Formation of compounds with alunite-like structure in the Bi2O3–Al2O3–Fe2O3–P2O5–H2O system under hydrothermal conditions

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Abstract

Under hydrothermal conditions in the Bi2O3-Al2O3–Fe2O3–P2O5–H2O system, variable-composition compounds Bi(Al1–xFex)3(PO4)2(OH)6 with an alunite-like structure were obtained. Based on experimental data on the miscibility limits of components in the (1–x)BiAl3(PO4)2(OH)6–xBiFe3(PO4)2(OH)6 system, the parameters of the subregular solution model (Q1 = 6.395, Q2 = 8.987 kJ/mol) were determined, and spinodal and binodal decomposition curves of solid solutions with an alunite-like structure were calculated. Thermodynamic calculations showed that individual BiAl3(PO4)2(OH)6 and BiFe3(PO4)2(OH)6 can form at temperatures above 122 and 170°C, respectively, which is consistent with the experimental data obtained in this study, indicating the absence of compounds with alunite-like structure at 160°C in the range 0.8 < x ≤ 1.

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About the authors

D. P. Elovikov

Petersburg Nuclear Physics Institute named by B.P. Konstantinov of National Research Centre “Kurchatov Institute”; St. Petersburg Electrotechnical University “LETI”

Author for correspondence.
Email: syncdima@mail.ru

Institute of Silicate Chemistry

Russian Federation, St. Petersburg, 199034; St. Petersburg, 197022

O. V. Proskurina

Ioffe Institute; St. Petersburg State Technological Institute

Email: syncdima@mail.ru
Russian Federation, St. Petersburg, 194021; St. Petersburg, 190013

V. V. Gusarov

Petersburg Nuclear Physics Institute named by B.P. Konstantinov of National Research Centre “Kurchatov Institute”; Ioffe Institute

Email: syncdima@mail.ru

Institute of Silicate Chemistry

Russian Federation, St. Petersburg, 199034; St. Petersburg, 194021

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Supplementary files

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2. Fig. 1. X-ray diffraction patterns of samples 1–10 (Table 1) after isothermal holding under hydrothermal conditions at 160°C and a pressure of ~6 MPa for 10 days.

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3. Fig. 2. X-ray diffraction patterns of samples obtained with different durations of isothermal holding of a water-salt suspension with a given stoichiometry of elements to form compounds of variable composition in the (1 – x)BiAl3(PO4)2(OH)6–xBiFe3(PO4)2(OH)6 system, where x0 = 0.5: a — 8, b — 14, c — 23, d — 30, d — 90 days. Line designations in the figure by color: red — calculation, black — experiment, purple — difference between calculation and experiment, blue and green — structure of the composition with a higher and lower iron content, respectively.

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4. Fig. 3. Dependence of the unit cell volume (V) of Bi(Al1–xFex)3(PO4)2(OH)6 solid solutions with alunite-like structure on the iron content in the (1 – x)BiAl3(PO4)2(OH)6–xBiFe3(PO4)2(OH)6 system. Black symbols are the iron content in the structure, according to X-ray diffraction analysis, for samples 1–7, red symbols are the iron content in the structure at different durations of isothermal holding for sample 5. Symbols with an unpainted middle correspond to the compositions of the (1–x)BiAl3(PO4)2(OH)6 system with non-single-phase samples.

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5. Fig. 4. Dependences of the Gibbs energy of formation of compounds with an alunite-like structure in the (1 – x)BiAl3(PO4)2(OH)6–xBiFe3(PO4)2(OH)6 system (a, solid line) and the Gibbs energy of mixing (b) on the temperature and iron content in the system; curves of spinodal and binodal decomposition of the phase with an alunite-like structure (c) in this system. Designations in figures (a) and (b): 1 — 122, 2 — 150, 3 — 160, 4 — 170°C. Points in figure c: diamonds — compositions 8 and 9 (Table 1).

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