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The quintet completed: The partitioning of sulfur between nominally volatile-free minerals and silicate melts

  • Sara Callegaro EMAIL logo , Kalotina Geraki , Andrea Marzoli , Angelo de Min , Victoria Maneta and Don R. Baker
Published/Copyright: April 29, 2020
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American Mineralogist
From the journal American Mineralogist Volume 105 Issue 5

Abstract

Magmatic systems are dominated by five volatiles, namely H2O, CO2, F, Cl, and S (the igneous quintet). Multiple studies have measured partitioning of four out of these five volatiles (H2O, CO2, F, and Cl) between nominally volatile-free minerals and melts, whereas the partitioning of sulfur is poorly known. To better constrain the behavior of sulfur in igneous systems we measured the partitioning of sulfur between clinopyroxene and silicate melts over a range of pressure, temperature, and melt composition from 0.8 to 1.2 GPa, 1000 to 1240 °C, and 49 to 66 wt% SiO2 (13 measurements). Additionally, we determined the crystal-melt partitioning of sulfur for plagioclase (6 measurements), orthopyroxene (2 measurements), amphibole (2 measurements), and olivine (1 measurement) in some of these same run products. Experiments were performed at high and low oxygen fugacities, where sulfur in the melt is expected to be dominantly present as an S6+ or an S2– species, respectively. When the partition coefficient is calculated as the total sulfur in the crystal divided by the total sulfur in the melt, the partition coefficient varies from 0.017 to 0.075 for clinopyroxene, from 0.036 to 0.229 for plagioclase, and is a maximum of 0.001 for olivine and of 0.003 for orthopyroxene. The variation in the total sulfur partition coefficient positively correlates with cation-oxygen bond lengths in the crystals; the measured partition coefficients increase in the order: olivine < orthopyroxene < clinopyroxene ≤ amphibole and plagioclase. At high oxygen fugacities in hydrous experiments, the clinopyroxene/melt partition coefficients for total sulfur are only approximately one-third of those measured in low oxygen fugacity, anhydrous experiments. However when the partition coefficient is calculated as total sulfur in the crystal divided by S2– in the melt, the clinopyroxene/melt partition coefficients for experiments with melts between ~51 and 66 wt% SiO2 can be described by a single mean value of 0.063 ± 0.010 (1σ standard deviation about the mean). These two observations support the hypothesis that sulfur, as S2–, replaces oxygen in the crystal structure. The results of hydrous experiments at low oxygen fugacity and anhydrous experiments at high oxygen fugacity suggest that oxygen fugacity has a greater effect on sulfur partitioning than water. Although the total sulfur clinopyroxene-melt partition coefficients are affected by the Mg/(Mg+Fe) ratio of the crystal, partition coefficients calculated using S2– in the melt display no clear dependence upon the Mg# of the clinopyroxene. Both the bulk and the S2– partition coefficients appear unaffected by IVAl in the clinopyroxene structure. No effect of anorthite content nor of iron concentration in the crystal was seen in the data for plagioclase-melt partitioning. The data obtained for orthopyroxene and olivine were too few to establish any trends. The partition coefficients of total sulfur and S2– between the crystals studied and silicate melts are typically lower than those of fluorine, higher than those of carbon, and similar to those of chlorine and hydrogen. These sulfur partition coefficients can be combined with analyses of volatiles in nominally volatile-free minerals and previously published partition coefficients of H2O, C, F, and Cl to constrain the concentration of the igneous quintet, the five major volatiles in magmatic systems.

Keywords: Clinopyroxene/melt sulfur partitioning; equilibrium melts; magmatic volatiles; synchrotron micro X‑ray fluorescence

Acknowledgments and Funding

We thank two anonymous reviewers for their insightful suggestions and K. Iacovino for her comments on an earlier version of this manuscript. This research was supported by an NSERC Discovery Grant to D.R.B. and by the 2014 SIMP prize grant dedicated to the memory of E.M. Piccirillo awarded to S.C. Further support from PRIN (PRIN 20178LPCP) to A. Marzoli is gratefully acknowledged. The synchrotron measurements were supported by Diamond Light Source.

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Received: 2019-07-01
Accepted: 2019-12-20
Published Online: 2020-04-29
Published in Print: 2020-05-26

© 2020 Walter de Gruyter GmbH, Berlin/Boston

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  28. Erratum
https://doi.org/10.2138/am-2020-7188
Keywords for this article
Clinopyroxene/melt sulfur partitioning; equilibrium melts; magmatic volatiles; synchrotron micro X‑ray fluorescence

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  1. Texture constraints on crystal size distribution methodology: An application to the Laki fissure eruption
  2. Hydrogenation reactions of carbon on Earth: Linking methane, margarine, and life
  3. Abiotic and biotic processes that drive carboxylation and decarboxylation reactions
  4. In-situ measurements of magmatic volatile elements, F, S, and Cl, by electron microprobe, secondary ion mass spectrometry, and heavy ion elastic recoil detection analysis
  5. MSA Centennial Symposium
  6. An evolutionary system of mineralogy. Part I: Stellar mineralogy (>13 to 4.6 Ga)
  7. A structural study of size-dependent lattice variation: In situ X-ray diffraction of the growth of goethite nanoparticles from 2-line ferrihydrite
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  12. 222Rn and 220Rn emanations from powdered samples of samarskite as a function of annealing temperature
  13. Polymerization during melting of ortho- and meta-silicates: Effects on Q species stability, heats of fusion, and redox state of mid-ocean range basalts (MORBs)
  14. Formation of native arsenic in hydrothermal base metal deposits and related supergene U6+ enrichment: The Michael vein near Lahr, SW Germany
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  21. Presentation of the Mineralogical Society of America Award for 2019 to Olivier Namur
  22. Acceptance of the Mineralogical Society of America Award for 2019
  23. Presentation of the 2019 MSA Distinguished Public Service Medal to Rodney C. Ewing
  24. Acceptance of Distinguished Public Service Award of the Mineralogical Society of America for 2019
  25. Presentation of the 2019 Roebling Medal of the Mineralogical Society of America to Peter R. Buseck
  26. Acceptance of the 2019 Roebling Medal of the Mineralogical Society of America
  27. Erratum
  28. Erratum
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