Ettringite surface chemistry: Interplay of electrostatic and ion specificity

This paper presents a detailed experimental study combined with Monte Carlo (MC) simulations within the primitive model of the physical chemistry at the ettringite–water interface over a wide range of pH and bulk conditions for which ettringite exists thanks to its solubility in aqueous solutions. Ettringite, which is an important phase in hydrated cement-based systems, bears a permanent and positive structural charge. In contrast with previous studies, electrokinetic measurements together with the careful chemical analysis of the equilibrium solutions of the dispersions have brought strong support to designate sulfate as being the ion determining the potential. Simulations showed that electrostatics, through ion–ion correlations, are not strong enough to explain the charge reversal of ettringite immersed in sulfate salt solutions. However, an excellent agreement between simulated and experimental data was obtained including a short-range nonelectrostatic adsorption potential for the sulfate ion. This result strongly suggests the existence of a chemical specificity of sulfate ions for an ettringite surface.

Graphical abstractA good fit is obtained adding a specific potential to the ettringite–sulfate interaction, which highlights the existence of a specific interaction.Figure optionsDownload full-size imageDownload high-quality image (51 K)Download as PowerPoint slideResearch highlights► Consistent picture of the ettringite–water interface over pH and bulk conditions. ► Charge reversal of ettringite immersed in sulfate salt solutions. ► Electrostatics, through ion–ion correlations, must be considered. ► Sulfate short-range adsorption potential must be considered too.