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PubMed2003

An analytical model for the interpretation of pulse injection experiments performed for testing the spatial variability of clay formations.

This paper presents an analytical model to describe pulse injection experiments. This model solves the advection-diffusion equation while taking into account back diffusion from the clay core to the inlet and from the outlet to the clay core. In most analytical models, back diffusion is neglected. For sufficiently high Péclet numbers, this is a good approximation. However, in experiments where the Péclet number is low, back diffusion is important and must be taken into account. An additional advantage of the present model is that both concentration and flux are conserved at the inlet and at the outlet of the clay core. This model is used to fit pulse injection experiments with iodide and tritiated water (HTO) in clay cores. The (new) model is required for fitting the experimental results since in clay layers advection is very slow leading to a low Péclet number. The experiments are performed on clay cores taken from different depths from the Boom Clay and the Ypres Clay layer under the site of the nuclear power plant of Doel (Belgium). The quality of all fits is excellent and the obtained parameter values are coherent. For HTO, the fitted value for the diffusion accessible porosity is consistent with measurements of the water content in Ypres Clay cores. In both types of clays, the apparent diffusion coefficient at zero flow is between 10(-10) and 2 x 10(-10) m(2)/s for iodide and between 2 x 10(-10) and 3 x 10(-10) m(2)/s for HTO. The dispersion length is in the order of 10(-3) m. The average value for the diffusion accessible porosity is between 0.35 and 0.4 for HTO and between 0.2 and 0.25 for iodide.

Aluminum Silicates↗
PubMed2003

Modelling of nonreactive tracer dipole tests in a shear zone at the Grimsel test site.

The investigation of the migration of a high pH plume in a fractured shear zone is foreseen by a long-term experiment at the Grimsel rock laboratory. In order to characterise the initial conditions for the long-term experiment and to evaluate an optimal hydraulic in situ set-up, several dipole experiments with nonreacting tracers have been performed. The dipole experiments differ in geometry, pumping rates and orientation to the background water flow. Several single and double-porosity models have been applied to fit the results of these dipole tracer tests in order to extract values for some transport parameters and discriminate for certain transport processes. A two-dimensional porous medium approach was successfully used to fit tracer breakthrough curves measured for a dipole experiment. A model based on a one-dimensional dual porous medium approach was also successful, although the applied hydraulic dipole, with similar injection and extraction rates, suggests the existence of an extended two-dimensional flow field. For the two-dimensional porous medium approach, tracer breakthrough could only be fitted with a complex flow field geometry within the heterogeneous fractured shear zone. The heterogeneity was generated by heterogeneous porosity and hydraulic permeability distributions. Predictions for further dipole geometries and a sorbing tracer have been calculated by means of both models using the flow and transport parameters deduced from fits for a single dipole experiment. This allows for comparison with the measured breakthrough of sorbing tracers. The foreseen experiment with sorbing (radionuclide) tracers will help decide on the appropriate approach that should be used to describe such dipole experiments in this shear zone. Additionally, the migration and spreading of a solution with high pH has been calculated taking into account mineral dissolution and precipitation in a two-dimensional porous medium approach in order to estimate the amount and character of the mineral reactions induced by the interaction between the high pH solution and the rock.

Geological Phenomena↗
PubMed2003

A sensibility analysis of model selection in modeling the reactive transport of cesium in crushed granite.

We performed a sensibility analysis of model selection in modeling the reactive transport of cesium in crushed granite through model calibration and validation. Based on some solid phase analysis data and kinetic batch experimental results, we hypothesized three two-site sorption models in the LEHGC reactive transport model to fit the breakthrough curves (BTCs) from the corresponding column experiments. The analysis of breakthrough curves shows that both the empirical two-site kinetic linear sorption model and the semi-mechanistic/semi-empirical two-site kinetic surface complexation model, regardless of their complexity, can match our experimental data fairly well under given test conditions. A numerical experiment to further compare the two models shows that they behave differently when the pore velocity is not of the same order of magnitude as our test velocities. This result indicates that further investigations to help determine a better model are needed. We suggest that a multistage column experiment, which tests over the whole range of practical flow velocities, should be conducted to help alleviate inadequate hypothesized models.

Calibration↗
PubMed2003

Determination of the flow-wetted surface in fractured media.

