Dynamic wetting of a CO2-H2O-montmorillonite system using molecular dynamics

Abstract

Injecting carbon dioxide into shale reservoirs achieves geological carbon sequestration (GCS), effectively reducing atmospheric carbon dioxide levels. Rock wetting characterizes the strength of the interaction between fluids and rocks, thereby determining fluid distribution, which is crucial for GCS trapping efficiency. In this study, the dynamic wetting of H2O-montmorillonite and CO2-H2O-montmorillonite systems was studied using molecular dynamics (MD) simulations. Montmorillonites with different lattice substitution arrangements based on pyrophyllite are strongly water-wet, and a precursor film forms at the leading edge of the bulk water. Na+ controls precursor film formation, which is rapidly spreading forward at a constant speed along the lattice substitution site lines based on Na+ distribution. The lower the proportion of Al3+/Si4+ lattice substitution in the Si-O tetrahedral layer on the fluid side, the higher the degree of water-wetness. The competitive adsorption of carbon dioxide and water molecules reduces the degree of spreading, resulting in a decrease in the degree of water-wetness. However, compared to the H2O-montmorillonite system, the spreading behavior remained unchanged. High carbon dioxide pressure caused the wetting to change from strongly water-wet to weakly water-wet, however no wetting reversal was exhibited. The wetting changes were particularly prominent near the supercritical carbon dioxide pressure, with a limit of 18 MPa. For the first time, this study distinguished the dynamic behaviors of bulk water and precursor films, revealed the formation mechanism of precursor films, and revealed the control mechanism of carbon dioxide pressure on dynamic wetting from a molecular perspective. The quantitative relationship between the contact angle and flow velocity at different carbon dioxide pressures presented in this study could effectively guide the establishment of a fluid force equation for infiltrating flow, providing theoretical support for GCS numerical simulation research.