『Abstract
Carbonation of partially serpentinized and weathered peridotites
was studied experimentally under hydrothermal conditions (T: 200℃,
PCO2: 130-180 bars).
Experiments were performed in a closed system using whole rock
drill core samples (height: 1 cm, diameter: 1 cm) as starting
material. The initial samples were composed mainly of meshwork
serpentine, relics of primary olivine and an olivine weathering
product (deweylite assemblage). Two types of solutions, each with
a total salt content corresponding to that of average seawater
(35 g/L dissolved salts), were used: (1) a Na-Ca-Cl solution (12.5
g/L CaCl2 + 22.5 g/L NaCl) and (2) a NaCl
solution (35 g/L NaCl). After 15-25 days of experimental treatment,
the samples were partly covered with carbonates. In addition,
noticeable carbonation reactions had occurred below the sample
surfaces within zones with thicknesses up to 250μm. In the Na-Ca-Cl
solution, both the olivine relicts and the deweylite assemblage
were partly replaced by calcite along the surrounding serpentine
veins. However, the extent of calcitization was found to be considerably
larger for the deweylite assemblage than for the olivine. Bulk
fluid analyses show an increase in the Mg and Si concentrations
with reaction time. In the NaCl solution, the deweylite assemblage
was partly dissolved resulting in large voids within the reaction
zone. In contrast, the olivine was replaced by magnesite. Under
the conditions of our experiments, the meshwork serpentine was
not reactive, but aided fluid infiltration into the rock samples.
The experimentally produced microtextures closely resemble those
found in natural examples. Our study elucidates the mechanisms
by which carbonates form in ultramafic rocks under relatively
high PCO2-T conditions
and particularly in the presence of Ca-bearing aqueous solutions.
The existence of a serpentine meshtexture and the presence of
weathering products formed from primary Mg-silicates may have
significant beneficial effects on in situ CO2
mineral sequestration in ultramafic rocks.』
1. Introduction
2. Materials and methods
2.1. Analytical methods
2.2. Description of the starting material
2.3. Experimental procedures
2.4. Aqueous speciation calculations
3. Results
3.1. Textural characteristics of the reacted peridotite samples
3.1.1. After reaction with the Na-Ca-Cl solution
3.1.2. After reaction with the NaCl solution
3.2. Changes in the chemistry of the aqueous solutions
4. Discussion
4.1. Reaction mechanisms
4.1.1. The formation of calcite
4.1.2. The formation of magnesite
4.2. Mobilization of Mg and Si
4.3. Comparison of the experimentally produced microtextures
with natural examples
4.4. The impact of weathering and serpentinization on the carbonation
of ultramafic rocks and some implications for in situ CO2 storage
5. Conclusions
Acknowledgments
References