Abstract
Carbonates are abundant sedimentary minerals at the surface and sub-surface of the Earth and they have been proposed as tracers of liquid water in extraterrestrial environments. Their formation mechanism is since generally associated with aqueous alteration processes. Recently, carbonate minerals have been discovered on Mars' surface by different orbitals or rover missions. In particular, the phoenix mission has measured from 1% to 5% of calcium carbonate (calcite type) within the soil (Smith et al., 2009). These occurrences have been reported in area where the relative humidity is significantly high (Boynton et al., 2009). The small concentration of carbonates suggests an alternative process on mineral grain surfaces (as suggested by Shaheen et al., 2010) than carbonation in aqueous conditions. Such an observation could rather point toward a possible formation mechanism by dust–gas reaction under current Martian conditions. To understand the mechanism of carbonate formation under conditions relevant to current Martian atmosphere and surface, we designed an experimental setup consisting of an infrared microscope coupled to a cryogenic reaction cell (IR-CryoCell setup). Three different mineral precursors of carbonates (Ca and Mg hydroxides, and a hydrated Ca silicate formed from Ca2SiO4), low temperature (from −10 to +30°C), and reduced CO2 pressure (from 100 to 2000mbar) were utilized to investigate the mechanism of gas–solid carbonation at mineral surfaces. These mineral materials are crucial precursors to form Ca and Mg carbonates in humid environments (0%<relative humidity<100%) at dust–CO2 or dust–water ice–CO2 interfaces. Our results reveal a significant and fast carbonation process for Ca hydroxide and hydrated Ca silicate. Conversely, only a moderate carbonation is observed for the Mg hydroxide. These results suggest that gas–solid carbonation process or carbonate formation at the dust–water ice–CO2 interfaces could be a currently active Mars' surface process. To the best of our knowledge, we report for the first time that calcium carbonate can be formed at a negative temperature (−10°C) via gas–solid carbonation of Ca hydroxide. We note that the carbonation process at low temperature (<0°C) described in the present study could also have important implications on the dust–water ice–CO2 interactions in cold terrestrial environments (e.g. Antarctic).
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