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Reimus, Paul W.

Publications and source records attributed to Reimus, Paul W..

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Uranium Retardation Capacity of Lithologies from the Negev Desert, Israel—Rock Characterization and Sorption Experiments

A series of batch experiments were performed to assess the uranium sorption capacity of four mineralogically distinct lithologies from the Negev Desert, Israel, to evaluate the suitability of a potential site for subsurface radioactive waste disposal. The rock specimens consisted of an organic-rich phosphorite, a bituminous marl, a chalk, and a sandstone. The sorption data for each lithology were fitted using a general composite surface complexation model (GC SCM) implemented in PHREEQC. Sorption data were also fitted by a non-mechanistic Langmuir sorption isotherm, which can be used as an alternative to the GC SCM to provide a more computationally efficient method for uranium sorption. This is because all the rocks tested have high pH/alkalinity/calcium buffering capacities that restrict groundwater chemistry variations, so that the use of a GC SCM is not advantageous. The mineralogy of the rocks points to several dominant sorption phases for uranyl (UO 2 2+ ), including apatite, organic carbon, clays, and iron-bearing phases. The surface complexation parameters based on literature values for the minerals identified overestimate the uranium sorption capacities, so that for our application, an empirical approach that makes direct use of the experimental data to estimate mineral-specific sorption parameters appears to be more practical for predicting uranium sorption.

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

Subsurface Radionuclide Transport: Northeastern Negev Desert Vadose Zone Model Development - 19285

The overarching goal of the research presented is to build a subsurface radionuclide transport model for the vadose zone in the northeastern Negev desert of Israel, in order to assist in evaluating its suitability for radioactive waste subsurface disposal. The Negev desert provides a unique geologic setting because of its arid conditions, deep vadose zone and the layered stratigraphy consisting of sandstones, limestones, chalks, shales, marls, phosphorites, clays and cherts. These lithologies form intercalated layers of impermeable and permeable rocks, some with a high adsorption capacity for radionuclides. This paper consists of year one results of a joint US-Israeli collaboration to construct a generic radionuclide transport model of the vadose zone of the northeastern Negev region, Israel. The work aims to (1) evaluate potential vadose zone sites for a nuclear waste disposal site in Israel, and (2) promote the exchange of information and experience in subsurface waste siting and management. First year results include a) measured hydrogeologic rock properties for rock and core samples taken from the Negev desert, Israel, b) sorption and kinetic data for uranium U(VI) on phosphorite, chalk, sandstone and oil-shale lithologies, and c) an updated geologic, stratigraphic, and hydrologic subsurface framework for the northeastern Negev region. Preliminary results on uranium adsorption for key subsurface lithologies are encouraging in terms of the potential suitability of the Negev vadose zone to act as an efficient medium for the retardation of radionuclides. The findings provide impetus for continued experimentation and the development of a northeastern Negev subsurface flow and transport model. (authors)

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DOE OSTI2018

Long-term stability of dithionite in alkaline anaerobic aqueous solution

Closed-system experiments were conducted to investigate the decomposition of sodium dithionite in aqueous solutions under varying pH and starting concentrations to simulate the deployment of dithionite as an in-situ redox barrier. Co-determination of dithionite and its degradation products was conducted using UV-Vis spectrometry, iodometric titration, and ion chromatography. In unbuffered solutions, dithionite reacted rapidly, whereas in near-neutral solutions (pH ~7), it persisted for ~ 50 days and in alkaline solution (pH ~9.5) for >100 days. As a result, these are the longest lifetimes reported to date, which we attribute to not only excluding oxygen but also preventing outgassing of H 2 S.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Inferring subsurface heterogeneity from push-drift tracer tests

In this study, we consider the late-time tailing in a tracer test performed with a push-drift methodology (i.e., quasi-radial injection followed by drift under natural gradient). Numerical simulations of such tests are performed on 1000 multi-Gaussian 2-D log-hydraulic conductivity field realizations of varying heterogeneity, each under eight distinct mean flow directions. The ensemble pdfs of solute return times are found to exhibit power law tails for each considered variance of the log-hydraulic conductivity field, σ$2\atop{ln K}$. The tail exponent is found to relate straightforwardly to σ$2\atop{ln K}$ and, within the parameter space we explored, to be independent of push-phase pumping rate, pumping duration, and local-scale dispersivity. We conjecture that individual push-drift tracer tests in wells with screened intervals much greater than the vertical correlation length of the aquifer will exhibit quasi-ergodicity and that their tail exponent may be used to infer σ$2\atop{ln K}$. Lastly, we calibrate a predictive relationship of this sort from our Monte Carlo study, and apply it to data from a push-drift test performed at a site of approximately known heterogeneity—closely matching the existing best estimate of heterogeneity.

