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Calorimetric study of skutterudite (CoAs2.92) and heazlewoodite (Ni3S2)

  • Juraj Majzlan ORCID logo , Stefan Kiefer , Kristina Lilova , Tamilarasan Subramani , Alexandra Navrotsky , Marek Tuhý , Anna Vymazalová , Dmitriy A. Chareev , Edgar Dachs and Artur Benisek
Published/Copyright: December 1, 2022
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American Mineralogist
From the journal American Mineralogist Volume 107 Issue 12

Abstract

Nickel and cobalt arsenides, sulfarsenides, and sulfides occur in many hydrothermal ore deposits, but their thermodynamic properties are not well known, in some cases not known at all. In this work, we determined a full set of thermodynamic properties for heazlewoodite and skutterudite. Both phases were synthesized in evacuated silica tubes at elevated temperatures, and electron microprobe analyses gave their compositions as Ni3S2 and CoAs2.92, respectively. Enthalpies of formation were measured by high-temperature oxide-melt solution calorimetry. The reference phases were pure elements, thus eliminating any systematic errors related to such phases. The enthalpies of formation at T = 298.15 K and P = 105 Pa are –216.0 ± 8.4(2σ) and –88.2 ± 6.1 kJ·mol−1 for Ni3S2 and CoAs2.92, respectively. Entropies were calculated from low-temperature heat capacity (CP) data from relaxation (PPMS) calorimetry and are 133.8 ± 1.6 and 106.4 ± 1.3 J·mol–1·K–1, respectively. The calculated Gibbs free energies of formation are –210.0 ± 8.4 and –79.9 ± 6.2 kJ·mol−1 for Ni3S2 and CoAs2.92, respectively. The PPMS CP data, together with a set of differential scanning calorimetry measurements, were used to derive CP polynomials up to 700 K with the Kiefer model based on previously published frequencies of acoustic and optic modes. Equilibrium constants for selected reactions with an aqueous phase were calculated up to 700 K. Geochemical modeling in these systems, however, should await until more reliable data for other phases from the system Co-Ni-As-S are available.

Keywords: Heazlewoodite; skutterudite; enthalpy; entropy; geochemical modeling

Acknowledgments

We are thankful to Valentina L. Stolyarova and Gleb Pokrovski for their constructive criticism and comments. The work presented here was financially supported by a Deutsche Forschungsgemeinschaft grant MA 3927/32-1. Oxide melt solution calorimetry was supported by the U.S. Department of Energy Office of Basic Energy Sciences, under grant DE-FG02-97ER14749. The work of DACh is supported by RFBR, No. 20-35-70049.

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Received: 2021-10-08
Accepted: 2021-12-07
Published Online: 2022-12-01
Published in Print: 2022-12-16

© 2022 Mineralogical Society of America

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https://doi.org/10.2138/am-2022-8337
Keywords for this article
Heazlewoodite; skutterudite; enthalpy; entropy; geochemical modeling

Articles in the same Issue

  1. Oxidation of arcs and mantle wedges: It’s not all about iron and water
  2. Paragenesis of Li minerals in the Nanyangshan rare-metal pegmatite, Northern China: Toward a generalized sequence of Li crystallization in Li-Cs-Ta-type granitic pegmatites
  3. The new mineral tomiolloite, Al12(Te4+O3)5[(SO3)0.5(SO4)0.5](OH)24: A unique microporous tellurite structure
  4. Authigenic anatase nanoparticles as a proxy for sedimentary environment and porewater pH
  5. Color effects of Cu nanoparticles in Cu-bearing plagioclase feldspars
  6. Expanding the speciation of terrestrial molybdenum: Discovery of polekhovskyite, MoNiP2, and insights into the sources of Mo-phosphides in the Dead Sea Transform area
  7. Sound speed and refractive index of amorphous CaSiO3 upon pressure cycling to 40 GPa
  8. Calorimetric study of skutterudite (CoAs2.92) and heazlewoodite (Ni3S2)
  9. Melting phase equilibrium relations in the MgSiO3-SiO2 system under high pressures
  10. Effects of hydrostaticity and Mn-substitution on dolomite stability at high pressure
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