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• W2337260596 abstract "Abstract A thermodynamic model of SiO 2 – H 2 O mixing in sub- and supercritical fluids has been developed based on new and existing experimental data on the solubility of quartz in H 2 O . To supplement previously published data, we conducted new solubility experiments at 15 and 20 kbar and 900–1100 °C using hydrothermal piston–cylinder methods. At concentrations below ∼ 10 mol% SiO 2 , solubility was measured by single-crystal weight loss. At higher concentrations, solubility was determined by bracketing the presence and absence of quartz in quenched charges using multiple isothermal and isobaric runs with varying SiO 2 – H 2 O ratios. These data were combined with previously published results to construct a thermodynamic model of SiO 2 – H 2 O mixing. Following studies of silicate melts, the model takes oxygen in the fluid to be in three forms: free, molecular H 2 O , Si-bridging oxygens ( O br 2 - ) , and the terminal hydroxyls ( OH tm - ) of silanol groups. The equilibrium exchange of oxygen between these forms can be written 1 2 H 2 O + 1 2 O br 2 - = OH tm - . The standard Gibbs free energy change of this reaction ( Δ G ∘ ) was incorporated into a subregular solution model for mixing of SiO 2 liquid and H 2 O fluid. The P–T dependences of Δ G ∘ and interchange energies were derived by an error minimization algorithm, producing thirteen independent fit parameters. The model is applicable from 5 to 20 kbar and 500 °C to the dry melting curve of quartz. It reproduces experimentally derived quartz solubility data to 3.8% on average (1 σ  = 5.3%). The model also predicts hydrous melting of quartz, critical melt–vapor mixing, activity–concentration relations, partial molar volume and entropy of aqueous silica, water speciation, and the thermal expansivity, isothermal compressibility, and isobaric heat capacity of a fluid in equilibrium with quartz. The model predicts a critical end point in the SiO 2 – H 2 O system at 1067 °C and 9.33 kbar, in very good agreement with the accepted location at ∼ 1080 °C and 9.5–10 kbar. The model is also in good agreement with previous estimates of the extent of silica polymerization. The results of this study clearly demonstrate that there is an explicit link between polymerization chemistry and critical mixing of silicate– H 2 O solutions." @default.
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• W2337260596 date "2011-08-01" @default.
• W2337260596 modified "2023-09-28" @default.
• W2337260596 title "A thermodynamic model for the system SiO2-H2O near the upper critical end point based on quartz solubility experiments at 500-1100 C and 5-20 kbar" @default.
• W2337260596 hasPublicationYear "2011" @default.
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