The influence of microorganisms on the immobilization of radionuclide in subsurface crystalline rock environments

In the underground rock characterization facility tunnel ONKALO in Finland, and in the Äspö Hard Rock Laboratory (HRL) in Sweden massive 5–10-mm thick biofilms were observed attached to tunnel walls where groundwater was seeping from bedrock fractures. The main goal of the study was to evaluate the relevance of microbial processes for the immobilization of radionuclides in a deep crystalline repository for high-level radioactive waste. In laboratory experiments the effect of uranium on biofilms was studied on site in the ONKALO tunnel by adding uranium to the fracture water in a self constructed flow cell by using detached biofilm samples. Biofilm specimens collected for transmission electron microscopy studies indicated that uranium in the biofilm was immobilized intracellularly in microorganisms as needle-shaped uranyl phosphate minerals, similar to meta-Autunite (Ca[UO2]2[PO4]2•10-12H2O).
Gallionella ferruginea dominated biofilms associated with bacteriogenic iron oxides (BIOS) from the Äspö HRL were used for laboratory experiments, in which uranium and neptunium, respectively, were added to the BIOS biofilms. The biofilms were submerged in Äspö groundwater in a flow cell under aerobic conditions. The results showed a substantial decrease of uranium and neptunium in the groundwater of approximately 85% and 95%, respectively. Thermodynamic calculation of the theoretical predominant fields of uranium species showed that the formation of an aqueous uranium carbonate species Ca2UO2(CO3)3 was predicted due to the high concentration of carbonate in the groundwater. Under the given pH conditions the uptake of uranium and neptunium in the BIOS biofilm depends predominantly on the high amount of ferrihydrite, which precipitated onto the ferrous iron-oxidizing and stalk-forming bacterium Gallionella ferruginea. Consequently, the combination of the biological material and iron oxides created an abundant surface area for bioaccumulation and adsorption of radionuclides.