Enhanced olivine carbonation within a basalt as compared to single-phase experiments: the impact of redox and bulk composition on the dissolution kinetics of olivine

Monday, 15 December 2014: 5:30 PM
Olivier Sissmann1, Fabrice Brunet2, Isabelle Martinez3, Francois J Guyot4,5, Anne Verlaguet6, Yves Pinquier7, Bruno Garcia1, Michel Chardin1, Eric Kohler1 and Damien Daval8, (1)IFP Énergies nouvelles, Rueil-Malmaison Cedex, France, (2)ISTerre Institute of Earth Sciences, Saint Martin d'Hères, France, (3)Institut de Physique du Globe de Paris, Paris, France, (4)IMPMC Institut de Minéralogie et de Physique des Milieux Condensés, Paris Cedex 05, France, (5)Muséum National d'Histoire Naturelle, Paris, France, (6)ISTeP Institut des Sciences de la Terre de Paris, Paris Cedex 05, France, (7)Laboratoire de Geologie de l' Ecole Normale Superieure, Paris, France, (8)LHyGeS Laboratoire d'Hydrologie et de Géochimie de Strasbourg, Strasbourg Cedex, France
Olivine (Mg,Fe)2SiO4, which is one of the major mineral constituents of mafic and ultramafic rocks, has an attractive potential for CO2 mineral sequestration, as it possesses a high content of carbonate-forming divalent cations and exhibits one of the highest dissolution rate amongst rock-forming minerals. This study reports drastic differences in carbonation yields between experiments performed on olivine-rich basalt samples and on olivine separates (a more restricted chemical system). Batch experiments were conducted in water at 150°C and pCO2 = 280 bars on a Mg-rich tholeiitic basalt (9.3 wt.% MgO and 12.2 wt.% CaO), composed of olivine, Ti-magnetite, plagioclase and clinopyroxene. After 45 days of reaction, 56 wt.% of the initial MgO has reacted with CO2 to form Fe-bearing magnesite (Mg0.8Fe0.2)CO3 along with minor calcium carbonates. The substantial decrease of olivine content upon carbonation supports the idea that ferroan magnesite formation mainly follows from olivine dissolution. In contrast, in experiments performed under similar run durations and P/T conditions with a San Carlos olivine separate (47.8 wt.% MgO) of similar grain size, only 5 wt.% of the initial MgO content reacted to form Fe-bearing magnesite. The overall carbonation kinetics of the basalt is enhanced by a factor of 40. It could be accounted for by differences in chemical and textural properties of the secondary-silica layer which covers reacted olivine grains in both types of sample. A TEM inspection of mineral surfaces shows that the thin amorphous silica layer (~100 nm) is porous in the case of the basalt sample and that it contains significant amounts of iron and aluminum. Thus, we propose that the composition of the olivine environment itself can strongly influence the olivine dissolution-carbonation process. Consequently, laboratory data obtained on olivine separates might yield a conservative estimate of the true carbonation potential of olivine-bearing basaltic rocks. More generally, this study questions the approach which consists in evaluating the carbonation potential of a rock based on experiments on separate minerals. It also emphasizes the impact of fO2 and potential co-injected gases on the olivine dissolution-carbonation process.