58 GEOSCIENCES↗
DOE OSTI2017

Laboratory column experiments and transport modeling to evaluate retardation of uranium in an aquifer downgradient of a uranium in-situ recovery site

The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47 relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.

58 GEOSCIENCES↗
DOE OSTI2017

Evaluation of multiple tracer methods to estimate low groundwater flow velocities

Here, four different tracer methods were used to estimate groundwater flow velocity at a multiple-well site in the saturated alluvium south of Yucca Mountain, Nevada: (1) two single-well tracer tests with different rest or “shut-in” periods, (2) a cross-hole tracer test with an extended flow interruption, (3) a comparison of two tracer decay curves in an injection borehole with and without pumping of a downgradient well, and (4) a natural-gradient tracer test. Such tracer methods are potentially very useful for estimating groundwater velocities when hydraulic gradients are flat (and hence uncertain) and also when water level and hydraulic conductivity data are sparse, both of which were the case at this test location. The purpose of the study was to evaluate the first three methods for their ability to provide reasonable estimates of relatively low groundwater flow velocities in such low-hydraulic-gradient environments. The natural-gradient method is generally considered to be the most robust and direct method, so it was used to provide a “ground truth” velocity estimate. However, this method usually requires several wells, so it is often not practical in systems with large depths to groundwater and correspondingly high well installation costs. The fact that a successful natural gradient test was conducted at the test location offered a unique opportunity to compare the flow velocity estimates obtained by the more easily deployed and lower risk methods with the ground-truth natural-gradient method. The groundwater flow velocity estimates from the four methods agreed very well with each other, suggesting that the first three methods all provided reasonably good estimates of groundwater flow velocity at the site. We discuss the advantages and disadvantages of the different methods, as well as some of the uncertainties associated with them.

58 GEOSCIENCES↗
DOE OSTI2015

Genome Sequence of a Chromium-Reducing Strain, Bacillus cereus S612

We report here the genome sequence of an effective chromium-reducing bacterium, Bacillus cereus strain S612. We found that the size of the draft genome sequence is approximately 5.4 Mb, with a G+C content of 35%, and it is predicted to contain 5,450 protein-coding genes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Reactive transport of uranium in fractured crystalline rock: Upscaling in time and distance

In this study, batch adsorption and breakthrough column experiments were conducted to evaluate uranium transport through altered material that fills fractures in a granite rock system at the Grimsel Test Site in Switzerland at pH 6.9 and 7.9. The role of adsorption and desorption kinetics was evaluated with reactive transport modeling by comparing one-, two-, and three-site models. Emphasis was placed on describing long desorption tails that are important for upscaling in time and distance. The effect of increasing pH in injection solutions was also evaluated. For pH 6.9, a three-site model with forward rate constants between 0.07 and 0.8 ml g –1 h –1 , reverse rate constants between 0.001 and 0.06 h –1 , and site densities of 1.3, 0.104, and 0.026 μmol g –1 for ‘weak/fast’, ‘strong/slow’, and ‘very strong/very slow’ sites provided the best fits. For pH 7.9, a three-site model with forward rate constants between 0.05 and 0.8 mL g –1 h –1 , reverse rate constants between 0.001 and 0.6 h –1 , and site densities of 1.3, 0.039, and 0.013 μmol g –1 for a ‘weak/fast’, ‘strong/slow’, and ‘very strong/very slow’ sites provided the best fits. Column retardation coefficients (R d ) were 80 for pH 6.9 and 10.3 for pH 7.9. Model parameters determined from the batch and column experiments were used in 50 year large-scale simulations for continuous and pulse injections and indicated that a three-site model is necessary at pH 6.9, although a K d -type equilibrium partition model with one-site was adequate for large scale predictions at pH 7.9. Batch experiments were useful for predicting early breakthrough times in the columns while column experiments helped differentiate the relative importance of sorption sites and desorption rate constants on transport.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine

