Assessment of radionuclide vapor-phase transport in unsaturated tuff

This report describes bounding calculations performed to investigate the possibility of radionuclide migration in a vapor phase associated with the emplacement of high-level waste canister in unsaturated tuff formations. Two potential radionuclide transport mechanisms in the vapor phase were examined: aerosol migration and convection/diffusion of volatile species. The former may have significant impact on the release of radionuclides to the accessible environment as the concentration in the aerosols will be equal to that in the ground water. A conservative analysis of air diffusion in a stagnant liquid film indicated that for all expected repository conditions, aerosol formation is not possible. The migration of volatile species was examined both in the vicinity of a waste canister and outside the thermally disturbed zone. Two-dimensional (radial) and three-dimensional (radial-vertical) coupled heat transfer-gas flow-liquid flow simulations were performed using the TOUGH computer code. The gas flow rate relative to the liquid flow rate predicted from the simulations allowed calculations of mobility ratios due to convection which led to the conclusion that, except for the immediate region near the canister, transport in the liquid phase will be dominant for radionuclides heavier than radon. Near the waste canister, iodine transport may also be important in the vapor phase. Bounding calculations for vertical mobility ratios were carried out as a function of saturation. These calculations are conservative and agree well with the two-dimensional simulations. Based on this analysis, it is clear that vapor-phase transport will not be important for radionuclides such as cesium and heavier species. Vapor transport for iodine may play a role in the overall release scenario depending on the particular repository conditions