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The use of calcium bearing resources to facilitate solvent regeneration and CO2 reuse via carbon mineralization offers a low energy pathway for the production of calcium carbonate. However, a crucial challenge is the lack of specificity in the formation of various calcium carbonate polymorphs during carbon mineralization. One of the less explored but highly effective approaches to tune the morphology and crystal structure of specific carbonate phases involves tuning vortex flows. This approach is an alternative to utilizing chemical reagents that need to be regenerated for tuning the morphologies and crystalline structures to direct the formation of specific carbonate phases. In this study, the efficacy of using homogeneous vortex flows in limiting the agglomeration of carbonate particles and directing the formation of metastable vaterite phases is discussed and contrasted with the influence of inhomogeneous conventional feed flow patterns on precipitated calcium carbonate (PCC). Herein, a TaylorCouette Carbonate Conversion (TC3 ) reactor is used to direct the formation of spherical vaterite particles with uniform particle size distribution preferentially over calcite and other phases. The formed vortex patterns inside TC3 reactor provide homogeneous reaction spaces conducive to PCC formation, ensuring uniform mixing throughout the process. By increasing the rotational speed and the residence time, higher purity carbonates with more uniform sizes are obtained. Furthermore, preferential vaterite formation is also observed in leachates obtained from alkaline industrial residues such as construction and demolition waste and steel slag. Thus, the proposed approach is effective in harnessing multiple waste streams such as CO2 emissions and alkaline industrial residues to produce calcium carbonate phases such as vaterite with structural and morphological specificity. 

Scalable efforts to remove anthropogenic CO 2 via the formation of durable carbonates require us to harness siliceous nanoporous geologic materials for carbon storage. While calcium carbonate formation has been extensively reported in bulk fluids, there is a limited understanding of the influence of nanoconfined fluids on the formation of specific stable and metastable polymorphs of calcium carbonates in siliceous materials that are abundant in subsurface environments. To address this challenge, silica nanochannels with diameters of 3.7 nm are architected and the formation of specific calcium carbonate phases is investigated using X-ray diffraction (XRD), and molecular dynamics (MD) simulations. The formation of stable calcium carbonate (or calcite) is noted in silica nanochannels. The presence of fewer water molecules in the first hydration shell of calcium ions in confinement compared to in bulk fluids contributes to stable calcium carbonate formation. These studies show that nanoporous siliceous environments favor the formation of stable calcium carbonate formation.