Summary: | The potential for mineral carbonation of CO<sub>2</sub> in plutonic mafic rocks is addressed through a set of laboratory experiments on cumulate gabbro and gabbro-diorite specimens from the Sines Massif (Portugal). The experiments were conducted in an autoclave, for a maximum of 64 days, using a CO<sub>2</sub> supersaturated brine under pressure and temperature conditions similar to those expected around an injection well during early-phase CO<sub>2</sub> injection. Multiple techniques for mineralogical and geochemical characterization were applied ante- and post-carbonation experiments. New mineralogical phases (smectite, halite and gypsum), roughness increase and material loss were observed after exposure to the CO<sub>2</sub> supersaturated brine. The chemical analysis shows consistent changes in the brine and rock specimens: (i) increases in iron (Fe) and magnesium (Mg) in the aqueous phase and decreases in Fe<sub>2</sub>O<sub>3</sub> and MgO in the specimens; (ii) a decrease in aqueous calcium (Ca) and an increase in CaO in the cumulate gabbro, whereas in the gabbro-diorite aqueous Ca increased and afterwards remained constant, whereas CaO decreased. The geochemical model using the CrunchFlow code was able to reproduce the experimental observations and simulate the chemical behavior for longer times. Overall, the study indicates that the early-stage CO<sub>2</sub> injection conditions adopted induce mainly a dissolution phase with mineralogical/textural readjustments on the external area of the samples studied.
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