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1.
The hydration of periclase to brucite was investigated experimentally. Single crystals of periclase machined to millimeter sized cubes with (100) surfaces were reacted with distilled water at temperatures of 350 to 620 °C and a pressure of 200 MPa for run durations of 5 to 40 minutes. Hydration produced a layer of brucite covering the surface of periclase. While the shrinking periclase largely retained its cube shape a surface roughness developed on the μm scale and eventually outward pointing spikes bounded by (111) faces emerged on the retreating faces of the periclase due to kinetic selection of less reactive (111) and (110) surfaces. The periclase to brucite conversion followed a linear rate law, where the reaction rate increased from 350 to 530 °C and then decreased towards higher temperature and finally vanished at about 630 °C, where periclase, brucite, and water are in equilibrium at 200 MPa. The overall kinetics of the hydration reaction is conveniently described in terms of a phenomenological interface mobility. Measuring the velocity of the hydration front relative to the lattice of the reactant periclase, the temperature dependence of its mobility is described by an Arrhenius relation with pre-exponential factor 1.7.10?12 m 4/s.J and activation energy of EA=55 kJ/mol.  相似文献   

2.
An empirical model is developed to predict the dissolution rate of calcite in saline solutions that are saturated with respect to dissolved \(\hbox {CO}_2\) over a broad range of both subcritical and supercritical conditions. The focus is on determining the rate of calcite dissolution within a temperature range of 50–100 \(^\circ \hbox {C}\) and pressures up to 600 bar, relevant for \(\hbox {CO}_2\) sequestration in saline aquifers. A general reaction kinetic model is used that is based on the extension of the standard Arrhenius equation with an added, solubility-dependent, pH term to account for the saturated concentration of dissolved \(\hbox {CO}_2\). On the basis of this kinetic model, a new rate equation is obtained using multi-parameter, nonlinear regression of experimental data to determine the dissolution of calcite as a function of temperature, pressure and salinity. Different models for the activity coefficient of \(\hbox {CO}_2\) dissolved in saline solutions are accounted for. The new rate equation helps us obtain good agreement with experimental data, and it is applied to study the geochemically induced alterations of fracture geometry due to calcite dissolution.  相似文献   

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