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Raman studies of Fe redox in Hanford low activity waste alumino-borosilicate glasses
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DOI：10.1016/j.jnoncrysol.2026.124094.png)
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Abstract
En 中文
Raman measurements were performed on two Fe-containing alumino-borosilicate waste glass series (one with Re as a surrogate for Tc, and the other without Re) synthesized under a wide range of redox conditions. Both series show similar Raman trends for two independent features sensitive to Fe valence. As the glasses become more reduced, most alumino-borosilicate features show minimal changes; however, a Fe3+-related feature near 950 cm-1 decreases area, while a Fe2+-related feature near 410 cm-1 appears at Fe2+/Fetotal ≥ 68% and increases area. The 950 cm-1 feature is correlated to Fe3+O4 tetrahedra polymerized to silicate tetrahedra from evidence presented here and elsewhere. To the best of our knowledge, the Fe2+-related 410 cm-1 peak is a new observation for silicate glasses, that may, in part, be due to motions within ferrous tetrahedra linked to silicate tetrahedra, according to the Raman spectra and lattice dynamics calculations for the crystalline Fe2+-silicate, pellyite. Raman also indicates Fe sites in these glasses are likely incorporated in the alumino-borosilicate network, and shows no evidence of isolated Fe sites surrounded by network modifying cations, such as Na+.
Keywords:
Fe redox
Raman spectroscopy
alumino-borosilicate glass
Fe2+
Fe3+
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3.5
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1.9W
Citations:
3.3W
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