Diffusion and sorption in the rock matrix are important retardation mechanisms for radionuclide transport in fractured media. For the conditions existing in a deep repository in crystalline rock, interaction with the rock matrix is controlled by the water flowrate in the fractures and the surface area in contact with the flowing water (the so-called "flow-wetted surface" (FWS)). The flow-wetted surface may be determined from the frequency of open fractures intersecting a borehole. The choice of packer distance used in these hydraulic measurements is crucial, however, since several open fractures may be found in one packer interval. The use of a packer distance that is too large may result in a considerable underestimation of the flow-wetted surface. This is especially important in zones with a high frequency of open fractures (fracture zones) where a small packer distance is a fundamental requirement. A large volume of hydraulic data has been compiled in Sweden from measurements using quite small packer distances. Over the last decade, the most common packer distance used for the hydraulic tests has been 3 m, although some new measurements using a shorter packer distance have also been performed. In several cases, the resolution of these measurements has been less than 0.5 m. All these data have been analysed in detail. From these data, the flow-wetted surface has been calculated and compared with the flow-wetted surface estimated in earlier studies. The results show the importance of using a small packer distance for carrying out borehole transmissivity measurements.

Adsorption↗
PubMed2003

Interpretation of out-diffusion experiments on crystalline rocks using random walk modeling.

Matrix diffusion in saturated rocks with very low permeability is one of the major mechanisms of solute transport. Laboratory out-diffusion experiments on rock samples may provide an estimate of the bulk diffusion coefficient. However, numerous results have shown that this average parameter does not really depict the complex mechanism of diffusion as a function of the internal heterogeneity of crystalline rocks. Two-dimensional images of the porosity distribution in a granite sample were obtained by impregnation with a radioactive resin and autoradiography. Some examples based on these images and synthetic images were used to perform numerical simulations of out-diffusion using two different random walk methods. The simulated shapes of the out-diffusion curves depend on the spatial distribution of the porosity and on the pore connectivity with the border of the sample. Such relations might explain the multiple nested slopes or the convex shapes often observed on real experimental curves.

Diffusion↗
PubMed2003

Sensitivity analysis of radionuclide migration in compacted bentonite: a mechanistic model approach.

Mechanistic model calculations for the migration of Cs, Ra, Am and Pb in compacted bentonite have been carried out to evaluate sensitivities with respect to different parameter variations. A surface chemical speciation/electric double layer model is used to calculate: (i) porewater composition and radionuclide speciation in solution and at the bentonite surface, yielding the distribution of mobile and sorbed species and (ii) interaction of diffusing species with negatively charged pore walls to obtain diffusion parameters. The basic scenario considers the interaction of compacted bentonite with a fresh-type groundwater; variations include the presence of bentonite impurities and saline groundwater. It is shown that these scenarios result in significant variations of porewater composition that affect migration via three mechanisms that can partly compensate each other: (1) effects on sorption through radionuclide complexation in solution, and competition of major cations for surface sites; (2) changes in radionuclide solution speciation leading to different diffusing species under different conditions; (3) effects on diffusion through changes in the electric double layer properties of the clay pores as a function of ionic strength.

Aluminum Silicates↗
PubMed2003

Release of uranium from rock matrix--a record of glacial meltwater intrusions?

Uranium release observed in a rock matrix around water-carrying fractures was studied using U-series disequilibrium (USD) modelling and mass balance calculations. Several release scenarios were tested, with specific attention to the glacial aspects. The release appears to have occurred in two or three violent episodes during the last 300 ky. A release after the last glaciation can be excluded on mass flow grounds. Continuous release for more than 300 ky can be excluded on radioactive disequilibrium grounds. Repeated inflows of oxic glacial meltwater seem to have triggered the release episodes.

Environmental Monitoring↗
PubMed2003

Swedish-German actinide migration experiment at ASPO hard rock laboratory.

