Petteri Pitkänen

Application of mass-balance and flow simulation calculations to interpretation of mixing at Äspö, Sweden

The hydrogeology of a vertical fracture zone at 70 m depth at the access tunnel to the Aspo Hard Rock Laboratory was monitored over 3 a for hydrochemical changes that could be effected by construction of a deep repository for high-level nuclear waste. Tunnel construction dramatically disturbed the hydrogeological system, but this provided an opportunity to integrate hydrogeochemical and hydrological evaluation of the zone. The objective of this study was to evaluate hydrogeochemical evolution, groundwater flow and surface water intrusion during the experiment using an integrated approach of geochemical mass-balance calculations and numerical flow simulations. The dilution of major ions was the dominant hydrochemical trend. However, HCO3 and SO4 showed significant enrichment. Increasing activity of 14C suggested that oxidation of organic C was the likely source of HCO3. Any mineral source dissolving during the experiment seemed insufficient to account for changes in SO4 and current intrusion of sea water was excluded according to the data. Cation exchange as well as minor calcite reactions in fractures were assumed probable in such temporary chemical conditions. Conservative two end-member mixing models with shallow groundwater in the zone and initial groundwater at tunnel level also assumed remarkable mass transfer (several mmol/l). Therefore a third SO4-rich end-member, a regional shallow groundwater type which may mix by lateral flow in the system, was tested. This was also expected from hydraulic measurements and preliminary flow simulations assuming homogeneity. Three end-member mixing calculations using Cl and SO4 as conservative tracers give a constant proportion of lateral water in all boreholes after 300 days, which is consistent with the steady state character of the flow field in the late part of the experiment. To predict reactions on plausible levels needs significant adjustments of initial and final waters, indicating uncertainties in the hydrochemical information of the fracture zone. In the flow simulations the transmissivities were selected so that the chemical mixing proportions would match simulated portions of flow as closely as possible. The simulated total recoveries (drawdowns) differ from the measurements mainly due to overly simple parametrisation of the transmissivity in the fracture zone. However, integrating hydrochemistry in flow modelling is considered encouraging in producing additional information of the heterogeneity of a flow structure.

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.

Interaction of Water and Compacted Sodium-Bentonite in Simulated Nuclear Waste Disposal Conditions

Alteration of compacted sodium-bentonite (Volclay MX-80) caused by groundwater in simulated repository conditions for high level radioactive waste, was studied in an experiment where bentonite (wrapped by a copper cylinder) was let to react with two types (A,B) of synthetic granitic groundwater that are distinguished by their initial concentration of potassium and chloride. The reaction took place in ambient conditions at a temperature of 75 °C and proceeded during several time intervals up to 36 months. At the end of each time interval the water was chemically analysed for determination of possible changes in composition. Chemical and mineralogical changes in the bentonite were investigated by using NH 4 Cl extractions, XRD and microprobe (SEM, EDS) analyses and were studied as a function of the reaction time (months) as well as of the distance (mm) from the contact front with water. Sodium ions were found to migrate out from the bentonite while being replaced by other cations such as calcium, magnesium and to some extent, particularly during the reaction of the bentonite with water B, by potassium. No clear evidence was found for the fixation of potassium ions in the interlayer position of montmorillonite clay and the transformation to illite. The main mineralogical change in the bentonite was from Na- to Ca-rich montmorillonite. Secondary processes were the dissolution-precipitation of sulphur compounds, dissolution of gypsum and carbonates and the dissolution-precipitation of copper compounds.

Determination of Porewater Chemistry in Compacted Bentonite

Laboratory experiments were performed to study the interaction between groundwater and compacted sodium bentonite (Volclay MX-80). The solutions used were the fresh and saline groundwater simulants. The experiments were carried out in aerobic and anaerobic conditions at elevated temperature. Of main interest in the present study were the chemical changes in the reacting solution, bentonite porewater, and bentonite itself. The results for major cations display a principal difference between the interactions with fresh and saline solutions, while the differences between aerobic and anaerobic conditions within each solution case seem to be minor. The experimental results for the bentonite-water equilibria were interpreted in terms of a multi-site surface complexation model and the computer program HYDRAQL. The apparent diffusivities for sodium and sulfate in bentonite samples sandwiched between two filter plates were also determined.