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Development and testing of radionuclide transport models for fractured rock: examples from the Nagra/JNC Radionuclide Migration Programme in the Grimsel Test Site, Switzerland.

The joint Swiss National Co-operative for the Disposal of Radioactive Waste (Nagra)/Japan Nuclear Cycle Development Institute (JNC) Radionuclide Migration Programme has now been on-going for over a decade in Nagra's Grimsel Test Site (GTS). The main aim of the programme has been the direct testing of radionuclide transport models in as realistic manner as possible. Although it will never be possible to fully test these models due to the large time and distance scales involved, tests of the model assumptions in scaled down but otherwise realistic conditions will contribute to developing confidence in the predictive power of the models. In this paper, the Nagra/JNC approach is highlighted with examples from a large programme of field, laboratory and natural analogue studies based around the GTS. The successes and failures are discussed as in the general approach to the thorough testing of predictive transport codes which will be used in repository performance assessment (PA). Some of the work is still on-going and this represents the first presentation of a unique set of results and conclusions.

Geological Phenomena↗

Removal of As, Mn, Mo, Se, U, V and Zn from groundwater by zero-valent iron in a passive treatment cell: reaction progress modeling.

Three treatment cells were operated at a site near Durango, CO. One treatment cell operated for more than 3 years. The treatment cells were used for passive removal of contamination from groundwater at a uranium mill tailings repository site. Zero-valent iron [Fe(0)] that had been powdered, bound with aluminosilicate and molded into plates was used as a reactive material in one treatment cell. The others used granular Fe(0) and steel wool. The treatment cells significantly reduced concentrations of As, Mn, Mo, Se, U, V and Zn in groundwater that flowed through it. Zero-valent iron [Fe(0)], magnetite (Fe3O4), calcite (CaCO3), goethite (FeOOH) and mixtures of contaminant-bearing phases were identified in the solid fraction of one treatment cell. A reaction progress approach was used to model chemical evolution of water chemistry as it reacted with the Fe(0). Precipitation of calcite, ferrous hydroxide [Fe(OH)2] and ferrous sulfide (FeS) were used to simulate observed changes in major-ion aqueous chemistry. The amount of reaction progress differed for each treatment cell. Changes in contaminant concentrations were consistent with precipitation of reduced oxides (UO2, V2O3), sulfides (As2S3, ZnS), iron minerals (FeSe2, FeMoO4) and carbonate (MnCO3). Formation of a free gas phase and precipitation of minerals contributed to loss of hydraulic conductivity in one treatment cell.

Arsenic↗

Flow and transport in unsaturated fractured rock: effects of multiscale heterogeneity of hydrogeologic properties.

The heterogeneity of hydrogeologic properties at different scales may have different effects on flow and transport processes in a subsurface system. A model for the unsaturated zone of Yucca Mountain, Nevada, is developed to represent complex heterogeneity at two different scales: (1) layer scale corresponding to geologic layering and (2) local scale. The layer-scale hydrogeologic properties are obtained using inverse modeling, based on the available measurements collected from the Yucca Mountain site. Calibration results show a significant lateral and vertical variability in matrix and fracture properties. Hydrogeologic property distributions in a two-dimensional, vertical cross-section of the site are generated by combining the average layer-scale matrix and fracture properties with local-scale perturbations generated using a stochastic simulation method. The unsaturated water flow and conservative (nonsorbing) tracer transport through the cross-section are simulated for different sets of matrix and fracture property fields. Comparison of simulation results indicates that the local-scale heterogeneity of matrix and fracture properties has a considerable effect on unsaturated flow processes, leading to fast flow paths in fractures and the matrix. These paths shorten the travel time of a conservative tracer from the source (repository) horizon in the unsaturated zone to the water table for small fractions of total released tracer mass. As a result, the local-scale heterogeneity also has a noticeable effect on global tracer transport processes, characterized by an average breakthrough curve at the water table, especially at the early arrival time of tracer mass. However, the effect is not significant at the later time after 20% tracer mass reaches the water table. The simulation results also verify that matrix diffusion plays an important role in overall solute transport processes in the unsaturated zone at Yucca Mountain.

