Identification of Secondary Phases Formed During Unsaturated Reaction of UO2 with EJ-13 Water

ABSTRACTA set of experiments, wherein UO2 has been contacted by dripping water, has been conducted over a period of 182.5 weeks. The experiments are being conducted to develop procedures to study spent fuel reaction under unsaturated conditions that are expected to exist over the lifetime of the proposed Yucca Mountain repository site. One half of the experiments have been terminated, while one half are ongoing. Analyses of solutions that have dripped from the reacted UO2 have been performed for all experiments, while reacted UO2 surfaces have been examined for the terminated experiments. A pulse of uranium release from the UO2 solid, combined with the formation of schoepite on the surface of the UO2, was observed between 39 and 96 weeks of reaction. Thereafter, the uranium release decreased and a second set of secondary phases was observed. The latter phases incorporated cations from the EJ-13 water and include boltwoodite, uranophane, sklodowskite, compreignacite, and schoepite. The experiments are continuing to monitor whether additional changes in solution chemistry or secondary phase formation occurs.