In situ recovery (ISR) uranium (U) mining mobilizes U in its oxidized hexavalent form (U(VI)) by oxidative dissolution of U from the roll-front U deposits. Post-mining natural attenuation of residual U(VI) at ISR mines is a potential remediation strategy. Detection and monitoring of naturally occurring reducing subsurface environments are important for successful implementation of this remediation scheme. We used the isotopic tracers ²³⁸U/²³⁵U (δ²³⁸U), ²³⁴U/²³⁸U activity ratio, and ³⁴S/³²S (δ³⁴S), and geochemical measurements of U ore and groundwater collected from 32 wells located within, upgradient, and downgradient of a roll-front U deposit to detect U(VI) reduction and U mobility at an ISR mining site at Rosita, TX, USA. The δ²³⁸U in Rosita groundwater varies from 0.61‰ to -2.49‰, with a trend toward lower δ²³⁸U in downgradient wells. The concurrent decrease in U(VI) concentration and δ²³⁸U with an ε of 0.48‰ ± 0.08‰ is indicative of naturally occurring reducing environments conducive to U(VI) reduction. Additionally, characteristic ²³⁴U/²³⁸U activity ratio and δ³⁴S values may also be used to trace the mobility of the ore zone groundwater after mining has ended. These results support the use of U isotope-based detection of natural attenuation of U(VI) at Rosita and other similar ISR mining sites.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Experimental Evaluation of Actinide Transport in a Fractured Granodiorite

The objective of this study was to demonstrate and evaluate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments have already been conducted with uranium and additional field experiments using other actinides are planned at the site. Thus, working on this system provides a unique opportunity to compare lab experiment results with fieldscale observations. Rock cores drilled from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption and column breakthrough experiments. Solutions with pH 6.8 and 8.8 were tested. Solutions were switched to radionuclide-free synthetic Grimsel groundwater after near-steady actinide/colloid breakthrough occurred in column experiments. We are currently evaluating actinide adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, and mineralogy in solutions and suspensions with bentonite colloids. (auth)

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DOE OSTI2013

Development of Models to Simulate Tracer Tests for Characterization of Enhanced Geothermal Systems

A recent report found that power and heat produced from enhanced (or engineered) geothermal systems (EGSs) could have a major impact on the U.S energy production capability while having a minimal impact on the environment. EGS resources differ from high-grade hydrothermal resources in that they lack sufficient temperature distribution, permeability/porosity, fluid saturation, or recharge of reservoir fluids. Therefore, quantitative characterization of temperature distributions and the surface area available for heat transfer in EGS is necessary for the design and commercial development of the geothermal energy of a potential EGS site. The goal of this project is to provide integrated tracer and tracer interpretation tools to facilitate this characterization. This project was initially focused on tracer development with the application of perfluorinated tracer (PFT) compounds, non-reactive tracers used in numerous applications from atmospheric transport to underground leak detection, to geothermal systems, and evaluation of encapsulated PFTs that would release tracers at targeted reservoir temperatures. After the 2011 midyear review and subsequent discussions with the U.S. Department of Energy Geothermal Technology Program (GTP), emphasis was shifted to interpretive tool development, testing, and validation. Subsurface modeling capabilities are an important component of this project for both the design of suitable tracers and the interpretation of data from in situ tracer tests, be they single- or multi-well tests. The purpose of this report is to describe the results of the tracer and model development for simulating and conducting tracer tests for characterizing EGS parameters.

EGS↗
DOE OSTI2012

Temperature dependence of cation exchange in geothermal applications

Geothermal energy is heat energy stored by the earth, and is currently being explored as a renewable energy resource. To extract energy efficiently from a geothermal reservoir it must be hot, close to the surface, and have good permeability. If a reservoir is lacking any of these it can be enhanced by creating fractures in the rock. These fractures increase surface area available for heat transfer, and allow water to flow more efficiently increasing energy output. In this study we determine if the effectiveness of the enhancement can be determined by the chemical indicator lithium (Li). We preformed simulations to study the amount of Li that absorbs onto the rock at different temperatures. From this data we determined the absorption of Li onto the rock does not change significantly with change in temperature and therefore can be used to determine change in surface area after enhancement.

Earth Sciences↗
DOE OSTI2012

Preliminary Interpretation of a Radionuclide and Colloid Tracer Test in a Granodiorite Shear Zone at the Grimsel Test Site, Switzerland

In February and March 2012, a tracer test involving the injection of a radionuclide-colloid cocktail was conducted in the MI shear zone at the Grimsel Test Site, Switzerland, as part of the Colloids Formation and Migration (CFM) project. The colloids were derived from FEBEX bentonite, which is mined in Spain and is being considered as a potential waste package backfill in a Spanish nuclear waste repository.

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