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At least 613 records · Page 34

Long-term Kinetics of Uranyl Desorption from Sediments Under Advective Conditions

Long-term (> 4 months) column experiments were performed to investigate the kinetics of uranyl (U(VI)) desorption in sediments collected from the Integrated Field Research Challenge (IFRC) site at the US Department of Energy (DOE) Hanford 300 Area. The experimental results were used to evaluate alternative multi-rate surface complexation reaction (SCR) approaches to describe the short- and long-term kinetics of U(VI) desorption under flow conditions. The SCR stoichiometry, equilibrium constants, and multi-rate parameters were independently characterized in batch and stirred flow-cell reactors. Multi-rate SCR models that were either additively constructed using the SCRs for individual size fractions (e.g., Shang et al., 2011), or composite in nature could effectively describe short-term U(VI) desorption under flow conditions. The long-term desorption results, however, revealed that using a labile U concentration measured by carbonate extraction under-estimated desorbable U(VI) and the long-term rate of U(VI) desorption. An alternative modeling approach using total U as the desorbable U(VI) concentration was proposed to overcome this difficulty. This study also found that the gravel size fraction (2-8 mm), which is typically treated as non-reactive in modeling U(VI) reactive transport because of low external surface area, can have an important effect on the U(VI) desorption in the sediment. This study demonstrates an approach to effectively extrapolate U(VI) desorption kinetics for field-scale application, and identifies important parameters and uncertainties affecting model predictions.

additivity approach↗

Composition of conglomerates analyzed by the Curiosity rover: Implications for Gale Crater crust and sediment sources

The Curiosity rover has analyzed various detrital sedimentary rocks at Gale Crater, among which fluvial and lacustrine rocks are predominant. Conglomerates correspond both to the coarsest sediments analyzed and the least modified by chemical alteration, enabling us to link their chemistry to that of source rocks on the Gale Crater rims. Here, we report the results of six conglomerate targets analyzed by Alpha-Particle X-ray Spectrometer and 40 analyzed by ChemCam. The bulk chemistry derived by both instruments suggests two distinct end-members for the conglomerate compositions. The first group (Darwin type) is typical of conglomerates analyzed before sol 540; it has a felsic alkali-rich composition, with a Na 2 O/K 2 O > 5. The second group (Kimberley type) is typical of conglomerates analyzed between sols 540 and 670 in the vicinity of the Kimberley waypoint; it has an alkali-rich potassic composition with Na 2 O/K 2 O < 2. The variety of chemistry and igneous textures (when identifiable) of individual clasts suggest that each conglomerate type is a mixture of multiple source rocks. Conglomerate compositions are in agreement with most of the felsic alkali-rich float rock compositions analyzed in the hummocky plains. The average composition of conglomerates can be taken as a proxy of the average igneous crust composition at Gale Crater. Finally, the differences between the composition of conglomerates and that of finer-grained detrital sediments analyzed by the rover suggest modifications by diagenetic processes (especially for Mg enrichments in fine-grained rocks), physical sorting, and mixing with finer-grained material of different composition.

58 GEOSCIENCES↗

The effect of hydrate saturation on water retention curves in hydrate‐bearing sediments

Abstract The experimental measurement of water retention curve in hydrate‐bearing sediments is critically important to understand the behavior of hydrate dissociation and gas production. In this study, tetrahydrofuran (THF) is selected as hydrate former. The pore habit of THF hydrates is investigated by visual observation in a transparent micromodel. It is confirmed that THF hydrates are not wetting phase on the quartz surface of the micromodel and occupy either an entire pore or part of pore space resulting in change in pore size distribution. And the measurement of water retention curves in THF hydrate‐bearing sediments with hydrate saturation ranging from S h = 0 to S h = 0.7 is conducted for excess water condition. The experimental results show that the gas entry pressure and the capillary pressure increase with increasing hydrate saturation. Based on the experimental results, fitting parameters for van Genuchten equation are suggested for different hydrate saturation conditions.

