Optimizing conditions for an accelerated leach test

An accelerated leach test for low-level radioactive waste forms is being developed to provide, in a short time, data that can be extrapolated to long time periods. The approach is to provide experimental conditions that will accelerate leaching without changing the dominant release mechanism. Experimental efforts have focused on combining individual factors that have been observed to accelerate leaching. These include elevated temperature, increased leachant volume, and reduced specimen size. The response of diffusion coefficients to various acceleration factors have been evaluated and provide information on experimental parameters that need to be optimized to increase leach rates. For example, these data show that large volumes of leachant are required when leaching portland cement waste forms at elevated temperatures because of high concentrations of dissolved species. Sr-85 leaching is particularly susceptible to suppression due to concentration effects while Cs-137 leaching is less so. Preliminary modeling using a diffusion mechanism (allowing for depletion) of a finite cylinder geometry indicates that during early portions of experiments (daily sampling intervals), leaching is diffusion controlled and more rapid than later in the same experiments (weekly or greater sampling intervals). For cement waste forms, this reduction in rate may be partially controlled by changes in physical structure and chemistry (sometimes related to environmental influences such as CO2), but it is more likely associated with the duration of the sampling interval. 9 refs., 6 figs