Fluid-Fluid Interfacial Effects in Multiphase Flow during Carbonated Waterflooding in Sandstone: Application of X-ray Microcomputed Tomography and Molecular Dynamics.

Fluid-fluid interfacial reactions in porous materials are pertinent to many engineering applications such as fuel cells, catalyst design, subsurface energy recovery (enhanced oil recovery), and CO storage. They have been identified to control physicochemical properties such as interfacial rheology, multiphase flow, and reaction kinetics. In recent years, engineered waterflooding has been identified as an effective way to increase hydrocarbon recovery and solid-fluid interaction has been assessed as the key mechanism. However, in this study, we demonstrated that in the absence of solid-fluid interactions (in strong hydrophilic porous media), fluid-fluid interfacial reactions can significantly affect multiphase flow and thus lead to an increased hydrocarbon recovery during engineered carbonated waterflooding. We designed a microwaterflooding system to evaluate the interfacial reactions during two phase flow with engineered carbonated waters. Given that salinity controls the amount of dissolved CO, we injected carbonated high salinity water and carbonated low salinity water to achieve different fluid-fluid reactions. We injected the carbonated water in a sandstone with 99.5% quartz under X-ray microcomputed tomography (μCT) scanning at a resolution of 3.43 μm per pixel. Image processing shows that carbonated low salinity waterflooding can recover 8% more oil than carbonated high salinity waterflooding, while the quartz-rich sandstone remains strongly hydrophilic in both samples. A gradual CT intensity distribution indicates an interfacial phase generation between carbonated brine and crude oil during carbonated waterflooding. Therefore, we attributed the additional hydrocarbon recoveries to the fluid-fluid interfacial reactions. To understand the effects of fluid-fluid reactions on interfacial properties, we performed molecular dynamics simulations to investigate the chemical species distribution at the interface, interfacial tension (IFT) changes, and CO diffusion. The MD simulation results revealed a layered structure of the interface, a lower CO diffusion coefficient in carbonated high salinity water, a lower IFT in carbonated low salinity water, a swelling hydrocarbon phase in carbonated low salinity water, and more CO accumulated at the interface between the hydrocarbon phase and carbonated low salinity water. This work provides a general and fundamental understanding of the influence of fluid-fluid interactions on the interfacial properties between carbonated water and the hydrocarbon interface.