In Situ Self-assembly of Nanoparticles into Waxberry-like Starch Microspheres Enhanced the Mechanical Strength, Fatigue Resistance, and Adhesiveness of Hydrogel
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Owing to the diminishing resources and growing awareness of environmental issues, significant scientific attention has been paid to the development of physical gel materials using renewable and low-cost natural resources. Inspired by the strengthened mechanism of double-network and nanocomposite gels, we report a facile and green method to realize a mechanically stiff, fatigue-resistant, and adhesive-debranched waxy corn starch/PVA double-crosslinked nanocomposite gel (W-Gel) skeleton material with dynamic non-covalent bonds. The in situ formation of DBS nanoparticles leads to self-assembly into 3D waxberry-like microspheres, which act as physical crosslinkers by embedding themselves within network skeleton structures. The resulting hydrogel exhibited excellently mechanical behavior, including a good stretchability over 1200% strain, a maximum compressive strength of up to 780.7 ± 27.8 kPa, and the ability to sustain as much weight as 4.6 kg (about 2,000 times its own weight). Notably, the recovery efficiency exceeded 93% after the 60th compressive successive loading-unloading cycle at 50% strain. The hydrogel successfully adhered onto soft and hard substrates, such as skins, plastics, gauzes, glasses, and metals, manifesting in long-term, stable sustained release of epigallocatechin gallate (EGCG). The EGCG-loaded W-Gels exhibited predominant antibacterial activity against both Gram-positive bacteria (S. aureus) and Gram-negative bacteria (E. coli and S. typhus).