Two-dimensional (2D) materials have been incorporated into calcium silicate hydrate (C-S-H) gel to enhance its mechanical performance for decades, while the modified C-S-H gel exhibits poor toughness, tensile strength, and ductility. In this work, we report a new design strategy and synthesis route to strengthen C-S-H interface by intercalating a silicene sheet of one atom thickness. The hybrid C-S-H/Silicene gel shows superb mechanical properties, with a remarkable enhancement in strength and other functional properties. By using density functional theory (DFT) and molecular dynamics (MD) simulations, we have demonstrated that Si-O bonds between silicene and C-S-H are stable and covalent, and the interaction energy of this bilayer gel nearly doubles by forming a 3D covalent network with a strong bridging effect. Owing to its better crystallinity enrichment and its induced dislocation dissipation mechanism, the hybrid C-S-H/Silicene gel possesses a higher tensile ductility (∼118% average enhancement and ∼228% in the c direction) and a much smaller elastic stiffness (59.04 GPa for average Young's modulus). This work offers an ingenuous route in turning brittle C-S-H gel into a soft gel, which provides opportunities for fabricating ultrahigh performance cementitious materials.
Keywords: DFT calculations; calcium silicate hydrate; interlayer; microstructure; molecular dynamics; nanomaterials; tensile stress.