Within the scope of a bilateral cooperation between Svensk Kärnbränslehantering (SKB) and Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung (FZK-INE), an actinide migration experiment is currently being performed at the Aspö Hard Rock Laboratory (HRL) in Sweden. This paper covers laboratory and in situ investigations on actinide migration in single-fractured granite core samples. For the in situ experiment, the CHEMLAB 2 probe developed by SKB was used. The experimental setup as well as the breakthrough of inert tracers and of the actinides Am, Np and Pu are presented. The breakthrough curves of inert tracers were analyzed to determine hydraulic properties of the fractured samples. Postmortem analyses of the solid samples were performed to characterize the flow path and the sorbed actinides. After cutting the cores, the abraded material was analyzed with respect to sorbed actinides. The slices were scanned optically to visualize the flow path. Effective volumes and inner surface areas were measured. In the experiments, only breakthrough of Np(V) was observed. In each experiment, the recovery of Np(V) was < or = 40%. Breakthrough of Am(III) and Pu(IV) as well as of Np(IV) was not observed.

Actinoid Series Elements↗
PubMed2003

Characterisation of HTO diffusion properties by an in situ tracer experiment in Opalinus clay at Mont Terri.

A long-term single borehole diffusion experiment using tritiated water as tracer was carried out in Opalinus clay, an argillaceous rock formation that is accessible at the Mont Terri Underground Research Laboratory, situated in the Swiss Jura. The tracer was diluted in reconstituted formation water and introduced into a packed-off section of a borehole located in saturated rock. Pressure in this interval was maintained equal to the pore pressure of the surrounding rock in order to prevent any hydraulic gradient around the borehole and to avoid advective transport processes. The evolution of the tracer concentration in the injection system was monitored over time. After 1 year of diffusion, the claystone surrounding the interval was retrieved by overcoring the whole borehole and packer system, and by an adjacent oblique borehole. Compressed air was used as drilling fluid to reduce rock disturbances. The recovered overcore was sampled along profiles perpendicular to the borehole wall with a view to determining the tracer-concentration profiles in the rock. To avoid further evaporation of tritiated water, subsamples were immediately transferred into polyethylene bottles and disaggregated by adding a known amount of tracer-free water. Fifteen profiles were determined and showed a decreasing tracer concentration with distance into the rock. The pore-water contents were constant along those profiles, confirming that only very little water was lost during overcoring operations. The evolution of tritium-tracer concentration in the injection system over time and in situ profiles were interpreted with a 3-D numerical simulation of the experiment. That allowed for the identification of the transport parameters (orthotropic diffusion tensor and porosity) by minimising the relative quadratic error between the experimental and simulated data. The fitting is good and the results are consistent with data obtained on drill-core samples. The result of tritiated water is discussed regarding (1) the potential effect of mechanical and/or chemical disturbances around the injection borehole and (2) the specific behaviour of tritiated water.

Aluminum Silicates↗
PubMed2003

In situ diffusion experiment in granite: phase I.

A program of in situ experiments, supported by laboratory studies, was initiated to study diffusion in sparsely fractured rock (SFR), with a goal of developing an understanding of diffusion processes within intact crystalline rock. Phase I of the in situ diffusion experiment was started in 1996, with the purpose of developing a methodology for estimating diffusion parameter values. Four in situ diffusion experiments, using a conservative iodide tracer, were performed in highly stressed SFR at a depth of 450 m in the Underground Research Laboratory (URL). The experiments, performed over a 2 year period, yielded rock permeability estimates of 2 x 10(-21) m(2) and effective diffusion coefficients varying from 2.1 x 10(-14) to 1.9 x 10(-13) m(2)/s, which were estimated using the MOTIF code. The in situ diffusion profiles reveal a characteristic "dog leg" pattern, with iodide concentrations decreasing rapidly within a centimeter of the open borehole wall. It is hypothesized that this is an artifact of local stress redistribution and creation of a zone of increased constrictivity close to the borehole wall. A comparison of estimated in situ and laboratory diffusivities and permeabilities provides evidence that the physical properties of rock samples removed from high-stress regimes change. As a result of the lessons learnt during Phase I, a Phase II in situ program has been initiated to improve our general understanding of diffusion in SFR.

Diffusion↗
PubMed2003

Solute transport in crystalline rocks at Aspö--II: blind predictions, inverse modelling and lessons learnt from test STT1.

