Reaction molecular dynamics study of calcium alumino-silicate hydrate gel in the hydration deposition process at the calcium silicate hydrate interface: The influence of Al/Si

Abstract

Supplementary cementitious materials (SCMs) can partially replace cement in concrete production, forming calcium alumino-silicate hydrate (C-A-S-H). This enhances concrete durability while recycling waste. However, the early hydration reaction process of C-A-S-H and its deposition and aggregation behavior at the interface with the primary hydration product of cement, calcium silicate hydrate (C–S–H), remain unknown. Therefore, this study utilizes reactive molecular dynamics to model the deposition and growth behaviors of C-A-S-H precursors with different Al/Si ratios on C–S–H, and discusses the effects of the Al/Si ratio on C-A-S-H gel aggregation behavior and structural evolution at the C–S–H interface. The results show that increasing Al content significantly promotes the early hydration reaction rate of C-A-S-H gel, the degree of polymerization of silicate chains, and the amount of Qn(n ≥ 2) species. Moreover, higher Al content leads to the precursors aggregating among themselves rather than depositing on the C–S–H substrate surface. The incorporation of Al–O polyhedra can effectively bridge silicate chains on the C–S–H surface and alter the growth patterns of hydration products from linear chains to three-dimensional networks. This work provides molecular-level insights into the influences of the Al/Si ratio on the early hydration reaction process and interfacial deposition behaviors of C-A-S-H gel.