The low-salinity waterflooding (LSWF) technique during enhanced oil recovery has received increasing attention over the last decade. Several studies have attempted to understand the effects of LSWF through both experiments and modelling, but their results are inconsistent due to a lack of understanding of the crude oil/brine and brine/rock interfaces. In this paper, the crude oil/brine interface was studied by developing a triple-layer surface complexation model. The carboxyl groups (–COOH) were attributed to the surface charge and electrical triple-layer development of the crude oil in LSWF. The zeta potentials of the emulsion at various pH levels and the calcium and magnesium concentrations were measured to examine the interface. These data were then directly fitted to the simulated zeta potentials to determine the surface site density of –COOH and the associated equilibrium constants for the dissociation and adsorption of calcium and magnesium. The –COOH site density was determined by fitting the pH-independent zeta potential, while the equilibrium constant values were estimated from the variations in the zeta potential with the changes in pH and the concentrations of calcium and magnesium. The determined surface complexation parameters were validated by comparing the experimental zeta potential data from different ionic solutions. The developed surface complexation model was used along with the estimated parameters to predict the interface of crude oil in seawater, formation water, and their dilutions. The simulated zeta potential results agreed well with the experimental data, demonstrating that the model is applicable to understand the crude oil/brine interface in LSWF. Finally, the importance of the prediction of the surface and zeta potentials in the evaluation of the interface and the estimation of electrostatic forces, and thus the wettability alteration, was discussed.
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