Limited reactivity of pyroxene and plagioclase in batch experiments with supercritical CO in the presence of NaCl and NaHCO in the context of CO sequestration via carbonation.

One-step high-pressure and high-temperature direct aqueous mineral carbonation of tailings derived from mining of Platinum Group Metals in South Africa requires a fundamental understanding of the reactivity of the most dominant mineral phases, i.e. pyroxene and plagioclase (66 wt. % and 12 wt. % of the bulk rock respectively) that are typically found in these tailings. The silicate minerals pyroxene and plagioclase were sampled from a pyroxenite footwall mined with the ore-bearing UG2 and from the Merensky Reefs outcropping in the eastern limb of the Bushveld Complex. These pyroxene and plagioclase grains were concentrated by gravity separation from the orthopyroxenite bulk rock and batch-reacted in a sodium chloride (NaCl) brine saturated with pure carbon dioxide (CO) gas-only or seeded with sodium bicarbonate (NaHCO; as an additional CO source) for 13 days at 100 °C and 10 MPa. Pyroxene dissolved slightly but no weathering features were observed in plagioclase. Analyses of the filtrates obtained from the pyroxene sample in the absence of NaHCO showed an increased concentration of magnesium and calcium ions in the solution. However, they had also reached a cation saturation sealing. On the other hand, liquid samples from reactions where both CO gas and NaHCO were added to the solution exhibited a pronounced decrease in dissolved magnesium and calcium ions. XRD patterns of some of the post-reaction solids collected from the cation-depleted solution aliquots showed peaks of newly formed secondary magnesite and vermiculite. Moreover, the presence of magnesite was further confirmed by Raman shift analysis of the dried solid products. The formation of secondary magnesite was observed only in the experiments seeded with NaHCO, specifically where the pre-reaction solid was pyroxene rich. Some of the resultant fluid chemistry was corroborated by the geochemical model that simulated the reaction parameters using the Geochemist Work Bench (GWB) software. Overall, the results indicate low pyroxene dissolution, which leads to limited carbonation. These findings suggest that the carbonation of PGM tailings may be constrained under the evaluated physicochemical conditions.