Abstract
The hydration process is a critical stage in the development of the properties of cement-based materials，however, the influence of cellulose nanocrystals (CNC) on cement during the early hydration is controversial. This study uses pure tricalcium silicate (C3S) as the object to analyze the influence of carboxyl CNC (CCNC) and sulfonic CNC (SCNC) on hydration parameters such as hydration rate, types, quality, and pore structure of hydration products during the early hydration period. The dissolution of C3S and the interaction between fluids and minerals at the C3S/CNC interface is the core mechanism of the early hydration. Ultraviolet and energy spectrum analyzed adsorption between CNC and C3S from a physical perspective, and molecular dynamics simulations deeply discussed the adsorption behavior between C3S/Water/CNC at nano-scale. The results show that CNC prolongs the hydration induction and acceleration period, delays the early hydration of C3S; CCNC exhibits a more significant effect than SCNC. Under the action of Ca-O and hydrogen bonds, CNC will adsorb on the surface of C3S and cover its surface, reducing the number of waters on the surface of C3S. Hydrophilic CNC molecules attract water molecules close to the CNC chain, and solidifying water molecules prevents it from entering the hydration surface. CNC also restricts the diffusion of Ca2+ on the surface of C3S to outside, improving the stability of Ca-O coordination, promoting the accumulation of hydration products at the C3S surface, and inhibiting the dissolution of C3S. Understanding the effect of functionalized CNCs on the diffusion and sedimentation mechanism of water molecules and Ca2+ during hydration can provide insights for guiding the design of nanomaterials with strong compatibility with cement systems and enlarging the application of functionalized nanomaterials in cement-based materials engineering fields.
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