Transport and selective uptake of radium into natural clay minerals

Understanding of the environmental behavior of Ra is important from the viewpoint of the long-termed repository safety of radioactive waste, but investigation of Ra behavior in natural environment is difficult to detect. We found isotopic evidence of Ra transportation and its selective uptake into clay minerals from Pb isotopic analyses. Illite grains found in calcite veins included in sandstone near the Oklo uranium deposit, Republic of Gabon, show extremely low 207Pb/206Pb (∼ 0.0158) isotopic ratios. Although the Pb isotopic ratios of calcite and quartz coexisting with illite indicate the formation age of each component, those of illite do not. In addition, illite grains having low 207Pb/206Pb isotopic ratios contain a strongly large amount of Ba (1230 to 6010 ppm) in contrast with low contents of Ba in calcite and quartz (< 0.26 ppm). Considering the chemical similarity between Ba and Ra, the 207Pb/206Pb isotopic data suggest an excess of 206Pb due to selective adsorption of 226Ra (and also Ba) into illite grains. This is a very rare example to show evidence of the selective adsorption behavior of Ra from the isotopic excesses of 206Pb, although the adsorption ability of Ra itself in nature was largely reported.