Microanalysis and optimization-based estimation of C–S–H contents of cementitious systems containing fly ash and silica fume

In this study, a new approach to characterize hardened pastes of pure portland cement as well as those containing cement with supplementary cementitious materials (SCM) was adopted using scanning electron microscopy (SEM) and energy dispersive X-ray spectra (EDS) microanalyses. The volume stoichiometry of the hydration reactions was used to estimate the quantities of the primary and secondary calcium silicate hydrate (C–S–H) and the calcium hydroxide produced by these reactions. The 3D plots of Si/Ca, Al/Ca and S/Ca atom ratios given by the microanalyses were compared with the estimated quantities of C–S–H to successfully determine the Ca/Si ratio of eleven different cementitious systems at four different ages using a constrained nonlinear least squares optimization formulation by General Algebraic Modeling System (GAMS). The estimated mass fraction of calcium hydroxide from the above method agreed well with the calcium hydroxide content determined from the thermogravimetric analyses (TGA).