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

Abstract

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) +more »« less

Authors:: 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.

Publication Date:: Sat Jan 07 00:00:00 EST 2017

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

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

OSTI Identifier:: 1374595

Alternate Identifier(s):: OSTI ID: 1397831

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

Resource Type:: Accepted Manuscript

Journal Name:: Geochimica et Cosmochimica Acta

Additional Journal Information:: Journal Volume: 203; Journal Issue: C; Journal ID: ISSN 0016-7037

Publisher:: The Geochemical Society; The Meteoritical Society

Country of Publication:: United States

Language:: English

Subject:: 58 GEOSCIENCES

Citation Formats


                    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., and Weber, J. K.R. Local structural variation with oxygen fugacity in Fe2SiO4+x fayalitic iron silicate melts.  United States: N. p., 2017. 
Web.  doi:10.1016/j.gca.2016.12.038.

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                    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. Local structural variation with oxygen fugacity in Fe2SiO4+x fayalitic iron silicate melts.  United States.  https://doi.org/10.1016/j.gca.2016.12.038

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                    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., and Weber, J. K.R. Sat .  
"Local structural variation with oxygen fugacity in Fe2SiO4+x fayalitic iron silicate melts".  United States.  https://doi.org/10.1016/j.gca.2016.12.038.  https://www.osti.gov/servlets/purl/1374595.

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@article{osti_1374595,

  title        = {Local structural variation with oxygen fugacity in Fe2SiO4+x fayalitic iron silicate melts},

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

  abstractNote = {Here, the structure of molten Fe2SiO4+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, nFeO, close to 5 for all Fe3+/ΣFe. Diffraction measurements yielded values of 4.4(2) < nFeO < 4.7(1). There is limited evidence for a linear trend nFeO(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 rFeO lie close to 2.06 Å, consistent with nFeO 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.},

  doi          = {10.1016/j.gca.2016.12.038},

  journal      = {Geochimica et Cosmochimica Acta},

  number       = C,

  volume       = 203,

  place        = {United States},

  year         = {Sat Jan 07 00:00:00 EST 2017},

  month        = {Sat Jan 07 00:00:00 EST 2017}

}

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Wilke, Max; Farges, François; Petit, Pierre-Emmanuel
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Variation in oxygen fugacity with depth in the upper mantle beneath the Kaapvaal craton, Southern Africa
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Woodland, A. B.; Koch, M.
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Zhang, H. L.; Hirschmann, M. M.; Cottrell, E.
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journal, May 2019

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International Journal of Applied Glass Science, Vol. 10, Issue 4
DOI: 10.1111/ijag.13479

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

Abstract

Citation Formats

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Laser hearth melt processing of ceramic materials journal, February 1996

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

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journal, October 2015

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Temperature-dependent structural heterogeneity in calcium silicate liquids
journal, December 2010

XANES calibrations for the oxidation state of iron in a silicate glass
journal, July 2003

Oxidation state of iron in komatiitic melt inclusions indicates hot Archaean mantle
journal, October 2008

The system, FeO-SiO 2
journal, September 1932

Bond-valence parameters obtained from a systematic analysis of the Inorganic Crystal Structure Database
journal, August 1985

Local structure and dynamics of high temperature SrO–Al2O3 liquids studied by 27Al NMR and Sr K-edge XAS spectroscopy
journal, November 2001

Physical properties of CaAl2Si2O8–CaMgSi2O6–FeO–Fe2O3 melts: Analogues for extra-terrestrial basalt
journal, May 2013

The oxidation state of Fe in MORB glasses and the oxygen fugacity of the upper mantle
journal, May 2011

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journal, November 2009

The System Iron-Oxygen. I. The Wüstite Field and Related Equilibria
journal, August 1945

The System Iron—Oxygen. II. Equilibrium and Thermodynamics of Liquid Oxide and Other Phases
journal, May 1946

The effect of oxidation state on the viscosity of melts in the system Na2O-FeO-Fe2O3-SiO2
journal, February 1987

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journal, December 2012

Structure of (Fe $_{x}$ Ca $_{1 - x}$ O) $_{y}$ (SiO $_{2}$ ) $_{1 - y}$ liquids and glasses from high-energy x-ray diffraction: Implications for the structure of natural basaltic magmas
journal, June 2013

Slag remains from the Na Slupi site (Prague, Czech Republic): evidence for early medieval non-ferrous metal smelting
journal, January 2015

The effect of redox state on the local structural environment of iron in silicate glasses: a combined XAFS spectroscopy, molecular dynamics, and bond valence study
journal, October 2004

The Redox State of Earth's Mantle
journal, May 2008

Quantification of rapid environmental redox processes with quick-scanning x-ray absorption spectroscopy (Q-XAS)
journal, September 2009

Resonant X-ray spectroscopy to study K absorption pre-edges in 3d transition metal compounds
journal, March 2009

A computer simulation study of natural silicate melts. Part I: Low pressure properties
journal, March 2007

