The influence of glass composition on crystalline phase stability in glass-ceramic wasteforms

Zirconolite glass-ceramic wasteforms were prepared using a suite of Na2O-Al2O3-B2O3-SiO2 glass matrices with variable Al:B ratios. Zirconolite was the dominant crystalline phase only for the most alumina rich glass compositions. As the Al:B ratio decreased zirconolite was replaced by sphene, zircon and rutile. Thermodynamic data were used to calculate a silica activity in the glass melt below which zirconolite is the favoured crystalline phase. The concept of the crystalline reference state of glass melts is then utilised to provide a physical basis for why silica activity varies with the Al:B ratio.