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Co-variability of S6+, S4+, and S2− in apatite as a function of oxidation state: Implications for a new oxybarometer

  • Brian A. Konecke EMAIL logo , Adrian Fiege , Adam C. Simon , Fleurice Parat and André Stechern
Published/Copyright: March 6, 2017
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American Mineralogist
From the journal American Mineralogist Volume 102 Issue 3

Abstract

In this study, we use micro-X-ray absorption near-edge structures (μ-XANES) spectroscopy at the S K-edge to investigate the oxidation state of S in natural magmatic-hydrothermal apatite (Durango, Mexico, and Mina Carmen, Chile) and experimental apatites crystallized from volatile-saturated lamproitic melts at 1000 °C and 300 MPa over a broad range of oxygen fugacities [(log(fO2) = FMQ, FMQ+1.2, FMQ+3; FMQ = fayalite-magnetite-quartz solid buffer]. The data are used to test the hypothesis that S oxidation states other than S6+ may substitute into the apatite structure. Peak energies corresponding to sulfate S6+ (~2482 eV), sulfite S4+ (~2478 eV), and sulfide S2− (~2470 eV) were observed in apatite, and the integrated areas of the different sulfur peaks correspond to changes in fO2 and bulk S content. Here, multiple tests confirmed that the S oxidation state in apatite remains constant when exposed to the synchrotron beam, at least for up to 1 h exposure (i.e., no irradiation damages). To our knowledge, this observation makes apatite the first mineral to incorporate reduced (S2−), intermediate (S4+), and oxidized (S6+) S in variable proportions as a function of the prevailing fO2 of the system.

Apatites crystallized under oxidizing conditions (FMQ+1.2 and FMQ+3), where the S6+/STotal peak area ratio in the coexisting glass (i.e., quenched melt) is ~1, are dominated by S6+ with a small contribution of S4+, whereas apatites crystallizing at reduced conditions (FMQ) contain predominantly S2−, lesser amounts of S6+, and possibly traces of S4+. A sulfur oxidation state vs. S concentration analytical line transect across hydrothermally altered apatite from the Mina Carmen iron oxide-apatite (IOA) deposit (Chile) demonstrates that apatite can become enriched in S4+ relative to S6+, indicating metasomatic overprinting via a SO2-bearing fluid or vapor phase. This XANES study demonstrates that as the fO2 increases from FQM to FMQ+1.2 to FMQ+3 the oxidation state of S in igneous apatite changes from S2− dominant to S6+ > S4+ to S6+ ≫ S4+. Furthermore, these results suggest that spectroscopic studies of igneous apatite have potential to trace the oxidation state of S in magmas. The presence of three S oxidations states in apatite may in part explain the non-Henrian partitioning of S between apatite and melt. Our study reveals the potential to use the S signature of apatite to elucidate both oxygen and sulfur fugacity in magmatic and hydrothermal systems.

Keywords: Apatite; sulfur oxidation state; XANES; oxybarometer; apatite crystallization experiments

Special collection papers can be found online at http://www.minsocam.org/MSA/AmMin/special-collections.html.

Acknowledgments

We acknowledge the experimental and analytical facilities at Leibniz University Hannover (LUH), University of Michigan (UM), American Museum of Natural History (AMNH), and GeoSoilEnviroCars (Sector 13), Advanced Photon Source (APS), Argonne National Laboratory. We thank M. Newville and T. Lanzarotti for assistance and discussion during S XANES analysis. We also thank T. Hudgins, P. Ruprecht, and N. La Cruz for their assistance in data collection; S. Wilke, and O. Namur for their assistance during experiments; and J. Knipping, T. Childress, M. Reich, and F. Barra for collecting the Carmen sample. Finally, we thank Z. Zajacz and J. Dilles for their constructive reviews, and are grateful for the editorial handling of J. Hughes. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This work was funded by the NSF, EAR-Grant No. 1524394. B.A.K acknowledges support from Rackham Graduate School (UM) and a Society of Economic Geologists Student Research Grant.

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Received: 2016-6-30
Accepted: 2016-10-26
Published Online: 2017-3-6
Published in Print: 2017-3-1

© 2017 by Walter de Gruyter Berlin/Boston

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https://doi.org/10.2138/am-2017-5907
Keywords for this article
Apatite; sulfur oxidation state; XANES; oxybarometer; apatite crystallization experiments

Articles in the same Issue

  1. Special collection: From magmas to ore deposits
  2. Sulfide-silicate textures in magmatic Ni-Cu-PGE sulfide ore deposits: Disseminated and net-textured ores
  3. Special collection: Olivine
  4. Nickel variability in Hawaiian olivine: Evaluating the relative contributions from mantle and crustal processes
  5. Special collection: Water in nominally hydrous and anhydrous minerals
  6. Hydrogen incorporation mechanisms in forsterite: New insights from 1H and 29Si NMR spectroscopy and first-principles calculation
  7. Special collection: Water in nominally hydrous and anhydrous minerals
  8. New SIMS reference materials for measuring water in upper mantle minerals
  9. Special collection: Apatite: A common mineral, uncommonly versatile
  10. Co-variability of S6+, S4+, and S2− in apatite as a function of oxidation state: Implications for a new oxybarometer
  11. Special collection: Apatite: A common mineral, uncommonly versatile
  12. Apatite in the dike-gabbro transition zone of mid-ocean ridge: Evidence for brine assimilation by axial melt lens
  13. Special collection: Apatite: A common mineral, uncommonly versatile
  14. LA-Q-ICP-MS apatite U/Pb geochronology using common Pb in plagioclase: Examples from layered mafic intrusions
  15. Special collection: Apatite: A common mineral, uncommonly versatile
  16. Chlorine and fluorine partitioning between apatite and sediment melt at 2.5 GPa, 800 °C: A new experimentally derived thermodynamic model
  17. Outlooks in earth and planetary materials
  18. On the mineralogy of the “Anthropocene Epoch”
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  22. Representative size distributions of framboidal, euhedral, and sunflower pyrite from high-resolution X-ray tomography and scanning electron microscopy analyses
  24. Phase relations of MgFe2O4 at conditions of the deep upper mantle and transition zone
  26. Thermodynamics and crystal chemistry of rhomboclase, (H5O2)Fe(SO4)2⋅2H2O, and the phase (H3O)Fe(SO4)2 and implications for acid mine drainage
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  30. A new high-pressure phase transition in clinoferrosilite: In situ single-crystal X-ray diffraction study
  32. Investigating nanoscale mineral compositions: Iron L3-edge spectroscopic evaluation of iron oxide and oxy-hydroxide coordination
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  36. Hollisterite (Al3Fe), kryachkoite (Al,Cu)6(Fe,Cu), and stolperite (AlCu): Three new minerals from the Khatyrka CV3 carbonaceous chondrite
  38. New Mineral Names
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