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

Bonding and structure in network glasses
journal, November 2016

X-Ray Diffraction and Near Edge Studies of Iron Oxides and Alumina at High Temperatures Using Aerodynamic Levitation and Laser Heating
journal, January 1999

The structure of sodium iron silicate glass – a multi-technique approach
journal, August 1999

Komatiites I: Eruption and Flow
journal, August 1985

Fluid flow effects in levitated droplets
journal, January 2005

Convection in Containerless Processing
journal, November 2004

High-Temperature XAS Study of Fe2SiO4 Liquid: Reduced Coordination of Ferrous Iron
journal, October 1993

Multi-spectroscopic study of Fe(II) in silicate glasses: Implications for the coordination environment of Fe(II) in silicate melts
journal, September 2005

A Mössbauer study of the oxidation state of Fe in silicate melts
journal, November 2004

Carbonate Melts and Carbonatites
journal, January 2013

Viscosity of Fayalite-Based Slags
journal, January 1977

A comparison of various commonly used correlation functions for describing total scattering
journal, April 2001

Effect of oxygen fugacity on the coordination and oxidation state of iron in alkali bearing silicate melts
journal, September 2015

Glass Formation at the Limit of Insufficient Network Formers
journal, March 2004

Mineralogical and Chemical Characterization of Roman Slag from the Archaeological Site of Castra (Ajdovščina, Slovenia): Roman slag from Castra (Ajdovščina, Slovenia)
journal, June 2014

Natural widths of atomic K and L levels, K α X‐ray lines and several K L L Auger lines
journal, April 1979

The compressibility of silicate liquids containing Fe2O3 and the effect of composition, temperature, oxygen fugacity and pressure on their redox states
journal, July 1991

A possible effect of melt structure on the Mg-Fe2+ partitioning between olivine and melt
journal, June 2002

Structure of liquid oxides at very high temperatures
journal, January 2003

Kinetics and mechanisms of iron redox reactions in silicate melts: The effects of temperature and alkali cations
journal, April 2008

Temperature-induced boron coordination change in alkali borate glasses and melts
journal, January 2003

The differentiation of the Skaergaard Intrusion: A discussion of Hunter and Sparks (Contrib Mineral Petrol 95:451?461)
journal, February 1990

Oxidation state of iron in hydrous mantle phases: implications for subduction and mantle oxygen fugacity
journal, June 2004

Petrology on Mars
journal, November 2015

Redox state of iron in peralkaline rhyolitic glass/melt: X-ray absorption micro-spectroscopy experiments at high temperature
journal, August 2006

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journal, July 2014

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journal, May 2006

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journal, March 2001

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journal, September 1959

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journal, June 2005

Amorphous materials: Properties, structure, and durability: Quantification of the kinetics of iron oxidation in silicate melts using Raman spectroscopy and assessment of the role of oxygen diffusion
journal, November 2008

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journal, March 2000

Environment of ferrous iron in CaFeSi2O6 glass; contributions of EXAFS and molecular dynamics
journal, August 2000

Ferric-ferrous equilibria in natural silicate liquids at 1 bar
journal, February 1981

Discordant Iron-Rich Ultramafic Pegmatites in the Bushveld Complex and their Relationship to Iron-Rich Intercumulus and Residual Liquids
journal, August 1994

Petrogenetic linkages among fO2, isotopic enrichments-depletions and crystallization history in Martian basalts. Evidence from the distribution of phosphorus in olivine megacrysts
journal, November 2013

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journal, February 2012

Area detector corrections for high quality synchrotron X-ray structure factor measurements
journal, January 2012

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journal, January 2013

A time resolved high energy X-ray diffraction study of cooling liquid SiO2
journal, January 2013

Low Cation Coordination in Oxide Melts
journal, April 2014

Molten uranium dioxide structure and dynamics
journal, November 2014

Extracting the pair distribution function from white-beam X-ray total scattering data
journal, June 2011

Viscosity of liquid fayalite up to 9 GPa
journal, January 2015

Volcanism on Mars controlled by early oxidation of the upper mantle
journal, June 2013

Core formation and the oxidation state of the Earth
journal, July 2005

Evidence from X-ray absorption for network-forming Fe2+ in molten alkali silicates
journal, March 1988

Spectral Absorption Coefficient of Molten Aluminum Oxide from.0.385 to 0.780 mum
journal, March 1995

Laser hearth melt processing of ceramic materials
journal, February 1996

Determination of Fe3+ sites in a NaFeSi2O6 glass by neutron diffraction with isotopic substitution coupled with numerical simulation
journal, October 2006

Intermediate-range order in the silicate network glasses ${NaFe}_{x} {Al}_{1 - x} {Si}_{2} O_{6}$ $(x = 0, 0.5, 0.8, 1)$ : A neutron diffraction and empirical potential structure refinement modeling investigation
journal, August 2008

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journal, December 2008

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journal, January 2010