The structural evolution of nanocrystalline calcium silicate hydrate (C-S-H) as a function of its calcium to silicon (Ca/Si) ratio has been probed using qualitative and quantitative X-ray atomic pair distribution function analysis of synchrotron X-ray scattering data. Whatever the Ca/Si ratio, the C-S-H structure is similar to that of tobermorite. When the Ca/Si ratio increases from ∼0.6 to ∼1.2, Si wollastonite-like chains progressively depolymerize through preferential omission of Si bridging tetrahedra. When the Ca/Si ratio approaches ∼1.5, nanosheets of portlandite are detected in samples aged for 1 d, while microcrystalline portlandite is detected in samples aged for 1 year. High-resolution transmission electron microscopy imaging shows that the tobermorite-like structure is maintained to Ca/Si > 3.
Keywords: C–S–H; calcium silicate hydrates; pair distribution function; transmission electron microscopy.