Experimental determination of zirconium speciation in hydrothermal solutions |
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| Authors: | B N Ryzhenko N I Kovalenko N I Prisyagina N P Starshinova V V Krupskaya |
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| Institution: | (1) Vernadsky Institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, ul. Kosygina 19, Moscow, 119991, Russia;(2) Institute of Geology of Ore Deposits, Petrography, Mineralogy, and Geochemistry (IGEM), Russian Academy of Sciences, Staromonetnyi per. 35, Moscow, 109017, Russia |
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| Abstract: | The solubility of ZrO2(baddeleyite) in HCl, HF, H2SO4, NaOH, and Na2CO3 solutions was determined by the capsule method at 500°C and 1000 bar. Baddeleyite is the only solid phase detected in the experimental products. Based on the ZrO2(baddeleyite) solubility measurements, the values of equilibrium constants at 500°C and 1000 bar (consistent with the Gibbs free energies of all the reactants) were obtained for the following reactions: ZrO2(cr) + H2SO 4 0 = Zr(OH)2OH 4 0 (pKo = 4.95), ZrO2(cr) + 2H2SO 4 0 = Zr(SO4) 2 0 ) + 2H2O (pKo = 3.74), ZrO2(cr) + H2O + HF0 = Zr(OH)3F0 (pKo = 3.35), ZrO2(cr) + 2HF0 = Zr(OH)2F 2 0 (pKo = 2.37), and ZrO2(cr) + 2H2O + OH? = Zr(OH) 5 ? (pKo = 4.39). Ionization constants were estimated for the chloride, fluoride, sulfate, and hydroxo complexes of zirconium. Using the experimental data and thermodynamic information derived from experiments and the electrostatic model of the ionization of electrolytes, it was shown that no more than n mg zirconium per one kilogram H2O can be accumulated in high-temperature fluids at 500°C and 1000 bar. |
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