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Liquid Immiscibility in the System NaF–H2O at 1073 K and 200–230 MPa and Its Effect on Microlite Solubility

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Abstract

New data have been obtained on the solubility of microlite (CaNa)Ta2O6F in the NaF–H2O system of P–Q type in a wide range of sodium fluoride concentrations (from 0 to 40 wt% NaF). The tantalum concentration in equilibrium with microlite and fluorite in the concentrations range of NaF from 0 to 8 mol·kg−1 H2O (25 wt% NaF) does not exceed 3 × 10−5 mol·kg−1. Sodium fluoride concentrations have been estimated in the immiscible fluids L1 (fluid of moderate density) and L2 (dense fluid) in the NaF–H2O system at 1073 K and 200–230 MPa. The L1 and L2 fluids at p = 200 MPa contain 5 ± 1 and 26 ± 1 wt% NaF, and at p = 230 MPa contain 12 ± 1 and 25 ± 1 wt% NaF. Thermodynamic analysis of the experimental data has shown that the best agreement with experimental microlite solubility in the homogeneous fluid field of NaF–H2O solutions takes place assuming the following aqueous Ta(V) species: \( {\text{HTaO}}_{3}^{\text{o}} \), TaO2F°, \( {\text{TaO(OH)F}}_{ 2}^{\text{o}} \), \( {\text{NaTaO}}_{ 3}^{\text{o}} \), and \( {\text{Na}}_{ 6} {\text{H}}_{ 2} {\text{Ta}}_{ 6} {\text{O}}_{ 1 9}^{\text{o}} \).

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Acknowledgments

The authors are grateful to V. K. Karandashev (IPTM RAS), A. N. Nekrasov, and O. L. Samokhvalova (IEM RAS) for their help in the experimental research. An earlier version of this manuscript was reviewed by Dr. Z. A. Kotelnikova (IGEM RAS) and an anonymous referee, who provided comments that have helped to noticeably improve the quality of this paper. The work is supported by Russian Fund of Basic Research Grants 14-05-00145, 15-05-03393, 14-05-00424, 14-05-91750-AF, and the program DES RAS No. 2.

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Redkin, A.F., Kotova, N.P. & Shapovalov, Y.B. Liquid Immiscibility in the System NaF–H2O at 1073 K and 200–230 MPa and Its Effect on Microlite Solubility. J Solution Chem 44, 2008–2026 (2015). https://doi.org/10.1007/s10953-015-0394-1

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