Abstract
The stabilities of uranyl-carbonate and uranyl-hydroxide aqueous complexes were experimentally determined at temperatures ranging from 25 to 125 °C using in situ UV–vis and Raman spectroscopic techniques. Combined with earlier determinations of the stability of chloride, sulfate, and hydroxide complexes at temperatures up to 250 °C, these data permit to create a consolidated dataset suitable for modeling of U(VI) mobilization in natural systems. The parameters of the Modified Ryzhenko-Bryzgalin and the Helgeson-Kirkham-Flowers (HKF) Equations of State (EoS) were derived based on this dataset and used for thermodynamic modeling different scenarios of U(VI) mobilization. These models suggest that at conditions relevant to natural systems, carbonate-mediated transport of U(VI) is likely suppressed by the high stability of solid UO2(OH)2 and Na2U2O7. In contrast, sulfate-mediated mobilization mechanisms are highly efficient at acidic and near-neutral pH conditions and can lead to effective hydrothermal mobilization of U(VI).
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