Density functional simulations as a tool to probe molecular interactions in wet supercritical CO₂

Recent advances in mixed Gaussian and plane wave algorithms have made possible the effective use of density functional theory (DFT) in ab initio molecular dynamics (AIMD) simulations for large and chemically complex models of condensed phase materials. In this chapter, we are reviewing recent progress on the modeling and characterization of co-sequestration processes and reactivity in wet supercritical CO₂ (sc-CO₂). We examine the molecular transformations of mineral and metal components of a sequestration system in contact with water-bearing scCO₂ media and aim to establish a reliable correspondence between experimental observations and theory models with predictive ability and transferability of results in large-scale geomechanical simulators.