Andrew Martin

Comparative modeling of an in situ diffusion experiment in granite at the Grimsel Test Site

An in situ diffusion experiment was performed at the Grimsel Test Site (Switzerland). Several tracers ((3)H as HTO, (22)Na(+), (134)Cs(+), (131)I(-) with stable I(-) as carrier) were continuously circulated through a packed-off borehole and the decrease in tracer concentrations in the liquid phase was monitored for a period of about 2years. Subsequently, the borehole section was overcored and the tracer profiles in the rock analyzed ((3)H, (22)Na(+), (134)Cs(+)). (3)H and (22)Na(+) showed a similar decrease in activity in the circulation system (slightly larger drop for (3)H). The drop in activity for (134)Cs(+) was much more pronounced. Transport distances in the rock were about 20cm for (3)H, 10cm for (22)Na(+), and 1cm for (134)Cs(+). The dataset (except for (131)I(-) because of complete decay at the end of the experiment) was analyzed with different diffusion-sorption models by different teams (IDAEA-CSIC, UJV-Rez, JAEA) using different codes, with the goal of obtaining effective diffusion coefficients (De) and porosity (ϕ) or rock capacity (α) values. From the activity measurements in the rock, it was observed that it was not possible to recover the full tracer activity in the rock (no activity balance when adding the activities in the rock and in the fluid circulation system). A Borehole Disturbed Zone (BDZ) had to be taken into account to fit the experimental observations. The extension of the BDZ (1-2mm) is about the same magnitude than the mean grain size of the quartz and feldspar grains. IDAEA-CSIC and UJV-Rez tried directly to match the results of the in situ experiment, without forcing any laboratory-based parameter values into the models. JAEA conducted a predictive modeling based on laboratory diffusion data and their scaling to in situ conditions. The results from the different codes have been compared, also with results from small-scale laboratory experiments. Outstanding issues to be resolved are the need for a very large capacity factor in the BDZ for (3)H and the difference between apparent diffusion coefficients (Da) from the in situ experiment and out-leaching laboratory tests.

Matrix diffusion and sorption of Cs+, Na+, I– and HTO in granodiorite: Laboratory-scale results and their extrapolation to the in situ condition

Matrix diffusion and sorption are important processes controlling radionuclide transport in crystalline rocks. Such processes are typically studied in the laboratory using borehole core samples however there is still much uncertainty on the changes to rock transport properties during coring and decompression. It is therefore important to show how such laboratory-based results compare with in situ conditions. This paper focuses on laboratory-scale mechanistic understanding and how this can be extrapolated to in situ conditions as part of the Long Term Diffusion (LTD) project at the Grimsel Test Site, Switzerland. Diffusion and sorption of (137)Cs(+), (22)Na(+), (125)I(-) and tritiated water (HTO) in Grimsel granodiorite were studied using through-diffusion and batch sorption experiments. Effective diffusivities (De) of these tracers showed typical cation excess and anion exclusion effects and their salinity dependence, although the extent of these effects varied due to the heterogeneous pore networks in the crystalline rock samples. Rock capacity factors (α) and distribution coefficients (Kd) for Cs(+) and Na(+) were found to be sensitive to porewater salinity. Through-diffusion experiments indicated dual depth profiles for Cs(+) and Na(+) which could be explained by a near-surface Kd increment. A microscopic analysis indicated that this is caused by high porosity and sorption capacities in disturbed biotite minerals on the surface of the samples. The Kd values derived from the dual profiles are likely to correspond to Kd dependence on the grain sizes of crushed samples in the batch sorption experiments. The results of the in situ LTD experiments were interpreted reasonably well by using transport parameters derived from laboratory data and extrapolating them to in situ conditions. These comparative experimental and modelling studies provided a way to extrapolate from laboratory scale to in situ condition. It is well known that the difference in porosity between laboratory and in situ conditions is a key factor to scale laboratory-derived De to in situ conditions. We also show that cation excess diffusion is likely to be a key mechanism in crystalline rocks and that high Kd in the disturbed surfaces is critically important to evaluate transport in both laboratory and in situ tests.

Sorption and diffusion of selenium oxyanions in granitic rock

The processes controlling diffusion and sorption of radionuclides have been studied extensively in the laboratory, whereas, only a few in-situ experiments have been carried out in order to study in-situ diffusion over the long-term (several years). This is largely due to the fact that in-situ experiments are typically time consuming and cost intensive, and it is commonly accepted that laboratory scale tests are well-established approaches to characterizing the properties of geological media. In order to assess the relevance of laboratory experiments, the Swiss National Cooperative for Disposal of Radioactive Waste (Nagra) have been conducting extensive experiments in the Underground Rock Laboratory (URL) at the Grimsel Test Site (GTS) in order to study radionuclide transport and retention in-situ. One of the elements used in these experiments is non-radioactive selenium, as an analog for the radiotoxic isotope Se-79, which is present in radioactive waste. In this work, two laboratory through-diffusion experiments using selenium as a tracer were carried out in block (decimeter) scale rock specimens to support one of the ongoing radionuclide transport and retention in-situ experiment at the GTS mentioned above. The though-diffusion tests of selenium were performed under atmospheric conditions in both Kuru grey granite (KGG) and Grimsel granodiorite (GG). The decrease of selenium concentration in an inlet hole drilled into each of the rock samples and the breakthrough of selenium into sampling holes drilled around the inlet were analyzed using Inductively Coupled Plasma Mass Spectrometry (ICP-MS). The effective diffusion (De) and distribution coefficients (Kd) of selenium were then determined from the changes of selenium concentration in the inlet and sampling holes using a Time-Domain Diffusion (TDD) simulations. In addition, Kd of selenium was measured by batch sorption experiments as a function of pH and Se concentration in atmospheric conditions and nitrogen atmosphere. The speciation of selenium was studied by HPLC-ICP-MS in simulated ground waters of each of the rock types. The Kd of selenium was found to be in the range of (6.2-7.0±2.0)×10(-3)m(3)/kg in crushed rock whereas the Kd obtained from block scale through diffusion experiment varied between (1.5±0.3)×10(-3)m(3)/kg and (1.0±0.6)×10(-4)m(3)/kg. The De of selenium was significantly higher for GG; De=(2.5±1.5)×10(-12)m(2)/s than for KGG; De=(7±2)×10(-13)m(2)/s due to the higher permeability of GG compared with KGG.

