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PubMedDate not supplied

Modeling unsaturated flow and transport processes at the Busted Butte Field Test Site, Nevada.

A numerical model was used to simulate the flow and transport processes at the Busted Butte Field Test Site for the purpose of quantifying the effects of hydrogeologic conditions beneath the potential Yucca Mountain repository horizon. In situ experiments were conducted on a 10 x 10 x 7 m block comprising a layered Topopah Springs/Calico Hills formation with two imbedded faults. Tracer solution was continuously injected in eight parallel boreholes arranged on two horizontal planes. Twelve collection boreholes were emplaced perpendicular to the injection holes and were both horizontal and inclined. Solution samples were collected regularly using a sampling assembly consisting of an inverted membrane and sorbing-paper sampling pads. Comparisons between measurements and predictions show that, except for the occasional drops of concentrations observed in the field, the current model is able to capture the general characteristics of the system with varying levels of agreement using laboratory-measured mean hydraulic properties. Simulation results and field observations revealed a capillary-driven flow in the system. Good quantitative agreement is generally observed for near-field boreholes, however, this agreement deteriorates and the simulated solute concentration is underestimated at boreholes farther away from the injection points. Increasing the spatial resolution of the simulation improves the model predictions only to a limited extent. Scaling issues may need to be considered to describe flow and transport events, as the travel distance becomes large.

Adsorption↗
PubMedDate not supplied

Fault-matrix interactions in nonwelded tuff of the Paintbrush Group at Yucca Mountain.

To investigate the potential for fast flow through altered tuff of the nonwelded unit of the Paintbrush Group (PTn) at Yucca Mountain, Nevada, we carried out in situ field experiments using water released directly into the matrix and along a minor subvertical normal fault at Alcove 4 in the Exploratory Studies Facility (ESF). During the experiments, changes in moisture content were monitored within the test bed, and a slot excavated below the test bed was visually inspected for seepage. Our field tests suggest that the dry porous PTn matrix is capable of attenuating episodic percolation fluxes in localized areas (such as around faults) where fast flow would be expected to dominate. Once wetted, the matrix is able to retain the moisture over a period of months. As saturation increases in the matrix, less water imbibes along the fault and more water travels farther along the fault. From this observation, we infer that a sequence of infiltration events separated by periods of up to a few months could convey water over increasing distances along the fault.

Filtration↗
PubMedDate not supplied

Performance assessment model development and analysis of radionuclide transport in the unsaturated zone, Yucca Mountain, Nevada.

This paper describes the development and use of a particle-tracking model to perform radionuclide-transport simulations in the unsaturated zone at Yucca Mountain, Nevada. The goal of the effort was to produce a computational model that can be coupled to the project's calibrated 3D site-scale flow model so that the results of that effort could be incorporated directly into the Total System Performance Assessment (TSPA) analyses. The transport model simulates multiple species (typically 20 or more) with complex time-varying and spatially varying releases from the potential repository. Water-table rise, climate-change scenarios, and decay chains are additional features of the model. A cell-based particle-tracking method was employed that includes a dual-permeability formulation, advection, longitudinal dispersion, matrix diffusion, and colloid-facilitated transport. This paper examines the transport behavior of several key radionuclides through the unsaturated zone using the calibrated 3D unsaturated flow fields. Computational results illustrate the relative importance of fracture flow, matrix diffusion, and lateral diversion on the distribution of travel times from the simulated repository to the water table for various climatic conditions. Results also indicate rapid transport through fractures for a portion of the released mass. Further refinement of the model will address several issues, including conservatism in the transport model, the assignment of parameters in the flow and transport models, and the underlying assumptions used to support the conceptual models of flow and transport in the unsaturated zone at Yucca Mountain.

Calibration↗
PubMedDate not supplied

Calibration of Yucca Mountain unsaturated zone flow and transport model using porewater chloride data.

