Uranium Behavior in the Process of Primary Pitchblende Ores Alteration by the Post-ore Hydro thermal Solutions: An Application to Assessment of Uranium Migration from Underground Spent Nuclear Fuel Repositories

摘要

It has been shown that the main uranium ore mineral, pitchblende (uranium dioxide), is a natural analog of synthetic uraninite (also uranium dioxide), which constitutes 96% of spent nuclear fuel (SNF). Geochrono-logical studies of the U-Pb isotope systems in unaltered pitchblende from the orebodies reveal that these systems remained completely closed over the entire period (approximately 135 Ma) since the formation of the deposits. The bulk of the primary uranium ores within the Streltsovskoye ore field was influenced to various degrees by post-ore hydrothermal solutions that led to pitchblende spherulites being replaced by pseudomor-phs of an amorphous phase with a U-Si composition; this phase also re-precipitated in veinlets proximal to the pitchblende pseudomorphs. A technique specially developed by the authors was used to carry out quantitative counts of the abundance of uranium minerals by calculating the uranium mass balance in one of the orebodies subjected to hydrothermal alteration. The calculations reveal minimal uranium loss from the orebody. Uranium liberated in the process of the pseudomorphic replacement of pitchblende was immediately fixed, in situ, in the newly formed coffinite-like amorphous U-Si phase as a result of the development of an efficient geochemical barrier that prevented the long-distance migration of uranium. In assessing the long-term safety of underground SNF repositories, the results of the present study give us confidence that SNF uraninite, in terms of the preservation of its integrity as a mineral phase, provides for the reliable long-term isolation of uranium, transuranium elements, and fission products that are "sealed" in the uraninite matrix. In the case of the mineral transformation of the uraninite matrix by hydrothermal solutions, the liberated uranium would be efficiently immobilized by the newly formed amorphous U-Si phase.