Spent fuel dissolution rates as a function of burnup and water chemistry

To help provide a source term for performance-assessment calculations, dissolution studies on light-water-reactor (LWR) spent fuel have been conducted over the past few years at Pacific Northwest National Laboratory in support of the Yucca Mountain Site Characterization Project. This report describes that work for fiscal years 1996 through mid-1998 and includes summaries of some results from previous years for completeness. The following conclusions were based on the results of various flowthrough dissolution rate tests and on tests designed to measure the inventories of {sup 129}I located within the fuel/cladding gap region of different spent fuels: (1) Spent fuels with burnups in the range 30 to 50 MWd/kgM all dissolved at about the same rate over the conditions tested. To help determine whether the lack of burnup dependence extends to higher and lower values, tests are in progress or planned for spent fuels with burnups of 13 and {approximately} 65 MWd/kgM. (2) Oxidation of spent fuel up to the U{sub 4}O{sub 9+x} stage does not have a large effect on intrinsic dissolution rates. However, this degree of oxidation could increase the dissolution rates of relatively intact fuel by opening the grain boundaries, thereby increasing the effective surface area that is available for contact by water. From a disposal viewpoint, this is a potentially more important consideration than the effect on intrinsic rates. (3) The gap inventories of {sup 129}I were found to be smaller than the fission gas release (FGR) for the same fuel rod with the exception of the rod with the highest FGR. Several additional fuels would have to be tested to determine whether a generalized relationship exists between FGR and {sup 129}I gap inventory for US LWR fuels