In this study, porewater chloride data from Yucca Mountain, NV are analyzed and modeled by three-dimensional chemical transport simulation and analytical methods. The simulation modeling approach is based on a continuum formulation of coupled multiphase fluid flow and tracer transport processes through fractured porous rock using a dual-continuum concept. Infiltration rate calibrations were performed using the porewater chloride data. Model results of chloride distributions were improved in matching the observed data with the calibrated infiltration rates. Statistical analyses of the frequency distribution for overall percolation fluxes and chloride concentration in the unsaturated zone system demonstrate that the use of the calibrated infiltration rates had an insignificant effect on the distribution of simulated percolation fluxes but significantly changed the predicted distribution of simulated chloride concentrations. An analytical method was also applied to model transient chloride transport. The method was verified by three-dimensional simulation results to be capable of capturing major chemical transient behavior and trends. Effects of lateral flow in the Paintbrush nonwelded unit on percolation fluxes and chloride distribution were studied by three-dimensional simulations with increased horizontal permeability. The combined results from these model calibrations furnish important information for the UZ model studies, contributing to performance assessment of the potential repository.

Calibration↗
PubMedDate not supplied

Modeling flow and transport in unsaturated fractured rock: an evaluation of the continuum approach.

Because the continuum approach is relatively simple and straightforward to implement, it has been commonly used in modeling flow and transport in unsaturated fractured rock. However, the usefulness of this approach can be questioned in terms of its adequacy for representing fingering flow and transport in unsaturated fractured rock. The continuum approach thus needs to be evaluated carefully by comparing simulation results with field observations directly related to unsaturated flow and transport processes. This paper reports on such an evaluation, based on a combination of model calibration and prediction, using data from an infiltration test carried out in a densely fractured rock within the unsaturated zone of Yucca Mountain, Nevada. Comparisons between experimental and modeling results show that the continuum approach may be able to capture important features of flow and transport processes observed from the test. The modeling results also show that matrix diffusion may have a significant effect on the overall transport behavior in unsaturated fractured rocks, which can be used to estimate effective fracture-matrix interface areas based on tracer transport data. While more theoretical, numerical, and experimental studies are needed to provide a conclusive evaluation, this study suggests that the continuum approach is useful for modeling flow and transport in unsaturated, densely fractured rock.

Calibration↗
PubMedDate not supplied

Conceptual evaluation of the potential role of fractures in unsaturated processes at Yucca Mountain.

A wide array of field observations, in situ testing, and rock and water sampling (and subsequent analyses) within the unsaturated zone (UZ) of Yucca Mountain demonstrate the importance of fractures to flow and transport in the welded tuffs. The abundance of fractures and the spatial variability in their hydraulic properties, along with the heterogeneity within lithologic formations, make evaluation of unsaturated processes occurring within the potential repository horizon complex. Fracture mapping and field testing show that fractures are well connected, yet considerable variation is seen within and between units comprising the potential repository horizon with regard to fracture trace length, spacing, permeability, and capillarity. These variations have important implications for the distribution and movement of water and solutes through the unsaturated zone. Numerical models designed to assess such phenomena as unsaturated flow, transport, and coupled thermal-hydrological processes each require their own conceptual model for fracture networks, in order to identify the subset of all fractures that is relevant to the particular study. We evaluate several process-dependent conceptual models for fractures and identify the relevant fracture subsets related to these processes.

Forecasting↗
PubMedDate not supplied

On the physics of unstable infiltration, seepage, and gravity drainage in partially saturated tuffs.

