Investigation of the surface charge behaviour of ettringite: Influence of pH, calcium, and sulphate ions

Ettringite is an important mineral that contributes to the overall performance of cementitious materials. Knowledge of the surface charge behaviour of a solid is necessary for a mechanistic description of surface processes such as adsorption or particle-particle interactions. The objective of this study was to develop a model capable of reproducing ettringite surface charge as a function of calcium, sulphate, and pH. Ettringite was synthesised and characterised using different analytical, microscopic, and spectroscopic techniques with the help of density functional theory. Electrophoretic mobility was measured using laser Doppler electrophoresis in alkaline waters representative of the cementitious environment. The behaviour of the ettringite surface charge was shown to be quite complex as sulphate and calcium acted in a competitive manner on the overall charge. The ζ-potential increases when the calcium content increases, whereas it decreases when sulphate increases. This is due to the possible adsorption of these ions at the surface, and the extent of the effect depends on the relative concentrations of Ca and SO₄ ^2-. An electrostatic double layer model (DLM) was used to calculate the surface potential, considering the adsorption of both calcium and sulphate, as possible ions determining the potential (IDP), and formation of different complexes with ettringite surface functional groups (SOH). The variations of the ζ-potential could be satisfactorily predicted under the different chemical conditions of interest in a cementitious environment.