Abstract

We have investigated mechanochemical reactions with the calcium silicate wollastonite to probe potential mechanisms of sequestration and long-term storage of CO2 as mineral carbonates in cement pastes. Wollastonite, CaSiO3, was milled under ambient and 13C enriched CO2 atmospheres. Milling induced a structure change from monoclinic wollastonite−2M to triclinic−1T, consistent with high pressure treatment. The results from solid-state 13C nuclear magnetic resonance (NMR) spectroscopy shows this process forms an extraordinarily stable amorphous calcium carbonate (ACC) phase that remains despite a high temperature dehydration treatment (130 °C) and persists in the same form after 3 yrs. of storage at ambient conditions. Thermogravimetric analysis (TGA) of these samples indicates that ACC is produced at the similar solid concentrations in both CO2-enriched and ambient atmospheres. The observation of meta-stable ACC due to wollastonite carbonation may play an important role in further exploration and optimization of mineral carbonation reactions for CO2 capturing cement formulations.

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