Calibration↗

A reaction-transport model for calcite precipitation and evaluation of infiltration fluxes in unsaturated fractured rock.

The percolation flux in the unsaturated zone (UZ) is an important parameter addressed in site characterization and flow and transport modeling of the potential nuclear-waste repository at Yucca Mountain, NV, USA. The US Geological Survey (USGS) has documented hydrogenic calcite abundances in fractures and lithophysal cavities at Yucca Mountain to provide constraints on percolation fluxes in the UZ. The purpose of this study was to investigate the relationship between percolation flux and measured calcite abundances using reactive transport modeling. Our model considers the following essential factors affecting calcite precipitation: (1) infiltration, (2) the ambient geothermal gradient, (3) gaseous CO(2) diffusive transport and partitioning in liquid and gas phases, (4) fracture-matrix interaction for water flow and chemical constituents, and (5) water-rock interaction. Over a bounding range of 2-20 mm/year infiltration rate, the simulated calcite distributions capture the trend in calcite abundances measured in a deep borehole (WT-24) by the USGS. The calcite is found predominantly in fractures in the welded tuffs, which is also captured by the model simulations. Simulations showed that from about 2 to 6 mm/year, the amount of calcite precipitated in the welded Topopah Spring tuff is sensitive to the infiltration rate. This dependence decreases at higher infiltration rates owing to a modification of the geothermal gradient from the increased percolation flux. The model also confirms the conceptual model for higher percolation fluxes in the fractures compared to the matrix in the welded units, and the significant contribution of Ca from water-rock interaction. This study indicates that reactive transport modeling of calcite deposition can yield important constraints on the unsaturated zone infiltration-percolation flux and provide useful insight into processes such as fracture-matrix interaction as well as conditions and parameters controlling calcite deposition.

Calcium Carbonate↗

Observation and characterization of colloids derived from leached cement hydrates.

The possibility of colloid generation from cement hydrates in a cementitious repository environment has been investigated through leaching experiments. Pulverized samples of High Flyash and Silica fume-content Cement (HFSC) and 1:9 ordinary portland cement/blast furnace slag (1:9 OPC/BFS) hydrate were leached in low-salinity groundwater at three solid-to-liquid (S/L) mass ratios (1:5, 1:50 and 1:100), and two temperatures (20 and 60 degrees C) for durations of nearly 2 and 8 months. Detailed characterization of colloid populations has been undertaken by TEM coupled with X-ray analysis. In addition, the surface charge and stability behavior of colloids have been investigated. The colloid concentrations in HFSC hydrate leachates generated at 20 and 60 degrees C show similar trends with S/L ratio. The colloid concentrations of leachates with the lower S/L ratio (1:50 and 1:100) are in the range of 10(11)-10(12) particles per liter. The majority of these particles are composed predominantly of Si, Ca, and Al; the mean particle size is less than 100 nm. The lowest colloid concentrations are found in the leachates with the highest S/L ratios, and the colloid populations tend to be dominated by larger particles. HFSC-derived colloid stability is due to a high negative zeta potential at alkaline pH values, combined with a calcium concentration that is below the critical coagulation concentration (CCC) for the colloids. A preliminary interpretation of HFSC-derived colloid stability based on classical DLVO theory provides a semi-quantitative explanation of the dependence of colloid populations on the S/L ratio in the leaching experiments.

Colloids↗

Study of the contaminant transport into granite microfractures using nuclear ion beam techniques.

Hydrated bentonite is a very plastic material and it is expected to enter in the rock microfractures at the granite/bentonite boundary of a deep geological high-level waste repository. This process is enhanced by the high swelling pressure of the clay. Since bentonite has a very good sorption capability for many radionuclides, the displacement of the clay might lead to a "clay-mediated" contaminant transport into the rock. The aim of this work is to study the contaminant transport into granite microfractures using nuclear ion beam techniques, and to determine to what extent the clay can favour it. To do so, bentonite previously doped with uranium, cesium and europium was put in contact with the surface of granite sheets. Granite sheets contacted with non-doped bentonite and with radionuclide solutions were also prepared as references. This allowed analysing the differences in the diffusion behaviour of the three systems: clay, radionuclides and clay plus radionuclides. A combination of Rutherford backscattering spectrometry (RBS) and other nuclear ion-beam techniques such as particle-induced X-ray emission (PIXE) and microPIXE was used to study the depth and lateral distribution of clay and contaminants inside granite. It was also tried to evaluate not only the diffusion depth and diffusion coefficients but also the different areas of the granite where the diffusants have a preferential access.

