Temperature-dependent rehydration of magnesium silicate hydrate (M-S-H): Development of no-cement binder through MD/DFT validation

The MgO–SiO 2 –H 2 O binding system was vital for the strength properties of magnesia castables. However, the low yield of magnesium silicate hydrate (M-S-H) during the curing process limited the further improvement in the service performance of magnesia castables. The introduce of synthesized M-S-H into magnesia castables was a potential approach to address the above issue, and it was explored in this work. The effect of dehydration temperature (from 200 to 800 °C) on the rehydration behavior of M-S-H and the strength of magnesia castables was investigated. The results indicated that the magnesia castables with pre-dehydrated M-S-H below 600 °C processed an enhanced binding property. The highest strength occurred in the sample with pre-dehydrated M-S-H at 200 °C, and the strength dramatically decreased in the presence of M-S-H calcinated at 800 °C. According to Molecular Dynamics (MD) simulations, structural distortion was generated from the dehydration process of M-S-H and was worsened by temperature increase. The minimum distortion occurred in the dehydration of M-S-H at 200 °C, which was confirmed as merely 8% physical water removal based on the Density Functional Theory (DFT) calculations. Ultimately, the appropriate structural distortion could increase the hydration reactivity and improve the strength of magnesia castables.