To improve understanding of the physics of dynamic instabilities in unsaturated flow processes within the Paintbrush nonwelded unit (PTn) and the middle nonlithophysal portion of the Topopah Spring welded tuff unit (TSw) of Yucca Mountain, we analyzed data from a series of infiltration tests carried out at two sites (Alcove 4 and Alcove 6) in the Exploratory Studies Facility (ESF), using analytical and empirical functions. The analysis of infiltration rates measured at both sites showed three temporal scales of infiltration rate: (1) a macro-scale trend of overall decreasing flow, (2) a meso-scale trend of fast and slow motion exhibiting three-stage variations of the flow rate (decreasing, increasing, and [again] decreasing flow rate, as observed in soils in the presence of entrapped air), and (3) micro-scale (high frequency) fluctuations. Infiltration tests in the nonwelded unit at Alcove 4 indicate that this unit may effectively dampen episodic fast infiltration events; however, well-known Kostyakov, Horton, and Philip equations do not satisfactorily describe the observed trends of the infiltration rate. Instead, a Weibull distribution model can most accurately describe experimentally determined time trends of the infiltration rate. Infiltration tests in highly permeable, fractured, welded tuff at Alcove 6 indicate that the infiltration rate exhibits pulsation, which may have been caused by multiple threshold effects and water-air redistribution between fractures and matrix. The empirical relationships between the extrinsic seepage from fractures, matrix imbibition, and gravity drainage versus the infiltration rate, as well as scaling and self-similarity for the leading edge of the water front are the hallmark of the nonlinear dynamic processes in water flow under episodic infiltration through fractured tuff. Based on the analysis of experimental data, we propose a conceptual model of a dynamic fracture flow and fracture-matrix interaction in fractured tuff, incorporating the time-dependent processes of water redistribution in the fracture-matrix system.

Filtration↗
PubMedDate not supplied

Chlorine-36 data at Yucca Mountain: statistical tests of conceptual models for unsaturated-zone flow.

An extensive set of chlorine-36 (36Cl) data has been collected in the Exploratory Studies Facility (ESF), an 8-km-long tunnel at Yucca Mountain, Nevada, for the purpose of developing and testing conceptual models of flow and transport in the unsaturated zone (UZ) at this site. At several locations, the measured values of 36Cl/Cl ratios for salts leached from rock samples are high enough to provide strong evidence that at least a small component of bomb-pulse 36Cl, fallout from atmospheric testing of nuclear devices in the 1950s and 1960s, was measured, implying that some fraction of the water traveled from the ground surface through 200-300 m of unsaturated rock to the level of the ESF during the last 50 years. These data are analyzed here using a formal statistical approach based on log-linear models to evaluate alternative conceptual models for the distribution of such fast flow paths. The most significant determinant of the presence of bomb-pulse 36Cl in a sample from the welded Topopah Spring unit (TSw) is the structural setting from which the sample was collected. Our analysis generally supports the conceptual model that a fault that cuts through the nonwelded Paintbrush tuff unit (PTn) that overlies the TSw is required in order for bomb-pulse 36Cl to be transmitted to the sample depth in less than 50 years. Away from PTn-cutting faults, the ages of water samples at the ESF appear to be a strong function of the thickness of the nonwelded tuff between the ground surface and the ESF, due to slow matrix flow in that unit.

Chlorine↗
PubMedDate not supplied

Development of discrete flow paths in unsaturated fractures at Yucca Mountain.

We have carried out numerical modeling studies to investigate the development of discrete-fracture flow paths and flow-focusing phenomena in the unsaturated rock of the potential repository horizon at Yucca Mountain, Nevada. These studies are based on two- and three-dimensional (2-D and 3-D) numerical models using site-specific parameters. The 2-D and 3-D models use high-resolution spatial discretization to explicitly include effects of discrete fractures with stochastically developed fracture permeabilities and a continuum approach. The permeability field is generated based on air permeability measurements at various scales. For most of the cases considered, uniform infiltration with different average rates (1-500 mm/year) is prescribed at the top of the model, while variability in outflow at the bottom of the model is used to evaluate the degree of flow focusing. In addition, scenarios involving nonuniform infiltration at the top boundary, different permeability correlation lengths and different flow-allocation schemes were analyzed. The modeling results obtained from all of the cases showed a remarkably similar flow-focusing pattern at the repository horizon. Furthermore, tracer transport simulation results also revealed additional features of focused flow and transport through the fracture network.

