Thermodynamic calculations of chemical solubilities of gases in oxide melts and glasses

Abstract

The Reddy-Blander thermodynamic model for calculating sulfide solubilities in oxide melts and glasses has been modified and extended to predict a priori solubilities of sulfide, sulfate, phosphate, carbonate and halides in multicomponent oxide melts and glasses, from a knowledge of the thermodynamic activities of the basic component oxides (SiO₂, Na₂O, K₂O, CaO, etc.), in most cases with no adjustable parameters. Agreement with measured solubilities is within or nearly within experimental uncertainties over wide ranges of composition in two-, three-, four- and five-component melts and glasses. Particularly good agreement is obtained for the dissolution of sulfur, SO₂ and SO₃ as sulfate. The oxide activities used in the computations are calculated from a database of model parameters obtained by optimizing thermodynamic and phase equilibrium data for oxide Systems. Sulfide, sulfate, phosphate, carbonate and halides as solutes have now been included in this database. Software for Gibbs energy minimization with automatic access to this and other databases permits the calculation of solubilides in multicomponent oxide melts and glasses in equilibrium with other phases such as gases, molten salts, solids and metals, and can be useful to model evaporation processes and bubble formation.