Aluminum Silicates↗

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↗

Porewater chemistry in compacted re-saturated MX-80 bentonite.

Bentonites of various types are being investigated in many countries as backfill materials in high-level radioactive waste disposal concepts. Being able to understand the chemistry of the porewater in compacted bentonite is very important since it is critical to predicting radionuclide solubilities and to the synthesis of sorption data bases, and hence to repository safety studies. In this paper, porewater compositions in compacted bentonites are calculated, taking into consideration such factors as montmorillonite swelling, semi-permeable membrane effects, very low "free water" volumes, and the highly effective buffering characteristics of the exchangeable cations and the amphoteric edge sites. The former buffer the cation concentrations and the latter fix the pH in the porewater of a re-saturated bentonite. The above considerations are used in conjunction with previously measured physico-chemical characterisation data on MX-80 powder to calculate porewater compositions in compacted bentonites. For the MX-80 material specified, the porewaters calculated for initial dry densities between 1200 and 1600 kg m(-3) had relatively high ionic strengths (I approximately 0.3 M), similar cation concentrations and a pH equal to 8.0. The porewaters changed from being Na(2)SO(4)-rich at 1200 kg m(-3) to a NaCl/Na(2)SO(4) type water at 1600 kg m(-3).

Adsorption↗

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↗

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↗

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↗

Seepage into drifts with mechanical degradation.

Seepage into drifts in unsaturated tuff is an important issue for the long-term performance of the proposed nuclear waste repository at Yucca Mountain, Nevada. Drifts in which waste packages will be emplaced are subject to degradation in the form of rockfall from the drift ceiling, induced by stress-relief, seismic, or thermal effects. The objective of this study is to calculate seepage rates, for various drift-degradation scenarios and for different values of percolation flux, in the Topopah Spring middle nonlithophysal (Tptpmn) and the Topopah Spring lower lithophysal (Tptpll) units at Yucca Mountain. Seepage calculations are conducted by (1) defining a heterogeneous drift-scale permeability model with field data, (2) selecting calibrated parameters associated with the Tptpmn and Tptpll units, and (3) simulating seepage, based on detailed degraded-drift profiles obtained from a separate rock mechanics engineering analysis. The simulation results indicate (1) that the seepage threshold (i.e., the percolation flux at which seepage first occurs) is not significantly changed by drift degradation and (2) the degradation-induced increase in seepage above the threshold is influenced probably more by the shape of the cavity created by rockfall than by rockfall volume.

Geological Phenomena↗

Flow and transport in the drift shadow in a dual-continuum model.

The current concept for high-level radioactive waste disposal at Yucca Mountain is for the waste to be placed in underground tunnels (or drifts) in the middle of a thick unsaturated zone. Flow modeling and field testing have shown that not all flow encountering a drift will seep into the drift. The underlying reason for the diversion of unsaturated flow around a drift is that capillary forces in the fractures and matrix prevent water entry into the drift unless the capillary pressure in the rock decreases sufficiently to allow for gravity forces to overcome the capillary barrier. As a result of the capillary barrier effect, flow tends to be diverted around the drift, affecting the flow pattern beneath the drift. For some distance beneath the drift, water saturation and flux are reduced. This drift shadow zone is much more pronounced in the fractures than in the matrix due to dominance of gravity over capillary forces in the fractures. Moving downward, away from the drift, the shadow zone asymptotically re-equilibrates to the undisturbed flow conditions due to capillary forces. The behavior of radionuclide transport in this zone of reduced flow is investigated here because this will affect the amount of time required for radionuclides to penetrate the unsaturated zone. The delay of radionuclide movement in the geosphere is one aspect of the potential repository system that could limit public exposure to radioactive waste. The behavior of flow and transport is calculated using a two-dimensional, drift-scale dual-permeability model extending to nine drift diameters below the potential waste emplacement drift. The flow model is first compared with an analytical model for a single continuum. Then, the dual-continuum flow model is investigated with respect to drift-scale and mountain-scale property sets. Transport calculations are performed for a wide range of flow conditions and for different aqueous radionuclides and colloids. Findings indicate that transport times for dissolved or colloidal material released from a drift without seepage are several orders of magnitude longer than if the releases occurred in the undisturbed flow field. Furthermore, the calculations indicate that the transport rate for radionuclides released in the drift shadow is relatively insensitive to flow rates in the fractures, but is sensitive to the flow rate in the matrix.

