『Abstract
The products of forsterite dissolution and the conditions favorable
for magnesite precipitation have been investigated in experiments
conducted at temperature and pressure conditions relevant to geologic
carbon sequestration in deep saline aquifers. Although forsterite
is not a common mineral in deep saline aquifers, the experiments
offer insights into the effects of relevant temperatures and PCO2 levels on silicate
mineral dissolution and subsequent carbonate precipitation. Mineral
suspensions and aqueous solutions were reacted at 30℃ and 95℃
in batch reactors, and at each temperature experiments were conducted
with headspaces containing fixed PCO2 values of 1 and 100 bar. Reaction products
and progress were determined by elemental analysis of the dissolved
phase, geochemical modeling, and analysis of the solid phase using
scanning electron microscopy, infrared spectroscopy, ad X-ray
diffraction. The extent of forsterite dissolution increased with
both increasing temperature and PCO2 . The release of Mg and Si from forsterite
was stoichiometric, but the Si concentration was ultimately controlled
by the solubility of amorphous silica. During forsterite dissolution
initiated in deionized water, the aqueous solution reached supersaturated
conditions with respect to magnesite; however, magnesite precipitation
was not observed for reaction times of nearly four weeks. Magnesite
precipitation was observed in a series of experiments with initial
solution compositions that simulated extensive forsterite dissolution.
The precipitation of magnesite appears to be limited by the process
of nucleation, and nucleation requires a critical saturation index
between 0.25 and 1.14 at 95℃ and 100 bar PCO2 . Magnesite precipitation is fastest in
the presence of an initial magnesite seed. Although magnesite
precipitates do form on the surfaces of forsterite particles,
the presence of the forsterite surface does not significantly
accelerate magnesite precipitation relative to solid-free systems.
Keywords: Carbon dioxide; Dissolution; Forsterite; Magnesite;
Precipitation; Sequestration』
1. Introduction
2. Experimental materials and methods
2.1. Materials
2.2. Experimental procedure
2.3. Analytical methods
2.4. Equilibrium modeling of speciation
3. Results
3.1. Fosterite dissolution
3.2. Magnesite precipitation
4. Discussion
4.1. Stoichiometry of forsterite dissolution and precipitation
of secondary phases
4.2. Trends in forsterite dissolution rate
4.3. Magnesite precipitation
4.4. Implications for carbon storage and sequestration in deep
saline aquifers
5. Conclusion
Acknowledgments
References