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Thermodynamic characterization of synthetic lead-arsenate apatites with different halogen substitutions

  • Bartosz Puzio ORCID logo , Lei Zhang , Jennifer E.S. Szymanowski , Peter C. Burns ORCID logo and Maciej Manecki
Published/Copyright: March 30, 2023
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American Mineralogist
From the journal American Mineralogist Volume 108 Issue 4

Abstract

Thermodynamic parameters have been measured for synthetic analogs of the mimetite- group minerals Pb5(AsO4)3X (X = OH, Cl, Br, I) belonging to the apatite supergroup. Phases precipitated from aqueous solutions under ambient conditions with well characterized structures and compositions were studied. For each phase, dissolution enthalpy was experimentally determined by oxide melt drop solution calorimetry in a molten solvent of sodium molybdate (3Na2O·4MoO3) at 976 K. The enthalpy of formation from the elements Δ H f , e l ∘ was calculated using thermochemical cycles and was −3030.6 ± 11.5, −3026.6 ± 15.8, −2967.6 ± 25.0, and −2993.1 ± 12.2 kJ/mol for Pb5.00(AsO4)3.00OH0.86(CO3)0.07, Pb5.00(AsO4)3.00Cl0.80(CO3)0.10, Pb5.00(AsO4)3.00Br0.80(CO3)0.10, and Pb5.00(AsO4)3.00I0.45OH0.35(CO3)0.10, respectively. These Δ H f , e l ∘ values exhibit typical trends for apatites: they increased (were less negative) with the increasing molar mass and ionic radius of X and decreased with the electronegativity and ionization energy of X. The compilation and comparison of data for Ca-, Pb-, P-, and As-apatites revealed correlations indicating that thermodynamic enthalpic stability is largely influenced by chemical factors (e.g., differences in electronegativities of the elements, ionization energy, or ionic characteristics of the bonds) and to a lesser extent by physical and geometric parameters in the crystal structure related to the mass and size of the X anion. Using the correlations, it was possible to estimate the value of hitherto unknown Δ H f , e l ∘ for Pb5(AsO4)3F, −3144.3 ± 66.5 kJ/mol. The observed relationships apply to the entire apatite supergroup and can be used to predict the values of Δ H f , e l ∘ for phases that have not been studied experimentally. The new data on environmentally significant phases will contribute to the modeling of mineral-water interactions, particularly for potential use in the remediation of soils and wastes contaminated with Pb and As and in the immobilization of radioactive waste containing I-129.

Keywords: Lead apatite; lead arsenates; calorimetry; enthalpy; mimetite; iodoapatites

Funding statement: Financial support for the research was provided to B.P. by the Polish National Science Center (NCN) [Grant No. 2017/27/N/ST10/00776]. The calorimetry portion of this work was funded by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [Grant No. DE-FG02-07ER15880].

Acknowledgments

We greatly appreciate the comments of Associate Editor Charles A. Geiger and the four anonymous reviewers, which have helped us to improve the manuscript. I am grateful for the brainstorming session with Małgorzata Lempart-Drozd, which helped to improve the quality of the discussion of the results obtained. Many thanks to my friend Grzegorz Rzepa for the time we spent together on the SEM/EDS analyses, which proved to be revealing.

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Received: 2020-01-23
Accepted: 2022-04-01
Published Online: 2023-03-30
Published in Print: 2023-04-25

© 2023 by Mineralogical Society of America

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https://doi.org/10.2138/am-2020-7452
Keywords for this article
Lead apatite; lead arsenates; calorimetry; enthalpy; mimetite; iodoapatites

Articles in the same Issue

  1. Mineralogy and geochemistry of hot spring deposits at Námafjall, Iceland: Analog for sulfate soils at Gusev crater, Mars
  2. The iron spin transition of deep nitrogen-bearing mineral Fe3N1.2 at high pressure
  3. Hydrogen occupation and hydrogen-induced volume expansion in Fe0.9Ni0.1Dx at high P-T conditions
  4. Volumes and spin states of FeHx: Implication for the density and temperature of the Earth’s core
  5. Thermodynamic characterization of synthetic lead-arsenate apatites with different halogen substitutions
  6. Structural changes in shocked tektite and their implications to impact-induced glass formation
  7. Characterization of vandenbrandeite: A potential alteration product of spent nuclear fuel
  8. The NaCl-CaCO3 and NaCl-MgCO3 systems at 6 GPa: Link between saline and carbonatitic diamond forming melts
  9. Single-crystal elasticity of (Al,Fe)-bearing bridgmanite up to 82 GPa
  10. Single-crystal X-ray diffraction of fluorapatite to 61 GPa
  11. Iron and aluminum substitution mechanism in the perovskite phase in the system MgSiO3-FeAlO3-MgO
  12. Ultrasonic studies of alkali-rich hydrous silicate glasses: Elasticity, density, and implications for water dissolution mechanisms
  13. Gadolinium-dominant monazite and xenotime: Selective hydrothermal enrichment of middle REE during low-temperature alteration of uraninite, brannerite, and fluorapatite (the Zimná Voda REE-U-Au quartz vein, Western Carpathians, Slovakia)
  14. Nucleation of Th-rich cerianite on halloysite surface in a regolith-hosted rare earth elements deposit in South China
  15. Presentation of the Dana Medal of the Mineralogical Society of America for 2022 to Cin-Ty Lee
  16. Acceptance of the Dana Medal of the Mineralogical Society of America for 2022
  17. Presentation of the Mineralogical Society of America Award for 2022 to Benjamin M. Tutolo
  18. Acceptance of the Mineralogical Society of America Award for 2022
  19. Presentation of the 2022 Roebling Medal of the Mineralogical Society of America to John W. Valley
  20. Acceptance of the 2022 Roebling Medal of the Mineralogical Society of America
  21. New Mineral Names
  22. Book Review
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