Structure of NaFeSiO4, NaFeSi2O6, and NaFeSi3O8 glasses and glass-ceramics
2020
The crystallization of iron-containing sodium silicate phases holds particular importance,
both in the management high-level nuclear wastes and in geosciences. Here, we study three asquenched glasses and their heat-treated chemical analogues, NaFeSiO4, NaFeSi2O6, and
NaFeSi3O8 (with nominal stoichiometries from feldspathoid, pyroxene, and feldspar mineral
groups – i.e., Si/Fe = 1, 2, and 3 respectively) – using a variety of techniques. Phase analyses
revealed that as-quenched NaFeSiO4 cannot accommodate all Fe in the glass phase (some Fe
crystallizes as Fe3O4), whereas as-quenched NaFeSi2O6 and NaFeSi3O8 form amorphous glasses
upon quenching. NaFeSi2O6 glass is the only composition that crystallizes into its respective
isochemical crystalline polymorph, i.e. aegirine, upon isothermal heat-treatment. As revealed by
Mossbauer spectroscopy, iron is predominantly present as 4-coordinated Fe3+ in all glasses, though
it is present as 6-coordinated Fe3+ in the aegirine crystals (NaFeSi2O6), as expected from
crystallography. Thus, Fe can form the crystalline phases 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.
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