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Title: Hydrothermal interactions of cesium and strontium phases from spent unreprocessed fuel with basalt phases and basalts

Technical Report ·
DOI:https://doi.org/10.2172/5306867· OSTI ID:5306867

This investigation is a segment of an extensive research program aimed at investigating the feasibility of long-term, subsurface storage of commercial nuclear waste. Specifically, it is anticipated that the waste will be housed in a repository mined from the basalt formations which lie beneath the Hanford Site. The elements monitored during the present experiments were Cs and Sr. These two elements represent significant biohazards if released from a repository and are the major heat producing radionuclides present in commercial radioactive waste. Several Cs phases and/or solutions were reacted with either isolated basalt phases or bulk-rock basalt, and the resulting solids and solutions were analyzed. The hydrothermal reactivity of SrZrO/sub 3/, which is believed to be a probable host for Sr in SFE was investigated. While so far no evidence exists which indicates that Sr is present in a water soluble phase in spent fuel elements (SFE), detailed investigation of a potential hazard is warranted. This investigation has determined that some Cs compounds likely to be stable components of spent fuel (i.e., CsOH, Cs/sub 2/MoO/sub 4/, Cs/sub 2/U/sub 2/O/sub 7/) have significant hydrothermal solubilities. These solubilities are greatly decreased in the presence of basalt and/or basalt minerals. The decrease in the amount of Cs in solution results from reactions which form pollucite and/or CsAlSiO/sub 4/, with the production of pollucite exceeding that of CsAlSiO/sub 4/. Dissolution of ..beta..-Cs/sub 2/U/sub 2/O/sub 7/ implies solubilizing a uranium species to an undetermined extent. The production of schoepite (UO/sub 3/.3H/sub 2/O) during some experiments containing basalt phases, indicates a tendency to oxidize U/sup 4 +/ to U/sup 6 +/. When diopside (nominally CaMgSi/sub 2/O/sub 6/) and ..beta..-Cs/sub 2/U/sub 2/O/sub 7/ were hydrothermally reacted, at 300/sup 0/C both UO/sub 2/ and UO/sub 3/.3H/sub 2/O were produced. Results of experiments on SrZrO/sub 3/ show it to be an unreactive phase.

Research Organization:
Pennsylvania State Univ., University Park, PA (United States); Atomics International Div., Richland, WA (USA). Rockwell Hanford Operations
DOE Contract Number:
AC06-77RL01030
OSTI ID:
5306867
Report Number(s):
RHO-BWI-C-70; TRN: 80-010440
Country of Publication:
United States
Language:
English