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Licensed Unlicensed Requires Authentication Published by De Gruyter September 20, 2020

Structure of NaFeSiO4, NaFeSi2O6, and NaFeSi3O8 glasses and glass-ceramics

Mostafa Ahmadzadeh ORCID logo , Alex Scrimshire , Lucy Mottram , Martin C. Stennett , Neil C. Hyatt , Paul A. Bingham and John S. McCloy
From the journal American Mineralogist


The crystallization of iron-containing sodium silicate phases holds particular importance, both in the management of high-level nuclear wastes and in geosciences. Here, we study three as-quenched glasses and their heat-treated chemical analogs, NaFeSiO4, NaFeSi2O6, and NaFeSi3O8 (with nominal stoichiometries from feldspathoid, pyroxene, and feldspar mineral groups, i.e., Si/Fe = 1, 2, and 3, respectively) using various techniques. Phase analyses revealed that as-quenched NaFeSiO4 could not accommodate all Fe in the glass phase (some Fe crystallizes as Fe3O4), whereas as-quenched NaFeSi2O6 and NaFeSi3O8 form amorphous glasses. NaFeSi2O6 glass is the only composition that crystallizes into its respective isochemical crystalline polymorph, i.e., aegirine, upon isothermal heat-treatment. As revealed by Mössbauer spectroscopy, iron is predominantly present as fourfold-coordinated Fe3+ in all glasses, though it is present as sixfold-coordinated Fe3+ in the aegirine crystals (NaFeSi2O6), as expected from crystallography. Thus, Na-Fe silicate can form a crystalline phase in which it is octahedrally coordinated, even though it is mostly tetrahedrally coordinated in the parent glasses. Thermal behavior, magnetic properties, iron redox state (including Fe K-edge X‑ray absorption), and vibrational properties (Raman spectra) of the above compositions are discussed.


The authors thank Daniel Neuville from the Institut de Physique du Globe de Paris (IPGP) for help with Raman spectroscopy measurements and interpretation.

  1. Funding

    This research was supported by the Department of Energy Waste Treatment and Immobilization Plant Federal Project Office, contract numbers DE-EM002904 and 89304017CEM000001, under the direction of Albert A. Kruger. A portion of this research used 6-BM of the National Synchrotron Light Source II (NSLSII), a U.S. DOE OS user facility operated for the DOE OS by Brookhaven National Laboratory (BNL) under contract DE-SC0012704. This work was, in part, performed in the HADES/MIDAS facility at the University of Sheffield, established with financial support of the Department for Business, Energy & Industrial Strategy and Engineering and Physical Sciences Research Council (EPSRC) under grant EP/T011424/1 (Hyatt et al. 2020). The U.K. portion of the research was sponsored, in part, by the UK Engineering and Physical Sciences Research Council under grants EP/N017870/1 and EP/S01019X/1.

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Received: 2019-09-13
Accepted: 2020-02-14
Published Online: 2020-09-20
Published in Print: 2020-09-25

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