Colloids↗

Inverse and predictive modeling of seepage into underground openings.

We discuss the development and calibration of a model for predicting seepage into underground openings. Seepage is a key factor affecting the performance of the potential nuclear-waste repository at Yucca Mountain, Nevada. Three-dimensional numerical models were developed to simulate field tests in which water was released from boreholes above excavated niches. Data from air-injection tests were geostatistically analyzed to infer the heterogeneous structure of the fracture permeability field. The heterogeneous continuum model was then calibrated against the measured amount of water that seeped into the opening. This approach resulted in the estimation of model-related, seepage-specific parameters on the scale of interest. The ability of the calibrated model to predict seepage was examined by comparing calculated with measured seepage rates from additional experiments conducted in different portions of the fracture network. We conclude that an effective capillary strength parameter is suitable to characterize seepage-related features and processes for use in a prediction model of average seepage into potential waste-emplacement drifts.

Calibration↗

Analytical solutions for reactive transport of N-member radionuclide chains in a single fracture.

Several numerical codes have been used to simulate radionuclide transport in fractured rock systems. The validation of such numerical codes can be accomplished by comparison of numerical simulations against appropriate analytical solutions. In this paper, we present analytical solutions for the reactive transport of N-member radionuclide chains (i.e., multiple species of radionuclides and their daughter species) through a discrete fracture in a porous rock matrix applying a system decomposition approach. We consider the transport of N-member radionuclide chains in a single-fracture-matrix system as a starting point to simulate more realistic and complex systems. The processes considered are advection along the fracture, lateral diffusion in the matrix, radioactive decay of multiple radionuclides, and adsorption in both the fracture and matrix. Different retardation factors can be specified for the fracture and matrix. However, all species are assumed to share the same retardation factors for the fracture and matrix, respectively. Although a daughter species may penetrate farther along the fracture than its parent species when a constant-concentration boundary condition is applied, our results indicate that all species retain the same transport speed in the fracture if a pulse of the first species is released into the fracture. This solution scheme provides a way to validate numerical computer codes of radionuclide transport in fractured rock, such as those being used to assess the performance of a potential nuclear-waste repository at Yucca Mountain.

Adsorption↗

Fluid flow and reactive transport around potential nuclear waste emplacement tunnels at Yucca Mountain, Nevada.

The evolution of fluid chemistry and mineral alteration around a potential waste emplacement tunnel (drift) is evaluated using numerical modeling. The model considers the flow of water, gas, and heat, plus reactions between minerals, CO(2) gas, and aqueous species, and porosity-permeability-capillary pressure coupling for a dual permeability (fractures and matrix) medium. Two possible operating temperature modes are investigated: a "high-temperature" case with temperatures exceeding the boiling point of water for several hundred years, and a "low-temperature" case with temperatures remaining below boiling for the entire life of the repository. In both cases, possible seepage waters are characterized by dilute to moderate salinities and mildly alkaline pH values. These trends in fluid composition and mineral alteration are controlled by various coupled mechanisms. For example, upon heating and boiling, CO(2) exsolution from pore waters raises pH and causes calcite precipitation. In condensation zones, this CO(2) redissolves, resulting in a decrease in pH that causes calcite dissolution and enhances feldspar alteration to clays. Heat also enhances dissolution of wall rock minerals leading to elevated silica concentrations. Amorphous silica precipitates through evaporative concentration caused by boiling in the high-temperature case, but does not precipitate in the low-temperature case. Some alteration of feldspars to clays and zeolites is predicted in the high-temperature case. In both cases, calcite precipitates when percolating waters are heated near the drift. The predicted porosity decrease around drifts in the high-temperature case (several percent of the fracture volume) is larger by at least one order of magnitude than in the low temperature case. Although there are important differences between the two investigated temperature modes in the predicted evolution of fluid compositions and mineral alteration around drifts, these differences are largely within to the model uncertainty and the variability of water compositions at Yucca Mountain.

