To maximize the high-value application of fly ash, this study investigates the incorporation of amorphous silica derived from fly ash as a silicon source and lime milk as a calcium source into microporous calcium silicate powders through dynamic hydrothermal synthesis at 100 °C for a duration of 2 h or less. The products were collected at various synthesis intervals and analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FT-IR), and thermogravimetric differential scanning calorimetry (TG-DSC). Results indicate that microporous calcium silicate forms through a dynamic reaction that disrupts Si-O bonds, enhancing the mobility of silica-oxygen tetrahedra and generating H2SiO42−groups. Ca2+ ions also interact with these bonds, resulting in Q1 and Q2 forms of silica-oxygen tetrahedra. Phase transformation of calcium silicate at various intervals was noted, beginning with 3CaO·2SiO2·3H2O, shifting to 2CaO·3SiO2·2.5H2O, and finally to CaO·2SiO2·2H2O at 90 min. Thus, microporous calcium silicate evolves from an amorphous C-S-H gel into a crystalline form, featuring diverse calcium silicate minerals with calcium-silicon ratios and particle sizes between 10 and 20 μm, with sizes increasing until the 80-min.
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