摘要
Steady-state dissolution rates of Haute Vallée de l'Aude dolomite were measured as a function of chemical affinity and aqueous solution composition in mixed-flow reactors at 80 °C. Experiments were performed in HCl–NaHCO3 bearing aqueous solutions with in-situ pH ranging from 6.36 to 7.17. Rates are found to be a strong function of aqueous carbonate concentrations at far-from-equilibrium conditions. Measured rates can be described using the dissolution mechanism of Pokrovsky and Schott [Pokrovsky, O.S., Schott, J., 2001. Kinetics and mechanism of dolomite dissolution in neutral to alkaline solutions revisited. Am. J. Sci., 301, 597–626] where rates are controlled by the detachment of the > MgOH2+ species at the dolomite surface. Within this mechanism, dolomite dissolution rates can be described using
where
r refers to the overall BET surface area normalized dolomite dissolution rate at both near and far-from-equilibrium conditions,
kMg+ designates a rate constant equal to 4.0 × 10
− 12 mol cm
− 2 s
− 1,
KCa and
KCO3 denote equilibrium constants equal to 3.5 × 10
− 5 and 4.5 × 10
− 5, respectively,
ai refers to the activity of the subscripted aqueous species,
A corresponds to the chemical affinity of the dissolving dolomite,
R represents the
gas constant,
T symbolizes absolute temperature and
n designates a stoichiometric coefficient equal to 1.9.