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A continuous and mechanistic representation of calcite reaction-controlled kinetics in dilute solutions at 25°C and 1 atm total pressure

A continuous and mechanistic representation of calcite reaction-controlled kinetics in dilute... Calcite dissolution rates were measured using a free-drift technique at 25°C, 1 atm total pressure, and various $$P_{CO_2 } $$ in deionized water. The data were corrected for gas phase disequilibrium and fitted to a kinetic expression derived by coupling the mechanistic models of Plummeret al. (1987a) and Chouet al. (1989) to the surface complexation model of Van Cappellenet al. (1993). Corrected dissolution and precipitation rate measurements from previous investigations were combined to our data set and fitted to the same expression. The following reactions provide an adequate description of the calcite dissolution and precipitation mechanism in dilute solutions:[Figure not available: see fulltext.] for which the overall reaction rate is given by[Figure not available: see fulltext.] where >i are the densities of surface complexes (mol/m2),a i are the activities of dissolved species and,k i are the rate constants corresponding to the above reactions. This rate equation satisfies the principle of microscopic reversibility and applies to both dissolution and precipitation reactions over a wide range of $$P_{CO_2 } $$ , pH and saturation states. The rate constants obtained from fitting the data set to Equation (3) are compatible with values reported by Plummeret al. and Chouet al., as well as yielding a very good estimate of the thermodynamic solubility constant of calcite, K 0 sp . http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Aquatic Geochemistry Springer Journals

A continuous and mechanistic representation of calcite reaction-controlled kinetics in dilute solutions at 25°C and 1 atm total pressure

Aquatic Geochemistry , Volume 1 (1) – Nov 11, 2004

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References (44)

Publisher
Springer Journals
Copyright
Copyright
Subject
Earth Sciences; Geochemistry; Hydrology/Water Resources; Hydrogeology; Water Quality/Water Pollution
ISSN
1380-6165
eISSN
1573-1421
DOI
10.1007/BF01025233
Publisher site
See Article on Publisher Site

Abstract

Calcite dissolution rates were measured using a free-drift technique at 25°C, 1 atm total pressure, and various $$P_{CO_2 } $$ in deionized water. The data were corrected for gas phase disequilibrium and fitted to a kinetic expression derived by coupling the mechanistic models of Plummeret al. (1987a) and Chouet al. (1989) to the surface complexation model of Van Cappellenet al. (1993). Corrected dissolution and precipitation rate measurements from previous investigations were combined to our data set and fitted to the same expression. The following reactions provide an adequate description of the calcite dissolution and precipitation mechanism in dilute solutions:[Figure not available: see fulltext.] for which the overall reaction rate is given by[Figure not available: see fulltext.] where >i are the densities of surface complexes (mol/m2),a i are the activities of dissolved species and,k i are the rate constants corresponding to the above reactions. This rate equation satisfies the principle of microscopic reversibility and applies to both dissolution and precipitation reactions over a wide range of $$P_{CO_2 } $$ , pH and saturation states. The rate constants obtained from fitting the data set to Equation (3) are compatible with values reported by Plummeret al. and Chouet al., as well as yielding a very good estimate of the thermodynamic solubility constant of calcite, K 0 sp .

Journal

Aquatic GeochemistrySpringer Journals

Published: Nov 11, 2004

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