Filtration↗
PubMedDate not supplied

Estimation of percolation flux from borehole temperature data at Yucca Mountain, Nevada.

Temperature data from the unsaturated zone (UZ) at Yucca Mountain are analyzed to estimate percolation-flux rates and overall heat flux. A multilayer, one-dimensional analytical solution is presented for determining percolation flux from temperature data. Case studies have shown that the analytical solution agrees very well with results from the numerical code, TOUGH2. The results of the analysis yield percolation fluxes in the range from 0 to 20 mm/year for most of the deep boreholes. This range is in good agreement with the results of infiltration studies at Yucca Mountain. Percolation flux for the shallower boreholes, however, cannot be accurately determined from temperature data alone because large gas flow in the shallow system alters the temperature profiles. Percolation-flux estimates for boreholes located near or intersecting major faults are significantly higher than those for other boreholes. These estimates may be affected by gas flow in the faults.

Forecasting↗
PubMedDate not supplied

Transport of a reactive tracer in saturated alluvium described using a three-component cation-exchange model.

A weakly sorbing cation, lithium, will be used as a reactive tracer in upcoming field tracer tests in the saturated alluvium south of Yucca Mountain, Nevada. One objective of the field tests is to determine how well field-scale reactive transport can be predicted using transport parameters derived from laboratory experiments. This paper describes several laboratory lithium batch sorption and column transport experiments that were conducted using ground water and alluvium obtained from the site of the planned field tests. In the batch experiments, isotherms were determined over 2.5 orders of magnitude of lithium concentrations, corresponding to the range expected in the field tests. In addition to measuring equilibrium lithium concentrations, concentrations of other cations, namely Na(+), K(+), and Ca(2+), were measured in the batch tests to determine Li(+)-exchangeable equilibria. This information was used in conjunction with alluvium cation exchange capacity measurements to parameterize a three-component cation-exchange model (EQUIL) that describes lithium sorption in the alluvium system. This model was then applied to interpret the transport behavior of lithium ion in saturated alluvium column tests conducted at three different lithium bromide injection concentrations. The concentrations were selected such that lithium ion either dominated, accounted for a little over half, or accounted for only a small fraction of the total cation equivalents in the injection solution. Although tracer breakthrough curves differed significantly under each of these conditions, with highly asymmetric responses occurring at the highest injection concentrations, the three-component cation-exchange model reproduced the observed transport behavior of lithium and the other cations in each case with a similar set of model parameters. In contrast, a linear K(d)-type sorption model could only match the lithium responses at the lowest injection concentration. The three-component model will be used to interpret the field tests, with the expectation that it will help refine estimates of effective flow porosity, particularly if the lithium response curves are asymmetric.

Adsorption↗
PubMedDate not supplied

Modeling dispersion in three-dimensional heterogeneous fractured media at Yucca Mountain.

Highly resolved numerical simulations are conducted to evaluate the longitudinal and transverse dispersivities proposed for use in the larger-scale Yucca Mountain saturated zone (SZ) site-scale model. Two different stochastic continuum models (SCM) that define the spatial variability of permeability are inferred from the observed fracture characteristics and the measured permeabilities. These models are created with a combination of indicator geostatistics and boolean simulation that allow for modeling different correlation lengths and anisotropy ratios at different permeability thresholds as well as the inclusion of large, high-permeability features. Longitudinal and transverse (horizontal and vertical) dispersion through the permeability realizations is evaluated for both distributed and focused source geometries using groundwater flow and streamline particle tracking. These numerical results are compared to behavior predicted by an analytical solution and to dispersivities estimated by an expert panel. Early time transport results are significantly non-Gaussian due to the strong heterogeneity of the fractured medium. At late times, travel distances of 23 correlation lengths, the longitudinal and transverse horizontal dispersivity results are well approximated by the analytical solution and the expert elicitation estimates. The calculated transverse vertical dispersivity values are smaller than those estimated from the analytical solution. Inclusion of high-permeability features of the same size as the model domain with a distributed planar source creates extreme values of the longitudinal and transverse horizontal dispersivity.

