In-situ study of phase changes in glass by impedance spectroscopy and scaling

Abstract

Transformation in “evolving glass” in ion-conducting silicate glasses, glass ceramics or ceramics containing an intergranular glass is studied by in-situ impedance spectroscopy and scaling laws. Approaches are developed to scale frequency-dependent electrical conductivity and dielectric properties of multiphase ion-conducting materials to derive temperature-independent information on bulk phases and interfaces in presence. A material's scaled electric conductivity provides a unique response over a range of temperature, if the material remains unaltered, but changes, once modifications in the material occur. Therefore, impedance spectroscopy in combination with scaling can be used for tracking modifications in structure, organization, chemistry and microstructure in “evolving (ion-conducting) glass”.In a first part of this work, our approach is validated through application to stable silicate glasses and glass ceramics. Then “evolving glass” is studied in bulk glasses and ceramics with intergranular glass. Examples include ceramming of glass under formation of a glass ceramic, glass-glass phase separation, modification of intergranular glass in ceramics as result of chemical reactions or melt corrosion.Our approach allows to determine onset of phase separation, nucleation or reaction with high precision. It further reveals that nucleation in our exemplary lithium aluminum silicate glass starts with formation of interfaces (phase separation) prior to forming a well-organized crystal lattice. During phase separation in glass, early capacitive contributions in the impedance spectra indicate that the formation of glass-glass interface precedes the compositional changes in the bulk glass.Impedance of refractories is monitored during thermal treatments or corrosion in glass melt at temperatures up to 1600 °C, and glass characteristics of refractories with glass content as low as 3% are extracted. Conductivity and/or level and/or interconnectivity of the refractory's glass are shown to change during thermal treatments due to reactions between glass and crystalline refractory phases, due to phase transformation or, in case of melt corrosion, due to melt infiltration and ion exchange with the melt.In-situ tracking of impedance and application of scaling laws is shown to be able to reveal changes in bulk glass and intergranular glass.