of uncertainty are considered, specifically geometric and hydraulic parameters of permeable fracture zones. Sensitivity analyses indicate that the existence and location of permeable fracture zones and the relationship between fracture zone permeability and depth from ground surface are the most significant factors for lifetime expectancy distribution in such a crystalline rock environment. As a consequence, it is successfully demonstrated that the concept of lifetime expectancy can be applied to siting and performance assessment studies for deep geologic repositories in crystalline fractured rock settings.