Multiscale Simulation and Structural Analysis of CO₂ Uptake in Clay-Based and Porous Materials for Carbon Management*

The Texas-Louisiana Carbon Management Center (TXLACMC), with support from the U.S. Department of Energy, acts as a key regional hub for promoting carbon capture and storage (CCS) technologies through simulation-driven research and educational outreach. This study explores the physicochemical behavior of CO₂ within geological substrates, emphasizing the integrity of caprock and the risks of fault reactivation linked to clay swelling and pore-scale transformations. By employing molecular dynamics simulations and crystallographic modeling, we investigate interlayer spacing shifts, adsorption energetics, and structural transitions in montmorillonite clays and metal-organic frameworks (MOFs). Our simulations reveal octahedral-to-tetrahedral phase transitions and microfracture propagation associated with CO₂ saturation, which have implications for permeability and long-term sequestration stability. Comparative uptake studies of Na-rich versus Mg/Ca/Al-rich clays highlight the cost-performance trade-offs in the scalable deployment of CCS. Additionally, we assessed MOFs for their tunable pore geometries and thermodynamic selectivity under varying pressure conditions. This research integrates simulation, experimental validation, and curriculum development to enhance physics-based education in carbon management and geological storage systems.