The incorporation of nano-reinforcements is believed to be a promising method to create high performance nanocomposites, which are largely dependent on the interfacial connections. In this work, the newly emerging two-dimensional (2D) material, 2Dsilica is intentionally intercalated into the interlayer defective sites of calcium silicate hydrate (C-S-H), which is the primary hydration product of ordinary portland cements. The reactive molecular simulation results indicate the nano-reinforcement can strongly interact with the inorganic matrix to form a high-ductility nanocomposite. The uniaxial tensile loading tests show the plastic stage of the C-S-H is considerably enhanced due to the intercalation of 2D-silica, which removes the intrinsic brittleness of cementbased materials at the nano-scale. It is observed that the dangling atoms at the edge of 2D-silica can react with non-bridging oxygen atoms of C-S-H, forming Si-O-Si bonds at interfaces. Those covalent bonds transform Q 1 and Q 2 in the C-S-H into high connectivity Q 3 and Q 4 species, which increases the integrity of the matrix and its resistance to crack propagation. During the tensile process, the elongation and breakage of those high-strength covalent bonds needs higher tensile stress and consumes higher energy, which leads to a strong plasticity and higher toughness. This work may shed new lights on the interaction mechanisms between 2D-materials and inorganic hosts, and provide solutions to modifying the brittleness of concrete.
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