Uraninite recrystallization and Pb loss in the Oklo and Bangombé natural fission reactors, Gabon

The Oklo and Bangombé natural fossil fission reactors formed ca. 2 Ga ago in the Franceville basin, Gabon. The response of uraninite in the natural reactors to different geological conditions has implications for the disposal of the UO2 in spent nuclear fuel. Uraninite and galena from two reactor zones, RZ16 at Oklo and RZB at Bangombé, were studied to clarify the chronology and effect of alteration events on the reactor zones. In addition, ion microprobe U-Pb analysis of zircons from a dolerite dyke in the Oklo deposit were completed to better constrain the age of the dyke, and thereby testing the link between the dyke and an important alteration event in the reactor zones. The analyzed uraninite from RZ16 and RZB contains ca. 6 wt% PbO, indicating a substantial loss of radiogenic Pb. Transmission electron microscopy showed that microscopic uraninite grains in the reactor zones consist of mainly defect-free nanocrystalline to microcrystalline aggregates. However, the nanocrystalline regions have elevated Si contents and lower Pb contents than coarser uraninite crystallites. Single stage model ages of large, millimeter-sized galena grains at both RZ16 and RZB correlate well with the age of the Oklo dolerite dyke, 860 ± 39 Ma (2σ). Thus, the first major Pb loss from uraninite occurred at both Oklo and Bangombé during regional extension and the intrusion of a dyke swarm in the Franceville basin, ~ 860–890 Ma ago. Uraninite Pb isotopes from RZ16 and RZB give lower ages of ca. 500 Ma. These ages agree with the “chemical” ages of the uraninite, and show that an ancient Pb loss occurred after the intrusion of the dolerite dykes. The presence of nanocrystallites in the reactor uraninite indicates internal recrystallization, which may have occurred around 500 Ma, resulting in the 6wt% PbO uraninite. It is suggested that leaching by fluid interaction triggered by the Pan-African orogeny was important during this second Pb-loss event. Thus, there are indications that uraninite at both the Oklo and Bangombé natural reactors has experienced at least two ancient episodes of Pb loss associated with internal recrystallization. These recrystallization events have occurred without significantly depleting the 2 Ga fission products compatible with the uraninite structure