Forecasting↗
PubMedDate not supplied

The site-scale saturated zone flow model for Yucca Mountain: calibration of different conceptual models and their impact on flow paths.

This paper presents several different conceptual models of the Large Hydraulic Gradient (LHG) region north of Yucca Mountain and describes the impact of those models on groundwater flow near the potential high-level repository site. The results are based on a numerical model of site-scale saturated zone beneath Yucca Mountain. This model is used for performance assessment predictions of radionuclide transport and to guide future data collection and modeling activities. The numerical model is calibrated by matching available water level measurements using parameter estimation techniques, along with more informal comparisons of the model to hydrologic and geochemical information. The model software (hydrologic simulation code FEHM and parameter estimation software PEST) and model setup allows for efficient calibration of multiple conceptual models. Until now, the Large Hydraulic Gradient has been simulated using a low-permeability, east-west oriented feature, even though direct evidence for this feature is lacking. In addition to this model, we investigate and calibrate three additional conceptual models of the Large Hydraulic Gradient, all of which are based on a presumed zone of hydrothermal chemical alteration north of Yucca Mountain. After examining the heads and permeabilities obtained from the calibrated models, we present particle pathways from the potential repository that record differences in the predicted groundwater flow regime. The results show that Large Hydraulic Gradient can be represented with the alternate conceptual models that include the hydrothermally altered zone. The predicted pathways are mildly sensitive to the choice of the conceptual model and more sensitive to the quality of calibration in the vicinity on the repository. These differences are most likely due to different degrees of fit of model to data, and do not represent important differences in hydrologic conditions for the different conceptual models.

Calibration↗
PubMed2001

Seabed gamma-ray spectrometry: applications at IAEA-MEL.

The technique of underwater gamma-ray spectrometry has been developed to complement or replace the traditional sampling-sample analysis approach for applications with space-time constraints, e.g. large areas of investigation, emergency response or long-term monitoring. IAEA-MEL has used both high-efficiency NaI(Tl) and high-resolution HPGe spectrometry to investigate contamination with anthropogenic radionuclides in a variety of marine environments. Surveys at the South Pacific nuclear test sites of Mururoa and Fangataufa have been used to guide sampling in areas of high contamination around ground zero points. In the Irish Sea offshore from the Sellafield nuclear reprocessing plant, a gamma-ray survey of seabed sediment was carried out to obtain estimates of the distribution and subsequently, for the inventory of 137Cs in the investigated area.

Air Pollution, Radioactive↗
PubMed2003

Immobilization of iodide on copper(I) sulfide minerals.

In the goal of finding efficient scavengers for radioiodide in conditions (pH, pE) close to those encountered in deep geological sites, sorption of iodide ions on cuprous sulfide minerals (especially roxbyite, Cu(1.75)S) has been studied. Surface analysis by X-ray photoelectron spectroscopy has shown that commercial cuprous sulfides are covered by an oxidized overlayer (mainly in the form of CuSO(4)). Therefore, a synthetic procedure to get roxbyite (typically by mixing Na(2)S with an aqueous suspension of commercial Cu(2)O) was applied to produce pure samples with clean surfaces. Batch equilibration of cuprous sulfide particles suspended in aqueous solutions containing iodide species has revealed significant consumption of iodide. The sorption mechanism involves the formation of a surface complex via the exchange of surface hydroxyl groups by iodide anions, as highlighted by a transient pH increase during the immobilization process. Other copper and mixed copper-iron sulfides (e.g. CuS, CuFeS(2)), which are stable over wide pH and potential ranges are also likely to accumulate iodide species. Because of the specific interaction between iodide and copper(I) centers on the minerals, high distribution coefficients (>1000 ml/g) were observed.

