This study is focused on elucidating the role and mechanism of hydroxyl-functionalized multi-walled carbon nanotubes (MWCNTs-OH) as a reinforcement material in cement-based composites. The dispersion of MWCNTs-OH within the cement composites was first assessed using Raman spectroscopy. Subsequently, SEM, FT-IR, TGA, XRD, and nano-indentation techniques were employed to investigate the structural transformation and phase changes occurring in the cement matrix upon incorporating MWCNTs-OH. The results reveal that MWCNTs-OH can significantly improve the macro-mechanical properties of cement composites by their capacity for pulling out, pore-filling, inducing multi-cracking, and promoting hydration. From a micro-perspective, observations of the micro-morphology demonstrate that MWCNTs-OH reinforces cement composites through crack-bridging and pull-out effects. Regarding the hydrated calcium silicate (C-S-H), the addition of MWCNTs-OH has a negligible impact on the ratio of low-density C-S-H (LD-CSH) to high-density C-S-H (HD-CSH). Moreover, the results obtained from FT-IR and XRD tests provide evidence that the bonding between MWCNTs-OH and the cement matrix is predominantly governed by physical interactions.
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