Electrostatic properties of C–S–H and C-A-S-H for predicting calcium and chloride adsorption

The adsorption capacity of cement hydrates considerably affects the ionic ingress into cementitious materials. In this study, the surface electrostatic properties of calcium silicate hydrate (C–S–H) and calcium aluminosilicate hydrate (C-A-S-H) were determined to understand the effects of the properties on calcium and chloride adsorption. The density of the surface functional groups was determined by analysing the structure of C–S–H and C-A-S-H through 27Al and 29Si MAS NMR. The surface sites of ≡SiOH and ≡AlOH are available in C-A-S-H whereas C–S–H has ≡SiOH groups for ionic adsorption. We found that the incorporation of aluminium decreases the number of total adsorption sites in C-A-S-H. Furthermore, the site density increased with Ca/(Si + Al). To understand the C-A-S-H/solution interface, a triple-layer surface complexation model was developed and the associated equilibrium constants for deprotonation, calcium, and chloride adsorption were determined by fitting the experimental data of potentiometric titration and zeta potential measurement results. The estimated surface complexation modelling parameters were verified by predicting the experimental data of calcium and chloride adsorption on C–S–H and C-A-S-H.