Mahabadi, Nariman↗

Evaluation of a Geotechnical Compaction Model to Estimate Sediment Deformation

When surface ruts from vehicle activity occur above archeological deposits, there is a potential for an impact to the archeological record to occur. While impacts to the soil surface are relatively straightforward to describe, sub-surface disturbances are more difficult to quantify. In particular, disturbances to buried archeological materials can be difficult to characterize. Materials can be damaged by surface disturbances, but they can also be impacted even if they stay intact. Interpretation of intact materials relocated within the sediment column can be problematic. Traditional characterization methods (e.g. excavation) can also disturb archaeological materials. Here, we present a geotechnical compaction model that can be used to assist with sub-surface characterization under vehicle ruts formed during off-road travel. The model is based on a Boussinesq analysis of stress increase below a surface load. The change in bulk density resulting from compaction is assumed to be proportional to the stress increase. The model results were compared against pilot scale tests conducted with homogeneous sediment and field scale in-situ tests. The results indicate that the model generally agreed with measurements to within 20%, although only a single soil type was evaluated in these studies, with a narrow range of initial bulk densities and rut depths. While application of the model across a broader matrix of soil types, bulk densities and rut depths would increase confidence in the model, it appears that the model may be suitable for use in archeological field investigations. Potential uses include both compliance and research based field applications.

Fritz, Brad G.↗

Mercury concentrations in Pacific lamprey ( Entosphenus tridentatus ) and sediments in the Columbia River basin: Mercury in Columbia River Pacific lamprey

We investigated mercury accumulation in Pacific lamprey and sediments in the Columbia River basin. Mercury concentrations in larval lamprey differed significantly among sample locations (P < 0.001) and were correlated with concentrations in sediments (r 2 = 0.83), whereas adult concentrations were highly variable (range 0.1–9.5 µg/g) and unrelated to holding time after collection. The results suggest that Pacific lamprey in the Columbia River basin may be exposed to mercury levels that have adverse ecological effects.

54 ENVIRONMENTAL SCIENCES↗

Quantitative guidance for efficient vertical flow measurements at the sediment–water interface using temperature–depth profiles

Upward discharge to surface water bodies can be quantified using analytical models based on temperature–depth (T-z) profiles. The use of sediment T-z profiles is attractive as discharge estimates can be obtained using point-in-time data that are collected inexpensively and rapidly. Previous studies have identified that T-z methods can only be applied at times of the year when there is significant difference between the streambed–water interface and deeper sediment temperatures (e.g., winter and summer). However, surface water temperatures also vary diurnally, and the influence of these variations on discharge estimates from T-z methods is poorly understood. For this study, synthetic T-z profiles were generated numerically using measured streambed interface temperature data to assess the influence of diurnal temperature variations on discharge estimation and provide insight into the suitable application of T-z methods. Results show that the time of day of data collection can have a substantial influence on vertical flux estimates using T-z methods. For low groundwater discharge fluxes (e.g., 0.1 m d -1 ), daily transience in streambed temperatures led to relatively large errors in estimated flow magnitude and direction. For higher discharge fluxes (1.5 m d -1 ), the influence of transient streambed temperatures on discharge estimates was strongly reduced. Discharge estimates from point-in-time T-z profiles were most accurate when the uppermost point in the T-z profile was near the bed interface daily mean (two time periods daily). Where temperature time series data are available, daily averaged T-z profiles can produce accurate discharge estimates across a wide range of discharge rates. Seasonality in shallow groundwater temperature generally had a negligible influence on vertical flow estimates. Finally, these findings can be used to plan field campaigns and provide guidance on the optimal application of T-z methods to quantify vertical groundwater discharge to surface water bodies.

