Abstract

Graphene oxide (GO) has been widely reported to enhance the mechanical performance of cementitious composites. However, the fundamental hydration mechanisms underlying these improvements, such as GO’s role as a nucleation site, remain poorly explored and quantified. This study presents a comprehensive, non-destructive investigation into the time-dependent hydration behaviour of GO-induced cement pastes using time-domain 1H Nuclear Magnetic Resonance (NMR) spectroscopy, supported by thermogravimetric analysis (TGA), humidity-controlled water-retention tests, and compressive strength tests. Cementitious composites containing 0.035%, 0.065%, and 0.08% GO by weight of cement (bwoc) were monitored from 4 h to 28 days to track the evolution of discrete water phases, including capillary, inter-hydrate, gel pore, and interlayer water. NMR results reveal that GO initially facilitates water redistribution by retaining free water within its layered structure, followed by a delayed but sustained release that promotes continued hydration and a progressive shift toward less mobile pore–water environments at later curing ages. TGA confirms enhanced formation of hydration products in GO-induced cementitious systems, with an optimal dosage of 0.035% bwoc achieving the most sustained hydration and highest compressive strength. Higher GO dosages accelerate early hydration but limit later-stage hydration due to diffusion barriers formed by hydration products. This study provides time-dependent scientific evidence of GO’s dual role as a hydration nucleation agent and water-release regulator, establishing a mechanistic basis for dosage optimization in nano-engineered cementitious composites.

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