『Abstract
Direct measurements of calcite (1014)(後の1の頭に-)
faces were performed using in situ atomic force microscopy (AFM)
to reveal the dissolution processes as a function of solution
saturation state and temperature. Time-sequential AFM images demonstrated
that step velocities at constant temperature increased with increasing
undersaturation. The anisotropy of obtuse and acute step velocities
appeared to become more significant as solutions approached equilibrium
and temperature increased. At saturation state Ω>0.02, a curvilinear
boundary was formed at the intersection of two acute steps and
the initially rhombohedral etch pit exhibited a nearly triangular
shape. This suggests that the [441(最初の4の頭に-)]a and [481(1の頭に-)]a
steps may not belong to the calcite-aqueous solution equilibrium
system. Further increase in the saturation state (Ω≧0.3) led to
a lack of each pit formation and dissolution primarily occurred
at existing steps, in accordance with Teng (2004). Analysis of
step kinetics at different temperatures yielded activation energies
of 25±6 kJ/mol and 14± 13 kJ/mol for obtuse and acute steps, respectively.
The inconsistencies in etch pit morphology, step anisotropy, and
step activation energies from the present study with those of
studies far-from-equilibrium can be explained by increased influence
of the backward reaction, or growth, near-equilibrium. We propose
that the backward reaction occurs preferentially at the acute-acute
kink sites. The kinetics and effective activation energies of
near-equilibrium calcite dissolution presented in this work provide
accurate experimental data under likely CO2
sequestration conditions, and thus are crucial to the development
of robust geochemical models that predict the long-term performance
of mineral-trapped CO2.』
1. Introduction
2. Experimental
2.1. Sample and solution preparation
2.2. AFM apparatus
3. Results and discussion
3.1. Etch pit formation and morphology
3.2. Step kinetics
3.3. Activation energy
4. Conclusion
Acknowledgments
References