Local structural variation with oxygen fugacity in Fe2SiO4+x fayalitic iron silicate melts

Alderman, O. L.G.; Lazareva, L.; Wilding, M. C.; Benmore, C. J.; Heald, S.; Johnson, C. E.; Johnson, J. A.; Hah, H. -Y.; Sendelbach, S.; Tamalonis, A.; Skinner, L. B.; Parise, J. B.; Weber, J. K.R.

doi:10.1016/j.gca.2016.12.038

Title: Local structural variation with oxygen fugacity in Fe₂SiO_4+x fayalitic iron silicate melts

Journal Article · Sat Jan 07 00:00:00 EST 2017 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2016.12.038· OSTI ID:1374595

Alderman, O. L.G.; Lazareva, L.; Wilding, M. C.; Benmore, C. J.; Heald, S.; Johnson, C. E.; Johnson, J. A.; Hah, H. -Y.; Sendelbach, S.; Tamalonis, A.; Skinner, L. B.; Parise, J. B.; Weber, J. K.R.

Here, the structure of molten Fe₂SiO_4+x has been studied using both high-energy X-ray diffraction and Fe K-edge X-ray absorption near-edge structure (XANES) spectroscopy, combined with aerodynamic levitation and laser beam heating. A wide range of Fe³⁺ contents were accessed by varying the levitation and atmospheric gas composition. Diffraction measurements were made in the temperature (T) and oxygen partial pressure ranges 1624(21) < T < 2183(94) K (uncertainties in parentheses) and –5.6(3) < ΔFMQ < +2.8(5) log units (relative to the Fayalite-Magnetite-Quartz buffer). Iron K-edge XANES measurements covered the ranges 1557(33) < T < 1994(36) K and –2.1(3) < ΔFMQ < +4.4(3) log units. Fe³⁺ contents, x = Fe³⁺/ΣFe, estimated directly from the pre-edge peaks of the XANES spectra varied between 0.15(1) and 0.40(2). While these agree in some cases with semi-empirical models, notable discrepancies are discussed in the context of the redox kinetics and the limitations in both the models and in the calibrations used to derive oxidation state from XANES spectra. XANES pre-edge peak areas imply average Fe–O coordination numbers, n_FeO, close to 5 for all Fe³⁺/ΣFe. Diffraction measurements yielded values of 4.4(2) < n_FeO < 4.7(1). There is limited evidence for a linear trend n_FeO(x) = 4.46(3) + 0.4(1)x. Asymmetric Fe–O bond length distributions peak at around 1.96 Å and have a shoulder arising from longer interatomic distances. Mean r_FeO lie close to 2.06 Å, consistent with n_FeO close to 5. These observations suggest that Fe²⁺ is less efficient at stabilizing tetrahedral Fe³⁺ compared to large monovalent alkali cations. Comparison of in-situ XANES estimates of Fe³⁺/ΣFe in the melts to those of the quenched solids obtained from XANES as well as Mössbauer spectroscopy indicate rapid oxidation during cooling, enabled by stirring of the melt by the levitation gas flow. As such, the oxidation state of hot komatiitic and other highly fluid melts may not be retained, even during rapid cooling, as it is for cooler basaltic and more silicic magmas.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SBIR DE-SC0007564; BES DE-FG02-09ER46650

OSTI ID:: 1374595

Alternate ID(s):: OSTI ID: 1397831

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 203, Issue C; ISSN 0016-7037

Publisher:: The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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