Radium isotopes in saline seepages,south-western Yilgarn,Western Australia

Water samples from saline seepages in the south-western Yilgarn Block of Western Australia contain high activities of the four naturally-occurring radium isotopes. Activities of up to 310 $\text{pCi}\text{l}$ for ²²⁶Ra and 1720 $\text{pCi}\text{l}$ for ²²⁸Ra were measured and the ${}^{228}\text{Ra}{}^{226}\text{Ra}$ ratio averaged 6.1. Activities of the two short-lived radium isotopes were also high. ²²³Ra activities of up to 94 $\text{pCi}\text{l}$ were found with an average ${}^{226}\text{Ra}{}^{223}\text{Ra}$ ratio of 3.3, considerably lower than the natural abundance ratio of 21.4. Activities of up to 23 $\text{pCi}\text{l}$²²⁷Ac, the long-lived ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 22 years}$) grandparent of ²²³Ra, were also measured. The analysis of surface granite samples, the probable source rocks of the radium, gave $\text{Th}\text{U}$ activity ratios of around 1.5. The higher ${}^{228}\text{Ra}{}^{226}\text{Ra}$ ratios of the waters were attributed to readily leached ²²⁸Ra in the weathered granites as a result of thorium remaining after weathering. Leach experiments on U-Th ore by NaCl solutions showed that all four radium isotopes were equally leached. Sulphate anions reduced the ²²⁶Ra and ²²⁸Ra leaching to a greater extent than for ²²³Ra and ²²⁴Ra, suggesting that the latter isotopes were being supported in solution by parent isotopes. In particular this suggested ²²⁷Ac was leached into the sulphate solution but this does not fully account for the amount of ²²⁷Ac seen in the seepage waters.