Solution to the Problems of Cementitious Materials Exposed to Silane-Based Hydrophobic Coatings

Silane-based hydrophobic coatings are widely used to improve the durability of cement-based materials in aggressive environments such as marine and hydraulic structures. However, their long-term effectiveness is strongly influenced by interfacial adhesion degradation under humid conditions, which remains a critical challenge in engineering applications. From a scientific perspective, the fundamental mechanisms governing how silane-based coatings interact with cement hydration products, particularly under varying moisture conditions, are still not fully understood. In particular, the role of interfacial water in regulating bonding strength and intermolecular force transfer at the nanoscale has not been quantitatively clarified. To address these issues, this study investigates the interfacial debonding behavior of polydimethylsiloxane (PDMS), a representative silane-based hydrophobic component, on calcium silicate hydrate (C–S–H) substrates using molecular dynamics simulations under controlled hydration states. The results show that the interfacial interaction is dominated by van der Waals forces, with a calculated binding energy of approximately 357 kcal/m2. As the interfacial water content increases from dry to high-humidity conditions, the maximum debonding force (F_max) decreases from approximately 1.6 × 103 pN to 1.3 × 103 pN, corresponding to a reduction of about 18–20%. Similarly, the debonding work (W_max) shows a consistent decreasing trend, indicating reduced energy required for interface separation. This reduction is attributed to the formation of a continuous water film, which increases the interfacial separation distance and reduces the efficiency of intermolecular force transfer. These findings demonstrate the humidity-dependent weakening of interfacial adhesion and provide new insights into the nanoscale mechanisms governing the performance of silane-based coatings. The results offer a theoretical basis for optimizing the durability and reliability of hydrophobic treatments in cement-based materials under realistic service conditions.