Mineral carbonation of New Caledonian ultramafic mine slag: Effect of glass and secondary silicates on the carbonation yield

New Caledonian nickel (Ni) mines produces ∼12 million metric tons of mine slag every year, that are considered undesired and uneconomic waste materials. However, due to the high content of Mg2+ and Fe2+, these slags exhibit a potential of carbon dioxide (CO2) storage by ex-situ aqueous mineral carbonation. We conducted laboratory batch experiments at 200 °C/ 150 bar, 250 °C/ 300 bar, 300 °C/ 300 bar, in CO2-saturated water to better understand the slag dissolution, secondary mineral formation at the fluid-mineral interface, and the effect of the secondary silicates on the carbonation yield. The slag contains olivine (45 wt%) and glass (55 wt%). Olivine in the slag dissolves faster than glass, contributing to carbonate precipitation (Fe-rich magnesite) at 200 °C/150 bar. At 250 °C/ 300 bar, olivine is almost completely dissolved while glass dissolves only partially, both contributing to the highest recorded carbonation yields of the slag of 44 wt%. Although both olivine and glass are completely dissolved at 300 °C/ 300 bar, the carbonate yield drops at a value half of that at 250 °C/ 300 bar. This is due to formation of large quantity of Mg-bearing phyllosilicates that reduces the amount of Mg2+ available for carbonation. These results emphasize that increasing temperature above 250 °C would not increase the carbonate yield of New Caledonian mine slags. However, as glass only partially reacts at T < 250 °C, mobilizing Mg2+ in glass could potentially increase the carbonation yield, for example by adding suitable organic ligands. Mg-bearing phyllosilicates and amorphous silica that are formed in these experiments do not exhibit passivation properties, and therefore do not affect the carbonation rate.