54 ENVIRONMENTAL SCIENCES↗

Membrane inlet laser spectroscopy to measure H and O stable isotope compositions of soil and sediment pore water with high sample throughput

Here, the fast and accurate measurement of H and O stable isotope compositions (δ 2 H and δ 18 O values) of soil and sediment pore water remains an impediment to scaling-up the application of these isotopes in soil and vadose hydrology. Here we describe a method and its calibration to measuring soil and sediment pore water δ 2 H and δ 18 O values using a water vapor-permeable probe coupled to an isotope ratio infrared spectroscopy analyzer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Sediment Containing Coal Ash from the Kingston Ash Release on Embryo-Larval Development in the Fathead Minnow, Pimephales promelas (Rafinesque, 1820)

The largest environmental release of coal ash in U.S. history occurred in December 2008 with the failure of a retention structure at the Tennessee Valley Authority (TVA) Kingston Fossil Plant in East Tennessee. A byproduct of coal-burning power plants, coal ash is enriched in metals and metalloids such as selenium and arsenic with known toxicity to fish including embryonic and larval stages. The effects of contact exposure to sediments containing up to 78 % coal ash from the Kingston spill on the early development of fish embryos and larvae were examined in 7-day laboratory tests with the fathead minnow (Pimephales promelas). No significant effects were observed on hatching success, incidences of gross developmental abnormalities, or embryo-larval survival. Results suggest that direct exposures to sediment containing residual coal ash from the Kingston ash release may not present significant risks to fish eggs and larvae in waterways affected by the spill.

Coal Ash Toxicity Fish Early Life Stages Selenium ↗

Diverse Bacterial Groups Contribute to the Alkane Degradation Potential of Chronically Polluted Subantarctic Coastal Sediments

We aimed to gain insight into the alkane degradation potential of microbial communities from chronically polluted sediments of a subantarctic coastal environment using a combination of metagenomic approaches. A total of 6178 sequences annotated as alkane-1-monooxygenases (EC 1.14.15.3) were retrieved from a shotgun metagenomic dataset that included two sites analyzed in triplicate. The majority of the sequences binned with AlkB described in Bacteroidetes (32 ± 13 %) or Proteobacteria (29 ± 7 %), although a large proportion remained unclassified at the phylum level. Operational taxonomic unit (OTU)-based analyses showed small differences in AlkB distribution among samples that could be correlated with alkane concentrations, as well as with site-specific variations in pH and salinity. A number of low-abundance OTUs, mostly affiliated with Actinobacterial sequences, were found to be only present in the most contaminated samples. On the other hand, the molecular screening of a large-insert metagenomic library of intertidal sediments from one of the sampling sites identified two genomic fragments containing novel alkB gene sequences, as well as various contiguous genes related to lipid metabolism. Both genomic fragments were affiliated with the phylum Planctomycetes, and one could be further assigned to the genus Rhodopirellula due to the presence of a partial sequence of the 23S ribosomal RNA (rRNA) gene. This work highlights the diversity of bacterial groups contributing to the alkane degradation potential and reveals patterns of functional diversity in relation with environmental stressors in a chronically polluted, high-latitude coastal environment. In addition, alkane biodegradation genes are described for the first time in members of Planctomycetes.

59 BASIC BIOLOGICAL SCIENCES↗

Effect of ion exchange on the rate of aerobic microbial oxidation of ammonium in hyporheic zone sediments

Microbially mediated ammonium oxidation is a major process affecting nitrogen transformation and cycling in natural environments. The dissolved ammonium concentration is also affected by ion exchange in geologic media, such as in soils and groundwater systems. This study investigated whether ion exchange process can affect microbially mediated aerobic oxidation of ammonium. Sediments from the Columbia River hyporheic zone at US Department Energy's Hanford site Washington State were used as an example for this study. Experiments were conducted using the sediments in synthetic groundwater and river water with different ionic strength and chemical compositions. Results indicated that ammonium sorption through ion exchange decreased the rate of ammonium oxidation, apparently resulting from the influence of the ion exchange on dissolved ammonium concentration, thus decreasing the bioavailability of ammonium for microbial oxidation. However, with the decrease of dissolved ammonium concentration, the sorbed ammonium released back to aqueous phase, and became bioavailable so that all the ammonium in the suspensions were oxidized. Low ionic strength enhanced ammonium sorption, and thus decreased the rate of ammonium oxidation. Our results implied a dynamic change in ammonium oxidation kinetics in an environment such as at HZ where river water and groundwater exchanges frequently that can change ionic strength, and thus ammonium sorption and desorption.

