Analysis Of Congruent Matrix Release, Precipitation, And Time-Distributed Containment Failure On Spent Fuel Performance

Abstract

AbstractThe Analytical Repository Source-Term (AREST) code has been developed for source-term evaluation of spent fuel as a final waste form in geologic repositories. AREST contains a set of analytical equations for the timedependent diffusional mass transport of both solubility-limited and inventory-limited radionuclides from a spent fuel in a failed container surrounded by a shell of packing or other porous material imbedded in a porous host rock. Three factors that affect release performance are examined: 1) congruent dissolution of the UO2 matrix, 2) chemical instability of the UO2 matrix, with precipitation of a more stable uranium phase within the waste package, and 3) the attenuation of release rate by distribution of containment failures with time.For congruent matrix dissolution, the release rates of included nuclides are proportional to the product of solubility-limited release of uranium and the fractional abundance of the nuclide. For certain conditions, congruent release rates are calculated to be up to 10 orders of magnitude lower than release rates assuming individual solubility-limits. Precipitation of a more stable, lower solubility uranium phase within the waste package is shown to increase release rates from the UO2 matrix compared to the non-precipitation case, in agreement with previous calculations. During the first 300 to 1000 years after repository closure, the distribution of containment failures with time will act to attenuate the peak average release rates of soluble, longlived nuclides, such as iodine-129, to values smaller than release rates below regulatory limits. However, for soluble nuclides with short half-lives, such as cesium-137, a broader distribution of containment failure with constant mean time of failure can actually cause an increase In the peak average release rates.