Revised Atomistic Models of the Crystal Structure of C–S–H with high C/S Ratio

Abstract The atomic structure of calcium-silicate-hydrate (C 1.67 –S–H x ) has been studied. Atomistic C–S–H models suggested in our previous study have been revised in order to perform a direct comparison of energetic stability of the different structures. An extensive set of periodic structures of C–S–H with variation of water content was created, and then optimized using molecular dynamics with reactive force field ReaxFF and quantum chemical semiempirical method PM6. All models show organization of water molecules inside the structure of C–S–H. The new geometries of C–S–H, reported in this paper, show lower relative energy with respect to the geometries from the original definition of C–S–H models. Model that corresponds to calcium enriched tobermorite structure has the lowest relative energy and the density closest to the experimental values.