Amorphous silica solubility and the thermodynamic properties of H 4SiO °4 in the range of 0° to 350°C at P sat

Abstract

The solubility of amorphous silica was determined in the temperature range 8° to 310°C at 1 bar below 100°C and at P sat at higher temperatures. Our results are consistent with previous experiments between 100° and 200°C, but at higher temperatures they indicate lower solubility. Below 100°C our result are lower than the results of some researchers, but in good agreement with others. Our solubility data have been combined with previously reported data to retrieve a temperature equation describing amorphous silica solubility. Quartz solubility data have also been assessed. The solubility equations for the reaction SiO 2,s + 2H 2O = H 4SiO ° 4 are: logK am.silica = −8.476− 485.24× T −1 − 2.268× 10 −6 × T 2 + 3.068× logT logK quartz = −34.188+ 197.47× T −1 − 5.851× 10 −6 × T 2 + 12.245× logT where T is in K. They are valid in the temperature range 0° to 350°C at 1 bar below 100°C and at P sat at higher temperatures. From the quartz solubility equation and the thermodynamic properties of quartz and liquid water, the standard partial molal Gibbs energy of formation and the third law entropy of H 4SiO ° 4 were calculated as −1,309,181 J/mole and 178.85 J/mole/K at 25°C. The difference in the standard apparent Gibbs energy of H 4SiO ° 4 as calculated from quartz solubility, on one hand, and amorphous silica solubility, on the other, is about the same over the temperature range 0° to 350°C indicating that the solubility temperature equations obtained for the two solids in this study are internally consistent. This indicates that the quartz solubility data of Rimstidt (1997), which were used in this study to retrieve the quartz solubility equation, are valid and also our data on ΔḠ ° f and S̄° for H 4SiO ° 4 at 25°C and 1 bar as well as the ΔḠ° temperature equation presented for this species. These new Gibbs energy values for H 4SiO ° 4 indicate that all silicate minerals are considerably more soluble under Earth’s surface conditions than generally accepted to date, or by about 0.6 log K units at 0°C per silicon atom in the unit formula.