Redistribution of REE, Pb and U by supergene weathering studied from in-situ isotopic analyses of the Bangombé natural reactor, Gabon

Abstract

The isotopic analyses of rare earth elements (REE), Pb and U in several kinds of minerals from the clay and black shale layers above the Bangombé natural reactor, Gabon, were performed using a sensitive high-resolution microprobe (SHRIMP) to investigate the migration and retardation processes of fission products released from the reactor. REE isotopic data of the secondary minerals found in clays and black shales show that most of fission products were effectively trapped in the clays and not distributed into the black shales over the clays, which reveals that the clays play an important role in preventing fission products from spreading. Zircon crystals in the clays heterogeneously contain high-U regions (up to 28.3 wt%) with normal 235U/ 238U ratios (=0.00725) and significant amounts of fissiogenic REE, which suggest the occurrence of significant chemical fractionation between REE and U during the dissolution of reactor uraninite and the recrystallization of secondary U minerals. The Pb data suggest that galena grains in the clays were also formed by the mixing of the two components during a recent alteration event, and that a significant amount of Pb was derived from 2.05-Ga-old original uraninite rather than reactor uraninite. The U–Pb systematics of zircon provide chronological information on the old igneous activity associated with the basement rock formation at 2.8 Ga and geochemical evidence of the incomplete mixing of independent Pb and U sources. This result is consistent with previous chronological results in this area.