The evolution of mineral reactive surface area is one of the primary phenomena controlling the progression and extent of mineral carbonation. The CO mineralization begins with nucleation of crystals that provide initial surface area for subsequent growth of the mineral. However, many reactive transport models (RTMs) for CO 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 CO mineralization data from the literature and models that ignore these processes. We observed that including nucleation and passivation lead to closer predictions of the CO 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, CO sequestration, chemical weathering, and concrete degradation.

中文翻译：

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表征成核驱动沉淀和二次钝化对碳矿化的综合影响


矿物反应表面积的演变是控制矿物碳酸化进程和程度的主要现象之一。 CO 矿化始于晶体成核，为矿物的后续生长提供初始表面积。然而，许多 CO 矿化的反应输运模型 (RTM) 不包括成核过程。少数确实包含它的 RTM 尚未根据实验数据进行验证。同样，许多 RTM 忽略了次要矿物的钝化作用，次生矿物覆盖溶解矿物的表面，减慢反应过程，并降低碳化的总程度。此外，成核和钝化对碳矿化的综合影响尚未得到适当的表征。在这项研究中，我们考虑了钝化和成核对矿化程度的耦合影响。成核驱动的沉淀模型依赖于核的形成来为晶体生长提供表面积，同时提出了一个新模型来解释钝化效应。我们的分析表明，(i) 忽略成核会导致高估矿化程度，(ii) 忽略钝化会导致高估围岩反应性。通过与文献中的 CO 矿化数据和忽略这些过程的模型进行比较来评估该模型。我们观察到，包括成核和钝化可以更准确地预测二氧化碳矿化程度。因此，本研究强调了在 RTM 中加入成核驱动沉淀和二次钝化的重要性。 该研究的结果可应用于各种科学和工程应用，例如石油生产、水泥碳化、二氧化碳封存、化学风化和混凝土降解。