Based on the results from detailed structural and petrological characterisation and on up-scaled laboratory values for sorption and diffusion, blind predictions were made for the STT1 dipole tracer test performed in the Swedish Aspö Hard Rock Laboratory. The tracers used were nonsorbing, such as uranine and tritiated water, weakly sorbing 22Na(+), 85Sr(2+), 47Ca(2+)and more strongly sorbing 86Rb(+), 133Ba(2+), 137Cs(+). Our model consists of two parts: (1) a flow part based on a 2D-streamtube formalism accounting for the natural background flow field and with an underlying homogeneous and isotropic transmissivity field and (2) a transport part in terms of the dual porosity medium approach which is linked to the flow part by the flow porosity. The calibration of the model was done using the data from one single uranine breakthrough (PDT3). The study clearly showed that matrix diffusion into a highly porous material, fault gouge, had to be included in our model evidenced by the characteristic shape of the breakthrough curve and in line with geological observations. After the disclosure of the measurements, it turned out that, in spite of the simplicity of our model, the prediction for the nonsorbing and weakly sorbing tracers was fairly good. The blind prediction for the more strongly sorbing tracers was in general less accurate. The reason for the good predictions is deemed to be the result of the choice of a model structure strongly based on geological observation. The breakthrough curves were inversely modelled to determine in situ values for the transport parameters and to draw consequences on the model structure applied. For good fits, only one additional fracture family in contact with cataclasite had to be taken into account, but no new transport mechanisms had to be invoked. The in situ values for the effective diffusion coefficient for fault gouge are a factor of 2-15 larger than the laboratory data. For cataclasite, both data sets have values comparable to laboratory data. The extracted K(d) values for the weakly sorbing tracers are larger than Swedish laboratory data by a factor of 25-60, but agree within a factor of 3-5 for the more strongly sorbing nuclides. The reason for the inconsistency concerning K(d)s is the use of fresh granite in the laboratory studies, whereas tracers in the field experiments interact only with fracture fault gouge and to a lesser extent with cataclasite both being mineralogically very different (e.g. clay-bearing) from the intact wall rock.

Calibration↗
PubMed2003

Influence of the mode of matrix porosity determination on matrix diffusion calculations.

The theoretical basis for matrix diffusion in fractured rocks and the methodology for the determination of diffusion coefficients in the laboratory are well established. One significant problem, however, remains in that it is difficult to quantify the degree of sample disturbance affecting the geometrical, geophysical and hydraulic properties of the rock matrix. A new technique, with in situ rock impregnation with resin, for examining the diffusion-accessible rock matrix has been developed and successfully adopted to the rock matrix behind a water-conducting fracture in host crystalline rocks at Nagra's Grimsel Test Site in Switzerland and JNC's Kamaishi In Situ Test Site in Japan. In line with the results of a large number of natural analogue and laboratory studies, the existence of an in situ interconnected pore network was substantiated. Matrix porosities determined on the laboratory samples from both the sites are 1.5-3 times higher than in situ values, irrespective of the technique applied. On the Grimsel granodiorite matrix, matrix porosity existing in situ and artefacts of stress release and physical disturbance, induced by sampling and sample preparation, were clearly distinguished, allowing in situ porosity to be quantified. Laboratory work with conventional techniques tends to overestimate the porosity of the rock matrix, hence leading to an overestimation of in situ matrix diffusion. The implications of these differences to a repository performance assessment are assessed with a couple of examples from existing assessments, and recommendations for future approaches to the examination of in situ matrix porosity are made.

Diffusion↗
PubMed2003

Modelling of silica diffusion experiments with 32Si in Boom Clay.

A mathematical model describing the dissolution of nuclear glass directly disposed in clay combines a first-order dissolution rate law with the diffusion of dissolved silica in clay. According to this model, the main parameters describing the long-term dissolution of the glass are etaR, the product of the diffusion accessible porosity eta and the retardation factor R, and the apparent diffusion coefficient D(app) of dissolved silica in clay. For determining the migration parameters needed for long-term predictions, four Through-Diffusion (T-D) experiments and one percolation test have been performed on undisturbed clay cores. In the Through-Diffusion experiments, the concentration decrease after injection of 32Si (radioactive labelled silica) was measured in the inlet compartment. At the end of the T-D experiments, the clay cores were cut in thin slices and the activity of labelled silica in each slice was determined. The measured activity profiles for these four clay cores are well reproducible. Since no labelled silica could be detected in the outlet compartments, the Through-Diffusion experiments are fitted by two In-Diffusion models: one model assuming linear and reversible sorption equilibrium and a second model taking into account sorption kinetics. Although the kinetic model provides better fits, due to the sufficiently long duration of the experiments, both models give approximately similar values for the fit parameters. The single percolation test leads to an apparent diffusion coefficient value about two to three times lower than those of the Through-Diffusion tests. Therefore, dissolved silica appears to be strongly retarded in Boom Clay. A retardation factor R between 100 and 300 was determined. The corresponding in situ distribution coefficient K(d) is in the range 25-75 cm(3) g(-1). The apparent diffusion coefficient of dissolved silica in Boom Clay is estimated between 2 x 10(-13) and 7 x 10(-13) m(2) s(-1). The pore diffusion coefficient is in the range from 6 x 10(-11) to 1 x 10(-10) m(2) s(-1).