Carbon Dioxide↗

Testing and parameterizing a conceptual solute transport model in saturated fractured tuff using sorbing and nonsorbing tracers in cross-hole tracer tests.

Two cross-hole tracer tests involving the simultaneous injection of two nonsorbing solute tracers with different diffusion coefficients (bromide and pentafluorobenzoate) and one weakly sorbing solute tracer (lithium ion) were conducted in two different intervals at the C-wells complex near the site of a potential high-level nuclear waste repository at Yucca Mountain, NV. The tests were conducted to (1) test a conceptual radionuclide transport model for saturated, fractured tuffs near Yucca Mountain and (2) obtain transport parameter estimates for predictive modeling of radionuclide transport. The differences between the responses of the two nonsorbing tracers and the sorbing tracer (when normalized to injection masses) were consistent with a dual-porosity transport system in which matrix diffusion was occurring. The concentration attenuation of the sorbing tracer relative to the nonsorbing tracers suggested that diffusion occurred primarily into matrix pores, not simply into stagnant water within the fractures. The K(d) values deduced from the lithium responses were generally larger than K(d) values measured in laboratory batch sorption tests using crushed C-wells cores. This result supports the use of laboratory-derived K(d) values for predicting sorbing species transport at the site, as the laboratory K(d) values would result in underprediction of sorption and hence conservative transport predictions. The tracer tests also provided estimates of effective flow porosity and longitudinal dispersivity at the site. The tests clearly demonstrated the advantages of using multiple tracers of different physical and chemical characteristics to distinguish between alternative conceptual transport models and to obtain transport parameter estimates that are better constrained than can be obtained using only a single tracer or using multiple nonsorbing tracers without a sorbing tracer.

Benzoates↗

Uncertainties in coupled thermal-hydrological processes associated with the Drift Scale Test at Yucca Mountain, Nevada.

Understanding thermally driven coupled hydrological, mechanical, and chemical processes in unsaturated fractured tuff is essential for evaluating the performance of the potential radioactive waste repository at Yucca Mountain, Nevada. The Drift Scale Test (DST), intended for acquiring such an understanding of these processes, has generated a huge volume of temperature and moisture redistribution data. Sophisticated thermal-hydrological (TH) conceptual models have yielded a good fit between simulation results and those measured data. However, some uncertainties in understanding the TH processes associated with the DST still exist. This paper evaluates these uncertainties and provides quantitative estimates of the range of these uncertainties. Of particular interest for the DST are the uncertainties resulting from the unmonitored loss of vapor through an open bulkhead of the test. There was concern that the outcome from the test might have been significantly altered by these losses. Using alternative conceptual models, we illustrate that predicted mean temperatures from the DST are within 1 degrees C of the measured mean temperatures through the first 2 years of heating. The simulated spatial and temporal evolution of drying and condensation fronts is found to be qualitatively consistent with measured saturation data. Energy and mass balance computation shows that no more than 13% of the input energy is lost because of vapor leaving the test domain through the bulkhead. The change in average saturation in fractures is also relatively small. For a hypothetical situation in which no vapor is allowed to exit through the bulkhead, the simulated average fracture saturation is not qualitatively different enough to be discerned by measured moisture redistribution data. This leads us to conclude that the DST, despite the uncertainties associated with open field testing, has provided an excellent understanding of the TH processes.

Forecasting↗