Influence of cerium addition and redox state on silicate structure and viscosity - Archive ouverte HAL
Article Dans Une Revue Journal of the American Ceramic Society Année : 2024

Influence of cerium addition and redox state on silicate structure and viscosity

Influence de l’addition de cérium et de l’état redox sur la structure et la viscosité des silicates

Résumé

The viscosities of Ce-free and Ce-bearing (∼1.3 mol%,∼6.5 wt.% Ce2O3) soda lime silicate (window glass) melts were measured with respect to oxidation state. Experiments were performed isothermally using a concentric-cylinder viscometer on melts equilibrated with successively reducing CO–CO2 gas mixtures within a gas tight vertical tube furnace at 1 atm. Viscosity measurement and sampling were performed at the end of each melt reduction step. Further, viscosities in the glass transition temperature range were estimated using the shift factor method applied to glass transition temperature values determined using differential scanning calorimetry (DSC) measurements on quenched glasses. The Ce speciation at each stepwise melt reduction was probed using Ce L3-edge X-ray absorption near-edge structure (XANES) spectroscopy, while structural information upon Ce addition and reduction was provided by Raman spectroscopy. The viscosities of these materials remain constant at this level of Ce addition and do not vary significantly with redox state at high temperature. Conversely, viscosity values in the glass transition temperature range increase upon both Ce addition and reduction. Our analysis, based on the glass composition analyses obtained via electron probe microanalyzer (EPMA), viscosity calculations, and observations of silicate structural changes, leads to the conclusion that the observed viscosity increase around the glass transition temperature is explained by the high ionic field strength of Ce ions as well as the polymerization behavior of the silicate matrix occurring during reduction of Ce. Because of its low concentration, resulting from its low solubility, Ce redox changes exert only minimal effects on the viscosity of this melt.
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samedi 1 mars 2025
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Dates et versions

hal-04751440 , version 1 (24-10-2024)

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Adrien Donatini, Luiz Pereira, Donald Dingwell, Kai‐uwe Hess, Dirk Müller, et al.. Influence of cerium addition and redox state on silicate structure and viscosity. Journal of the American Ceramic Society, In press, ⟨10.1111/jace.20113⟩. ⟨hal-04751440⟩
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