Synergistic Dynamic Hydrogen-Bond Interlocking Networks for Ultrafast Self-Healing and Water-Resistant Organosilicon–Epoxy Elastomers

Achieving a rational design of polymer networks that simultaneously integrates structural robustness, rapid self-healing, and environmental tolerance is critical for the long-term protection of marine engineering and infrastructure. This study presents a molecular engineering strategy based on a nanosilica (SNSi)-induced bulk three-dimensional dynamic hydrogen-bonded network to construct a high-performance organosilicon–epoxy adaptive elastomer (PDEP-SNSi15). By synergistically coupling intrinsic resin hydrogen bonds with multiple hydrogen bonds provided by the SNSi surface, a hybrid supramolecular network, characterized by a concentrated energy level distribution and markedly enhanced bond-exchange cooperativity, was formed. This unique network architecture enables rapid chain rearrangement by overcoming low energy barriers at room temperature, resulting in ultrafast self-healing with complete recovery within 20 s. Furthermore, the elastomer forms a strong interfacial adhesion and a dense water-resistant structure on rough inorganic substrates. This work establishes design principles for nanosilica-induced dynamic networks in high-performance self-healing materials and offers a theoretical foundation for developing next-generation protective coatings that integrate self-healing, environmental resistance, and high reliability.