Reaction of water with a simulated high-level nuclear waste glass at 300/sup 0/C, 300 bars

Abstract

The hydrothermal stability of high-level nuclear wastes is an important consideration in establishing waste form acceptance criteria for a geological repository in basalt. A detailed examination of the stability of a typical simulated high-level waste glass and pressurized water at 300/sup 0/C in a closed system has shown that extensive reaction occurred within a few weeks. The water acted first as a catalyst-solvent in devitrification of the glass and in dissolution, transport, and recrystallization of some of its constituents, and, second, as a reactant in forming hydrated and hydroxylated phases. This reaction with water resulted in the conversion of a solid shard of glass into a fragmented and partially dispersed mass of crystalline and noncrystalline material plus dissolved species within two weeks. The major crystalline reaction products were found to be analogs of naturally occurring minerals: (Cs,Na,Rb)/sub 2/(UO/sub 2/)/sub 2/.(Si/sub 2/O/sub 5/)/sub 3/.4H/sub 2/O (weeksite) and a series of pyroxene-structure phases, (Na,Ca) (Fe,Zn,Ti)Si/sub 2/O/sub 6/ (acmite, acmite--augites). Weeksite, however, is not expected to have long-term stability in the basalt environment. Much of the Na and Mo, and almost all of the B, in the original glass was identified in the product solutions. Of the elements or analogs of long-lived, hazardous radionuclides studied in this work, only Cs was observed in these solutions in substantial amounts. Although the comparatively rapid and extensive reactions at 300/sup 0/C would appear to require that an acceptable glass would have low waste and heat loading, it is suggested that there is good potential for favorable glass--basalt--water hydrothermal interactions. Favorable interactions would mean that, in the event of a hydrothermal incident, the interaction products would be more stable than the original waste form and would remain in the immediate repository.