Yan, Ailan↗

Characterization and modeling of the cemented sediment surrounding the Iulia Felix glass

About 1800 years ago a Roman Corbita sunk off the coast of Italy carrying a barrel of glass cullet to the floor of the Adriatic Sea. Samples of glass cullet and the cemented surrounding sediment have been characterized and the reaction between the glass and the sea water saturated with respect to calcite and dolomite has been modeled. Results from characterization and modeling show that the cement phase surrounding the sediment grains is a high-Mg calcite. The origin of the cement phase is likely the reaction between the glass and the sea water to from a Mg-silicate, here modeled as sepiolite.

archaeological glass↗

Scale-Dependent Rates of Uranyl Surface Complexation Reaction in Sediments

Scale-dependency of uranyl[U(VI)] surface complexation rates was investigated in stirred flow-cell and column systems using a U(VI)-contaminated sediment from the US Department of Energy, Hanford site, WA. The experimental results were used to estimate the apparent rate of U(VI) surface complexation at the grain-scale and in porous media. Numerical simulations using molecular, pore-scale, and continuum models were performed to provide insights into and to estimate the rate constants of U(VI) surface complexation at the different scales. The results showed that the grain-scale rate constant of U(VI) surface complexation was over 3 to 10 orders of magnitude smaller, dependent on the temporal scale, than the rate constant calculated using the molecular simulations. The grain-scale rate was faster initially and slower with time, showing the temporal scale-dependency. The largest rate constant at the grain-scale decreased additional 2 orders of magnitude when the rate was scaled to the porous media in the column. The scaling effect from the grain-scale to the porous media became less important for the slower sorption sites. Pore-scale simulations revealed the importance of coupled mass transport and reactions in both intragranular and inter-granular domains, which caused both spatial and temporal dependence of U(VI) surface complexation rates in the sediment. Pore-scale simulations also revealed a new rate-limiting mechanism in the intragranular porous domains that the rate of coupled diffusion and surface complexation reaction was slower than either process alone. The results provided important implications for developing models to scale geochemical/biogeochemical reactions.

uranium, desorption, kinetics, scaling, pore-scale↗

Cobalt-60, Barium-133, Cesium-137, and Europium-152 migration from cementitious sources through sediment under field conditions

Safe and effective storage of radioactive waste is essential to protect human and environmental health. Due to the potential for accidental releases and the severity of the associated risks, it is imperative to further understand radionuclide transport should an accident occur. This study was the second set of measurements conducted in 2022 of an ongoing experiment that has analyzed the vadose zone migration of radionuclides from cementitious wasteforms at the Savannah River Site over the last ten years. The radionuclides introduced within the sources are prominent constituents of radioactive waste or analogs for other groups or series of radionuclides. Lysimeters were first analyzed in 2016 using a collimated high-purity germanium gamma-ray spectrometer to non-destructively measure the concentration of each radionuclide in the sediment column as a function of depth. Following these measurements, the lysimeters were redeployed for another 4 years. All radionuclides in all lysimeters were observed to transport further during the redeployment period; however, the extent of migration varied with the material used for introduction. Except for 137Cs, migration through the sediment control system increased with decreasing ionic potential (ionic charge/radius); migration order: 152Eu<137Cs<60Co<133Ba. Overall, the cementitious wasteforms were observed to decrease radionuclide migration extent relative to natural vadose zone conditions. In both cementitious wasteforms, the migration extent increased in the order 152Eu<133Ba<60Co<137Cs. However, less migration was measured when the radionuclides were incorporated into a reducing grout wasteform. The novelty of this paper is the demonstration of a technique capable of creating non-destructive measurements over decade time scales. Ultimately, this work provides insight into the long-term migration of alkali, alkali earth, divalent transition metal, and trivalent (e.g., lanthanide and actinide element) isotopes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Permeability and porosity of hydrate-bearing sediments in the northern Gulf of Mexico

