Analysis of factors affecting the stability of backfill materials

Storage of high-level nuclear waste in subsurface repositories involves a backfill material as a physical/chemical barrier between the solid waste canisters and host rock. Chemical, structural, and textural changes due to hydrothermal reaction may degrade the backfill performance over the life of the repository. In order to evaluate the potential for such changes, we have: (1) carried out hydrothermal experiments on candidate backfill materials (smectite, illite, basalt) under conditions analogous to those at the repository, (2) performed a complete characterization of these materials before and after hydrothermal treatment using EMPA, XRD, SEM/EDS, and, especially, STEM/AEM techniques, and (3) reviewed and analyzed geologic systems which are analogous to the backfill systems. These serve as natural experimental systems with ages up to many tens of millions of years. The Umtanum basalt contains up to 25% of immiscible, two-phase glasses and late opal and nontronite in fractures. These materials are especially subject to solution effects and the glass may provide K to groundwater. The kinetics of the smectite to illite and illite to muscovite transitions are primarily controlled by Al/Si diffusion which is sluggish, rather than by rapid alkali ion diffusion. Thus, even though smectite (bentonite), mixed-layer illite/smectite and illite are all metastable phases transitional to muscovite plus other phases, reactions occur so slowly that these phases are retained even within a geologic time scale for temperatures of approximately 150, 200 and 3000C, respectively. A high ratio of Ca/K (perhaps supplied by solution of calcite) inhibits the transitions. If clay layers are compacted to form a continuous matrix, water may be prevented from penetrating the backfill and promoting the clay mineral transition