Abstract
The evolution of mineral reactive surface area is one of the primary phenomena controlling the progression and extent of mineral carbonation. The CO2 mineralization begins with nucleation of crystals that provide initial surface area for subsequent growth of the mineral. However, many reactive transport models (RTMs) for CO2 mineralization do not include the nucleation process. The few RTMs that do include it are yet to be validated against experimental data. Similarly, many RTMs ignore passivating effects of the secondary mineral, which coats the surface of the dissolving mineral, slow down the reaction process, and reduce the total extent of carbonation. Furthermore, the combined impact of nucleation and passivation on carbon mineralization is yet to be properly characterized. In this study, we consider the coupled effects of passivation and nucleation on the mineralization extent. The nucleation-driven precipitation model relies on the formation of nuclei to provide a surface area for crystal growth, while a new model is proposed to account for passivation effects. Our analysis shows that (i) omission of nucleation leads to overestimation of extent of mineralization, and (ii) omission of passivation leads to overestimation of host rock reactivity. The model was evaluated via comparison with CO2 mineralization data from the literature and models that ignore these processes. We observed that including nucleation and passivation lead to closer predictions of the CO2 mineralization extent. Therefore, this study highlights the importance of including the coupled nucleation-driven precipitation and secondary passivation in RTMs. The findings from the study can be applied in various scientific and engineering applications such as petroleum production, cement carbonation, CO2 sequestration, chemical weathering, and concrete degradation.
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