Hydrate-bearing sands are being actively explored because they contain the highest concentrations of hydrate and are the most economically recoverable hydrate resource. However, relatively little is known about the mechanisms or timescales of hydrate formation, which are related to methane supply, fluid flux, and host sediment properties such as permeability. We used logging-while-drilling data from locations in the northern Gulf of Mexico to develop an effective medium theory-based model for predicting permeability based on clay-sized sediment fraction. The model considers permeability varying between sand and clay endpoint permeabilities that are defined from laboratory data. We verified the model using permeability measurements on core samples from three boreholes, and then used the model to predict permeability in two wells drilled in Walker Ridge Block 313 during the Gulf of Mexico Gas Hydrate Joint Industry Project Leg II expedition in 2009. We found that the cleanest sands (clay-sized fraction <0.05) had intrinsic (hydrate-free) permeability contrasts of 5-6 orders of magnitude with the surrounding clays, which is sufficient to provide focused hydrate formation due to advection of methane from a deep source or diffusion of microbial methane from nearby clay layers. In sands where the clay-sized fraction exceeds 0.05, the permeability reduces significantly and focused flow is less pronounced. In these cases, diffusion of dissolved microbial methane is most likely the preferred mode of methane supply for hydrate formation. In conclusion, our results provide important constraints on methane supply mechanisms in the Walker Ridge area and have global implications for evaluating rates of methane migration and hydrate formation in hydrate-bearing sands.

58 GEOSCIENCES↗

Pore habit of methane hydrate and its evolution in sediment matrix – Laboratory visualization with phase-contrast micro-CT

Describing the pore habit of methane hydrate in sediment matrices is essential for understanding natural distribution of methane hydrate, methane trace (transport and solidification) in the hydrate stability zone, physical properties of hydrate-bearing sediments, and the associated influence on potential gas production. Pore habit visualization in natural media at pore scale even with laboratory synthesized cores has been challenging due to the similar densities of methane hydrate from pore liquid. In this work, we used phase-contrast assisted micro-CT with potassium iodine-doped brine to visualize four phases: sand particles, pore fluid, methane hydrate and methane gas. This study visualizes the pore habit of methane hydrate at various stages including during hydrate formation in excess-gas systems, its evolution after brine injection to replace pore fluid, and hydrate formation in excess-water systems. Hydrate tends to adopt round and smooth surfaces when in contact with water while exhibits relatively angular interfaces when in contact with methane gas. Hydrate formation in excess-gas systems results in a partial cementing and partial mineral-coating pore habit, while hydrate in excess-water systems develops mainly as pore-filling, and locally cementing or mineral-coating where big gas pockets exist at the initial state. Pore liquid replacement from methane gas to brine triggers a shift of hydrate pore habit towards pore-filling. Methane hydrate evolution over time produces bigger hydrate particles but with less contact area with sand particles. The effects of hydrate pore habit become less important as hydrate particle size exceeds the pore size. Additionally, hydrate formation could trap residual methane gas and brine as inclusions.

