Zeta potential of CO2-rich aqueous solutions in contact with intact sandstone sample at temperatures of 23 °C and 40 °C and pressures up to 10.0 MPa

Abstract

Despite the broad range of interest and applications, controls on the electric surface charge and the zeta potential of silica in contact with aqueous solutions saturated with dissolved CO₂ at conditions relevant to natural systems, remains unreported. There have been no published zeta potential measurements conducted in such systems at equilibrium, hence the effect of composition, pH, temperature and pressure remains unknown. We describe a novel methodology developed for the streaming potential measurements under these conditions, and report zeta potential values for the first time obtained with Fontainebleau sandstone core sample saturated with carbonated NaCl, Na₂SO₄, CaCl₂ and MgCl₂ solutions under equilibrium conditions at pressures up to 10 MPa and temperatures up to 40 °C. The results demonstrate that pH of solutions is the only control on the zeta potential, while temperature, CO₂ pressure and salt type affect pH values. We report three empirical relationships that describe the pH dependence of the zeta potential for: i) dead (partial CO₂ pressure of 10^-3.44 atm) NaCl/Na₂SO₄, ii) dead CaCl₂/MgCl₂ solutions, and iii) for all live (fully saturated with dissolved CO₂) solutions. The proposed new relationships provide essential insights into interfacial electrochemical properties of silica-water systems at conditions relevant to CO₂ geological storage.

Keywords: Carbonated aqueous solution; Elevated temperature; High pressure; Sandstone; Streaming potential method; Supercritical CO(2) conditions; Zeta potential.