Can Spent Nuclear Fuel Decay Heat Prevent Radionuclide Release?

Abstract

Heat generated by radioactive decay of spent fuel represents a potentially important barrier to water accumulation on commercial spent nuclear fuel in breached waste packages. In the absence of water, fuel degradation and radionuclide release will be negligible. Thermal models for the proposed Yucca Mountain Repository suggest that, after a period of approximately 1000-4000 years (depending on loading and ventilation conditions), the repository drift walls may decline to sub-boiling temperatures, thus allowing humidity in the drift to increase. The question thus arises, is the thermal gradient between the fuel and the drift sufficient to prevent water accumulation in a humid drift environment throughout the regulatory period? The answer depends on the balance between processes that oppose water condensation onto the fuel (decay heat) and those that promote condensation such as the deliquescence of hygroscopic phases within the fuel.

Our experimental results indicate that deliquescence could lead to the condensation of water onto spent fuel despite the thermal “self-drying” effect if the following criteria are met: (1) the fission product salt Csl is present in the fuel or in the fuel-cladding gap, (2) the relative humidity in the drift exceeds 80% while temperatures in the waste package are around 90^oC. Previous work suggests that these criteria may be met for some fuel pins within the proposed Yucca Mountain Repository. However, experiments that account for the role of U(VI) alteration phases suggest that deliquescence may be a self-limiting process in the sense that deliquescent components (e.g. Cs, Ba, Sr) may be incorporated into nondeliquescent U(VI) phases that form from the corrosion of spent fuel.