Applying Tools from Glass Science to Study Calcium-Silicate- Hydrates

To explain the similarities between a glass and amorphous C-S-H, a C-S-H molecular structure with stoichiometry of (CaO)1.7(SIO 2)1(H2O)1.9 is produced using a mixed reactive-nonreactive force field modeling. As the consequence of reactive modeling using REAXFF potential, part of water molecules in the interlayer spacing dissociate into hydroxyl groups and proton, which produces Ca-OH bonds. In addition, it is shown that monomers condensate to produce dimmers. This reduces the monomer content and increases the mean silicate chain length. Comprehensive topological analysis is performed to identify the local environment of each atom, which is indicative of short range order in C-S-H. Specially, the topological analysis is shown to be essential to distinguish between oxygen atoms in water, hydroxyl groups, silica chain and calcium oxide sheets. The medium range order in C-S-H is shown to exist using first sharp diffraction pattern derived from structure factor calculations. © 2013 American Society of Civil Engineers

Densification of the interlayer spacing governs the nanomechanical properties of calcium-silicate-hydrate

Calciuam-silicate-hydrate (C-S-H) is the principal binding phase in modern concrete. Molecular simulations imply that its nanoscale stiffness is 'defect-driven', i.e., dominated by crystallographic defects such as bridging site vacancies in its silicate chains. However, experimental validation of this result is difficult due to the hierarchically porous nature of C-S-H down to nanometers. Here, we integrate high pressure X-ray diffraction and atomistic simulations to correlate the anisotropic deformation of nanocrystalline C-S-H to its atomic-scale structure, which is changed by varying the Ca-to-Si molar ratio. Contrary to the 'defect-driven' hypothesis, we clearly observe stiffening of C-S-H with increasing Ca/Si in the range 0.8 ≤ Ca/Si ≤ 1.3, despite increasing numbers of vacancies in its silicate chains. The deformation of these chains along the b-axis occurs mainly through tilting of the Si-O-Si dihedral angle rather than shortening of the Si-O bond, and consequently there is no correlation between the incompressibilities of the a- and b-axes and the Ca/Si. On the contrary, the intrinsic stiffness of C-S-H solid is inversely correlated with the thickness of its interlayer space. This work provides direct experimental evidence to conduct more realistic modelling of C-S-H-based cementitious material

Is cement a glassy material?

The nature of Calcium-Silicate-Hydrate (C-S-H), the binding phase of cement, remains a controversial question. In particular, contrary to the former crystalline model, it was recently proposed that its nanoscale structure was actually amorphous. To elucidate this issue, we analyzed the structure of a realistic simulation of C-S-H, and compared the latter to crystalline tobermorite, a natural analogue to cement, and to an artificial ideal glass. Results clearly support that C-S-H is amorphous. However, its structure shows an intermediate degree of order, retaining some characteristics of the crystal while acquiring an overall glass-like disorder. Thanks to a detailed quantification of order and disorder, we show that its amorphous state mainly arises from its hydration. © 2014 Taylor & Francis Group

Is cement a glassy material?

The nature of Calcium-Silicate-Hydrate (C-S-H), the binding phase of cement, remains a controversial question. In particular, contrary to the former crystalline model, it was recently proposed that its nanoscale structure was actually amorphous. To elucidate this issue, we analyzed the structure of a realistic simulation of C-S-H, and compared the latter to crystalline tobermorite, a natural analogue to cement, and to an artificial ideal glass. Results clearly support that C-S-H is amorphous. However, its structure shows an intermediate degree of order, retaining some characteristics of the crystal while acquiring an overall glass-like disorder. Thanks to a detailed quantification of order and disorder, we show that its amorphous state mainly arises from its hydration. © 2014 Taylor & Francis Group

Applying tools from glass science to study calcium-Silicate- Hydrates

To explain the similarities between a glass and amorphous C-S-H, a C-S-H molecular structure with stoichiometry of (CaO) 1.7 (SIO 2 ) 1 (H 2 O) 1.9 is produced using a mixed reactive-nonreactive force field modeling. As the consequence of reactive modeling using REAXFF potential, part of water molecules in the interlayer spacing dissociate into hydroxyl groups and proton, which produces Ca-OH bonds. In addition, it is shown that monomers condensate to produce dimmers. This reduces the monomer content and increases the mean silicate chain length. Comprehensive topological analysis is performed to identify the local environment of each atom, which is indicative of short range order in C-S-H. Specially, the topological analysis is shown to be essential to distinguish between oxygen atoms in water, hydroxyl groups, silica chain and calcium oxide sheets. The medium range order in C-S-H is shown to exist using first sharp diffraction pattern derived from structure factor calculations. © 2013 American Society of Civil Engineers