Development of a universal atomistic cement model incorporating nanomaterials: From laboratory investigation to molecular simulation

Hydrated cement is considered one of the most complex binder systems. The development of models that suitably represent hydrated cement is still far from established due to the complexity of the hydration process, as well as the multiscale phase and different morphological properties. Therefore, this study attempts to develop a hydrated cement model using molecular-level simulation and laboratory testing. This model aimed to predict the mechanical properties of cement paste between 0.25 and 0.65 w/c ratios. In this regard, five cement paste mixtures with various w/c ratios were prepared and tested to evaluate their mechanical properties and micro-structures. Then, a novel modeling methodology using molecular dynamics (MD) simulation was carried out to develop an ingredient-based atomistic cement model. In this regard, the Dreiding force field (DFF) was used in all the simulation processes, starting from the cement clinker phases to the hydrated cement. The experimental results of cement paste mixtures revealed some useful data that was supportive of the simulations. Radial distribution function (RDF) and fractional free volume (FFV) were utilized to investigate the local atomic structure of the cement paste models. The calcium-silicate-hydrated (C-S-H) of the developed model was characterized through RDF and benchmarked to a well-known mineral analog, namely tobermorite. The developed model was computationally tested under different w/c ratios, and reliable results in terms of microstructural matrix as well as mechanical properties were obtained. Then, the cement models incorporating different ratios of nano-silica were developed, and a good estimation of the mechanical properties was obtained. Because of the universal nature of the reported model in this research, it could be utilized to further predict the mechanical behavior and durability performance of the cement paste.