Adsorption↗
PubMed2003

Sorption of selenium anionic species on apatites and iron oxides from aqueous solutions.

The sorption of selenite and selenate ions from aqueous solutions was investigated on hydroxyapatite, fluorapatite, goethite and hematite, in order to simulate the behavior of radioactive selenium in natural or artificial sorbing media. Correlation studies with acido-basic properties and solubility of the solids were also performed. The sorption is pH dependant, but these solids are very efficient for retaining selenite at pH values generally encountered in natural waters, with however higher K(d) values for oxides than apatites. Selenate ions are much less sorbed than selenite. Several methods such as electron microscopy and spectroscopic techniques were used to identify the sorption mechanisms. In the case of hydroxyapatite, sorption proceeds by substitution of phosphate groups in the lattice of the apatite crystal in the superficial layers of the solid. In the case of goethite and hematite, sorption can be interpreted and modeled by a surface complexation process, but there is a discrepancy between sorption site densities for selenite and for protons.

Adsorption↗
PubMed2002

Oxidative pyrolysis of organic ion exchange resins in the presence of metal oxide catalysts.

Pretreatment of the organic ion exchange resins by oxidative pyrolysis is effective for volume reduction before vitrification. In this work, pyrolysis of two nuclear-grade resins, Purolite NRW100 (cationic) and NRW400 (anionic), was examined using a laboratory-scale theromgravimetric analyzer (TGA) in air. It was shown that the cationic resin was harder to degrade and was less volatile compared to anionic resin. Off-gas data revealed the presence of SO2, CO2, CO, and H2O during oxidative pyrolysis of cationic resin from 30 to 800 degrees C. Trimethylamine, CO2, CO, and ethyl formate were found in the case of anionic resin. In addition, oxidative pyrolysis of the mixed resins (50/50 wt.%) showed the existence of the gases nearly at the temperatures where the gases would evolve if the results of two different resins were superimposed. Several metal salts including CuSO4*5H2O, CuO, and FeSO4*7H2O, as well as the ions Cu2+ pre-loaded on the resins had a catalytic effect on the oxidative pyrolysis of cationic resins, in which the decomposition of functional groups and polymer matrices was enhanced. Such catalytic effect was highlighted by a large decrease in activation energy calculated according to a degradation mechanism involving four consecutive reactions.

Catalysis↗
PubMed2003

Thorium removal by different adsorbents.

The removal of radiotoxic Th(4+) from aqueous solutions has been explored using two different groups of adsorptive materials (e.g. two activated carbons and four zeolites-two natural and two synthetic). The activated carbons were prepared from solvent extracted olive pulp (SEOP) and olive stone (OS) by a two-step physical activation method with steam. They were characterized by N(2) at 77K adsorption, Hg porosimetry and by determination of their iodine number. All carbons prepared are of the H-type (e.g. contain mainly basic surface oxides) confirmed by the results of the Boehm's method. The natural zeolites, clinoptilolite (NaCLI) and mordenite (NaMOR), were pretreated with Na(+) before the adsorption experiments, while the synthetic ones, NaX and NaA, were provided in their commercial sodium form. The natural zeolites, NaCLI and NaMOR, utilized 11.5 and 38.6% of the theoretical ion-exchange capacity, based on Al content, respectively, while NaX and NaA utilized 41.5 and 45.9%, respectively. The activated carbons showed better removal capability than NaCLI. NaMOR, showed comparable results to the carbon originated from OS, but lower removal capability than the carbon originated from SEOP. The synthetic zeolites showed the highest removal ability for thorium ions due to their increased ion-exchange capacity because of their cleaner and larger framework channels and their higher number of ion-exchange sites. The carbons adsorption capacity mainly depends on the content and nature of functional surface groups. The adsorption data were fitted to Langmuir and Freundlich models. The former achieved best fits and was further applied to obtain the respective Langmuir constant and maximum adsorption capacity for each system.

Adsorption↗