Alkaline silicate solutions were prepared with varying. SiO2-Na2O ratios, R
m = [SiO2]/[Na2O] = 2 or 3, with a constant silica concentration equal to 1
.5 M. The structure and the number fraction of different silicate molecular
species present in the solutions were classically determined for molar rat
io Rm = 2 using Si-29 nuclear magnetic resonance (Si-29 NMR). In the case o
f the sample with Rm = 3, for which no NMR data was available, we used smal
l-angle X-ray scattering (SAXS) experiments to get this information. The SA
XS model was previously tested with Rm = 2 silicate solution. When Ca++ is
added to alkaline silicate solutions, a gel is obtained under well-defined
conditions. The gel formation was studied by SAXS, small-angle neutron scat
tering (SANS) and elastic light scattering (ELS). For gelling solutions, du
ring aggregation of the initial particles in the sol and for the resulting
gels, the scattering data were fitted using a fractal model for the structu
re including a correlation cut-off distance and a contribution of remaining
individual sol particles. Experimental and calculated scattering curves ar
e in agreement for all studied samples. The results obtained may help to un
derstand the mechanism of formation of silico-calco-alkaline gels in concre
te chemistry. (C) 1999 Elsevier Science B.V. All rights reserved.