Assessing the durability of nuclear glass with respect to silica controlling processes in a clayey underground disposal

Abstract

ABSTRACTThe long-term behaviour of vitrified high-level waste in an underground clay repository was assessed by using the reactive transport model HYTEC with respect to silica diffusion, sorption and precipitation processes. Special attention was given to the chemical interactions between glass, corroded steel and the host-rock considering realistic time scale and repository design. A kinetic and congruent dissolution law of R7T7 nuclear glass was used assuming a first-order dissolution rate, which is chemistry dependent, as well as a long-term residual rate. Without silica sorption and precipitation, glass dissolution is diffusion-driven and the fraction of altered glass after 100,000 years ranges from 5% to 50% depending on the fracturation degree of the glass block. Corrosion products may limit glass dissolution by controlling silica diffusion, whereas silica sorption on such products has almost no effect on glass durability. Within the clayey host-rock, precipitation of silicate minerals such as chalcedony may affect glass durability much more significantly than sorption. In that case, however, a concomitant porosity drop is predicted that could progressively reduce silica diffusion and subsequent glass alteration.