Clay mineral mediated dynamics of CO2 hydrate formation and dissociation: Experimental insights for carbon sequestration

Marine sediment-based CO2 sequestration through hydrate formation is a promising approach for long-term CO2 storage. Despite the prevalence of clay minerals in marine sediments, their impact on CO2 hydrate dynamics remains disputed and necessitates validation. This study systematically investigated the effect of clay minerals, specifically Ca-montmorillonite (Ca-mmt) and illite, on CO2 hydrates nucleation, growth, and dissociation in clay suspensions (0–10 wt% concentrations). Clay minerals significantly promoted CO2 hydrate nucleation by providng additional nucleation sites and influencing water distribution through the surface electric field. Ca-mmt exhibited a more pronounced nucleation effect due to stronger hydration ability of Ca2+ increasing nucleation sites and local CO2 concentration. Both clay minerals enhanced CO2 hydrate growth, with concentration-dependent effects that differ between clay types. Ca-mmt exhibited a higher growth rate at lower concentrations (≤1 wt%), but a lower rate at higher concentrations (>1 wt%) due to the stronger swelling and aggregation ability upon water contact. Morphological analysis revealed the clay minerals’ impact on fluid behavior and mass transfer during hydrate growth. During dissociation, clay minerals impeded the process, prolonging overall dynamics. This study highlights the impact of physicochemical disparities between Ca-mmt and illite on CO2 hydrate dynamics, underscoring the importance of these interactions for CO2 sequestration.