Modeling Transport of Cesium in Grimsel Granodiorite With Micrometer Scale Heterogeneities and Dynamic Update of Kd

Transport and retardation of cesium in Grimsel granodiorite taking into account heterogeneity of mineral and pore structure was studied using rock samples overcored from an in situ diffusion test at the Grimsel Test Site. The field test was part of the Long-term Diffusion project (LTD) designed to characterize retardation properties (diffusion and distribution coefficients) under in situ conditions. Results of the LTD experiment for cesium showed that in-diffusion profiles and spatial concentration distributions were strongly influenced by the heterogeneous pore structure and mineral distribution. In order to study the effect of heterogeneity on the in-diffusion profile and spatial concentration distribution, a Time Domain Random Walk (TDRW) method was applied along with a feature for modeling chemical sorption in geological materials. A heterogeneous mineral structure of Grimsel granodiorite was constructed using X-ray micro computed tomography (X-μCT) and the map was linked to previous results for mineral specific porosities and distribution coefficients (Kd) that were determined using C-14-PMMA autoradiography and batch sorption experiments, respectively. After this the heterogeneous structure contains information on local porosity and Kd in 3D. It was found that the heterogeneity of the mineral structure on the micrometer scale affects significantly the diffusion and sorption of cesium in Grimsel granodiorite at the centimeter scale. Furthermore, the modeled in-diffusion profiles and spatial concentration distributions show similar shape and pattern to those from the LTD experiment. It was concluded that the use of detailed structure characterization and quantitative data on heterogeneity can significantly improve the interpretation and evaluation of transport experiments.

Trends in Scenario Development Methodologies and Integration in NUMO’s Approach

The development of scenarios for quantitative or qualitative analysis is a key element of the assessment of the safety of geological disposal systems. As an outcome of an international workshop attended by European and the Japanese implementers, a number of features common to current methodologies could be identified, as well as trends in their evolution over time. In the late nineties, scenario development was often described as a bottom-up process, whereby scenarios were said to be developed in essence from FEP databases. Nowadays, it is recognised that, in practice, the approaches actually adopted are better described as top-down or “hybrid”, taking as their starting point an integrated (top-down) understanding of the system under consideration including uncertainties in initial state, sometimes assisted by the development of “storyboards”. A bottom-up element remains (hence the term “hybrid”) to the extent that FEP databases or FEP catalogues (including interactions) are still used, but the focus is generally on completeness checking, which occurs parallel to the main assessment process. Recent advances focus on the consistent treatment of uncertainties throughout the safety assessment and on the integration of operational safety and long term safety.Copyright

Studies on radionuclide transport behaviour–The next generation of in-situ experiments at the Grimsel Test Site

Two recent ongoing major projects at the Grimsel Test Site (GTS) ( www.grimsel.com ) that were initiated to simulate the long-term behaviour of radionuclides in the repository near-field and the surrounding host rock are presented: the Colloid Formation and Migration (CFM) project, which focuses on colloid generation and migration from a bentonite source doped with radionuclides and the Long-Term Diffusion (LTD) project, which aims at in-situ verification and understanding of the processes that control the long-term diffusion of repository-relevant radionuclides. So far, the CFM project has principally involved: development and implementation of a state-of-the-art sealing concept to control hydraulic gradients in a shear zone to imitate repository-relevant conditions; extensive laboratory studies to examine bentonite erosion and colloid formation in a shear zone; and, development of models to estimate colloid formation and migration. The next stage will be to assess the behavior of bentonite colloids generated from a radionuclide spiked bentonite source-term emplaced into the controlled flow field of the shear zone. This will be coupled with further extensive laboratory studies in order to refine and evaluate the colloid models currently used in performance assessments. The LTD project consists of: a monopole diffusion experiment where weakly sorbing and non-sorbing radionuclides ( 3 H, 22 Na, 131 I, 134 Cs) have been circulating and diffusing into undisturbed rock matrix since June 2007; experiments to characterise pore space geometry, including determination of in-situ porosity with 14 C doped MMA resin for comparison with laboratory derived data; a study of natural tracers to elucidate evidence of long-term diffusion processes; and, an investigation of the in-situ matrix diffusion paths in core material from earlier GTS experiments. Future experiments will focus on diffusion processes starting from a water-conducting feature under realistic boundary conditions.