Uranium sequestration in fracture filling materials from fractured granite aquifers

Abstract

The migration of the uranium (U) in high-level radioactive waste that is held in deep geological repositories via fractures in deep granite aquifers is a serious safety concern, thus, this study investigates the effect of fracture filling materials designed to mitigate these concerns. Geochemical analysis was conducted on granite rock core and groundwater samples collected from boreholes located in granite areas. Sequential extraction tests on fracture filling material (FFM) samples were also conducted. The rock core samples were classified as two-mica granite that had uranium (U) content ranging from 1900 to 22,100 μg/kg with an arithmetic mean of 8500 μg/kg. The total U concentration in the FFM samples was found to range from 790 to 80,781 μg/kg. The U in the FFM samples was mainly associated with a carbonate phase that made up from 29.9 to 100% of the total U in the FFM. The U fraction of carbonate phase was closely correlated with the Ca fraction. U associated with crystalline inorganic FFM constituents (e.g, clay minerals and metal oxyhydroxides) was also found in FFM samples in fractions ranging from 21.1 to 70.1%. U in FFM is mainly incorporated via Ca-carbonate, which might have not been formed in modern groundwater, but the time and temperature during formation are unknown. In addition, the Fe, Si, Al, Ca, K, and U levels were found to be well correlated with each other, suggesting that U can also become geochemically associated with crystalline clay minerals or Fe-oxyhydroxides.