Aluminum Silicates↗
PubMedDate not supplied

Experimental and numerical simulation of dissolution and precipitation: implications for fracture sealing at Yucca Mountain, Nevada.

Plugging of flow paths caused by mineral precipitation in fractures above the potential repository at Yucca Mountain, Nevada could reduce the probability of water seeping into the repository. As part of an ongoing effort to evaluate thermal-hydrological-chemical (THC) effects on flow in fractured media, we performed a laboratory experiment and numerical simulations to investigate mineral dissolution and precipitation under anticipated temperature and pressure conditions in the repository. To replicate mineral dissolution by vapor condensate in fractured tuff, water was flowed through crushed Yucca Mountain tuff at 94 degrees C. The resulting steady-state fluid composition had a total dissolved solids content of about 140 mg/l; silica was the dominant dissolved constituent. A portion of the steady-state mineralized water was flowed into a vertically oriented planar fracture in a block of welded Topopah Spring Tuff that was maintained at 80 degrees C at the top and 130 degrees C at the bottom. The fracture began to seal with amorphous silica within 5 days.A 1-D plug-flow numerical model was used to simulate mineral dissolution, and a similar model was developed to simulate the flow of mineralized water through a planar fracture, where boiling conditions led to mineral precipitation. Predicted concentrations of the major dissolved constituents for the tuff dissolution were within a factor of 2 of the measured average steady-state compositions. The mineral precipitation simulations predicted the precipitation of amorphous silica at the base of the boiling front, leading to a greater than 50-fold decrease in fracture permeability in 5 days, consistent with the laboratory experiment.These results help validate the use of a numerical model to simulate THC processes at Yucca Mountain. The experiment and simulations indicated that boiling and concomitant precipitation of amorphous silica could cause significant reductions in fracture porosity and permeability on a local scale. However, differences in fluid flow rates and thermal gradients between the experimental setup and anticipated conditions at Yucca Mountain need to be factored into scaling the results of the dissolution/precipitation experiments and associated simulations to THC models for the potential Yucca Mountain repository.

Chemical Precipitation↗
PubMedDate not supplied

Parallel computing simulation of fluid flow in the unsaturated zone of Yucca Mountain, Nevada.

This paper presents the application of parallel computing techniques to large-scale modeling of fluid flow in the unsaturated zone (UZ) at Yucca Mountain, Nevada. In this study, parallel computing techniques, as implemented into the TOUGH2 code, are applied in large-scale numerical simulations on a distributed-memory parallel computer. The modeling study has been conducted using an over-1-million-cell three-dimensional numerical model, which incorporates a wide variety of field data for the highly heterogeneous fractured formation at Yucca Mountain. The objective of this study is to analyze the impact of various surface infiltration scenarios (under current and possible future climates) on flow through the UZ system, using various hydrogeological conceptual models with refined grids. The results indicate that the 1-million-cell models produce better resolution results and reveal some flow patterns that cannot be obtained using coarse-grid modeling models.

Environmental Monitoring↗
PubMedDate not supplied

Chemical analyses of pore water from boreholes USW SD-6 and USW WT-24, Yucca Mountain, Nevada.

