Atomic-level insights into the influence of zinc incorporation on clinker hydration reactivity

The issues of chemical doping effects on cement clinker properties have long been investigated but are not fully understood. This work aims to provide an atomic-level understanding of the essential relations between clinker reactivity and its electronic structure and clarify the mechanism of doping effect on clinker reactivity. The Fukui functions reveal that zinc doping reduces the number of reactive sites and effective charges of silicate and aluminate phases dramatically, which accounts for the significant hydration retardation as observed in previous experiments. However, Zn doping scarcely changes the number of reactive sites but increases the effective charges and the total localization index of the ferrite phase due to the strong localization capacity of Fe 3d states, which implies a slight reactivity promotion. The comprehensive and in-depth methodology demonstrated in this paper is significant to facilitate the innovation of cementitious materials with desirable properties.