Cellulose-based dynamically entangled supramolecular assembly (DESA) gels for impact resistance and vibration damping

Impact resistance and vibration damping are crucial for protective materials in personal protection, industrial security, and flexible electronics. We present DESA-Gels, Dynamically Entangled Supramolecular Assembly Gels, as a fundamentally different class of soft material. These gels are formed through evaporation-driven self-assembly of poly(vinyl alcohol) (PVA) and deep eutectic solvent (DES: choline chloride, and citric acid)-treated cellulose micro/nanofibers (CMNF). The fabrication uses a green deep-eutectic solvent to extract and disperse cellulose fibers, avoiding harsh chemicals. Through hierarchical hydrogen-bonding interactions, DESA-Gels develop a unique polymer-fluid duality: a percolating PVA polymer network serves as an elastic skeleton, while the DES-CMNF phase remains mobile and viscous, effectively acting as a dissipative fluid within the network. All achieved without any chemical crosslinkers or phase separation in the material. As a result of this supramolecular design, DESA-Gels show good mechanical properties (such as high tear resistance, puncture tolerance, and fatigue durability), room-temperature self-healing, extraordinary adhesion combined with ultra-broad operational conditions. They remain stable and functional from about -70 ℃ up to 80 ℃ and demonstrate broadband viscoelastic damping across a wide frequency spectrum. Our findings provide a novel perspective on the synthesis of tailored gels and offer valuable insights into the development of next-generation intelligent protective materials.