REE mobility in groundwater proximate to the natural fission reactor at Bangombé (Gabon)

Abstract

The natural nuclear fission reactor at Bangombé is located at a depth of approximately 12 m and has undergone supergene weathering and chemical exchange with groundwater under moderately oxidizing conditions. This reactor has been studied as an analogue for the migration of radionuclides in a geologic repository. Five water samples were taken from a drill hole in the reactor zone and from drill holes that are situated along the direction of the groundwater flow. Dissolution of phosphates in the weathering profile provided an important mechanism for the mobilization of phosphorous and REE. This phosphorous allowed the formation of secondary minerals, e.g., phosphatian coffinites and Fe-uranyl phosphate hydroxide hydrates. The filtered groundwaters (dissolved phase) obtained directly from the reactor zone had anomalous 143Nd/ 146Nd, 145Nd/ 146Nd and 149Sm/ 147Sm isotope ratios of 0.7235, 0.4933 and 0.843, respectively, confirming mixing between a fissiogenic and normal REE component. In this dissoved phase, a small fraction of the Nd (2.3 at.%) is of fissiogenic origin. The suspended loads (filtered particulates) of the same groundwater from within the reactor show similar isotopic anomalies with a fissiogenic Nd contribution of 3.2 at.%. Similar fissiogenic Nd contributions are observable for groundwater samples from outside the reactor zone (3 m distance). Both dissolved and suspended load samples from the more distant well (25 m) have normal isotopic ratios. Thus, the prevailing physico-chemical conditions within this groundwater system allow the migration of the fissiogenic REE over at least 3 m but less than 25 m. Although REE phases are abundant in the reactor zone, the REE concentrations of the water in contact with the sediments of this zone are very low (<17 ppt). The most important lanthanide- and actinide-bearing phases are uraninite, coffinites and Fe-uranyl phosphate hydroxide hydrate. The presence of all of these phases retards the mobility of the fissiogenic lanthanides and actinides.