Secondary Uranium-Phase Paragenesis and Incorporation of Radionuclides into Secondary Phase

The purpose of this analysis/model report (AMR) is to assess the potential for uranium (U) (VI) compounds, formed during the oxidative corrosion of spent uranium-oxide (UO{sub 2}) fuels, to sequester certain radionuclides and, thereby, limit their release. The ''unsaturated drip tests'' being conducted at Argonne National Laboratory (ANL) provide the basis of this AMR (Table 1). The ANL drip tests on spent fuel are the only experiments on fuel corrosion from which solids have been analyzed for trace levels of radionuclides. Brief summaries are provided of the results from other selected corrosion and dissolution experiments on spent UO{sub 2} fuels, specifically those conducted under nominally oxidizing conditions. Discussions of the current understanding of thermodynamic and kinetic properties of U(VI) compounds is provided in order to outline the scientific basis for modeling precipitation and dissolution of potential radionuclide-bearing phases under repository-relevant conditions. Attachment I provides additional information on corrosion mechanisms and behaviors of radionuclides in the tests at ANL. Attachment II reviews occurrence, formation, and alteration (collectively known as paragenesis) of naturally occurring U(VI) minerals because natural mineral occurrences can be used to assess the possible long-term behaviors of U(VI) compounds formed in short-term laboratory experiments and to extrapolate experimental results to repository-relevant time scales. This AMR develops a model for calculating dissolved concentrations of radionuclides that are incorporated into U(VI) compounds, which is an alternative to models currently used in TSPA to calculate dissolved concentration limits for certain radionuclides. In particular, the model developed in this AMR applies to Np (neptunium) concentrations being controlled by solid uranyl oxyhydroxides that are known to contain trace levels of Np. The results of this AMR and the conceptual model developed from it and presented in Section 6.7.2.3 are primarily intended to support sensitivity evaluations in performance assessment. This AMR was developed in accordance with the ''Technical Work Plan for Waste Form Degradation Process Model Report for SR'' (CRWMS M&O 2000a). The scope of this AMR is outlined in the section ''Mixed Phase Dissolved Radionuclide Concentration Limits'' of the technical work plan