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The potential importance of tetraborate complexation on lanthanide(III) and actinide(III) solubility is recognized in the literature but a systematic study of f-element complexation has not been performed. In neodymium solubility studies in WIPP brines, the carbonate complexation effect is not observed since tetraborate ions form a moderately strong complex with neodymium(III). The existence of these tetraborate complexes was established for low and high ionic strength solutions. Changes in neodymium(III) concentrations in undersaturation experiments were used to determine the neodymium with tetraborate stability constants as a function of NaCl ionic strength. As very low Nd(III) concentrations have to be measured, it was necessary to use an extraction pre-concentration step combined with ICP-MS analysis to extend the detection limit by a factor of 50. The determined Nd(III) with borate stability constants at infinite dilution and 25 °C are equal to logβ1=4.55±0.06 using the SIT approach, equal to logβ1=4.99±0.30 using the Pitzer approach, with an apparent logβ1=4.06±0.15 (in molal units) at I=5.6 m NaCl. Pitzer ion-interaction parameters for neodymium with tetraborate and SIT interaction coefficients were also determined and reported.

Environmental context. The aqueous geochemistry of thallium is not well known in comparison with cadmium and lead, although it is more highly toxic, and at the same time has a wide range of industrial applications. A database allowing us to reliably predict the speciation and solubility of thallium in various environments in low temperature systems would be invaluable in providing some understanding of thallium’s mobilisation and mitigation. We propose here such a thermodynamic database based on critical reviews. Abstract. Thallium is a highly toxic element, and at the same time it has a wide range of applications in industry. Therefore, it is important to know its speciation and solubility under low temperature conditions. This study expands the thermodynamic database of the first paper of this series on the aqueous geochemistry of thallium by providing the formation constants of some important thallium complexes, including TlEDTA3–, TlOx– (Ox: oxalate), TlSuc– (Suc: succinate), TlMal– (Mal: malonate) and TlHPO4–. This study also recommends the solubility product constant of TlCl(s) as 10–3.65. The combined database allows us to model reliably the speciation and solubility of thallium in the Earth surface environments. As an example, the speciation and solubility of thallium in soil solutions are presented based on thermodynamic calculations.