Mineralogical and chemical characteristics of the bentonite in the A2 test parcel of the LOT field experiments at Äspö HRL, Sweden

Abstract

The Long Term Test of Buffer Material (LOT) project at the Äspö Hard Rock Laboratory, Sweden, is a series of medium-scale field experiments focused on validating models and hypotheses concerning long term processes in the bentonite buffer of a repository for high-level radioactive waste. The test parcels emplaced in crystalline bedrock consist of blocks of compacted MX80 bentonite embedding a Cu-tube equipped with a heater to simulate the heat generation from radionuclide decay. The A2 test parcel had been subjected to elevated temperature (up to 130 °C) and hydration by a Na–Ca–Cl type groundwater for almost 6 years when it was retrieved to be analysed. The analyses included determinations of chemical composition, cation exchange capacity (CEC), exchangeable cations and mineralogy. Both the bulk bentonite and dialysed, homo-ionic Na-clay (<2 μm and <0.2 μm fractions) were analysed when relevant. Sulphate was redistributed in the heated part of the buffer under the thermal and hydration gradients that prevailed during the test period. Anhydrite accumulated in the warmer parts, whereas gypsum was dissolved in the peripheral parts of the buffer where water was supplied. Carbonate dissolution increased with temperature in the warmest parts, whereas chloride behaved conservatively in all blocks. Cu was incorporated in the bentonite matrix at the surface of the Cu-tube indicating some corrosion, which may be explained by reactions in an early stage of the test when trapped oxygen existed in the system. Along with the dissolution/precipitation reactions the porewater composition changed, which resulted in replacement of exchangeable sodium by calcium and magnesium in the warmest zone. Also Mg in the clay (<2 μm and <0.2 μm fractions) displays a clear gradient with peak values at the heater. Because several of the alternative sinks for Mg were eliminated in the sample preparation prior to the chemical analysis (purified clay fractions, removal of carbonates, Na-saturation) the smectite is suggested a candidate sink for Mg. Parallel with the increase in Mg, a loss in Si is indicated and CEC tends to increase in the clay that had been heated at 130 °C. A loss in tetrahedral Si that is balanced by Al, and replacement of Al by Mg in the octahedral sheet would imply that the layer charge of the smectite increased, which would be consistent with the higher CEC values of these samples. The changes in CEC are, however, close to the analytical resolution of the CEC method and no effect of the changes in chemical composition can be detected in the XRD-characteristics of the clay. Therefore, supplementary high-resolution analyses are required to verify whether the structure of montmorillonite has altered in the test period.