The nature of mineral precipitations in terrestrial alkaline soda lakes provides insights into the water chemistry of subsurface oceans on icy bodies in the outer solar system. Saturation analyses of terrestrial alkaline lakes have shown that the solution chemistries of lake waters are generally controlled by the presence of monohydrocalcite (MHC) and amorphous Mg-carbonate (AMC). However, direct observations of the formation of these metastable carbonates in natural alkaline lakes have been limited. This study provides evidence of in situ MHC formation in alkaline lakes, based on the water chemistry and mineralogy of suspended matter in Olgoy, Boon Tsagaan, and Orog Lakes (Valley of Gobi Lakes, Mongolia). The solution chemistries were close to saturation with respect to MHC and AMC, consistent with other alkaline lakes worldwide. Suspended matter was separated by the ultracentrifugation of lake water following freeze-drying. Our results show that MHC is the common mineral phase in the suspended matter. These observations confirm that MHC is the direct authigenic product of evaporation in alkaline lakes. The carbonate fraction in suspended matter from Olgoy Lake has a Mg/Ca ratio of 0.4, suggesting the formation of AMC in association with MHC. Based on the dissolution equilibria of AMC and MHC, we predict the Mg2+, Ca2+, and total dissolved carbonate concentrations in Enceladus’ ocean to be ~1 mmol/kg, ~10 μmol/kg, and 0.06–0.2 mol/kg, respectively, in the presence of AMC and MHC. We propose that the measurements of Mg contents in plumes will be key to constraining the total dissolved carbonate concentrations and chemical affinities of subsurface oceans on Enceladus and other alkaline-carbonate ocean worlds.
Monohydrocalcite (MHC) is a metastable hydrous calcium carbonate that requires Mg in the mother solution during formation in the laboratory. MHC prepared by previously reported methods always contains a large amount of Mg (Mg/Ca ratio up to 0.4) because of the simultaneous formation of amorphous Mg carbonate during synthesis, which has hindered detailed elucidation of the mineralogical characteristics of MHC. Here, we synthesized MHC at low temperature (5 °C) and found that it contained little Mg (Mg/Ca ratio < 0.01). X-ray absorption near-edge structure analysis of synthesized MHC revealed that the Mg present was structurally incorporated within the MHC, and that the chemical speciation of this Mg was similar to that of Mg in aragonite. Thus, low-temperature synthesis is an effective means of producing MHC without also producing amorphous Mg carbonate.
Observations by spacecraft and ground-based telescopes have found non-ice, salt materials, including halite and carbonate, on the surface of icy bodies, such as Europa and Ceres (e.g.,
Previous studies suggested that, generally, the climate of early Mars would have been semi-arid when the surface temperatures were above freezing. On early Mars, closed-basin lakes would have been created; however, the hydrogeochemical cycles of the lake systems are poorly constrained. Here we report results of our field surveys to terrestrial analogs of closed-basin lake systems that developed in cold and semi-arid climates: The Valley of the Gobi Lakes of Mongolia. Our results show that groundwater plays a central role not only in hydrology, but also in geochemical cycles in the lake systems. We find that groundwater predominantly flows into the lakes through local seepage and regional flows in semi-arid climates. Through the interactions with calcite-containing soils, local groundwater seepage provides Ca2+ and HCO3− to the lakes. In the wetland located in between the lakes, high-salinity shallow pools would provide Cl− and Na+ to the groundwater through infiltration. If similar processes occurred on early Mars, local seepage of groundwater would have provided magnesium and alkalinity to the early Jezero lakes, possibly leading to authigenic precipitation of lacustrine carbonates. On early Mars, infiltration of surface brine may have transported salts and oxidants on the surface to lakes via regional groundwater flows. We suggest that inflows of multiple types of groundwater in semi-arid climates could have caused redox disequilibria in closed-basin lakes on early Mars.
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