Analyses of pore water extracted from cores of boreholes USW SD-6 in the central part and USW WT-24 in the northern part of Yucca Mountain, Nevada, show significant vertical and lateral variations in dissolved-ion concentrations. Analyses of samples of only a few milliliters of pore water extracted by uniaxial or triaxial compression and by ultracentrifugation methods from adjacent core samples are generally in agreement, within the analytical error of 10% to 15%. However, the values of silica for water obtained by ultracentrifugation are consistently lower than values for water obtained by compression. The larger concentrations probably are due to localized pressure solution of silicate minerals during compression. The shallower water from core in borehole USW SD-6 was extracted from nonwelded units collectively referred to as the Paintbrush Tuff nonwelded (PTn). The deeper water was from core in both boreholes USW SD-6 and USW WT-24 in the nonwelded units referred to as the Calico Hills nonwelded (CHn). Significant differences in mean dissolved-ion concentrations in pore water between the PTn and CHn are (1) decreases in Ca, Mg, SO(4), and NO(3) and (2) increases in HCO(3) and (Na+K)/(Ca+Mg) ratios. The decrease in NO(3) and the increase in HCO(3) could be the result of denitrification through the oxidation of organic matter. The decrease in Ca and associated increase in (Na+K)/(Ca+Mg) is the result of ion exchange with zeolites in the CHn in borehole USW WT-24. This effect is not nearly as pronounced in borehole USW SD-6, probably reflecting a smaller amount of zeolitization of the CHn in USW SD-6. Geochemical calculations using the PHREEQC code indicate that the pore water from both boreholes USW SD-6 and USW WT-24 is uniformly undersaturated in anhydrite, gypsum, and amorphous silica, but supersaturated in quartz and chalcedony. The saturation of calcite, aragonite, sepiolite, and dolomite is more variable from sample to sample.

Environmental Monitoring↗
PubMedDate not supplied

Evolution of the unsaturated zone testing at Yucca Mountain.

The evaluation of the Yucca Mountain site has evolved from intensive surface-based investigations in the early 1980s to current focus on testing in underground drifts. Different periods of site characterization activities and prominent issues concerning the unsaturated zone (UZ) are summarized. Data collection activities have evolved from mapping of faults and fractures to estimation of percolation through tuff layers, and to quantification of seepage into drifts. Evaluation of discrete flow paths in drifts has led to fracture-matrix interaction and matrix diffusion tests over different scales. The effects of tuff interfaces and local faults are evaluated in fractured-welded and porous-nonwelded units. Mobilization of matrix water and redistribution of moisture are measured in thermal tests. Lessons learned from underground tests are used to focus on processes needed for additional quantification. Migration through the drift shadow zone and liquid flow through faults are two important issues that have evolved from current knowledge.

Environmental Monitoring↗
PubMedDate not supplied

A geostatistical modeling study of the effect of heterogeneity on radionuclide transport in the unsaturated zone, Yucca Mountain.

Retardation of certain radionuclides due to sorption to zeolitic minerals is considered one of the major barriers to contaminant transport in the unsaturated zone of Yucca Mountain. However, zeolitically altered areas are lower in permeability than unaltered regions, which raises the possibility that contaminants might bypass the sorptive zeolites. The relationship between hydrologic and chemical properties must be understood to predict the transport of radionuclides through zeolitically altered areas. In this study, we incorporate mineralogical information into an unsaturated zone transport model using geostatistical techniques to correlate zeolitic abundance to hydrologic and chemical properties. Geostatistical methods are used to develop variograms, kriging maps, and conditional simulations of zeolitic abundance. We then investigate, using flow and transport modeling on a heterogeneous field, the relationship between percent zeolitic alteration, permeability changes due to alteration, sorption due to alteration, and their overall effect on radionuclide transport. We compare these geostatistical simulations to a simplified threshold method in which each spatial location in the model is assigned either zeolitic or vitric properties based on the zeolitic abundance at that location. A key conclusion is that retardation due to sorption predicted by using the continuous distribution is larger than the retardation predicted by the threshold method. The reason for larger retardation when using the continuous distribution is a small but significant sorption at locations with low zeolitic abundance. If, for practical reasons, models with homogeneous properties within each layer are used, we recommend setting nonzero K(d)s in the vitric tuffs to mimic the more rigorous continuous distribution simulations. Regions with high zeolitic abundance may not be as effective in retarding radionuclides such as Neptunium since these rocks are lower in permeability and contaminants can only enter these regions through molecular diffusion.

Adsorption↗