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Dissolution kinetics of magnesite in acidic aqueous solution: A hydrothermal atomic force microscopy study assessing step kinetics and dissolution flux

Geochimica Et Cosmochimica Acta 66(18): 3201-3210

Autoren/Herausgeber: Higgins SR
Jordan G
Eggleston CM
Erschienen: 2002

Magnesite (104) dissolution kinetics were studied in acidic aqueous solutions (2.0 < pH < 4.2) at temperatures between 60 and 90degreesC by atomic force microscopy (AFM). Comparison of dissolution fluxes obtained by AFM and chemical methods revealed six to seven times larger dissolution fluxes obtained by chemical analysis. Corresponding empirical activation energies were found to be 74 +/- 22 kJ/mol and 41 +/- 4 kJ/mol (at pH 4.2) for the AFM and chemical methods, respectively. The empirical reaction order with respect to proton concentration was 0.36 +/- 0.13 and 0.47 +/- 0.03 for AFM and chemical methods, respectively. These comparisons suggest that the two experimental measurement methods differ as a result of the different sampling length scales associated with the methods. Negligible changes in step dissolution velocity with changes in bulk pH were found, suggesting that the principal source of increasing dissolution flux with decreasing pH is an increase in step density. However, the observed stable step orientation, which is dependent on pH, suggests that more than one proton adsorption equilibrium should be used to describe the surface chemistry of magnesite in acidic solution. Copyright (C) 2002 Elsevier Science Ltd.