Measurement of Glass Corrosion in Boom Clay Disposal Conditions: First Results of the Experimental Programme 2000-2003 of SCK•CEN

Abstract

To estimate the lifetime of vitrified high level waste (HLW-glass) in Boom Clay disposal conditions, the dissolution behaviour of waste glass has been studied with experiments performed in surface laboratories and in the HADES underground research facility of SCK·CEN since 1980. We present the main topics and first results of the SCK·CEN programme 2000–2003. This programme focuses on the following items: (1) the diffusion/sorption/precipitation of silica in Boom clay or backfill clay, (2) demonstration of glass dissolution behaviour in realistic test conditions, (3) the effect of presaturation of the clay with silica, and (4) the estimation of near field concentrations of critical isotopes. The experiments have shown so far that Si, released by the glass, is effectively immobilized by Boom Clay, but it can nevertheless diffuse into the clay without immediately precipitating. The dissolution rate of glass SON68 and SM539 is determined in Boom Clay at in situ density and at 30°C (this is the long-term temperature expected near the waste glass packages in a Boom Clay repository). The dissolution rates, based on glass mass losses, are constant during the first year, at ∼ 0.010 g.m−2.day−1 for glass SON68 and ∼ 0.012 g.m−2.day−1 for glass SM539. The addition of glass frit causes a decrease of the glass dissolution rate, both with glass SON68 and SM539, and both in Boom Clay and in FoCa-clay. In FoCa-clay at high density with glass frit, the dissolution rates, based on glass mass losses, after 8 months at 30°C are ∼ 0.001 g.m−2.day−1 (SM539) and ∼0.005 g.m−2.day−1 (SON68). Because the experiments performed in Boom Clay and FoCa-clay with glass frit simulate realistic conditions (high clay density, low temperature), they can be used to estimate the maximum glass dissolution rate in a (Boom) clay repository. The corresponding minimum lifetime of a glass canister, calculated with the SCK·CEN code for lifetime predictions, is of the order of 105 to 106 years, if we neglect the internal glass surface area (due to cracking). In more diluted clay suspensions with glass frit, the glass dissolution rate is 10−4 to 10−5 g.m−2.day−1 or even zero. This would correspond to a lifetime of >>106 years. So far, there is no indication that the addition of glass frit leads to secondary phase formation at low temperature (30–40°C). Leach experiments with doped glasses SON68 and SM539 suggest that the maximum concentrations of most critical radionuclides in near field conditions are lower than the best estimate solubilities used for performance assessment studies in Boom Clay. For Se, relatively high concentrations were measured, though. The research programme for the underground laboratory is not discussed.