Radionuclide concentrations in underground waters of Mururoa and Fangataufa Atolls

In 1997 an expedition to Mururoa and Fangataufa Atolls was carried out to sample underground waters from cavity-chimneys and carbonate monitoring wells. The aim of this study was to determine the prevailing concentration and distribution status of radionuclides. Elemental analysis of interstitial waters was carried out in the water fraction as well as in particles collected at 11 underground monitoring wells. 238Pu, 239,240Pu, 241Am, 137Cs, 90Sr, 3H, 125Sb, 155Eu and 60Co were analyzed in both fractions by alpha-, beta- and gamma-spectrometry. Measurements showed that at 60% of the sites, pH and Eh seemed to be related to tidal cycles; in contrast HTO was constant during the sampling time. Interstitial waters from carbonates and transition zones shared similar chemical composition that were not different from that of the surrounding seawater. Waters collected from basalt cavities left after nuclear tests, (Aristee and Ceto) have a different chemical signature characterized by a deficiency in Mg, K and SO4 as well as enrichment in Sr, Si, Al and Cl compared to the rest of the stations. Radionuclide concentrations present in both, water and particulate fractions, were significantly higher at Ceto and Aristee than at any other monitoring wells, except for Fuseau and Mitre monitoring wells (Fangataufa) where values similar to Ceto were found (e.g. 239,240Pu: > 20 mBq g-1). Considering that Pu isotopes showed high Kd values compared to non-sorbing radionuclides such as 3H, 90Sr and 137Cs it is very unlikely that migration from cavities to monitoring wells accounts for the concentration of Pu isotopes and Am at Fuseau 30 and Mitre 27. Perhaps the contact of lagoon waters with the well before sealing could be a possible source of the transuranics found at these sites. The 238Pu/239,240Pu ratios measured in the particles were similar to that of the lagoon (0.38), thus supporting this hypothesis. The fact that transuranics were found only in the particle fraction, in the water (colloids included) these radionuclides were below detection limits, may be accounted for the conspicuous quantity of iron oxy-hydroxides present in the particulate fraction that under the appropriate redox conditions may be interacting selectively with elements in solution (scavenging) resulting in the enhanced transuranic signal. While transuranics have been found in places of their origin, radionuclides with low Kd values (3H, 90Sr, 137Cs) have already been transported to monitoring wells, as well as to the atolls' lagoons and the open ocean.