58 GEOSCIENCES↗

Complex exposure-burial history and Pleistocene sediment recycling in the dead sea rift with implications for the age of the Acheulean site of ‘Ubeidiya

Here, we present early Pleistocene burial ages of the ‘Ubeidiya Formation sediments in the Jordan Valley, a segment of the Dead Sea Rift Valley. A minimum age of ∼1.1 Ma is constrained both by paleomagnetic analysis and U-Pb dating of Melanopsis shells. Simple cosmogenic burial ages (i.e., one very long exposure period followed by one period of burial) calculated from the ratios of 26 Al to 10 Be and 10 Be concentrations indicate ages of ∼3 Ma, contradicting the geological and paleomagnetic constraints as well as a reasonable age of the ‘Ubeidiya archeological site, as it contains human remains. A more sophisticated way of treating the results, by combining numerical modeling of cosmogenic nuclide build up during repeated burial-exposure cycles, paleomagnetic analysis (indicating reverse polarity) and a minimum burial age of 1.1 Ma set by U-Pb dating of Melanopsis shells, suggests two most probable time slots (1.19-1.77 and 1.93- 2.14 Ma) for the absolute age of the ‘Ubeidiya Formation. However, the skewed distribution of cosmogenic isotope burial ages, with a median age of 2.05 Ma, indicates a much higher probability of the older ages, most likely >1.9 Ma. The exposure-burial history that emerges from the model implies recycling of sediments previously deposited and buried in the rift valley, between 4.5 and 3.2 Ma, and subsequently exhumed, eroded, transported and then redeposited along the ‘Ubeidiya paleo lake shoreline.

Acheulean↗

Surge Block Method for Controlling Well Clogging and Sampling Sediment during Bioremediation

A surge block treatment method (i.e. inserting a solid rod plunger with a flat seal that closely fits the casing interior into a well and stocking it up and down) was performed for the rehabilitation of wells clogged with biomass and for the collection of time series sediment samples during in situ bioremediation tests for U(VI) immobilization at a the U.S. Department of Energy site in Oak Ridge, TN. The clogging caused by biomass growth had been controlled by using routine surge block treatment for18 times over a nearly four year test period. The treatment frequency was dependent of the dosage of electron donor injection and microbial community developed in the subsurface. Hydraulic tests showed that the apparent aquifer transmissivity at a clogged well with an inner diameter (ID) of 10.16 cm was increased by 8 13 times after the rehabilitation, indicating the effectiveness of the rehabilitation. Simultaneously with the rehabilitation, the surge block method was successfully used for collecting time series sediment samples composed of fine particles (clay and silt) from wells with ID 1.9 10.16 cm for the analysis of mineralogical and geochemical composition and microbial community during the same period. Our results demonstrated that the surge block method provided a cost-effective approach for both well rehabilitation and frequent solid sampling at the same location.

Wu, Wei-min↗

Sedimentation and shear-induced dynamics of spheroids in fluids with spatial viscosity variations

A generalized reciprocal theorem is used to relate the force and torque induced on a particle in an inertia-less fluid with small variation in viscosity to integrals involving Stokes flow fields and the spatial dependence of viscosity. These resistivity expressions are analytically evaluated using spheroidal harmonics and then used to obtain the mobility of the spheroid during sedimentation, and in linear flows, of a fluid with linear viscosity stratification. The coupling between the rotational and translational motion induced by stratification rotates the spheroid’s centerline, creating a variety of rotational and translational dynamics dependent upon the particle’s aspect ratio, κ, and the component of the stratification unit vector in the gravity direction, d g . Spheroids with 0.55 ⪅ κ ⪅ 2.0 exhibit the largest variety of settling behaviors. Interestingly, this range covers most microplastics and typical microorganisms. One of the modes include a stable orientation dependent only on κ and d g , but independent of initial orientation, thus allowing for the potential control of settling angles and sedimentation rates. In a simple shear flow, cross-streamline migration occurs due to the stratification-induced force generated on the particle. Similarly, a particle no longer stays at the stagnation point of a uniaxial extensional flow. While fully analytical results are obtained for spheroids, numerical simulations provide a source of validation. These simulations also provide additional insights into the stratification-induced force- and torque-producing mechanisms through the stratification-induced stress, which is not accessed in the reciprocal theorem-based analytical calculations.

Geophysical and Geological Flows: Stratified flows↗