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Calcium–alumino–silicate–hydrate (CaO–Al2O3–SiO2–H2O, or C–A–S–H) gel, which is the binding phase of cement-based materials, greatly influences concrete mechanical properties and durability. However, the atomic-scale kinetics of the aluminosilicate network condensation remains puzzling. Here, based on reactive molecular dynamics simulations of C–A–S–H systems formation with varying Al/Ca molar ratios, we study the kinetic mechanism of the hydrated aluminosilicate gels upon precipitation. We show that the condensation activation energy decreases with the Al/Ca molar ratio, which suggests that the concentration of the Al polytopes has a great effect on controlling the kinetics of the gelation reaction. Significantly, we demonstrate that 5-fold Al atoms are mainly forming at high Al/Ca molar ratios since there are insufficient hydrogen cations or extra calcium cations to compensate the negatively charged Al polytopes at high Al/Ca molar ratios during accelerated aging.more » « less
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