Glass-forming ability and structural features of melt-quenched and gel-derived SiO2-TiO2 glasses

SiO2-TiO2 glasses produced by aerodynamic levitation coupled to laser heating or by sol-gel spray-drying were compared to highlight their structural differences. Glass formation was possible by melt-quenching up to 10 mol% TiO2, while higher contents led to devitrification. Raman spectroscopy and solid-state 17 O and 29 Si magic-angle-spinning nuclear magnetic resonance confirmed the clear emergence of Ti-O-Si bonds and a tetrahedral oxygen coordination of Ti 4+ leading to full network connectivity, as also substantiated by the synthesis of TiO2-doped cristobalite. In gel-derived glasses, water content induced partial network depolymerization, thereby enhancing the solubility of TiO2 in the hydrous silicate matrix. However, full dehydration during heating proved challenging due to a competing tendency towards devitrification: the glass-forming range in the anhydrous binary SiO2-TiO2 system does not therefore appear to be significantly enlarged by the sol-gel synthesis route.