Geochemical behaviour study of radionuclides and their radiogenic daughters in the vicinity of Oklo 10 and 13 natural nuclear reactors (Gabon) - Application to high-level radioactive waste disposal

Since 1981, the discovery of new and almost unaltered natural nuclear reactors in the uranium mine of Oklo (Gabon) renewed the interest of scientific community. Indeed, due to their specific features, these reactors could be extensively investigated as natural analogues to better understand the geochemical processes which may occur in a high level nuclear waste repository. The aim of this PhD thesis is to determine the present distribution of a few radionuclides or their radiogenic daughters initially formed within the reaction zones and to infer their geochemical behaviour, subsequently to the stopping of nuclear reactions. Our study was focused on reactors 10 and 13 and their immediate sandstone surroundings in order to decipher the fate of U, Y and light rare earth elements which are assumed to be chemical analogues of actinides and fission products. Mineralogical observations, chemical and isotopic analyses on bulk rocks, led us to conclude that a part of radionuclides, as well as their daughters, remained confined within the reactions zones, in association with secondary mineral phases, whereas another part migrated towards tbe reactor rims. The radionuclides were concentrated at the reactor border or migrated within the first few metres of the surrounding sandstone, according to the intensity of nuclear reactors and the presence of the so-called 'facies argile de pile' which constitutes an intermediate facies between that of reactor cores and that of the surrounding sandstone. In the latter, long range elemental transfers occurred via fissures. Some of them, contemporaneous to the nuclear reactions drained radionuclides-rich fluids at temperatures of about 150-170 deg. C. More recent fissures, observed only in the environment of reactor 13, have allowed the transport of hotter hydrothermal fluids (about 310 deg. C), likely related to the nearby intrusion of dolerite dyke. The principal implications of this work for the disposal of nuclear wastes concern notably the long term stability of U dioxide in a reducing geological environment and its retention capability for various radionuclides. Our results also suggest that interfaces within the near field of a repository may act as sinks for radionuclides. Finally, this study confirms that fissures are likely to play an essential role in the transport of fluids and thus in the dispersion of radionuclides. (author)