Atomistic origin of kinetics in hydrated aluminosilicate gels upon precipitation

C Zhao and JH Yu and XY Chen and QY Wu and W Zhou and M Bauchy, JOURNAL OF CHEMICAL PHYSICS, 159, 144501 (2023).

DOI: 10.1063/5.0165937

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.

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