Zeta Potential in Intact Natural Carbonates at Elevated Temperatures

Abstract:

Measurements of zeta potential have been used to monitor subsurface flows in many natural brine systems. Numerous studies report zeta potentials in carbonates using crushed samples at low ionic strength and laboratory temperatures. However, natural brines have much higher salinity; moreover, temperatures are considerably higher in many subsurface settings. The variation of zeta potentials with temperature has not been examined in natural carbonates. We report zeta potential values interpreted from streaming potential measurements in two intact carbonate rock samples, saturated with artificial brines at elevated temperatures. We measure streaming potential using an experimental set-up that incorporates in-situ measurements of saturated rock conductivity, brine temperature, brine pH, brine electrical conductivity, pressure difference and voltage at temperatures up to 120^oC. The streaming potential measurements are complemented with brine effluent studies.

We find that the interpreted zeta potential is negative and decreases in magnitude with increasing temperature at low ionic strength (0.01M) and independent of temperature at high ionic strength (0.5M); consistent with published zeta potential in intact natural sandstones. The concentration of Ca²⁺ (main potential determining ion) also decreases with temperature at low ionic strength, but remains constant at high ionic strength. The temperature dependence of the zeta potential is consistent between two different natural carbonate samples and can be explained by the temperature dependence of pCa²⁺. We suggest that zeta potential of carbonate is independent of temperature or pH when pCa²⁺ remains constant. A linear variation of pH vs. pCa²⁺ is exhibited, at ambient and elevated temperatures, when pCa²⁺ is allowed to change with pH. This linear variation explains the numerous published data that shows apparent relationship between zeta potential of carbonates and pH.