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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)

  • H. Wayne Nesbitt EMAIL logo , G. Michael Bancroft and Grant S. Henderson
Published/Copyright: April 29, 2020
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American Mineralogist
From the journal American Mineralogist Volume 105 Issue 5

Abstract

29Si NMR and Raman spectroscopic studies demonstrate that fusion of crystalline orthosilicates and metasilicates produces melts more polymerized than their precursor crystals. Forsterite, for example, consists of 100% Q0 species, whereas its melt consists of ~50 mol% of Q1 species (Q = a Si tetrahedron and the superscript indicates the number of bridging oxygen atoms in the tetrahedron). Polymerization during melting can be rationalized from an energetics perspective. Si-NBO-M moieties of Q species are more susceptible to librational, rotational, and vibrational modes than are Si-BO-Si moieties (NBO = non-bridging oxygen; BO = bridging oxygen; M = counter cation). Thermal agitation activates these additional modes, thus increasing the CP and free energy of melts. The reaction of Qn to Qn+1 species during melting eliminates Si-NBO-M moieties and produces Si-O-Si moieties that are less susceptible to the additional modes, thereby minimizing the CP of melts. By decreasing the abundances of Q0, Q1, and Q2 species in favor of Q3 and Q4 species, melts become more stable. In the absence of polymerization, melting temperatures of minerals would be appreciably greater than observed.

Polymerization involves formation of Si-O bonds, which are strongly endothermic (Si-O bond dissociation is ~798 kJ/mol). The large heats of fusion (ᐃHf) of orthosilicates result primarily from polymerization reactions during melting (ᐃHf of forsterite, fayalite, and tephroite are ~142, ~92, and ~90 kJ/mol). The fusion of metasilicates and sorosilicates (e.g., pyroxenes and melilites) involves endothermic polymerization and exothermic depolymerization reactions, although the former dominates. These reactions tend to negate each other during melting, yielding less positive ᐃHf values than observed for orthosilicate fusion (e.g., ᐃHf of enstatite, diopside, pseudowollastonite, and åkermanite are ~73, ~69, ~57, and ~62 kJ/mol). Where polymerization and depolymerization reactions are absent ᐃHf is low and is due mostly to disordering during melting (e.g., ᐃHf of cristobalite is ~8.9 kJ/mol).

Experimental evidence indicates that ferric iron is present as a negatively charged oxyanionic complex in melts (e.g., [FeO2]1–) so that oxidation of Fe2+ should proceed according to: 4Femelt2++1O2+6Omelt2−→4[FeO2]melt1−.

Free oxygen (O2–), a by-product of polymerization reactions, drives the reaction to the right. Mid-ocean ridge basalts (MORBs) consequently should be more oxidized than their source (e.g., lherzolites) or their residues (e.g., harzburgites). Extraction of melt from the upper mantle and deposition in the crust should produce a crust more oxidized than its upper mantle source. Production of O2– during melting and its presence in alkali-rich magmas also explains the alkali-ferric iron effect.

Keywords: Silicate melting; mantle melting; Q species energetics; heats of fusion; polymerization reactions; MORB redox reactions

Acknowledgments

The authors thank Tony Withers for insightful discussion and for reading the manuscript. We also thank B. Mysen and another anonymous reviewer for reading the manuscript and offering numerous comments that resulted in a substantially improved manuscript. The authors thank their respective Universities and departments for logistical support during the conduct of this research.

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Received: 2018-10-08
Accepted: 2019-12-07
Published Online: 2020-04-29
Published in Print: 2020-05-26

© 2020 Walter de Gruyter GmbH, Berlin/Boston

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https://doi.org/10.2138/am-2020-6841
Keywords for this article
Silicate melting; mantle melting; Q species energetics; heats of fusion; polymerization reactions; MORB redox reactions

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  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
  8. Cassiterite crystallization experiments in alkali carbonate aqueous solutions using a hydrothermal diamond-anvil cell
  9. New insights into the nature of glauconite
  10. Kaolinization of 2:1 type clay minerals with different swelling properties
  11. The quintet completed: The partitioning of sulfur between nominally volatile-free minerals and silicate melts
  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
  15. Lingbaoite, AgTe3, a new silver telluride from the Xiaoqinling gold district, central China
  16. Oxygen isotope fractionation between gypsum and its formation waters: Implications for past chemistry of the Kawah Ijen volcanic lake, Indonesia
  17. Presentation of the 2018 MSA Award of the Mineralogical Society of America to Laura Nielsen Lammers
  18. Acceptance of the 2018 MSA Award of the Mineralogical Society of America
  19. Presentation of the Dana Medal of the Mineralogical Society of America for 2019 to Matthew J. Kohn
  20. Acceptance of the Dana Medal of the Mineralogical Society of America for 2019
  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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