Modeling of Elemental Species

Aqueous Solubility Diagrams for Cementitious Waste Stabilization Systems: II, End-Member Stoichiometries of Ideal Calcium Silicate Hydrate Solid Solutions

Solubility in the fully hydrated CaO–SiO2–H2O system can be best described using two ideal C-S-H-(I) and C-S-H-(II) binary solid solution phases. The most recent structural ideas about the C-S-H gel permit one to write stoichiometries of polymerized C-S-H-(II) end-members as hydrated precursors of the stable tobermorite and jennite minerals in the form of 5Ca(OH)2·6SiO2·5H2O and 10Ca(OH)2·6SiO2·6H2O, respectively. For thermodynamic modeling purposes, it is more convenient to express the number of basic silica and portlandite units in these stoichiometries using the coefficients nSi and nCa. Thermodynamic solid-solution aqueous-solution equilibrium modeling by applying the Gibbs energy minim…

Aqueous Solubility Diagrams for Cementitious Waste Stabilization Systems. 4. A Carbonation Model for Zn-Doped Calcium Silicate Hydrate by Gibbs Energy Minimization

A thermodynamic Gibbs energy minimization (GEM) solid solution-aqueous solution (SSAS) equilibrium model was used to determine the solubility of Zn from calcium silicate hydrate (CSH) phases doped with 0, 0.1, 1, 5, and 10% Zn at a unity (Ca+Zn)/Si molar ratio. Both the stoichiometry and standard molar Gibbs energy (G(o)298) of the Zn-bearing end-member in the ideal ternary Zn-bearing calcium silicate hydrate (CZSH) solid solution were determined by a "dual-thermodynamic" (GEM-DT) estimation technique. The SSAS model reproduces a complex sequence of reactions suggested to occur in a long-term weathering scenario of cementitious waste forms at subsurface repository conditions. The GEM model …