Effect of Different Initial CaO/SiO2 Molar Ratios and Curing Times on the Preparation and Formation Mechanism of Calcium Silicate Hydrate

Abstract

To better understand the pozzolanic activity in fly ash used as a supplementary cementitious material in cement or concrete, calcium silicate hydrate (C-S-H) has been synthesized by adding silica fume to a supersaturated calcium hydroxide solution prepared by mixing calcium oxide and ultrapure water. Thermogravimetric analysis results have revealed the variation in the weight loss due to C-S-H in the samples and the conversion ratio of calcium oxide (the μCaO value), which represents the proportion of calcium oxide in the initial reaction mixture used to produce C-S-H, with curing time. The weight loss due to C-S-H and the μCaO value were both maximized (13.5% and 90.4%, respectively) when the initial C/S molar ratio was 1.0 and the curing time was 90 d. X-ray diffraction (XRD) analysis has indicated that C-S-H in the samples after curing for 7 d had the composition Ca1.5SiO3.5·xH2O. 29Si magic angle spinning (MAS) nuclear magnetic resonance (NMR) analysis has revealed that the degree of polymerization of C-S-H increased with an increase in curing time for samples with an initial C/S molar ratio of 1.0. The ratio of internal to terminal tetrahedra (Q2/Q1) increased from 2.29 to 4.28 with the increase in curing time from 7 d to 90 d. At curing times ≥ 28 d, a leaf-like C-S-H structure was observed by scanning electron microscopy (SEM). An ectopic nucleation–polymerization reaction process is proposed for the formation mechanism of C-S-H.