Atomistic insights into the effect of temperature on capillary transport of water molecules in epoxy-modified calcium silicate hydrate nanopore: diffusion, kinetics, and mechanism

Abstract The movement of water molecules at the atomic scale within the calcium silicate hydrate (C–S–H) gel pores serves a dual role: it creates an environment for harmful chemical reactions within the pores and functions as a carrier for the transport of detrimental ions, thereby affects the mechanical properties and durability of cementitious materials. However, direct experimental observation poses substantial challenges. This study offers new insights into how temperature (253 K, 273 K, 293 K, and 313 K) affects the capillary transport of water molecules in epoxy-modified C–S–H. The findings demonstrate that the pore size undergoes continuous changes during immersion due to epoxy clustering or detachment, resulting in three scenarios: narrowing of epoxy/C–S–H channels (253 K, 273 K), channel blockage (293 K), and complete detachment (313 K). Moreover, the interactions between water molecules and epoxy lead to epoxy detachment or cluster formation on the C–S–H surface. As the temperature increases, the interaction between C–S–H and cross-linked epoxy resin weakens. The coordination between C–S–H and epoxy resin decreases, while the coordination with water increases. This paper provides valuable insights into the transport behavior of liquids within the epoxy-modified C–S–H pores of cement-based materials. It contributes to a better understanding of how liquids move and interact within the modified pore structure, which is beneficial for enhancing the performance and properties of cement-based materials.